A radiation-resistant supermacroporous aerogel for ultrafast and high-capacity gaseous iodine capture

A radiation-resistant supermacroporous aerogel for ultrafast and high-capacity gaseous iodine capture | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Research Article A radiation-resistant supermacroporous aerogel for ultrafast and high-capacity gaseous iodine capture Meng Ji, Dagang Li, Zilei Zhang, Haocun Tan, Xiyue Zhang, Yingjun Dong, and 3 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8836259/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted 9 You are reading this latest preprint version Abstract Efficient capture of radioactive gaseous iodine is crucial for the safe management of nuclear waste. However, most existing adsorbents suffer from low capacity, slow kinetics, high cost, or poor radiation stability. Herein, a simple aqueous cryo-polymerization strategy was developed to construct a polyethyleneimine-functionalized poly (acrylic acid) aerogel (PEI@PAA), enabling simultaneous ice-templated macropore formation, in-situ polymerization, and crosslinking. The resulting aerogel features a highly interconnected three-dimensional (3D) macroporous network (10~100 μm), which facilitates the rapid diffusion of iodine vapor. Meanwhile, abundant amino groups (RNH2, R2NH, R3N) act as chemical adsorption sites through charge-transfer interactions. The PEI@PAA aerogel exhibits an exceptionally high iodine uptake of 6.01 g·g-1 and achieves 90% of its saturation capacity within 4 h, which demonstrates a 10-fold kinetic enhancement over that of Ag-loaded zeolites. Benefiting from the robust gel network and continuous pore structure, the aerogel maintains a high capacity of 5.14~5.28 g·g-1 after exposure to 50 kGy of β/γ irradiation, with negligible structural degradation. This green and energy-efficient method eliminates the need for freeze-drying, offering a scalable and sustainable platform for the next generation of iodine adsorbents in nuclear waste treatment. Radioactive iodine capture Radiation-resistant adsorbents aerogel cryo-polymerization nuclear waste management Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Highlights λ A 3D supermacroporous PEI@PAA aerogel via facile cryo-polymerization. λ Record-high iodine capture capacity of 6.01 g·g achieved. λ Rapid adsorption: 90% equilibrium reached within 4 h. λ Excellent resistance to β/γ-irradiation demonstrated. λ Cost significantly lower than conventional silver-loaded adsorbents. 1. Introduction As a crucial component of the global low-carbon energy system, nuclear energy is essential in advancing the energy transition and achieving carbon neutrality [ 1 ]. However, the release of radioactive iodine isotopes (such as 129 I with a half-life of 1.57×10 7 years and 131 I with a half-life of 8.02 days) during spent fuel reprocessing is characterized by high volatility and significant bioaccumulation [ 2 ]. 129 I migrates through the atmosphere into water bodies and soil [ 3 ]. It tends to persist in the environment for prolonged periods and accumulates in the human thyroid gland, posing health risks [ 4 ]. Consequently, the development of efficient, stable, and economically viable technologies for radioactive iodine capture represents a core scientific and engineering challenge essential for the sustainable advancement of nuclear energy [ 5 ]. Among various treatment technologies, the adsorption method has garnered significant attention due to its simplicity and cost-effectiveness [ 6 ]. However, traditional adsorbents, such as silver-loaded zeolite (Ag-MOR), exhibit high selectivity but possess a limited adsorption capacity of only 0.22 g·g − 1 , relying on the precious metal silver, which contributes to elevated costs [ 7 ]. In contrast, metal sulfide composites like CuS/AC can enhance the adsorption capacity to 0.49 g·g − 1 , but they pose a flammability risk [ 8 ]. Recently emerged porous materials (MOFs [ 9 – 11 ], COFs [ 12 – 14 ], POPs [ 15 , 16 ]) demonstrate potential for iodine capture. However, they encounter challenges, including complex preparation, high costs, slow kinetics, and inadequate radiation stability. ZIF-8 is susceptible to structural collapse in humid environments [ 17 ], while UiO-66-NH 2 incurs high preparation cost [ 18 ]. Although TpPa-1 [ 19 ] and COF-TAPA [ 20 ] exhibit high specific surface areas, they necessitate high-temperature vacuum synthesis, and their adsorption equilibrium times extend to dozens of hours. Furthermore, most studies also overlook the influence of β/γ-irradiation on adsorption performance, which is particularly critical in the context of nuclear waste treatment [ 15 ]. To simultaneously enhance the adsorption rate and capacity for gaseous iodine, researchers have sought to introduce 3D porous aerogels, leveraging their supermacro interconnected pores to facilitate molecular transport. Zhu et al . prepared Catechin@3DCF aerogels via freeze-drying, achieving an iodine adsorption capacity of 2.23 g·g − 1 , although equilibrium required up to 20 h [ 21 ]. The UiO-66-NH 2 @WCA aerogels developed by Tian’ team shortened the adsorption equilibrium time to 15 h; however, their fabrication still relied on energy-intensive freeze-drying with prolonged processing cycles [ 22 ]. Consequently, developing energy-efficient strategies for the controllable construction of 3D interconnected macroporous structures remains a critical and unresolved challenge. The cryo-polymerization technique induces solvent crystallization under low-temperature conditions to template macropore formation, while in situ polymerization and simultaneous crosslinking construct a fully interconnected macroporous network, thereby overcoming the limitations of conventional freeze-drying and enabling drying and shaping under ambient temperature and pressure [ 23 ]. A series of 3D continuous porous adsorbents for uranium extraction from seawater have been developed via organic/aqueous phase cryo-polymerization [ 24 – 29 ]. Research on uranium has demonstrated that cryo-polymerization can rapidly construct continuous supermacro pores, significantly enhancing mass transfer flux and adsorption capacity. Building on this concept, we propose a green aqueous phase cryo-polymerization strategy. Using acrylic acid (AA) as the monomer to create a polyacrylic acid (PAA) framework, and employing an EDC/NHS-mediated amidation reaction for covalent grafting of polyethyleneimine (PEI), we prepared a 3D aerogel (PEI@PAA) with interconnected pores of 10–100 µm (Fig. 1a and 1b). The PEI@PAA aerogel exhibits both ultrahigh adsorption capacity (6.01 g·g − 1 ) and rapid kinetics, achieving 90% equilibrium within 4 h. The highly cross-linked 3D network within the gel phase of PEI@PAA confers excellent radiation resistance stability, maintaining an adsorption capacity of 5.14 ~ 5.28 g·g − 1 after 50 kGy β/γ irradiation. Furthermore, this method circumvents the energy-intensive freeze-drying process, facilitating low-cost and scalable preparation, and offering a practical new approach for efficient radioactive iodine capture and nuclear waste treatment. 2. Results and Discussion 2.1 Formation mechanism of the 3D continuous pore microstructure of PEI@PAA aerogel In Fig. 1a, the aqueous solvent of the AA solution gradually cools to form ice crystals at -20°C. These ice crystals serve as templates for the formation of supermacro pores, confining the reaction components to the amorphous regions between the ice crystals [ 30 ]. Within these amorphous regions, free radicals generated by the redox initiator trigger the polymerization reaction: on one hand, AA monomers polymerize into long PAA molecular chains. On the other hand, N,N'-methylenebisacrylamide (MBA) forms high-density chemical cross-links with AA through covalent bonding (Fig. S1 ). This combination constitutes the framework of the PAA gel phase with a 3D network structure [ 31 ]. The Fourier Transform Infrared Spectroscopy (FT-IR) spectrum indicates that the broad absorption peak at 3390 cm − 1 and the strong absorption peak at 1720 cm − 1 are attributed to the O-H stretching vibration and C = O asymmetric stretching vibration in the COOH group [ 32 ], respectively. The characteristic peak at 2950 cm − 1 corresponds to the C-H stretching vibration [ 33 ] (Fig. 1c). These characteristic peaks confirm the occurrence of the polymerization reaction. Notably, the framework of the PAA gel phase is formed through high-density cross-linking. Following drying under ambient temperature and pressure, the ice crystals melt, leaving behind interconnected supermacro pores in situ, thereby yielding a PAA framework with a continuous 3D supermacro pore structure. Figure 1 Preparation and characterization of the PAA matrix and PEI@PAA. a. Schematic diagram of PAA matrix synthesis, including solvent cryo-polymerization, chemical cross-linking, and pore templating, which together form continuous 3D pores. b. EDC/NHS-mediated coupling reaction: the amino groups in PEI react with the carboxyl groups in PAA to form amide bonds, leading to the synthesis of PEI@PAA; after drying under ambient pressure, PEI@PAA aerogel are obtained. c. FT-IR spectra of the PAA matrix and PEI@PAA. d. Full XPS spectra of PAA and PEI@PAA. e. High-resolution XPS spectra of C 1s for PAA and PEI@PAA. f. High-resolution XPS spectra of O 1s for PAA and PEI@PAA. g. High-resolution XPS spectrum of N 1s for PEI@PAA. As evidenced by the Scanning Electron Microscope (SEM) characterization in Fig. S3, both the xy cross-sections (Fig. S3 a ~ c) and xz cross-sections (Fig. S3 d ~ f) of the PAA aerogel demonstrate a continuous macroporous channel structure, with a pore size of approximately 10–100 µm and a wall thickness of about 2 ~ 20 µm. In particular, the surface of the PAA matrix (Fig. S3 g ~ i) exhibits a regular and continuous pore structure with comparable pore sizes. This phenomenon is attributed to the continuous distribution of ice crystals during the cryo-polymerization process, which generates a 3D interconnected pore structure of PAA from the surface to the interior and exhibits a uniform pore distribution state, facilitating the diffusion and adsorption mass transfer of gaseous iodine. The pore size distribution curve of the PAA framework surface indicates a significant presence of mesopores with sizes of 2 ~ 50 nm on the pore wall surface (Fig. S7). These fine pore structures enhance the adsorption capacity. Figure 1b illustrates the grafting process of PEI onto the PAA framework via the EDC/NHS-mediated coupling reaction. Firstly, the abundant COOH groups on PAA react with EDC to form a highly reactive acyl isourea intermediate. This intermediate subsequently reacts with NHS to produce a more stable NHS ester, which further reacts with the NH 2 groups in PEI to form CO-NH bonds, ultimately yielding the PEI@PAA aerogel (Fig. S2). As shown in Fig. 1c, the FT-IR spectra of PEI@PAA exhibit a characteristic peak at 3420 cm − 1 , corresponding to the amino groups (RNH 2 ) in PEI. Furthermore, the peak at 1650 cm − 1 , 1560 cm − 1 , 1310 cm − 1 are assigned to the amide I band (C = O stretching vibration), the amide II band (N-H bending vibration) [ 34 ], and the amide III band (C-N stretching vibration) [ 35 ], respectively. These results confirm that CO-NH bonds are formed between COOH and NH 2 groups, thereby verifying the successful grafting of PEI onto PAA. The elevated nitrogen (N) content of 18.2%, revealed by Energy Dispersive Spectroscopy (EDS) in Fig. S6b, further corroborates this successful grafting. Furthermore, the X-ray Photoelectron Spectroscopy (XPS) spectrum exhibits a sharp peak near a binding energy of 400 eV, corresponding to the characteristic N 1s peak associated with the amino groups in PEI (Fig. 1d). Specifically, the high-resolution N 1s spectrum identifies binding energies at 398.82 eV and 400.61 eV, corresponding to N in amino groups and CO-NH bonds, respectively (Fig. 1g). As illustrated in Fig. 1e, following PEI grafting, the binding energy of C = O shifts from 288.47 eV (COOH) to 286.79 eV (CO-NH), while the binding energy of C-O shifts from 285.67 eV to 285.02 eV (C-N). In the O 1s spectrum (Fig. 1f), the peak at 531.74 eV matches that of carbonyl oxygen (C = O) in carboxyl groups, whereas the peak at 533.24 eV corresponds to hydroxyl oxygen (C-OH). Following PEI grafting, a new peak emerges at 530.32 eV, consistent with the binding energy of carbonyl oxygen in amide bonds (CO-NH) [ 36 ]. In Fig. 1f, the peak at 531.74 eV corresponds to carbonyl oxygen (C = O) in carboxyl groups, while the peak at 533.24 eV corresponds to hydroxyl oxygen (C-OH). Following PEI grafting, a new peak emerges at 530.32 eV, consistent with the binding energy of carbonyl oxygen in amide bonds (CO-NH) [ 36 ]. Collectively, these findings confirm that the amino groups in PEI participate in a dehydration reaction, forming C-N bonds. The SEM images in Fig. 2 a ~ f and Fig. S4 illustrate the microstructure of the PEI@PAA aerogel. The PEI@PAA aerogel exhibit a highly consistent 3D interconnected supermacro pore structures across the xy cross-sections (Fig. 2 a ~ c), xz cross-sections (Fig. 2 d ~ f), and surface views (Fig. S4a ~ c). The pore size distributionran ges from 10 ~ 100 µm, with a corresponding wall thickness of approximately 2 ~ 20 µm. This isotropic, interconnected pore structure ensures efficient gaseous iodine diffusion into the interior of the PEI@PAA aerogel from all directions. Figure 2 h shows that the C, O, and N elements are uniformly distributed on the surface of the PEI@PAA aerogel. In particular, after grafting PEI, the nitrogen content increases to 18.2%, further confirming the successful grafting of PEI. As indicated by the pore size distribution curve in Fig. 2 i, mesopores with sizes of 2 ~ 50 nm exist on the framework surface, thereby increasing the specific surface area and providing additional attachment sites for iodine molecules. The connectivity of the pore structure of PEI@PAA aerogel was assessed via dynamic contact angle measurements. As illustrated in Fig. 2 j, the droplet penetration time for the PAA aerogel with a 3D supermacro pore structure (2.56 s) is significantly shorter than that of non-porous PAA-T (12.12 s). This stark contrast highlights the core advantage of an interconnected macropores in enhancing mass transfer rates. Furthermore, the PEI@PAA aerogel demonstrates an exceptionally rapid droplet penetration time of 0.02 s, which is primarily attributed to its higher nitrogen content and the highly interconnected 3D pore architecture extending from the surface to the interior of the aerogel[ 37 , 38 ]. As shown in Fig. 3 a, both the PEI@PAA and PAA XRD spectrums exhibit broad diffraction peaks, conforming they are both amorphous structures. Compared with PAA, the amorphous diffraction peak of the PEI@PAA aerogel is slightly enhanced, which may be attributed to the local ordered arrangement of PEI molecular chains or the improvement of the amorphous state by the PAA-PEI cross-linked network [ 38 ].The Thermogravimetric Analysis (TGA) curve (Fig. 3 b) reveals that the thermal decomposition of PEI@PAA occurs in three distinct stages. Stage 1 (< 150°C) is associated with the desorption of physically adsorbed water, accounting for a weight loss of approximately 5%. Stage 2 (200 ~ 350°C) corresponds to the cleavage of the PAA main chain [ 39 ]. Stage 3 (350 ~ 500°C) results from the decomposition of PEI chains [ 40 ]. The TGA results indicate that the PEI@PAA aerogel exhibits good thermal stability below 200°C, satisfying the requirements of practical applications. The N 2 adsorption-desorption isotherms (Fig. 3 c ~ d) reveal pronounced hysteresis loops for both PAA and PEI@PAA, confirming the presence of mesoporous structures within their gel frameworks [ 41 ]. After PEI grafting, the specific surface area decreased from 26.66 m 2 ·g − 1 to 15.52 m 2 ·g − 1 (Table S6), whereas the average size of the micropores within the gel framework increased from 1.31 nm to 6.85 nm (Table S9). The observed alteration can be attributed to the partial occlusion of smaller pores by PEI molecules and the coalescence of neighboring pores. 2.2 Adsorption properties 2.2.1 Relationship between reaction conditions and adsorption capacity The effects of the NHS, EDC and PEI dosages as well as the grafting time on the adsorption capacity were investigated (Tables S2 ~ S5). As the dosages of NHS and EDC increased, the adsorption capacity of the PEI@PAA aerogel exhibited a declining trend (Fig. S8a and Fig. S8b). Specifically, when the NHS concentration increased from 1 g·L − 1 to 60 g·L − 1 , the adsorption capacity decreased correspondingly from 6.01 g·g − 1 to 3.14 g·g − 1 . This decrease could be attributed to the fact that a high NHS concentration promotes the formation of by-products, which consume the activated intermediates [ 42 ]. Furthermore, an excessive amount of NHS may accelerate the hydrolysis of the intermediate products, thereby diminishing the grafting efficiency [ 43 ]. As shown in Fig. S8c, the adsorption capacity initially increases before declinging with the increasing PEI dosage, peaking at a PEI concentration is 120 g·L-1. An excessive PEI dosage could impede the diffusion of PEI molecules within the aqueous phase, resulting in diminished grafting efficiency [ 44 ]. Similarly, the grafting time exhibits an optimal range, with the adsorption capacity peaking at approximately 9 h. The decline in adsorption capacity beyond the optimal grafting time can be attributed to two primary factors: Upon surpassing the reaction equilibrium, the active groups are fully consumed, precluding the formation of new active sites; and the pre-established bonding structures may be compromised [ 43 ]. Furthermore, prolonged reaction durations may promote the formation of by-products, which consequently reduces the availability of active sites [ 44 ]. Based on the above results, the optimal synthesis conditions for the PEI@PAA aerogel were determined to be: [(NHS)]: [(EDC)]: [(PEI)] = 1 g·L − 1 :1 g·L − 1 :120 g·L − 1 , with a grafting time of 9 h. 2.2.2 Rapid adsorption kinetics characteristics Figure 4 a illustrates the color evolution of the PEI@PAA aerogel over time during the gaseous iodine adsorption process. Initially white, the sample undergoes a noticeable color change after merely 5 minutes of exposure to iodine vapor. It’s color then transitions sequentially to bright yellow (30 min), orange (1 h), gradually darkens to dark red (4 h), and finally turns black after 12 h. This color progression provides a visual demonstration of the rapid iodine adsorption by the PEI@PAA aerogel. the elemental mapping image reveals a uniform distribution of iodine throughout the pores of the aerogel (Fig. 4 b). Furthermore, the XPS spectrum exhibits distinct characteristic peaks at binding energies of 630.52 eV and 619.32 eV, corresponding to I 3d 3 / 2 and I 3d 5 / 2 , respectively, which confirms the successful capture of iodine [ 45 ] (Fig. 4 d). SEM analysis shows that after iodine adsorption, the pore structure of PEI@PAA remains undistorted and unbroken, exhibiting good stability during the adsorption process (Fig. S5). As depicted in Fig. 4 c, the PEI@PAA aerogel attains 90% of its equilibrium adsorption capacity (5.49 g·g − 1 ) within 4 h, corresponding to an average initial adsorption rate of 1.53 g·g − 1 ·h − 1 ; the final equilibrium capacity is determined to be 6.01 g·g − 1 . A comparative analysis of the iodine adsorption kinetics for various adsorbents is presented in Fig. 5 b. The data reveal that most reported adsorbents typically require 10 ~ 20 h or longer to achieve the same level of adsorption (90% of equilibrium), whereas the PEI@PAA aerogel achieves this within merely 4 hours, demonstrating a pronounced kinetic advantage. The adsorption kinetics were analyzed by fitting the experimental data to three prevalent kinetic models: the pseudo-first-order (PFO), pseudo-second-order (PSO), and Weber-Morris intraparticle diffusion models. As summarized in Fig. S9 and Tables S8 ~ S9, the PSO model yielded a higher correlation coefficient ( R 2 = 0.95) compared to the PFO model ( R 2 = 0.91), suggesting that chemisorption is likely the rate-controlling step [ 46 ]. The adsorption kinetics were further analyzed using the Weber-Morris intraparticle diffusion model, which typically delineates the process into three consecutive stages: the initial rapid surface adsorption stage ( k 3 = 4.35 g·g − 1 ·h − 0.5 ), the gradual intraparticle diffusion stage ( k 3 = 0.49 g·g − 1 ·h − 0.5 ), and the final adsorption equilibrium stage ( k 3 = 0.15 g·g − 1 ·h − 0.5 ). As illustrated in the structural schematic (Fig. 5 a), the three-dimensional network of interconnected supermacro pores within the aerogel provides efficient mass transport channels for iodine molecules. This unique porous architecture is responsible for the remarkably high diffusion rate observed in the initial stage. During the subsequent intraparticle diffusion stage, the abundant amino groups (RNH 2 ) grafted onto the pore surfaces of PEI@PAA facilitate rapid chemical capture (chemisorption) of iodine molecules, contributing to the overall high adsorption efficiency and kinetics [ 47 ]. 2.2.3 Adsorption Isotherms The adsorption isotherms of the PEI@PAA aerogel for gaseous iodine are presented in Fig. 4 f. The adsorption capacity increased rapidly with rising equilibrium concentration before gradually leveling off and eventually reaching saturation, indicating a typical monolayer adsorption profile. As shown in Fig. S10 and summarized in Table S11, the experimental data at all three temperatures (80, 100 and 120 ℃) were better described by the Freundlich model, with correlation coefficients ( R 2 ) of 0.95, 0.91 and 0.94, respectively. In contrast, the Langmuir model exhibited relatively lower correlation coefficients ( R 2 = 0.87, 0.79, and 0.86 at 80, 100, and 120°C, respectively; Table S10). The Temkin model provided a good fit only at 80°C ( R 2 = 0.95), whereas its fitting performance was poor at the higher temperatures of 100 and 120°C (Table S12). The Langmuir model describes adsorption on a homogeneous surface, whereas the Freundlich and Temkin models are typically applied to heterogeneous surface adsorption [ 48 ]. The superior fit of the Freundlich and Temkin models therefore suggests that iodine adsorption onto the PEI@PAA aerogel occurs on a heterogeneous surface, characterized by active sites with a distribution of adsorption energies. This heterogeneity can likely be attributed to the varying affinities and steric accessibility of the different amino groups within the grafted PEI chains toward iodine molecules. As illustrated in Fig. 5 b, the PEI@PAA aerogel demonstrates a superior iodine adsorption capacity of 6.01 g·g − 1 , which is notably higher than that of many other types of adsorbents. A comparative summary of the chemical reagents required for synthesizing various iodine adsorbents is provided in Table S1 . It reveals that key reagents such as silver nitrate for silver-based adsorbents and the organic ligands for constructing covalent organic frameworks (COFs) incur substantially higher material costs. In stark contrast, the PEI@PAA aerogel is fabricated from low-cost AA and PEI. Furthermore, its synthesis features mild reaction conditions, straightforward procedures, and low energy consumption, all of which are favorable factors for scalable manufacturing. As demonstrated in Fig. S14, the kilogram-scale rapid preparation of PEI@PAA aerogel monoliths with dimensions of 50 cm (L) × 35 cm (W) × 4 cm (H) has been achieved at the laboratory scale. This result preliminarily verifies the potential of the PEI@PAA aerogel for scalable manufacturing. 2.3 Adsorption mechanism Following iodine adsorption, the intensity of the XRD diffraction peak for the PEI@PAA aerogel at approximately 22° decreases markedly (Fig. 6 a). This observation can be ascribed to segmental disorder induced by the incorporation of I 2 molecules into the polymer network [ 49 ]. Concurrently, the diffraction peak shifts to a higher angle (ca. 24°). This shift is likely due to the formation of N + -I − charge-transfer complexes between I₂ and the amino groups, which reduces the interchain spacing [ 50 ]. In the FT-IR spectrum after adsorption, the intensity of the N-H bending vibration peak located at 1560 cm − 1 is notably reduced (Fig. 6 b). This attenuation indicates a strong interaction between the amino groups and the adsorbed iodine molecules [ 49 ]. A significant weight loss appears in the TGA curve of PEI@PAA-I 2 within the temperature range of 150 ~ 300°C, which corresponds to the desorption process of iodine (Fig. 6 c). The C 1s XPS spectrum in Figure d shows that after PEI@PAA adsorbed I₂, the binding energies of the characteristic peaks of C-C, C-O and C = O all shifted positively by approximately 0.6 ~ 0.7 eV. Especially, the C-C peak moved from 283.71 eV to 284.38 eV, which directly confirmed that the iodine species had a strong chemical interaction with the surface functional groups of the material, resulting in a decrease in the electron cloud density around the carbon atoms (Fig. 6 d). The O 1s XPS spectrum in Figure e shows that after adsorbing I₂, the main peak binding energy of PEI@PAA significantly shifted from 530.32 eV to 531.38 eV, indicating a decrease in the electron cloud density around the oxygen atoms. This confirms that iodine has a strong chemical interaction with the oxygen-containing functional groups in the material (Fig. 6 e). The high-resolution N 1s XPS spectrum reveals that the binding energy shifts from 398.82 eV to 399.98 eV after iodine adsorption (Fig. 6 f). This positive shift implies a decrease in electron density around the N atoms, consistent with electron transfer [ 51 ]. Concurrently, the appearance of characteristic peaks for I 3d 5 / 2 and I 3d 3 / 2 (Fig. 4 e) confirms the presence of iodine species on the adsorbent. Together, these results suggest that charge transfer occurs from the lone pair electrons of the amino N atoms to the adsorbed iodine molecules. The transferred charge can subsequently facilitate the formation of polyiodide species (I- 3and I- 5) with neighboring iodine molecules [ 52 ]. Raman spectroscopy further corroborates the XPS findings. As shown in Fig. S11, the spectrum of PEI@PAA-I 2 exhibits characteristic peaks not only for molecular iodine (I 2 ) at 159 cm − 1 but also for polyiodide species, specifically I- 3 at 109 cm − 1 and I- 5 at 158 cm − 1 [ 53 ]. Collectively, the spectroscopic evidence confirms that the adsorbed iodine exists within the PEI@PAA aerogel in multiple forms, including molecular iodine (I 2 ) and polyiodide anions (I- 3 and I- 5). The above conclusions regarding the adsorption mechanism were further verified through density functional theory (DFT) calculations. To elucidate this at the molecular level, a simplified molecular model of the PEI@PAA aerogel was constructed, and its electrostatic potential (ESP) distribution was calculated (Fig. 6 g). The calculated ESP map revealed that regions proximal to the N-containing functional groups (RNH 2 , R 2 NH, R 3 N) all exhibit relatively low ESP values. The binding energies between I 2 and these different active sites were then calculated (Fig. 6 h, Table S7). Interestingly, the secondary amine site exhibits the highest binding energy with I 2 (-22.78 kJ·mol − 1 ), a finding that appears inconsistent with the amide group possessing the most negative ESP. This apparent discrepancy can be rationalized by considering the distinct electronic structures. For the amide group, the conjugation effect between the lone pair electrons on the N atom and the adjacent carbonyl (C = O) group delocalizes the electron density, thereby reducing the local electron cloud density and nucleophilic reactivity of the N lone pair towards I 2 [ 54 ]. In contrast, the secondary amine, while having a less negative ESP, does not experience such pronounced electron delocalization. Furthermore, the electron-withdrawing nature of the nearby amide group may create an electron buffer effect, polarizing and enhancing the electron-donating ability of the adjacent secondary amine, ultimately strengthening its interaction with I 2 [ 55 ]. The weak interaction analysis (Fig. 6 i) indicates that the interaction between I 2 and active sites is mainly electrostatic, and adjacent amino groups can synergistically enhance the adsorption of I 2 . 2.4 Radiation resistance performance Radioactive isotopes of iodine, such as 131 I and 129 I, emit high-energy radiation during their radioactive decay. During its decay, 131 I undergoes β decay to form stable 131 Xe [ 56 ], releasing β particles with a maximum energy of 0.606 MeV and an average energy of 0.192 MeV [ 57 ]. This process is also accompanied by the emission of γ photons. The most abundant γ photon emitted has an energy of 364 keV, with an emission probability of 81.2% [ 58 ]. Similarly, the long-lived isotope 129 I decays via β emission to 129 Xe. This high-energy radiation can induce ionization and excitation within the adsorbent material, potentially leading to radiation damage. Such damage may manifest as alterations in molecular structure, degradation of functional groups, and a consequent decline in adsorption performance [ 59 ]. Consequently, for prospective applications in radioactive environments, evaluating the radiation resistance of PEI@PAA aerogels is of paramount importance. As shown in Fig. 7 a, exposure to β and γ irradiation induced a color change in the aerogel samples, which became light yellow. SEM characterization reveals that the macropore size and wall thickness of the PEI@PAA aerogel remained largely unchanged after irradiation, thereby preserving the integrity of its three-dimensional porous network (Fig. 7 b ~ g). Furthermore, the EDS elemental mapping (Fig. S12) demonstrated a homogeneous distribution of C, N, and O within the pore structure of PEI@PAA-β and PEI@PAA-γ. The elemental compositions, particularly the N content, showed negligible variation (PEI@PAA: 18.2%; PEI@PAA-β: 18.88%; PEI@PAA-γ: 20.03%), indicating no significant elemental loss or redistribution occurred due to the irradiation. Collectively, these structural and compositional analyses confirm the excellent radiation-resistant stability of the PEI@PAA aerogel, which is attributed to the inherent radiation resistance of the PEI polymer matrix. The iodine adsorption performance of the irradiated samples was evaluated. As shown in Fig. 7 h, the irradiated PEI@PAA-β and PEI@PAA-γ samples retained high adsorption capacities of 5.28 g·g − 1 and 5.14 g·g − 1 , respectively. The robust 3D framework and highly cross-linked network of the PEI@PAA aerogel contribute to its radiation tolerance by mitigating damage to the active sites and preserving the structural integrity upon irradiation. FT-IR spectrum confirmed that the persistence of the characteristic peaks associated with amides at 1310 cm − 1 , 1560 cm − 1 , 1650 cm − 1 and the characteristic peak of amino groups at 3420 cm − 1 in the PEI@PAA aerogel after irradiation, although with a reduction in their intensities (Fig. 7 i). Figure 7 l shows that, the N 1s binding energy shifted from 398.82 eV to 399.55 eV after β irradiation, indicating a loss of electrons density around the N atoms. Similarly, Fig. 7 o shows that after γ irradiation, the binding energy of N 1s increased from 398.82 eV to 399.94 eV, which also indicates that γ rays caused N to lose electrons. These spectroscopic analyses collectively indicate that irradiation induces partial chemical conversion of the amino groups, which is likely responsible for the observed slight decrease in the iodine adsorption capacity of the PEI@PAA aerogel [ 60 ]. For comparison, the iodine adsorbent BiMgO-2MBD from a previous study was subjected to identical irradiation conditions, and its post-irradiation adsorption capacity was subsequently measured [ 61 ]. The pristine adsorption capacity of the BiMgO-2MBD adsorbent was 5.15 g·g − 1 at 150°C. After irradiation, the capacities of BiMgO-2MBD-β and BiMgO-2MBD-γ decreased to 3.68 g·g − 1 and 2.16 g·g − 1 , respectively (Fig. S13), corresponding to significant reduction of 28.5% and 58.1% relative to the pristine material. This substantial reduction of capacities can be attributed to the powdered morphology of BiMgO-2MBD, leading to its active groups being more susceptible to radiation damage. In contrast, the spatial network framework of the PEI@PAA aerogel enhances the integrity of the material and reduces radiation damage to the active groups. The monolithic structure of the PEI@PAA aerogel makes it more conducive to resisting the effects of radiation. 3. Conclusions In this work, a 3D interconnected porous PEI@PAA aerogel was successfully fabricated via a facile cryo-polymerization strategy for efficient gaseous iodine capture. By inducing solvent crystallization and enabling simultaneous in situ polymerization and crosslinking, this approach eliminates the reliance on energy-intensive freeze-drying, thereby significantly reducing the preparation cost. The unique 3D continuous macro porous architecture of the aerogel provides efficient mass transfer pathways, enabling the adsorption process to reach 90% of its equilibrium capacity within merely 4 h. Concurrently, the high grafting density of PEI provides an abundance of active sites, endowing the aerogel with an exceptional equilibrium iodine adsorption capacity of up to 6.01 g·g − 1 . Notably, systematic irradiation tests demonstrated that the PEI@PAA aerogel maintained its core porous framework and retained a high iodine adsorption capacity (5.14 ~ 5.28 g·g − 1 ) after exposure to β and γ irradiation. This confirms its excellent structural stability and radiation resistance, fulfilling a key prerequisite for practical deployment in radioactive environments. In summary, the PEI@PAA aerogel synergistically integrates outstanding iodine adsorption capacity, rapid adsorption kinetics, cost-effectiveness, excellent stability, and remarkable radiation resistance. Coupled with its demonstrated capability for scalable production, this material demonstrates great promise as a high-performance aerogel-based adsorbent for the capture of radioactive iodine. 4. Experimental 4.1 Methods 4.1.1 Synthesis of PAA matrix and non-porous PAA-T A porous PAA matrix was prepared via cryo-polymerization and denoted as PAA. As a contrast, a non-porous PAA matrix was prepared via room-temperature polymerization and denoted as PAA-T. AA monomer solution and MBA crosslinker were first pre-mixed at 0°C. Subsequently, APS solution (initiator) and VC solution (co-initiator) were added sequentially to the mixture under continuous stirring. After thorough homogenization, the mixture was promptly transferred into two silicone molds (dimension: length × width × height = 60 mm × 30 mm × 40 mm). The mass concentrations of each component in the reaction solution were as follows: AA (8 ~ 10%), MBA (1.6 ~ 2%), APS (0.0825%), and VC (0.056%). One silicone mold of the mixed solution was immediately transferred to a -20°C freezer to rapidly freeze and crystallize the solvent. Polymerization was then allowed to proceeded at -20°C for 12 h. Subsequently, the resulting polymer was demolded, thoroughly washed with deionized water, and dried under ambient temperature and pressure to yield the porous PAA matrix. The other silicone mold was polymerized at ambient temperature and pressure for 12 h. After demolding, it underwent identical washing and drying procedures to obtain the non-porous PAA-T matrix. 4.1.2 PEI@PAA synthesis of aerogels The PEI@PAA aerogel was synthesized by grafting PEI onto the PAA matrix via an EDC/NHS-mediated amidation reaction. PAA matrix (0.2 g, dry weight), NHS (0.01 g), EDC (0.01 g), and deionized water (10 mL) were sequentially added to a sample vial. The mixture was sonicated for 15 min to ensure complete dispersion. Subsequently, PEI (1.2 g) was added, followed by another 15-min sonication. The mixture was then transferred to a water bath and reacted at 60°C for 9 h. After the reaction, the solution was decanted, and the product was thoroughly washed with deionized water. Finally, the product was dried under ambient conditions, yielding the white, monolithic PEI@PAA aerogel. Detailed characterization methods and computational details for the density functional theory (DFT) calculations are provided in the Supporting Information. 4.2 Iodine Adsorption Experiments Detailed experimental parameters and results regarding the determination of adsorption capacity, batch adsorption experiments, adsorption kinetics, and fitting of adsorption isotherms as well as data processing can be found in the Supporting Information. 4.3 Radiation Resistance Tests The PEI@PAA aerogel and the reference iodine adsorbent BiMgO-2MBD [ 61 ] were irradiated with β and γ rays at a total dose of 50 kGy. The resulting samples were designated as PEI@PAA-β, PEI@PAA-γ, BiMgO-2MBD-β, and BiMgO-2MBD-γ, respectively. The irradiated materials were then characterized by FT-IR, SEM, XPS, and iodine adsorption performance tests. Declarations Conflict of Interest The authors declare no interest conflict. They have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. Funding This work was supported by National Natural Science Foundation of China (22476010), Higher Education Research Project of the Education Department of Guangdong Province (2024ZDZX3015) and State Key Laboratory for Modification of Chemical Fibers and Polymer Materials (KF2212). Author Contribution Meng Ji : Writing - original draft, Methodology, Formal analysis, Visualization，Data curation. Dagang Li : Methodology, Formal analysis, Writing - review & editing. Zilei Zhang : Data curation, Formal analysis. Haocun Tan : Writing - review & editing, Software. Xiyue Zhang : Software, Data curation. Yingjun Dong : Data curation, Investigation. Chuanle Lu : Data curation, Investigation. Jinying Li : Supervision, Project administration. Dongxiang Zhang : Writing - review & editing, Funding acquisition, Resources. Acknowledgement This work was supported by National Natural Science Foundation of China (22476010), Higher Education Research Project of the Education Department of Guangdong Province (2024ZDZX3015) and State Key Laboratory for Modification of Chemical Fibers and Polymer Materials (KF2212). References Yang X, Cai B, Xue Y (2022) Review on Optimization of Nuclear Power Development: A Cyber-Physical-Social System in Energy Perspective. J Mod Power Syst Clean Energy 10:547–561. https://doi.org/10.35833/MPCE.2021.000272 Beck CL, Cervantes J, Chiswell S, Greaney AT, Johnson KR, Levitskaia TG, Martin LR, McDaniel G, Noble S, Rakos JM, Riley BJ, Ritzmann A, Tingey JM (2024) Review of iodine behavior from nuclear fuel dissolution to environmental release. 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J Hazard Mater 474:134688. https://doi.org/10.1016/j.jhazmat.2024.134688 Additional Declarations No competing interests reported. Supplementary Files SupportingInformation.docx floatimage1.png Cite Share Download PDF Status: Under Review Version 1 posted Editorial decision: Revision requested 29 Mar, 2026 Reviews received at journal 23 Mar, 2026 Reviews received at journal 19 Mar, 2026 Reviewers agreed at journal 28 Feb, 2026 Reviewers agreed at journal 24 Feb, 2026 Reviewers invited by journal 23 Feb, 2026 Editor assigned by journal 13 Feb, 2026 Submission checks completed at journal 12 Feb, 2026 First submitted to journal 09 Feb, 2026 You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-8836259","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":598564951,"identity":"a392df63-07a1-41df-876b-9366842bf8c8","order_by":0,"name":"Meng Ji","email":"","orcid":"","institution":"Beijing Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Meng","middleName":"","lastName":"Ji","suffix":""},{"id":598564952,"identity":"c2829028-8ef7-46bc-ab19-e7cbc2858b0c","order_by":1,"name":"Dagang Li","email":"","orcid":"","institution":"Beijing Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Dagang","middleName":"","lastName":"Li","suffix":""},{"id":598564953,"identity":"ae22fc2e-af44-47f3-b293-0d25683772dd","order_by":2,"name":"Zilei Zhang","email":"","orcid":"","institution":"Beijing Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Zilei","middleName":"","lastName":"Zhang","suffix":""},{"id":598564954,"identity":"fbfa4a4f-0071-4967-a940-ba957d80936b","order_by":3,"name":"Haocun Tan","email":"","orcid":"","institution":"Beijing Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Haocun","middleName":"","lastName":"Tan","suffix":""},{"id":598564955,"identity":"f8b94ae4-1f75-4e3f-b33a-a9b97ea58e76","order_by":4,"name":"Xiyue Zhang","email":"","orcid":"","institution":"Beijing Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Xiyue","middleName":"","lastName":"Zhang","suffix":""},{"id":598564956,"identity":"b17b69cc-0eb8-45ce-a5ac-5bf374952e9c","order_by":5,"name":"Yingjun Dong","email":"","orcid":"","institution":"Beijing Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Yingjun","middleName":"","lastName":"Dong","suffix":""},{"id":598564957,"identity":"4ac278e6-cb57-489c-9b0a-e39ac8ab7f1b","order_by":6,"name":"Chuanle Lu","email":"","orcid":"","institution":"Beijing Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Chuanle","middleName":"","lastName":"Lu","suffix":""},{"id":598564958,"identity":"ba7be25c-ab96-47cb-8d25-831a2c075b4e","order_by":7,"name":"Jinying Li","email":"","orcid":"","institution":"China National Nuclear Corporation","correspondingAuthor":false,"prefix":"","firstName":"Jinying","middleName":"","lastName":"Li","suffix":""},{"id":598564959,"identity":"494c6d7d-a873-41ac-9f32-f19917765d6a","order_by":8,"name":"Dongxiang Zhang","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAsklEQVRIiWNgGAWjYBACAyA+wFBxgAfEkSBBy5kDPDwkaWFgbDvAQLwWc/behwd/zrsjY8/AfPA2D4NdHkEtlj3HDQ7zbnsGdBhbsjUPQ3IxYYfdSGM4zLjtMFALj5k0D8OBxAZitBz8OQekhf8b8VoO8DaAbWEjTotlzzGGwzzHgH45zGZsOccgmbAWc/Y25o8/au7Ys7c3P7zxpsKOsBYEYAa7k3j1o2AUjIJRMArwAADzZTe/5xWUVQAAAABJRU5ErkJggg==","orcid":"","institution":"Beijing Institute of Technology","correspondingAuthor":true,"prefix":"","firstName":"Dongxiang","middleName":"","lastName":"Zhang","suffix":""}],"badges":[],"createdAt":"2026-02-10 04:38:18","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-8836259/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-8836259/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":103778035,"identity":"9a8be289-eecd-44d4-9423-d5dc838cdaa4","added_by":"auto","created_at":"2026-03-02 19:29:29","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":412845,"visible":true,"origin":"","legend":"\u003cp\u003ePreparation and characterization of the PAA matrix and PEI@PAA. a. Schematic diagram of PAA matrix synthesis, including solvent cryo-polymerization, chemical cross-linking, and pore templating, which together form continuous 3D pores. b.EDC/NHS-mediated coupling reaction: the amino groups in PEI react with the carboxyl groups in PAA to form amide bonds, leading to the synthesis of PEI@PAA; after drying under ambient pressure, PEI@PAA aerogel are obtained. c.FT-IR spectra of the PAA matrix and PEI@PAA. d. Full XPS spectra of PAA and PEI@PAA. e. High-resolution XPS spectra of C 1s for PAA and PEI@PAA. f.High-resolution XPS spectra of O 1s for PAA and PEI@PAA. g.High-resolution XPS spectrum of N 1s for PEI@PAA.\u003c/p\u003e","description":"","filename":"floatimage2.png","url":"https://assets-eu.researchsquare.com/files/rs-8836259/v1/921c2b3559cfd0611df5eb22.png"},{"id":103778036,"identity":"54978a7c-ec92-4f44-a6b7-d492fa046bbf","added_by":"auto","created_at":"2026-03-02 19:29:29","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":508524,"visible":true,"origin":"","legend":"\u003cp\u003eMicroscopic pore structure of PEI@PAA. a–c. SEM images of the PEI@PAA xy cross-section. d–f. SEM images of the PEI@PAA xz cross-section. g. Optical image of the PEI@PAA aerogel. h. EDS-Mapping analysis of PEI@PAA. i. Pore size distribution curve of the PEI@PAA aerogel framework obtained via BET measurement. j. Dynamic contact angle test for pore connectivity of PAA, PEI@PAA, and PAA-T (non-porous).\u003c/p\u003e","description":"","filename":"floatimage3.png","url":"https://assets-eu.researchsquare.com/files/rs-8836259/v1/68d89304667b4b81e5279d43.png"},{"id":103778037,"identity":"3c822846-962b-4a9e-9ed1-a410c2548358","added_by":"auto","created_at":"2026-03-02 19:29:29","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":372505,"visible":true,"origin":"","legend":"\u003cp\u003ePhysicochemical property characterization of PEI@PAA. a. XRD patterns of PAA and PEI@PAA. b. TGA curve of PEI@PAA. c. N\u003csub\u003e2\u003c/sub\u003e adsorption isotherm of the PAA matrix obtained via BET measurement. d. N\u003csub\u003e2\u003c/sub\u003e adsorption isotherm of the PEI@PAA aerogel Obtained via BET measurement.\u003c/p\u003e","description":"","filename":"floatimage4.png","url":"https://assets-eu.researchsquare.com/files/rs-8836259/v1/8b9e18185ddc72c3a4838070.png"},{"id":104400178,"identity":"65c54762-48ab-4041-8f28-c1e8e4067496","added_by":"auto","created_at":"2026-03-11 12:09:07","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":359229,"visible":true,"origin":"","legend":"\u003cp\u003eAdsorption characteristics of PEI@PAA aerogel for gaseous iodine. a. Apparent changes of PEI@PAA over time during the iodine adsorption process. b. EDS-Mapping elemental analysis of PEI@PAA-I\u003csub\u003e2\u003c/sub\u003e. c. Adsorption kinetic curve of PEI@PAA for iodine vapor.\u003csup\u003e \u003c/sup\u003ed. XPS spectra of PEI@PAA before and after iodine adsorption.\u003csup\u003e \u003c/sup\u003ee. High-resolution XPS spectrum of iodine in PEI@PAA-I\u003csub\u003e2\u003c/sub\u003e.\u003csup\u003e \u003c/sup\u003ef. Adsorption isotherm of PEI@PAA for gaseous iodine.\u003c/p\u003e","description":"","filename":"floatimage5.png","url":"https://assets-eu.researchsquare.com/files/rs-8836259/v1/46b8bc376d412e3535781f37.png"},{"id":104400278,"identity":"c7546181-a54a-4612-9741-cbe71eb58312","added_by":"auto","created_at":"2026-03-11 12:09:28","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":378829,"visible":true,"origin":"","legend":"\u003cp\u003ea. Mechanism of rapid kinetics for gaseous iodine adsorption by PEI@PAA aerogel. b. Performance comparison (adsorption capacity and kinetics) between PEI@PAA aerogel and other iodine-adsorbing materials; detailed adsorption characteristics of each adsorbent are provided in Table S13.\u003c/p\u003e","description":"","filename":"floatimage6.png","url":"https://assets-eu.researchsquare.com/files/rs-8836259/v1/6d00ee7c7d740c30d96b0d0f.png"},{"id":103778042,"identity":"238888dc-f67d-4f8b-97f9-4777834f2af4","added_by":"auto","created_at":"2026-03-02 19:29:29","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":467893,"visible":true,"origin":"","legend":"\u003cp\u003eAdsorption mechanism of PEI@PAA aerogel for iodine vapor. a. XRD patterns of PEI@PAA before and after iodine adsorption. b. FT-IR spectra of PEI@PAA before and after iodine adsorption. c. TGA curve of PEI@PAA-I\u003csub\u003e2\u003c/sub\u003e. d. High-resolution XPS C 1s spectra of PEI@PAA before and after iodine adsorption. e. High-resolution XPS O 1s spectra of PEI@PAA before and after iodine adsorption. f. High-resolution XPS N 1s spectra of PEI@PAA before and after iodine adsorption. g. Electrostatic potential (ESP) distribution map of PEI@PAA. h. Different molecular conformations of PEI@PAA adsorbing I\u003csub\u003e2\u003c/sub\u003e simulated by DFT. Here, black represents C (carbon), white represents H (hydrogen), red represents O (oxygen), blue represents N (nitrogen), and purple represents I (iodine). h-1. I\u003csub\u003e2\u003c/sub\u003e approaching NH\u003csub\u003e2\u003c/sub\u003e-R. h-2. I\u003csub\u003e2\u003c/sub\u003e approaching NH-R. h-3. I\u003csub\u003e2\u003c/sub\u003e approaching N-R. h-4. I\u003csub\u003e2\u003c/sub\u003e approaching NH-C=O. i. Weak interaction analysis between PEI@PAA and I\u003csub\u003e2\u003c/sub\u003e via the IRI method. i-1. I\u003csub\u003e2\u003c/sub\u003e approaching NH\u003csub\u003e2\u003c/sub\u003e-R. i-2. I\u003csub\u003e2\u003c/sub\u003e approaching NH-R. i-3. I\u003csub\u003e2\u003c/sub\u003e approaching N-R. i-4. I\u003csub\u003e2\u003c/sub\u003e approaching NH-C=O\u003c/p\u003e","description":"","filename":"floatimage7.png","url":"https://assets-eu.researchsquare.com/files/rs-8836259/v1/c99bc37f92cb363218cd8b14.png"},{"id":103778039,"identity":"6893c7d6-31b9-45b1-a2df-750ac08faf9d","added_by":"auto","created_at":"2026-03-02 19:29:29","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":566711,"visible":true,"origin":"","legend":"\u003cp\u003ePerformance changes of PEI@PAA aerogel after irradiation. a. Photographs of PEI@PAA aerogel before and after irradiation. b~g. SEM characterization of PEI@PAA-β and PEI@PAA-γ. h. Comparison of adsorption capacities before and after irradiation. i. FT-IR spectra of PEI@PAA before and after irradiation. j. C 1s spectrum of PEI@PAA-β. k. O 1s spectrum of PEI@PAA-β. l. N 1s spectrum of PEI@PAA-β. m. C 1s spectrum of PEI@PAA-γ. n. O 1s spectrum of PEI@PAA-γ. o. N 1s spectrum of PEI@PAA-γ.\u003c/p\u003e","description":"","filename":"floatimage8.png","url":"https://assets-eu.researchsquare.com/files/rs-8836259/v1/54a41ff1470d5fb8f9eeafad.png"},{"id":104407782,"identity":"5c71cc4a-2dc0-492e-bb35-9c227848a2bf","added_by":"auto","created_at":"2026-03-11 12:40:03","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":3931408,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-8836259/v1/4f4dc978-e908-4e3e-9a27-4fbdd9bfab47.pdf"},{"id":103778044,"identity":"28d55153-c95b-4ba9-8247-3d45265f25ad","added_by":"auto","created_at":"2026-03-02 19:29:29","extension":"docx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":6422606,"visible":true,"origin":"","legend":"","description":"","filename":"SupportingInformation.docx","url":"https://assets-eu.researchsquare.com/files/rs-8836259/v1/da4c4877016b1c33de27cfb0.docx"},{"id":103778041,"identity":"b52a01fa-33bf-4f58-849e-0743621d1741","added_by":"auto","created_at":"2026-03-02 19:29:29","extension":"png","order_by":2,"title":"","display":"","copyAsset":false,"role":"supplement","size":985135,"visible":true,"origin":"","legend":"","description":"","filename":"floatimage1.png","url":"https://assets-eu.researchsquare.com/files/rs-8836259/v1/d7d0b1280a19307f191120b6.png"}],"financialInterests":"No competing interests reported.","formattedTitle":"A radiation-resistant supermacroporous aerogel for ultrafast and high-capacity gaseous iodine capture","fulltext":[{"header":"Highlights","content":"\u003cp\u003eλ A 3D supermacroporous PEI@PAA aerogel via facile cryo-polymerization.\u003c/p\u003e\u003cp\u003eλ Record-high iodine capture capacity of 6.01 g\u0026middot;g achieved.\u003c/p\u003e\u003cp\u003eλ Rapid adsorption: 90% equilibrium reached within 4 h.\u003c/p\u003e\u003cp\u003eλ Excellent resistance to β/γ-irradiation demonstrated.\u003c/p\u003e\u003cp\u003eλ Cost significantly lower than conventional silver-loaded adsorbents.\u003c/p\u003e"},{"header":"1. Introduction","content":"\u003cp\u003eAs a crucial component of the global low-carbon energy system, nuclear energy is essential in advancing the energy transition and achieving carbon neutrality [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e]. However, the release of radioactive iodine isotopes (such as \u003csup\u003e129\u003c/sup\u003eI with a half-life of 1.57\u0026times;10\u003csup\u003e7\u003c/sup\u003e years and \u003csup\u003e131\u003c/sup\u003eI with a half-life of 8.02 days) during spent fuel reprocessing is characterized by high volatility and significant bioaccumulation [\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e].\u003csup\u003e129\u003c/sup\u003eI migrates through the atmosphere into water bodies and soil [\u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e]. It tends to persist in the environment for prolonged periods and accumulates in the human thyroid gland, posing health risks [\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e]. Consequently, the development of efficient, stable, and economically viable technologies for radioactive iodine capture represents a core scientific and engineering challenge essential for the sustainable advancement of nuclear energy [\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eAmong various treatment technologies, the adsorption method has garnered significant attention due to its simplicity and cost-effectiveness [\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e]. However, traditional adsorbents, such as silver-loaded zeolite (Ag-MOR), exhibit high selectivity but possess a limited adsorption capacity of only 0.22 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, relying on the precious metal silver, which contributes to elevated costs [\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e]. In contrast, metal sulfide composites like CuS/AC can enhance the adsorption capacity to 0.49 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, but they pose a flammability risk [\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e]. Recently emerged porous materials (MOFs [\u003cspan additionalcitationids=\"CR10\" citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e], COFs [\u003cspan additionalcitationids=\"CR13\" citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e], POPs [\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e, \u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e]) demonstrate potential for iodine capture. However, they encounter challenges, including complex preparation, high costs, slow kinetics, and inadequate radiation stability. ZIF-8 is susceptible to structural collapse in humid environments [\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e], while UiO-66-NH\u003csub\u003e2\u003c/sub\u003e incurs high preparation cost [\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e]. Although TpPa-1 [\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e] and COF-TAPA [\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e] exhibit high specific surface areas, they necessitate high-temperature vacuum synthesis, and their adsorption equilibrium times extend to dozens of hours. Furthermore, most studies also overlook the influence of β/γ-irradiation on adsorption performance, which is particularly critical in the context of nuclear waste treatment [\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eTo simultaneously enhance the adsorption rate and capacity for gaseous iodine, researchers have sought to introduce 3D porous aerogels, leveraging their supermacro interconnected pores to facilitate molecular transport. Zhu \u003cem\u003eet al\u003c/em\u003e. prepared Catechin@3DCF aerogels via freeze-drying, achieving an iodine adsorption capacity of 2.23 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, although equilibrium required up to 20 h [\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e]. The UiO-66-NH\u003csub\u003e2\u003c/sub\u003e@WCA aerogels developed by Tian\u0026rsquo; team shortened the adsorption equilibrium time to 15 h; however, their fabrication still relied on energy-intensive freeze-drying with prolonged processing cycles [\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e]. Consequently, developing energy-efficient strategies for the controllable construction of 3D interconnected macroporous structures remains a critical and unresolved challenge.\u003c/p\u003e \u003cp\u003eThe cryo-polymerization technique induces solvent crystallization under low-temperature conditions to template macropore formation, while in situ polymerization and simultaneous crosslinking construct a fully interconnected macroporous network, thereby overcoming the limitations of conventional freeze-drying and enabling drying and shaping under ambient temperature and pressure [\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e]. A series of 3D continuous porous adsorbents for uranium extraction from seawater have been developed via organic/aqueous phase cryo-polymerization [\u003cspan additionalcitationids=\"CR25 CR26 CR27 CR28\" citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e]. Research on uranium has demonstrated that cryo-polymerization can rapidly construct continuous supermacro pores, significantly enhancing mass transfer flux and adsorption capacity. Building on this concept, we propose a green aqueous phase cryo-polymerization strategy. Using acrylic acid (AA) as the monomer to create a polyacrylic acid (PAA) framework, and employing an EDC/NHS-mediated amidation reaction for covalent grafting of polyethyleneimine (PEI), we prepared a 3D aerogel (PEI@PAA) with interconnected pores of 10\u0026ndash;100 \u0026micro;m (Fig.\u0026nbsp;1a and 1b). The PEI@PAA aerogel exhibits both ultrahigh adsorption capacity (6.01 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) and rapid kinetics, achieving 90% equilibrium within 4 h. The highly cross-linked 3D network within the gel phase of PEI@PAA confers excellent radiation resistance stability, maintaining an adsorption capacity of 5.14\u0026thinsp;~\u0026thinsp;5.28 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e after 50 kGy β/γ irradiation. Furthermore, this method circumvents the energy-intensive freeze-drying process, facilitating low-cost and scalable preparation, and offering a practical new approach for efficient radioactive iodine capture and nuclear waste treatment.\u003c/p\u003e"},{"header":"2. Results and Discussion","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003e2.1 Formation mechanism of the 3D continuous pore microstructure of PEI@PAA aerogel\u003c/h2\u003e \u003cp\u003eIn Fig.\u0026nbsp;1a, the aqueous solvent of the AA solution gradually cools to form ice crystals at -20\u0026deg;C. These ice crystals serve as templates for the formation of supermacro pores, confining the reaction components to the amorphous regions between the ice crystals [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. Within these amorphous regions, free radicals generated by the redox initiator trigger the polymerization reaction: on one hand, AA monomers polymerize into long PAA molecular chains. On the other hand, N,N'-methylenebisacrylamide (MBA) forms high-density chemical cross-links with AA through covalent bonding (Fig. \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e). This combination constitutes the framework of the PAA gel phase with a 3D network structure [\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eThe Fourier Transform Infrared Spectroscopy (FT-IR) spectrum indicates that the broad absorption peak at 3390 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and the strong absorption peak at 1720 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e are attributed to the O-H stretching vibration and C\u0026thinsp;=\u0026thinsp;O asymmetric stretching vibration in the COOH group [\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e], respectively. The characteristic peak at 2950 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e corresponds to the C-H stretching vibration [\u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e] (Fig.\u0026nbsp;1c). These characteristic peaks confirm the occurrence of the polymerization reaction. Notably, the framework of the PAA gel phase is formed through high-density cross-linking. Following drying under ambient temperature and pressure, the ice crystals melt, leaving behind interconnected supermacro pores in situ, thereby yielding a PAA framework with a continuous 3D supermacro pore structure.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003cb\u003eFigure\u0026nbsp;1 Preparation and characterization of the PAA matrix and PEI@PAA. a.\u003c/b\u003e Schematic diagram of PAA matrix synthesis, including solvent cryo-polymerization, chemical cross-linking, and pore templating, which together form continuous 3D pores. \u003cb\u003eb.\u003c/b\u003e EDC/NHS-mediated coupling reaction: the amino groups in PEI react with the carboxyl groups in PAA to form amide bonds, leading to the synthesis of PEI@PAA; after drying under ambient pressure, PEI@PAA aerogel are obtained. \u003cb\u003ec.\u003c/b\u003e FT-IR spectra of the PAA matrix and PEI@PAA. \u003cb\u003ed.\u003c/b\u003e Full XPS spectra of PAA and PEI@PAA. \u003cb\u003ee.\u003c/b\u003e High-resolution XPS spectra of C 1s for PAA and PEI@PAA. \u003cb\u003ef.\u003c/b\u003e High-resolution XPS spectra of O 1s for PAA and PEI@PAA. \u003cb\u003eg.\u003c/b\u003e High-resolution XPS spectrum of N 1s for PEI@PAA.\u003c/p\u003e \u003cp\u003eAs evidenced by the Scanning Electron Microscope (SEM) characterization in Fig. S3, both the xy cross-sections (Fig. S3 a\u0026thinsp;~\u0026thinsp;c) and xz cross-sections (Fig. S3 d\u0026thinsp;~\u0026thinsp;f) of the PAA aerogel demonstrate a continuous macroporous channel structure, with a pore size of approximately 10\u0026ndash;100 \u0026micro;m and a wall thickness of about 2\u0026thinsp;~\u0026thinsp;20 \u0026micro;m. In particular, the surface of the PAA matrix (Fig. S3 g\u0026thinsp;~\u0026thinsp;i) exhibits a regular and continuous pore structure with comparable pore sizes. This phenomenon is attributed to the continuous distribution of ice crystals during the cryo-polymerization process, which generates a 3D interconnected pore structure of PAA from the surface to the interior and exhibits a uniform pore distribution state, facilitating the diffusion and adsorption mass transfer of gaseous iodine. The pore size distribution curve of the PAA framework surface indicates a significant presence of mesopores with sizes of 2\u0026thinsp;~\u0026thinsp;50 nm on the pore wall surface (Fig. S7). These fine pore structures enhance the adsorption capacity.\u003c/p\u003e \u003cp\u003eFigure\u0026nbsp;1b illustrates the grafting process of PEI onto the PAA framework via the EDC/NHS-mediated coupling reaction. Firstly, the abundant COOH groups on PAA react with EDC to form a highly reactive acyl isourea intermediate. This intermediate subsequently reacts with NHS to produce a more stable NHS ester, which further reacts with the NH\u003csub\u003e2\u003c/sub\u003e groups in PEI to form CO-NH bonds, ultimately yielding the PEI@PAA aerogel (Fig. S2).\u003c/p\u003e \u003cp\u003eAs shown in Fig.\u0026nbsp;1c, the FT-IR spectra of PEI@PAA exhibit a characteristic peak at 3420 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, corresponding to the amino groups (RNH\u003csub\u003e2\u003c/sub\u003e) in PEI. Furthermore, the peak at 1650 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, 1560 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, 1310 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e are assigned to the amide I band (C\u0026thinsp;=\u0026thinsp;O stretching vibration), the amide II band (N-H bending vibration) [\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e], and the amide III band (C-N stretching vibration) [\u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e], respectively. These results confirm that CO-NH bonds are formed between COOH and NH\u003csub\u003e2\u003c/sub\u003e groups, thereby verifying the successful grafting of PEI onto PAA. The elevated nitrogen (N) content of 18.2%, revealed by Energy Dispersive Spectroscopy (EDS) in Fig. S6b, further corroborates this successful grafting.\u003c/p\u003e \u003cp\u003eFurthermore, the X-ray Photoelectron Spectroscopy (XPS) spectrum exhibits a sharp peak near a binding energy of 400 eV, corresponding to the characteristic N 1s peak associated with the amino groups in PEI (Fig.\u0026nbsp;1d). Specifically, the high-resolution N 1s spectrum identifies binding energies at 398.82 eV and 400.61 eV, corresponding to N in amino groups and CO-NH bonds, respectively (Fig.\u0026nbsp;1g). As illustrated in Fig.\u0026nbsp;1e, following PEI grafting, the binding energy of C\u0026thinsp;=\u0026thinsp;O shifts from 288.47 eV (COOH) to 286.79 eV (CO-NH), while the binding energy of C-O shifts from 285.67 eV to 285.02 eV (C-N). In the O 1s spectrum (Fig.\u0026nbsp;1f), the peak at 531.74 eV matches that of carbonyl oxygen (C\u0026thinsp;=\u0026thinsp;O) in carboxyl groups, whereas the peak at 533.24 eV corresponds to hydroxyl oxygen (C-OH). Following PEI grafting, a new peak emerges at 530.32 eV, consistent with the binding energy of carbonyl oxygen in amide bonds (CO-NH) [\u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e]. In Fig.\u0026nbsp;1f, the peak at 531.74 eV corresponds to carbonyl oxygen (C\u0026thinsp;=\u0026thinsp;O) in carboxyl groups, while the peak at 533.24 eV corresponds to hydroxyl oxygen (C-OH). Following PEI grafting, a new peak emerges at 530.32 eV, consistent with the binding energy of carbonyl oxygen in amide bonds (CO-NH) [\u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e]. Collectively, these findings confirm that the amino groups in PEI participate in a dehydration reaction, forming C-N bonds.\u003c/p\u003e \u003cp\u003eThe SEM images in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e2\u003c/span\u003ea\u0026thinsp;~\u0026thinsp;f and Fig. S4 illustrate the microstructure of the PEI@PAA aerogel. The PEI@PAA aerogel exhibit a highly consistent 3D interconnected supermacro pore structures across the xy cross-sections (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e2\u003c/span\u003ea\u0026thinsp;~\u0026thinsp;c), xz cross-sections (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e2\u003c/span\u003ed\u0026thinsp;~\u0026thinsp;f), and surface views (Fig. S4a\u0026thinsp;~\u0026thinsp;c). The pore size distributionran ges from 10\u0026thinsp;~\u0026thinsp;100 \u0026micro;m, with a corresponding wall thickness of approximately 2\u0026thinsp;~\u0026thinsp;20 \u0026micro;m. This isotropic, interconnected pore structure ensures efficient gaseous iodine diffusion into the interior of the PEI@PAA aerogel from all directions. Figure\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e2\u003c/span\u003eh shows that the C, O, and N elements are uniformly distributed on the surface of the PEI@PAA aerogel. In particular, after grafting PEI, the nitrogen content increases to 18.2%, further confirming the successful grafting of PEI. As indicated by the pore size distribution curve in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e2\u003c/span\u003ei, mesopores with sizes of 2\u0026thinsp;~\u0026thinsp;50 nm exist on the framework surface, thereby increasing the specific surface area and providing additional attachment sites for iodine molecules.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe connectivity of the pore structure of PEI@PAA aerogel was assessed via dynamic contact angle measurements. As illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e2\u003c/span\u003ej, the droplet penetration time for the PAA aerogel with a 3D supermacro pore structure (2.56 s) is significantly shorter than that of non-porous PAA-T (12.12 s). This stark contrast highlights the core advantage of an interconnected macropores in enhancing mass transfer rates. Furthermore, the PEI@PAA aerogel demonstrates an exceptionally rapid droplet penetration time of 0.02 s, which is primarily attributed to its higher nitrogen content and the highly interconnected 3D pore architecture extending from the surface to the interior of the aerogel[\u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e, \u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e].\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eAs shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e3\u003c/span\u003ea, both the PEI@PAA and PAA XRD spectrums exhibit broad diffraction peaks, conforming they are both amorphous structures. Compared with PAA, the amorphous diffraction peak of the PEI@PAA aerogel is slightly enhanced, which may be attributed to the local ordered arrangement of PEI molecular chains or the improvement of the amorphous state by the PAA-PEI cross-linked network [\u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e].The Thermogravimetric Analysis (TGA) curve (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e3\u003c/span\u003eb) reveals that the thermal decomposition of PEI@PAA occurs in three distinct stages. Stage 1 (\u0026lt;\u0026thinsp;150\u0026deg;C) is associated with the desorption of physically adsorbed water, accounting for a weight loss of approximately 5%. Stage 2 (200\u0026thinsp;~\u0026thinsp;350\u0026deg;C) corresponds to the cleavage of the PAA main chain [\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e]. Stage 3 (350\u0026thinsp;~\u0026thinsp;500\u0026deg;C) results from the decomposition of PEI chains [\u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e40\u003c/span\u003e]. The TGA results indicate that the PEI@PAA aerogel exhibits good thermal stability below 200\u0026deg;C, satisfying the requirements of practical applications. The N\u003csub\u003e2\u003c/sub\u003e adsorption-desorption isotherms (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e3\u003c/span\u003ec\u0026thinsp;~\u0026thinsp;d) reveal pronounced hysteresis loops for both PAA and PEI@PAA, confirming the presence of mesoporous structures within their gel frameworks [\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e]. After PEI grafting, the specific surface area decreased from 26.66 m\u003csup\u003e2\u003c/sup\u003e\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e to 15.52 m\u003csup\u003e2\u003c/sup\u003e\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e(Table S6), whereas the average size of the micropores within the gel framework increased from 1.31 nm to 6.85 nm (Table S9). The observed alteration can be attributed to the partial occlusion of smaller pores by PEI molecules and the coalescence of neighboring pores.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec4\" class=\"Section2\"\u003e \u003ch2\u003e2.2 Adsorption properties\u003c/h2\u003e \u003cdiv id=\"Sec5\" class=\"Section3\"\u003e \u003ch2\u003e2.2.1 Relationship between reaction conditions and adsorption capacity\u003c/h2\u003e \u003cp\u003eThe effects of the NHS, EDC and PEI dosages as well as the grafting time on the adsorption capacity were investigated (Tables S2\u0026thinsp;~\u0026thinsp;S5). As the dosages of NHS and EDC increased, the adsorption capacity of the PEI@PAA aerogel exhibited a declining trend (Fig. S8a and Fig. S8b). Specifically, when the NHS concentration increased from 1 g\u0026middot;L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e to 60 g\u0026middot;L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, the adsorption capacity decreased correspondingly from 6.01 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e to 3.14 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. This decrease could be attributed to the fact that a high NHS concentration promotes the formation of by-products, which consume the activated intermediates [\u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e]. Furthermore, an excessive amount of NHS may accelerate the hydrolysis of the intermediate products, thereby diminishing the grafting efficiency [\u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e43\u003c/span\u003e].\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eAs shown in Fig. S8c, the adsorption capacity initially increases before declinging with the increasing PEI dosage, peaking at a PEI concentration is 120 g\u0026middot;L-1. An excessive PEI dosage could impede the diffusion of PEI molecules within the aqueous phase, resulting in diminished grafting efficiency [\u003cspan citationid=\"CR44\" class=\"CitationRef\"\u003e44\u003c/span\u003e]. Similarly, the grafting time exhibits an optimal range, with the adsorption capacity peaking at approximately 9 h. The decline in adsorption capacity beyond the optimal grafting time can be attributed to two primary factors: Upon surpassing the reaction equilibrium, the active groups are fully consumed, precluding the formation of new active sites; and the pre-established bonding structures may be compromised [\u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e43\u003c/span\u003e]. Furthermore, prolonged reaction durations may promote the formation of by-products, which consequently reduces the availability of active sites [\u003cspan citationid=\"CR44\" class=\"CitationRef\"\u003e44\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eBased on the above results, the optimal synthesis conditions for the PEI@PAA aerogel were determined to be: [(NHS)]: [(EDC)]: [(PEI)]\u0026thinsp;=\u0026thinsp;1 g\u0026middot;L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e:1 g\u0026middot;L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e:120 g\u0026middot;L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, with a grafting time of 9 h.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec6\" class=\"Section3\"\u003e \u003ch2\u003e2.2.2 Rapid adsorption kinetics characteristics\u003c/h2\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e4\u003c/span\u003ea illustrates the color evolution of the PEI@PAA aerogel over time during the gaseous iodine adsorption process. Initially white, the sample undergoes a noticeable color change after merely 5 minutes of exposure to iodine vapor. It\u0026rsquo;s color then transitions sequentially to bright yellow (30 min), orange (1 h), gradually darkens to dark red (4 h), and finally turns black after 12 h. This color progression provides a visual demonstration of the rapid iodine adsorption by the PEI@PAA aerogel. the elemental mapping image reveals a uniform distribution of iodine throughout the pores of the aerogel (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e4\u003c/span\u003eb). Furthermore, the XPS spectrum exhibits distinct characteristic peaks at binding energies of 630.52 eV and 619.32 eV, corresponding to I 3d\u003csub\u003e3\u003c/sub\u003e/\u003csub\u003e2\u003c/sub\u003e and I 3d\u003csub\u003e5\u003c/sub\u003e/\u003csub\u003e2\u003c/sub\u003e, respectively, which confirms the successful capture of iodine [\u003cspan citationid=\"CR45\" class=\"CitationRef\"\u003e45\u003c/span\u003e] (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e4\u003c/span\u003ed). SEM analysis shows that after iodine adsorption, the pore structure of PEI@PAA remains undistorted and unbroken, exhibiting good stability during the adsorption process (Fig. S5).\u003c/p\u003e \u003cp\u003eAs depicted in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e4\u003c/span\u003ec, the PEI@PAA aerogel attains 90% of its equilibrium adsorption capacity (5.49 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) within 4 h, corresponding to an average initial adsorption rate of 1.53 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e\u0026middot;h\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e; the final equilibrium capacity is determined to be 6.01 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. A comparative analysis of the iodine adsorption kinetics for various adsorbents is presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e5\u003c/span\u003eb. The data reveal that most reported adsorbents typically require 10\u0026thinsp;~\u0026thinsp;20 h or longer to achieve the same level of adsorption (90% of equilibrium), whereas the PEI@PAA aerogel achieves this within merely 4 hours, demonstrating a pronounced kinetic advantage.\u003c/p\u003e \u003cp\u003eThe adsorption kinetics were analyzed by fitting the experimental data to three prevalent kinetic models: the pseudo-first-order (PFO), pseudo-second-order (PSO), and Weber-Morris intraparticle diffusion models. As summarized in Fig. S9 and Tables S8\u0026thinsp;~\u0026thinsp;S9, the PSO model yielded a higher correlation coefficient (\u003cem\u003eR\u003c/em\u003e\u003csup\u003e2\u003c/sup\u003e\u0026thinsp;=\u0026thinsp;0.95) compared to the PFO model (\u003cem\u003eR\u003c/em\u003e\u003csup\u003e2\u003c/sup\u003e\u0026thinsp;=\u0026thinsp;0.91), suggesting that chemisorption is likely the rate-controlling step [\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e]. The adsorption kinetics were further analyzed using the Weber-Morris intraparticle diffusion model, which typically delineates the process into three consecutive stages: the initial rapid surface adsorption stage (\u003cem\u003ek\u003c/em\u003e\u003csub\u003e3\u003c/sub\u003e\u0026thinsp;=\u0026thinsp;4.35 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e\u0026middot;h\u003csup\u003e\u0026minus;\u0026thinsp;0.5\u003c/sup\u003e), the gradual intraparticle diffusion stage (\u003cem\u003ek\u003c/em\u003e\u003csub\u003e3\u003c/sub\u003e\u0026thinsp;=\u0026thinsp;0.49 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e\u0026middot;h\u003csup\u003e\u0026minus;\u0026thinsp;0.5\u003c/sup\u003e), and the final adsorption equilibrium stage (\u003cem\u003ek\u003c/em\u003e\u003csub\u003e3\u003c/sub\u003e\u0026thinsp;=\u0026thinsp;0.15 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e\u0026middot;h\u003csup\u003e\u0026minus;\u0026thinsp;0.5\u003c/sup\u003e). As illustrated in the structural schematic (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e5\u003c/span\u003ea), the three-dimensional network of interconnected supermacro pores within the aerogel provides efficient mass transport channels for iodine molecules. This unique porous architecture is responsible for the remarkably high diffusion rate observed in the initial stage. During the subsequent intraparticle diffusion stage, the abundant amino groups (RNH\u003csub\u003e2\u003c/sub\u003e) grafted onto the pore surfaces of PEI@PAA facilitate rapid chemical capture (chemisorption) of iodine molecules, contributing to the overall high adsorption efficiency and kinetics [\u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e47\u003c/span\u003e].\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec7\" class=\"Section3\"\u003e \u003ch2\u003e2.2.3 Adsorption Isotherms\u003c/h2\u003e \u003cp\u003eThe adsorption isotherms of the PEI@PAA aerogel for gaseous iodine are presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e4\u003c/span\u003ef. The adsorption capacity increased rapidly with rising equilibrium concentration before gradually leveling off and eventually reaching saturation, indicating a typical monolayer adsorption profile. As shown in Fig. S10 and summarized in Table S11, the experimental data at all three temperatures (80, 100 and 120 ℃) were better described by the Freundlich model, with correlation coefficients (\u003cem\u003eR\u003c/em\u003e\u003csup\u003e2\u003c/sup\u003e) of 0.95, 0.91 and 0.94, respectively. In contrast, the Langmuir model exhibited relatively lower correlation coefficients (\u003cem\u003eR\u003c/em\u003e\u003csup\u003e2\u003c/sup\u003e\u0026thinsp;=\u0026thinsp;0.87, 0.79, and 0.86 at 80, 100, and 120\u0026deg;C, respectively; Table S10). The Temkin model provided a good fit only at 80\u0026deg;C (\u003cem\u003eR\u003c/em\u003e\u003csup\u003e2\u003c/sup\u003e\u0026thinsp;=\u0026thinsp;0.95), whereas its fitting performance was poor at the higher temperatures of 100 and 120\u0026deg;C (Table S12).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe Langmuir model describes adsorption on a homogeneous surface, whereas the Freundlich and Temkin models are typically applied to heterogeneous surface adsorption [\u003cspan citationid=\"CR48\" class=\"CitationRef\"\u003e48\u003c/span\u003e]. The superior fit of the Freundlich and Temkin models therefore suggests that iodine adsorption onto the PEI@PAA aerogel occurs on a heterogeneous surface, characterized by active sites with a distribution of adsorption energies. This heterogeneity can likely be attributed to the varying affinities and steric accessibility of the different amino groups within the grafted PEI chains toward iodine molecules.\u003c/p\u003e \u003cp\u003eAs illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e5\u003c/span\u003eb, the PEI@PAA aerogel demonstrates a superior iodine adsorption capacity of 6.01 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, which is notably higher than that of many other types of adsorbents. A comparative summary of the chemical reagents required for synthesizing various iodine adsorbents is provided in Table \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e. It reveals that key reagents such as silver nitrate for silver-based adsorbents and the organic ligands for constructing covalent organic frameworks (COFs) incur substantially higher material costs. In stark contrast, the PEI@PAA aerogel is fabricated from low-cost AA and PEI. Furthermore, its synthesis features mild reaction conditions, straightforward procedures, and low energy consumption, all of which are favorable factors for scalable manufacturing. As demonstrated in Fig. S14, the kilogram-scale rapid preparation of PEI@PAA aerogel monoliths with dimensions of 50 cm (L) \u0026times; 35 cm (W) \u0026times; 4 cm (H) has been achieved at the laboratory scale. This result preliminarily verifies the potential of the PEI@PAA aerogel for scalable manufacturing.\u003c/p\u003e \u003c/div\u003e \u003c/div\u003e \u003cdiv id=\"Sec8\" class=\"Section2\"\u003e \u003ch2\u003e2.3 Adsorption mechanism\u003c/h2\u003e \u003cp\u003eFollowing iodine adsorption, the intensity of the XRD diffraction peak for the PEI@PAA aerogel at approximately 22\u0026deg; decreases markedly (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e6\u003c/span\u003ea). This observation can be ascribed to segmental disorder induced by the incorporation of I\u003csub\u003e2\u003c/sub\u003e molecules into the polymer network [\u003cspan citationid=\"CR49\" class=\"CitationRef\"\u003e49\u003c/span\u003e]. Concurrently, the diffraction peak shifts to a higher angle (ca. 24\u0026deg;). This shift is likely due to the formation of N\u003csup\u003e+\u003c/sup\u003e-I\u003csup\u003e\u0026minus;\u003c/sup\u003e charge-transfer complexes between I₂ and the amino groups, which reduces the interchain spacing [\u003cspan citationid=\"CR50\" class=\"CitationRef\"\u003e50\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eIn the FT-IR spectrum after adsorption, the intensity of the N-H bending vibration peak located at 1560 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e is notably reduced (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e6\u003c/span\u003eb). This attenuation indicates a strong interaction between the amino groups and the adsorbed iodine molecules [\u003cspan citationid=\"CR49\" class=\"CitationRef\"\u003e49\u003c/span\u003e]. A significant weight loss appears in the TGA curve of PEI@PAA-I\u003csub\u003e2\u003c/sub\u003e within the temperature range of 150\u0026thinsp;~\u0026thinsp;300\u0026deg;C, which corresponds to the desorption process of iodine (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e6\u003c/span\u003ec). The C 1s XPS spectrum in Figure d shows that after PEI@PAA adsorbed I₂, the binding energies of the characteristic peaks of C-C, C-O and C\u0026thinsp;=\u0026thinsp;O all shifted positively by approximately 0.6\u0026thinsp;~\u0026thinsp;0.7 eV. Especially, the C-C peak moved from 283.71 eV to 284.38 eV, which directly confirmed that the iodine species had a strong chemical interaction with the surface functional groups of the material, resulting in a decrease in the electron cloud density around the carbon atoms (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e6\u003c/span\u003ed). The O 1s XPS spectrum in Figure e shows that after adsorbing I₂, the main peak binding energy of PEI@PAA significantly shifted from 530.32 eV to 531.38 eV, indicating a decrease in the electron cloud density around the oxygen atoms. This confirms that iodine has a strong chemical interaction with the oxygen-containing functional groups in the material (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e6\u003c/span\u003ee). The high-resolution N 1s XPS spectrum reveals that the binding energy shifts from 398.82 eV to 399.98 eV after iodine adsorption (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e6\u003c/span\u003ef). This positive shift implies a decrease in electron density around the N atoms, consistent with electron transfer [\u003cspan citationid=\"CR51\" class=\"CitationRef\"\u003e51\u003c/span\u003e]. Concurrently, the appearance of characteristic peaks for I 3d\u003csub\u003e5\u003c/sub\u003e/\u003csub\u003e2\u003c/sub\u003e and I 3d\u003csub\u003e3\u003c/sub\u003e/\u003csub\u003e2\u003c/sub\u003e (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e4\u003c/span\u003ee) confirms the presence of iodine species on the adsorbent. Together, these results suggest that charge transfer occurs from the lone pair electrons of the amino N atoms to the adsorbed iodine molecules. The transferred charge can subsequently facilitate the formation of polyiodide species (I- 3and I- 5) with neighboring iodine molecules [\u003cspan citationid=\"CR52\" class=\"CitationRef\"\u003e52\u003c/span\u003e]. Raman spectroscopy further corroborates the XPS findings. As shown in Fig. S11, the spectrum of PEI@PAA-I\u003csub\u003e2\u003c/sub\u003e exhibits characteristic peaks not only for molecular iodine (I\u003csub\u003e2\u003c/sub\u003e) at 159 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e but also for polyiodide species, specifically I- 3 at 109 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and I- 5 at 158 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e [\u003cspan citationid=\"CR53\" class=\"CitationRef\"\u003e53\u003c/span\u003e]. Collectively, the spectroscopic evidence confirms\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003ethat the adsorbed iodine exists within the PEI@PAA aerogel in multiple forms, including molecular iodine (I\u003csub\u003e2\u003c/sub\u003e) and polyiodide anions (I- 3 and I- 5).\u003c/p\u003e \u003cp\u003eThe above conclusions regarding the adsorption mechanism were further verified through density functional theory (DFT) calculations. To elucidate this at the molecular level, a simplified molecular model of the PEI@PAA aerogel was constructed, and its electrostatic potential (ESP) distribution was calculated (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e6\u003c/span\u003eg). The calculated ESP map revealed that regions proximal to the N-containing functional groups (RNH\u003csub\u003e2\u003c/sub\u003e, R\u003csub\u003e2\u003c/sub\u003eNH, R\u003csub\u003e3\u003c/sub\u003eN) all exhibit relatively low ESP values. The binding energies between I\u003csub\u003e2\u003c/sub\u003e and these different active sites were then calculated (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e6\u003c/span\u003eh, Table S7). Interestingly, the secondary amine site exhibits the highest binding energy with I\u003csub\u003e2\u003c/sub\u003e (-22.78 kJ\u0026middot;mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e), a finding that appears inconsistent with the amide group possessing the most negative ESP. This apparent discrepancy can be rationalized by considering the distinct electronic structures. For the amide group, the conjugation effect between the lone pair electrons on the N atom and the adjacent carbonyl (C\u0026thinsp;=\u0026thinsp;O) group delocalizes the electron density, thereby reducing the local electron cloud density and nucleophilic reactivity of the N lone pair towards I\u003csub\u003e2\u003c/sub\u003e [\u003cspan citationid=\"CR54\" class=\"CitationRef\"\u003e54\u003c/span\u003e]. In contrast, the secondary amine, while having a less negative ESP, does not experience such pronounced electron delocalization. Furthermore, the electron-withdrawing nature of the nearby amide group may create an electron buffer effect, polarizing and enhancing the electron-donating ability of the adjacent secondary amine, ultimately strengthening its interaction with I\u003csub\u003e2\u003c/sub\u003e [\u003cspan citationid=\"CR55\" class=\"CitationRef\"\u003e55\u003c/span\u003e]. The weak interaction analysis (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e6\u003c/span\u003ei) indicates that the interaction between I\u003csub\u003e2\u003c/sub\u003e and active sites is mainly electrostatic, and adjacent amino groups can synergistically enhance the adsorption of I\u003csub\u003e2\u003c/sub\u003e.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec9\" class=\"Section2\"\u003e \u003ch2\u003e2.4 Radiation resistance performance\u003c/h2\u003e \u003cp\u003eRadioactive isotopes of iodine, such as \u003csup\u003e131\u003c/sup\u003eI and \u003csup\u003e129\u003c/sup\u003eI, emit high-energy radiation during their radioactive decay. During its decay, \u003csup\u003e131\u003c/sup\u003eI undergoes β decay to form stable \u003csup\u003e131\u003c/sup\u003eXe [\u003cspan citationid=\"CR56\" class=\"CitationRef\"\u003e56\u003c/span\u003e], releasing β particles with a maximum energy of 0.606 MeV and an average energy of 0.192 MeV [\u003cspan citationid=\"CR57\" class=\"CitationRef\"\u003e57\u003c/span\u003e]. This process is also accompanied by the emission of γ photons. The most abundant γ photon emitted has an energy of 364 keV, with an emission probability of 81.2% [\u003cspan citationid=\"CR58\" class=\"CitationRef\"\u003e58\u003c/span\u003e]. Similarly, the long-lived isotope \u003csup\u003e129\u003c/sup\u003eI decays via β emission to \u003csup\u003e129\u003c/sup\u003eXe. This high-energy radiation can induce ionization and excitation within the adsorbent material, potentially leading to radiation damage. Such damage may manifest as alterations in molecular structure, degradation of functional groups, and a consequent decline in adsorption performance [\u003cspan citationid=\"CR59\" class=\"CitationRef\"\u003e59\u003c/span\u003e]. Consequently, for prospective applications in radioactive environments, evaluating the radiation resistance of PEI@PAA aerogels is of paramount importance.\u003c/p\u003e \u003cp\u003eAs shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e7\u003c/span\u003ea, exposure to β and γ irradiation induced a color change in the aerogel samples, which became light yellow. SEM characterization reveals that the macropore size and wall thickness of the PEI@PAA aerogel remained largely unchanged after irradiation, thereby preserving the integrity of its three-dimensional porous network (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e7\u003c/span\u003eb\u0026thinsp;~\u0026thinsp;g). Furthermore, the EDS elemental mapping (Fig. S12) demonstrated a homogeneous distribution of C, N, and O within the pore structure of PEI@PAA-β and PEI@PAA-γ. The elemental compositions, particularly the N content, showed negligible variation (PEI@PAA: 18.2%; PEI@PAA-β: 18.88%; PEI@PAA-γ: 20.03%), indicating no significant elemental loss or redistribution occurred due to the irradiation. Collectively, these structural and compositional analyses confirm the excellent radiation-resistant stability of the PEI@PAA aerogel, which is attributed to the inherent radiation resistance of the PEI polymer matrix.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe iodine adsorption performance of the irradiated samples was evaluated. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e7\u003c/span\u003eh, the irradiated PEI@PAA-β and PEI@PAA-γ samples retained high adsorption capacities of 5.28 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 5.14 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively. The robust 3D framework and highly cross-linked network of the PEI@PAA aerogel contribute to its radiation tolerance by mitigating damage to the active sites and preserving the structural integrity upon irradiation. FT-IR spectrum confirmed that the persistence of the characteristic peaks associated with amides at 1310 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, 1560 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, 1650 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and the characteristic peak of amino groups at 3420 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e in the PEI@PAA aerogel after irradiation, although with a reduction in their intensities (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e7\u003c/span\u003ei). Figure\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e7\u003c/span\u003el shows that, the N 1s binding energy shifted from 398.82 eV to 399.55 eV after β irradiation, indicating a loss of electrons density around the N atoms. Similarly, Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e7\u003c/span\u003eo shows that after γ irradiation, the binding energy of N 1s increased from 398.82 eV to 399.94 eV, which also indicates that γ rays caused N to lose electrons. These spectroscopic analyses collectively indicate that irradiation induces partial chemical conversion of the amino groups, which is likely responsible for the observed slight decrease in the iodine adsorption capacity of the PEI@PAA aerogel [\u003cspan citationid=\"CR60\" class=\"CitationRef\"\u003e60\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eFor comparison, the iodine adsorbent BiMgO-2MBD from a previous study was subjected to identical irradiation conditions, and its post-irradiation adsorption capacity was subsequently measured [\u003cspan citationid=\"CR61\" class=\"CitationRef\"\u003e61\u003c/span\u003e]. The pristine adsorption capacity of the BiMgO-2MBD adsorbent was 5.15 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e at 150\u0026deg;C. After irradiation, the capacities of BiMgO-2MBD-β and BiMgO-2MBD-γ decreased to 3.68 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 2.16 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively (Fig. S13), corresponding to significant reduction of 28.5% and 58.1% relative to the pristine material. This substantial reduction of capacities can be attributed to the powdered morphology of BiMgO-2MBD, leading to its active groups being more susceptible to radiation damage. In contrast, the spatial network framework of the PEI@PAA aerogel enhances the integrity of the material and reduces radiation damage to the active groups. The monolithic structure of the PEI@PAA aerogel makes it more conducive to resisting the effects of radiation.\u003c/p\u003e \u003c/div\u003e"},{"header":"3. Conclusions","content":"\u003cp\u003eIn this work, a 3D interconnected porous PEI@PAA aerogel was successfully fabricated via a facile cryo-polymerization strategy for efficient gaseous iodine capture. By inducing solvent crystallization and enabling simultaneous in situ polymerization and crosslinking, this approach eliminates the reliance on energy-intensive freeze-drying, thereby significantly reducing the preparation cost. The unique 3D continuous macro porous architecture of the aerogel provides efficient mass transfer pathways, enabling the adsorption process to reach 90% of its equilibrium capacity within merely 4 h. Concurrently, the high grafting density of PEI provides an abundance of active sites, endowing the aerogel with an exceptional equilibrium iodine adsorption capacity of up to 6.01 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. Notably, systematic irradiation tests demonstrated that the PEI@PAA aerogel maintained its core porous framework and retained a high iodine adsorption capacity (5.14\u0026thinsp;~\u0026thinsp;5.28 g\u0026middot;g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) after exposure to β and γ irradiation. This confirms its excellent structural stability and radiation resistance, fulfilling a key prerequisite for practical deployment in radioactive environments. In summary, the PEI@PAA aerogel synergistically integrates outstanding iodine adsorption capacity, rapid adsorption kinetics, cost-effectiveness, excellent stability, and remarkable radiation resistance. Coupled with its demonstrated capability for scalable production, this material demonstrates great promise as a high-performance aerogel-based adsorbent for the capture of radioactive iodine.\u003c/p\u003e"},{"header":"4. Experimental","content":"\u003cdiv id=\"Sec12\" class=\"Section2\"\u003e \u003ch2\u003e4.1 Methods\u003c/h2\u003e \u003cdiv id=\"Sec13\" class=\"Section3\"\u003e \u003ch2\u003e4.1.1 Synthesis of PAA matrix and non-porous PAA-T\u003c/h2\u003e \u003cp\u003eA porous PAA matrix was prepared via cryo-polymerization and denoted as PAA. As a contrast, a non-porous PAA matrix was prepared via room-temperature polymerization and denoted as PAA-T.\u003c/p\u003e \u003cp\u003eAA monomer solution and MBA crosslinker were first pre-mixed at 0\u0026deg;C. Subsequently, APS solution (initiator) and VC solution (co-initiator) were added sequentially to the mixture under continuous stirring. After thorough homogenization, the mixture was promptly transferred into two silicone molds (dimension: length \u0026times; width \u0026times; height\u0026thinsp;=\u0026thinsp;60 mm \u0026times; 30 mm \u0026times; 40 mm). The mass concentrations of each component in the reaction solution were as follows: AA (8\u0026thinsp;~\u0026thinsp;10%), MBA (1.6\u0026thinsp;~\u0026thinsp;2%), APS (0.0825%), and VC (0.056%).\u003c/p\u003e \u003cp\u003eOne silicone mold of the mixed solution was immediately transferred to a -20\u0026deg;C freezer to rapidly freeze and crystallize the solvent. Polymerization was then allowed to proceeded at -20\u0026deg;C for 12 h. Subsequently, the resulting polymer was demolded, thoroughly washed with deionized water, and dried under ambient temperature and pressure to yield the porous PAA matrix. The other silicone mold was polymerized at ambient temperature and pressure for 12 h. After demolding, it underwent identical washing and drying procedures to obtain the non-porous PAA-T matrix.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec14\" class=\"Section3\"\u003e \u003ch2\u003e4.1.2 PEI@PAA synthesis of aerogels\u003c/h2\u003e \u003cp\u003eThe PEI@PAA aerogel was synthesized by grafting PEI onto the PAA matrix via an EDC/NHS-mediated amidation reaction. PAA matrix (0.2 g, dry weight), NHS (0.01 g), EDC (0.01 g), and deionized water (10 mL) were sequentially added to a sample vial. The mixture was sonicated for 15 min to ensure complete dispersion. Subsequently, PEI (1.2 g) was added, followed by another 15-min sonication. The mixture was then transferred to a water bath and reacted at 60\u0026deg;C for 9 h. After the reaction, the solution was decanted, and the product was thoroughly washed with deionized water. Finally, the product was dried under ambient conditions, yielding the white, monolithic PEI@PAA aerogel.\u003c/p\u003e \u003cp\u003eDetailed characterization methods and computational details for the density functional theory (DFT) calculations are provided in the Supporting Information.\u003c/p\u003e \u003c/div\u003e \u003c/div\u003e \u003cdiv id=\"Sec15\" class=\"Section2\"\u003e \u003ch2\u003e4.2 Iodine Adsorption Experiments\u003c/h2\u003e \u003cp\u003eDetailed experimental parameters and results regarding the determination of adsorption capacity, batch adsorption experiments, adsorption kinetics, and fitting of adsorption isotherms as well as data processing can be found in the Supporting Information.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec16\" class=\"Section2\"\u003e \u003ch2\u003e4.3 Radiation Resistance Tests\u003c/h2\u003e \u003cp\u003eThe PEI@PAA aerogel and the reference iodine adsorbent BiMgO-2MBD [\u003cspan citationid=\"CR61\" class=\"CitationRef\"\u003e61\u003c/span\u003e] were irradiated with β and γ rays at a total dose of 50 kGy. The resulting samples were designated as PEI@PAA-β, PEI@PAA-γ, BiMgO-2MBD-β, and BiMgO-2MBD-γ, respectively. The irradiated materials were then characterized by FT-IR, SEM, XPS, and iodine adsorption performance tests.\u003c/p\u003e \u003c/div\u003e"},{"header":"Declarations","content":" \u003cp\u003e \u003cstrong\u003eConflict of Interest\u003c/strong\u003e \u003cp\u003eThe authors declare no interest conflict. They have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.\u003c/p\u003e \u003c/p\u003e\u003ch2\u003eFunding\u003c/h2\u003e \u003cp\u003eThis work was supported by National Natural Science Foundation of China (22476010), Higher Education Research Project of the Education Department of Guangdong Province (2024ZDZX3015) and State Key Laboratory for Modification of Chemical Fibers and Polymer Materials (KF2212).\u003c/p\u003e\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eMeng Ji : Writing - original draft, Methodology, Formal analysis, Visualization，Data curation. Dagang Li : Methodology, Formal analysis, Writing - review \u0026amp; editing. Zilei Zhang : Data curation, Formal analysis. Haocun Tan : Writing - review \u0026amp; editing, Software. Xiyue Zhang : Software, Data curation. Yingjun Dong : Data curation, Investigation. Chuanle Lu : Data curation, Investigation. Jinying Li : Supervision, Project administration. Dongxiang Zhang : Writing - review \u0026amp; editing, Funding acquisition, Resources.\u003c/p\u003e\u003ch2\u003eAcknowledgement\u003c/h2\u003e\u003cp\u003eThis work was supported by National Natural Science Foundation of China (22476010), Higher Education Research Project of the Education Department of Guangdong Province (2024ZDZX3015) and State Key Laboratory for Modification of Chemical Fibers and Polymer Materials (KF2212).\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eYang X, Cai B, Xue Y (2022) Review on Optimization of Nuclear Power Development: A Cyber-Physical-Social System in Energy Perspective. 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J Hazard Mater 474:134688. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.jhazmat.2024.134688\u003c/span\u003e\u003cspan address=\"10.1016/j.jhazmat.2024.134688\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"advanced-composites-and-hybrid-materials","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"achm","sideBox":"Learn more about [Advanced Composites and Hybrid Materials](https://link.springer.com/journal/42114)","snPcode":"42114","submissionUrl":"https://submission.nature.com/new-submission/42114/3","title":"Advanced Composites and Hybrid Materials","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"Radioactive iodine capture, Radiation-resistant adsorbents, aerogel, cryo-polymerization, nuclear waste management","lastPublishedDoi":"10.21203/rs.3.rs-8836259/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-8836259/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eEfficient capture of radioactive gaseous iodine is crucial for the safe management of nuclear waste. However, most existing adsorbents suffer from low capacity, slow kinetics, high cost, or poor radiation stability. Herein, a simple aqueous cryo-polymerization strategy was developed to construct a polyethyleneimine-functionalized poly (acrylic acid) aerogel (PEI@PAA), enabling simultaneous ice-templated macropore formation, in-situ polymerization, and crosslinking. The resulting aerogel features a highly interconnected three-dimensional (3D) macroporous network (10~100 μm), which facilitates the rapid diffusion of iodine vapor. Meanwhile, abundant amino groups (RNH2, R2NH, R3N) act as chemical adsorption sites through charge-transfer interactions. The PEI@PAA aerogel exhibits an exceptionally high iodine uptake of 6.01 g·g-1 and achieves 90% of its saturation capacity within 4 h, which demonstrates a 10-fold kinetic enhancement over that of Ag-loaded zeolites. Benefiting from the robust gel network and continuous pore structure, the aerogel maintains a high capacity of 5.14~5.28 g·g-1 after exposure to 50 kGy of β/γ irradiation, with negligible structural degradation. This green and energy-efficient method eliminates the need for freeze-drying, offering a scalable and sustainable platform for the next generation of iodine adsorbents in nuclear waste treatment.\u003c/p\u003e","manuscriptTitle":"A radiation-resistant supermacroporous aerogel for ultrafast and high-capacity gaseous iodine capture","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2026-03-02 19:29:24","doi":"10.21203/rs.3.rs-8836259/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Revision requested","date":"2026-03-30T03:05:50+00:00","index":"","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2026-03-23T08:28:40+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2026-03-19T11:54:52+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"202965469105126481916865189541047756631","date":"2026-02-28T14:32:31+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"273248870373137113490531377782697617632","date":"2026-02-25T01:31:41+00:00","index":"hide","fulltext":""},{"type":"reviewersInvited","content":"","date":"2026-02-23T13:15:04+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2026-02-13T14:52:28+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2026-02-12T12:36:44+00:00","index":"","fulltext":""},{"type":"submitted","content":"Advanced Composites and Hybrid Materials","date":"2026-02-10T04:17:13+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"advanced-composites-and-hybrid-materials","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"achm","sideBox":"Learn more about [Advanced Composites and Hybrid Materials](https://link.springer.com/journal/42114)","snPcode":"42114","submissionUrl":"https://submission.nature.com/new-submission/42114/3","title":"Advanced Composites and Hybrid Materials","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"0a3b9df3-5f80-4caf-8471-d582e498f6c1","owner":[],"postedDate":"March 2nd, 2026","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[],"tags":[],"updatedAt":"2026-05-11T09:55:34+00:00","versionOfRecord":[],"versionCreatedAt":"2026-03-02 19:29:24","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-8836259","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-8836259","identity":"rs-8836259","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}