Fabrication and Characterization of Humic Acid-Modified Fe 3 O 4 /Waterborne Polyurethane Nanocomposite Emulsions

Fabrication and Characterization of Humic Acid-Modified Fe 3 O 4 /Waterborne Polyurethane Nanocomposite Emulsions | 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 Fabrication and Characterization of Humic Acid-Modified Fe 3 O 4 /Waterborne Polyurethane Nanocomposite Emulsions lei lin, Xiaofen Zhao, Zemin He, Xiangbo Feng, Zongcheng Miao, and 1 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8832982/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted 4 You are reading this latest preprint version Abstract Humic acid (HA)-modified Fe 3 O 4 /waterborne polyurethane (HA-FWPU) nanocomposite emulsions were successfully fabricated via a dual-modification strategy. Isophorone diisocyanate (IPDI), polycaprolactone diol (PCL-1000), and 2,2-bis(hydroxymethyl)propionic acid (DMPA) served as the primary reactants, while HA and nano-Fe 3 O 4 were incorporated as functional modifiers. The optimal modifier content was systematically determined. Comprehensive characterization revealed that HA significantly reduced the average emulsion particle size and improved colloidal stability. Fe 3 O 4 nanoparticles were surface-functionalized with (3-isocyanatopropyl)triethoxysilane (IPTS) to enhance compatibility and dispersibility within the polyurethane matrix. The incorporation of nano-Fe 3 O 4 not only improved the mechanical properties and thermal stability of the films but also imparted notable electrical conductivity and magnetic responsiveness. At an optimal Fe 3 O 4 loading of 2.0 wt%, the HA-FWPU3 film exhibited a tensile strength of 23.01 MPa—a 67.7% increase over the unmodified counterpart and a saturation magnetization of 6.01 emu/g. This work presents a feasible approach to designing multifunctional waterborne polyurethane composites for potential applications in electromagnetic shielding, sensors, and functional coatings. Waterborne polyurethane Organic-inorganic modification Humic acid Fe3O4 Nanocomposite Magnetic properties Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Figure 8 Figure 9 1. Introduction Waterborne polyurethane (WPU) has emerged as an environmentally benign alternative to solvent-based polyurethanes, employing water as the dispersion medium to significantly reduce volatile organic compounds (VOCS) [ 1 – 5 ] . Owing to its low toxicity, biocompatibility, and versatile processability, WPU is widely utilized in coatings, adhesives, textile finishing, and biomedical applications [ 6 – 11 ] . However, its practical deployment is often constrained by inherent limitations such as poor water resistance, moderate mechanical strength, and limited functionality [ 12 – 15 ] . To address these shortcomings, researchers have explored various modification strategies, including the incorporation of organic and inorganic fillers, to enhance the comprehensive performance and expand the application scope of WPU [ 16 – 20 ] . Among inorganic modifiers, magnetic Fe 3 O 4 nanoparticles have attracted considerable attention due to their superparamagnetic behavior, high surface area, and unique electronic properties [ 21 – 23 ] . These features make them promising candidates for developing polymer composites with tailored electromagnetic characteristics, suitable for electromagnetic interference (EMI) shielding, wave-absorbing materials, and sensors [ 24 – 26 ] . Nevertheless, the high density, strong aggregation tendency, and lack of surface functional groups of Fe 3 O 4 nanoparticles often lead to poor dispersion and phase separation within polymer matrices, compromising the stability and performance of the resulting composites [ 27 ] . Therefore, improving the interfacial compatibility between Fe 3 O 4 and the WPU matrix remains a critical challenge. Humic acid (HA), a natural macromolecule derived from lignite, is rich in reactive functional groups such as carboxyl (-COOH), hydroxyl (-OH), and aromatic rings [ 28 ] . Its incorporation into polymer systems can enhance emulsion stability, mechanical reinforcement, and thermal resistance, while offering a cost-effective and sustainable modification pathway [ 29 ] . Previous studies have demonstrated that HA can act as a cross-linking agent and stabilizer in WPU systems, improving both colloidal and mechanical properties [ 30 ] . In this study, we propose a synergistic modification strategy to fabricate high-performance HA-FWPU magnetic nanocomposite emulsions. Fe 3 O 4 nanoparticles were first surface-functionalized with IPTS to introduce reactive isocyanate groups, enabling covalent integration into the WPU network during prepolymerization. Simultaneously, HA was incorporated as a hydrophilic cross-linker to enhance emulsion stability and interfacial adhesion. The effects of HA and surface-modified Fe 3 O 4 on the emulsion properties, film morphology, mechanical performance, thermal stability, and magnetic behavior were systematically investigated. The optimized composite exhibited significantly enhanced mechanical strength and magnetic responsiveness, demonstrating its potential as a multifunctional material for advanced applications. 2. Experimental 2.1 Materials Polycaprolactone diol (PCL, Mₙ= 1000 g/mol) was supplied by Jining Baiyi Chemical Co., Ltd. (China). Isophorone diisocyanate (IPDI, 99%) was obtained from Bayer AG. Dibutyltin dilaurate (DBTDL, 95%), triethylamine (TEA, 99%), N-methyl-2-pyrrolidone (NMP, 99%), trimethylolpropane (TMP, 98%), 2,2-bis(hydroxymethyl)propionic acid (DMPA, 98%), and (3-isocyanatopropyl)triethoxysilane (IPTS, 95%) were purchased from Shanghai Macklin Biochemical Co., Ltd. Ferric chloride hexahydrate (FeCl 3 •6H 2 O, 99%), ferrous chloride tetrahydrate (FeCl 2 •4H 2 O, 99%), ammonia solution (25-28%), nitric acid (HNO 3 , 65-68%), hydrochloric acid (HCl, 36-38%), sodium hydroxide (NaOH, 96%), potassium hydroxide (KOH, 85%), and ethanol (99.7%) were provided by Tianjin Comio Chemical Reagent Co., Ltd. Lignite was sourced from Yunnan province. All chemicals were used as received without further purification. Deionized water was used throughout the experiments. 2.2 Methods 2.2.1 Synthesis of Fe 3 O 4 nanoparticles Fe 3 O 4 nanoparticles were synthesized via a co-precipitation method [31] . Briefly, FeCl 2 •4H 2 O and FeCl 3 •6H 2 O(molar ratio 1:2) were dissolved in 100 mL deionized water under vigorous stirring. The solution was heated to 80°C under nitrogen atmosphere, followed by the dropwise addition of ammonia solution to adjust the pH to 9. The reaction was maintained at 80°C for 60 min. The resulting black precipitate was separated magnetically, washed repeatedly with ethanol and deionized water, and dried under vacuum at 40 °C for 12 h. 2.2.2 Surface modification of Fe 3 O 4 with IPTS The as-synthesized Fe 3 O 4 powder (1.5 g) was dispersed in 100 mL toluene via ultrasonication for 30 min. IPTS (6.5 mL) was then added under nitrogen protection. The mixture was refluxed at 130 °C for 60 h with continuous stirring. After cooling to room temperature, the modified nanoparticles (denoted as Fe 3 O 4 -IPTS) were magnetically separated, washed with toluene and acetone, and dried under vacuum at 40 °C for 12 h. 2.2.3 Extraction of humic acid HA was extracted from lignite using an alkaline dissolution-acid precipitation protocol [32] . Briefly, 10 g of nitric acid-oxidized coal powder (120 mesh) was mixed with 100 mL of a 2 wt% mixed alkali solution (KOH:NaOH = 1:1) and stirred at 80 °C for 50 min. The mixture was filtered, and the filtrate was centrifuged at 8000 rpm for 5 min. The supernatant was acidified to pH 3 using HCl, leading to HA precipitation. The precipitate was collected, washed to neutrality, and dried at 50 °C under vacuum for 24 h. 2.2.4 Preparation of HA-FWPU nanocomposite emulsions The HA-FWPU emulsions were synthesized via a prepolymer emulsification method. Fe 3 O 4 -IPTS (varying amounts: 0, 0.5, 1.0, 2.0, and 4.0 wt% relative to total solids) was dispersed in 2 mL NMP via ultrasonication for 15 min. The dispersion was transferred to a three-necked flask equipped with a mechanical stirrer, condenser, and nitrogen inlet. PCL (15.01 g, 15.01 mmol), IPDI (7.48 g, 33.6 mmol), DMPA (1.0 g, 7.46 mmol), and 2-3 drops of DBTDL catalyst were added sequentially. The reaction was carried out at 80 °C for 2 h under nitrogen. HA (0.3g, predetermined as the optimal content based on prior optimization [33] ) was then added, and the reaction continued for another 1 h. The temperature was lowered to 40 °C, and TEA (0.9 g, 8.91 mmol) was added for neutralization. After 30 min, deionized water was added under high-speed stirring to emulsify the prepolymer, yielding an emulsion with 25% solid content. The resulting emulsions were designated as HA-FWPU0, HA-FWPU1, HA-FWPU2, HA-FWPU3, and HA-FWPU4, corresponding to Fe 3 O 4 -IPTS loadings of 0, 0.5, 1.0, 2.0, and 4.0 wt%, respectively. Table 1 Table of different HA-FWPU emulsion formulas Sample raw material /（g/mmol） w (Fe 3 O 4 )/% IPDI PCL DMPA TMP TEA HA HA-FWPU0 7.48/33.6 15.01/15.01 1.0/7.46 0.2/1.49 0.9/8.91 0.3 0 HA-FWPU1 7.48/33.6 15.01/15.01 1.0/7.46 0.2/1.49 0.9/8.91 0.3 0.5 HA-FWPU2 7.48/33.6 15.01/15.01 1.0/7.46 0.2/1.49 0.9/8.91 0.3 1.0 HA-FWPU3 7.48/33.6 15.01/15.01 1.0/7.46 0.2/1.49 0.9/8.91 0.3 2.0 HA-FWPU4 7.48/33.6 15.01/15.01 1.0/7.46 0.2/1.49 0.9/8.91 0.3 4.0 2.2.5 Film preparation The emulsions were cast onto polytetrafluoroethylene plates and dried at room temperature for 5 days, followed by vacuum drying at 50 °C for 24 h. The films were peeled off and stored in a desiccator for further characterization. 2.3 Characterization The morphologies of Fe 3 O 4 and Fe 3 O 4 -IPTS were characterized by scanning electron microscopy (SEM, S4800, Rigaku, Japan) and transmission electron microscopy (TEM, JEM-F200, JEOL, Japan). The FT-IR test was characterized by a Fourier infrared spectrometer (VECTOR-22, Bruker, Germany). The stability of the HA-FWPU emulsion was characterized by a stability tester (Turbiscan Lab, Formulaction, France). The emulsion particle size was characterized by a dynamic laser light scattering instrument (Zetasizer Nano-ZS, Malver, UK). The crystal structures of Fe 3 O 4 , Fe 3 O 4 -IPTS and HA-FWPU films were characterized by X-ray powder diffraction (XRD, CARY 800, Thermo Fisher). The mechanical properties of the HA-FWPU film are characterized by a universal testing machine (XWW-20B, Chengde Jinjian Testing Instrument Co., Ltd., China), the sensor is 500N, and the tensile speed is 20 mm/min. The thermal stability of the film was characterized by a thermogravimetric differential thermal analyzer (Q500, TA Corporation, USA), with a heating rate of 10 °C/min and a temperature range of 25 ~ 600 °C. The magnetic properties of Fe 3 O 4 and HA-FWPU films were characterized by a vibrating sample magnetometer (VSM, 7304, LAKE-SHORE, USA). 3. Results and discussion 3.1 FI-IR analysis Fig. 1. shows the FT-IR spectra of Fe 3 O 4 -IPTS, FPPU, HA, and HA-FWPU。Among them, Fe 3 O 4 -IPTS is used to represent IPTS modified Fe 3 O 4 , and FPPU is used to represent the prepolymer formed by introducing only Fe 3 O 4 without adding HA. In the Fe 3 O 4 -IPTS spectrum, the peak at 576 cm -1 was attributed to the stretching vibration of the Fe-O bond. The characteristic absorption peak of Si-O-Si can be clearly observed at 1055 cm -1 . The strong absorption peak observed at 2270 cm -1 was the characteristic peak of the -NCO group. C-H stretching vibration absorption peaks on -CH 3 and -CH 2 - and stretching vibration peaks of N-H bonds on amino groups were observed at 2930 cm -1 and 3329 cm -1 , respectively [34] . The above analysis shows that Fe 3 O 4 has been successfully modified using IPTS. In the FPPU spectrum, in addition to some characteristic peaks of the WPU prepolymer, the stretching vibration peaks of Fe-O bonds were also observed at 576cm -1 , which indicates that Fe 3 O 4 has been introduced into the aqueous polyurethane system. In addition, a characteristic peak of -NCO was also observed at 2270 cm -1 , which indicates that there was still unreacted -NCO in the FPPU. In the HA spectrum, the broad peak at 3700 ~ 3200cm -1 was due to the stretching vibration of the phenolic hydroxyl group, and the in-plane bending vibration peak of the hydroxyl group was observed at 1370 cm -1 .The C-C stretching vibration peak of benzene ring skeleton appeared at 1600 cm -1 , an in-plane bending vibration peak of C-H was observed at 1240 cm -1 , the peak at 1710 cm -1 was due to the stretching vibration of the C=O double bond of -COOH. Finally, in the HA-FWPU spectrum, the strong peak at 576 cm -1 was attributed to the stretching vibration of the Fe-O bond. In addition, the -NCO characteristic peak at 2270 cm -1 disappeared, it indicates that -NCO from the IPTS and the reactive monomer has been completely reacted by -OH in humic acid. In summary, HA-FWPU magnetic nanocomposites have been successfully prepared. 3.2 TEM analysis of surface modified Fe 3 O 4 Fig. 2-1 shows the TEM image of Fe 3 O 4 and Fe 3 O 4 -IPTS nanoparticles. It can be seen from the figure that the agglomeration of pure Fe 3 O 4 was more serious, but after the surface modification of IPTS, the agglomeration phenomenon between the particles weakens, which also proves that IPTS has been successfully modified on the surface of Fe 3 O 4 . Fig.2-2 was the effect of the dispersibility experiment of Fe 3 O 4 and Fe 3 O 4 -IPTS nanoparticles in ethanol solution. The modification effect of IPTS can be seen intuitively from the figure, which greatly improves the dispersion of Fe 3 O 4 nanoparticles in organic systems. 3.3 HA-FWPU emulsion properties 3.3.1 Emulsion stability analysis The TSI value reflects the degree of stability of the emulsion. The smaller the TSI value, the better the emulsion stability. When the TSI value exceeds 1, the emulsion stability was poor [35] . It can be seen from Fig.3. that compared with WPU, the TSI of HA-FWPU0 modified with HA was decreased by 43.4%, and the stability of the emulsion was significantly improved. It can be seen that the introduction of HA improves the stability of WPU emulsion. In addition, with the introduction of Fe 3 O 4 and the continuous increase of the amount, the TSI index of HA-FWPU emulsion also showed an increasing trend, and the stability of the emulsion gradually decreased. When Fe 3 O 4 was added in a small amount, the TSI index of HA-FWPU emulsion was less than 1, and the emulsion still has good stability. This was attributed to the reactive group -NCO grafted on the surface of Fe 3 O 4 -IPTS particles, which reacts with -OH in the system to graft onto the WPU matrix, emulsifies with WPU, and disperses uniformly. However, when the Fe 3 O 4 addition amount exceeds 2%, the TSI index of the HA-FWPU emulsion will all exceed 1, and the stability of the prepared emulsion was poor. This was due to the fact that agglomeration is easy to occur when the amount of Fe 3 O 4 introduced was too large, and it was easy to separate from the WPU system under the effect of gravity, which eventually leads to poor emulsion stability [36] . 3.3.2 Emulsion particle size analysis Fig. 4. was particle size distribution diagram of a series of HA-FWPU emulsions corresponding to different Fe 3 O 4 additions. It can be seen from the figure that the particle size distribution index of each emulsion shows a continuously increasing trend with the increase of the Fe 3 O 4 addition amount, but all remain within a small value. This shows that the particle size distribution of each emulsion was narrow and the particle size of the emulsion is relatively uniform. This was due to the introduction of HA increased the -COOH content in the prepolymer, making it easier to emulsify and disperse. In addition, as the amount of Fe 3 O 4 added increases, the average particle size of the emulsion also increases. This was due to the increasing amount of nano Fe 3 O 4 added, which will increase its agglomeration effect, and eventually lead to a slight increase in particle size of HA-FWPU emulsion. 3.4 HA-FWPU films properties 3.4.1 SEM analysis Fig. 5 shows the SEM micrographs of the fractured sections of the HA-FWPU film samples. Among them, (a), (b), (c), and (d) represent cross-sectional TEM images of HA-FWPU0, HA-FWPU1, HA-FWPU3, and HA-FWPU4 adhesive films, respectively. It can be seen from the figure that the cross-section of the HA-WPU0 film shown in Fig. 5 (a) is relatively flat, and no nanoparticles are present. Fig.5 (b), Fig.5 (c), and Fig.5 (d) the film cross sections were interspersed with many white particles, and the white particles are Fe 3 O 4 nanoparticles grafted onto the WPU matrix through chemical bonding. Among them, the distribution of white particles in Fig.5 (b) and Fig.5 (c) is relatively uniform, the agglomeration phenomenon is not obvious, and Fig.5 (c) has a lot more white particles than Fig.5 (b). In Fig.5(d), obvious agglomeration of nanoparticles appears. The reason for this phenomenon was that as the amount of Fe 3 O 4 nanoparticles added continues to increase, the number of Fe 3 O 4 nanoparticles present in the section of the film increases. However, when the addition amount exceeds the optimal addition amount (2.0%), the agglomeration of Fe 3 O 4 nanoparticles was severe, which eventually leads to uneven distribution in the cross section. 3.4.2 XRD analysis Fig. 6 shows the XRD patterns of Fe 3 O 4 , Fe 3 O 4 -IPTS and HA-FWPU. Fe 3 O 4 and Fe 3 O 4 -IPTS all show diffraction peaks at 2θ = 30.2, 35.3, 43.2, 53.6, 57.2, and 62.7. These correspond to the (220), (311), (400), (511), and (440) crystal planes in the Fe 3 O 4 cubic lattice, respectively. This shows that the prepared Fe 3 O 4 has a magnetite spinel structure [37] , and the modification of IPTS does not change the crystal structure of Fe 3 O 4 . A new broad absorption peak appears at 2θ = 19.8 in HA-FWPU, which was due to the orderly arrangement of the hard segments of HA-FWPU polymer. In addition, a diffraction peak appears at the same position as Fe 3 O 4 , indicating that Fe 3 O 4 has been introduced into the WPU system. However, the peak intensities were weakened and some of the peak positions are not obvious. This was because Fe 3 O 4 -IPTS was added in a small amount and the broad absorption peak at 2θ = 19.8 also has a certain masking effect on other peaks. 3.4.3 Mechanical performance analysis It can be seen from Fig. 7-1 that the introduction of nano Fe 3 O 4 has a certain degree of influence on the mechanical properties of HA-FWPU film. The specific performance was that with the increasing amount of Fe 3 O 4 added, the tensile strength of HA-FWPU film shows a trend of first increase and then decrease, while the elongation at break decreases. As shown in Fig.7-2 and 7-3, where the Fe 3 O 4 addition amount is 0% (mass fraction, the same applies hereinafter), the minimum tensile strength of the HA-FWPU film is 13.72Mpa and the maximum elongation at break is 1001.02 %；When the added amount of Fe 3 O 4 is 2.0%, the tensile strength of HA-FWPU3 film reaches a maximum of 23.01Mpa and the elongation at break is 671.37%. The change in the tensile strength of the above HA-FWPU film can be attributed to the following two points :(1) Nano-Fe 3 O 4 surface modified by IPTS in polyurethane matrix through strong interfacial force (covalent bond) formed between them, so that it achieves good dispersion in the polyurethane body, the addition of nano-Fe 3 O 4 Improve the tensile strength of Waterborne polyurethane materials. (2) When the amount of nano Fe 3 O 4 introducedwas too large, its large density and nano effect will cause agglomeration, affect its interaction with the polymer, and deteriorate compatibility. When the agglomeration of nanoparticles was severe, fracture stress points will be generated, which will seriously affect the mechanical properties of the polymer and eventually lead to a decrease in tensile strength [38] . In addition, with the continuous increase of the amount of nano Fe 3 O 4 introduced, the breaking elongation of waterborne polyurethane has decreased, and the minimum was 614.83% of HA-FWPU4 (4.0%) film. This effect may be related to the rigidity of the inorganic nanomaterial itself, so the plasticity of the polyurethane material was suppressed to a certain extent, resulting in a continuous decrease in elongation at break. 3.4.4 VSM analysis Fig. 8-1 shows the hysteresis loops of Fe 3 O 4 and Fe 3 O 4 -IPTS. It can be seen from the Figure that with the increase of the magnetic field, the magnetization increases continuously until it reaches the saturation magnetization (Ms). The coercivity (Hc) of both is zero, indicating that the prepared nanoparticles are superparamagnetic [39] . The maximum saturation magnetization of pure Fe 3 O 4 was 62 emu/g, while the maximum saturation magnetization of Fe 3 O 4 modified by IPTS decreased to 41 emu/g, which further indicates that Fe 3 O 4 -IPTS has been successfully obtained. Fig. 8-2 shows the hysteresis loops of HA-FWPU with different Fe 3 O 4 additions. As shown in figure, HA-FWPU with different Fe 3 O 4 additions has excellent magnetic properties. With the increase of Fe 3 O 4 -IPTS, the saturation magnetization of HA-FWPU also increases. When Fe 3 O 4 -IPTS was added in an amount of 2.0%, the saturation magnetization can reach 6.01 emu/g , indicating that the prepared magnetic composite material has excellent magnetic properties. 3.4.5 Thermogravimetric analysis Table 2 TG data of HA-FWPU film with different Fe 3 O 4 -IPTS additions Sample Decomposition temperature / ℃ T 10% T 50% T 90% HA-FWPU0 279.65 313.06 349.13 HA-FWPU1 282.04 322.25 356.01 HA-FWPU2 287.89 324.70 362.13 HA-FWPU3 284.75 324.08 361.32 HA-FWPU4 285.71 341.2 367.94 Thermogravimetry was used to characterize the thermal stability of HA-FWPU film. It can be known from FIG. 9 that the thermal decomposition processes of the respective HA-FWPU films before and after the introduction of Fe 3 O 4 are similar, and they all consist of three weightless stages. Before 200℃, the moisture and organic solvents are volatile and lost, then the decomposition of the hard part of the polymer, and finally the decomposition of the soft part [40] . The decomposition temperature of HA-FWPU film (HA-FWPU1~ 4) with Fe 3 O 4 -IPTS was higher than that of HA-FWPU film (HA-FWPU0) without Fe 3 O 4 -IPTS. On the one hand, the introduction of nano Fe 3 O 4 increases the crosslink density of the polymer. on the other hand, Fe 3 O 4 itself also has good thermal stability. This can also explain that when the temperature reaches 800℃, the adhesive film has not been decomposed 100% (the remaining part was the introduced Fe 3 O 4 ). According to Table 2, when the weight loss rate was 50%, the corresponding thermal decomposition temperatures of HA-FWPU0 and HA-FWPU4 are 313.06℃and 341.2℃, respectively, an increase of 10%, This shows that the introduction of nano Fe 3 O 4 has improved the thermal stability of waterborne polyurethane to a certain extent. 4. Conclusion A novel humic acid-modified Fe 3 O 4 /waterborne polyurethane (HA-FWPU) magnetic nanocomposite emulsion was successfully developed through a dual-modification strategy. Surface functionalization of Fe 3 O 4 with IPTS improved its dispersibility and covalent integration into the WPU matrix, while HA acted as an effective cross-linker and emulsion stabilizer. The optimized composite (2.0 wt% Fe 3 O 4 -IPTS) exhibited a tensile strength of 23.01 MPa, a 67.7% improvement over the unmodified film, along with a saturation magnetization of 6.01 emu/g. The emulsion demonstrated good colloidal stability, and the films showed enhanced thermal resistance. This work provides a sustainable and effective approach to designing multifunctional WPU-based nanocomposites with potential applications in electromagnetic shielding, sensors, functional coatings, and beyond. Declarations CRediT authorship contribution statement Lei Lin: Writing-original draft, Formal analysis, Data curation. Xiaofen Zhao: Writing- original draft, Methodology, Investigation, Formal analysis. Zemin He: Formal analysis, Data curation. Xiangbo Feng: Visualization. Yuzhen Zhao: Writing - review & editing, Writing-original draft, Funding acquisition. Zongcheng Miao: Writing-review & editing, Writing-original draft, Supervision. Declaration of competing interest The authors have no competing financial interests or personal relationships that might be construed as influencing the work reported herein. Acknowledgments This work was sponsored by the National Natural Science Founda-tion of China (52306165), the Scientific and Technical Innovation demonstration project for social development of Xi’an Municipal Bureau of Science and Technology (2024JH-CXSF-0020), the Key R&D Program Project of Xianyang (L2023-ZDYF-QYCX-029), Xi Jing University Research Fund (XJ240211) and the Youth Innovation Team of Shaanxi Universities (23JP186). Data availability Data will be made available on request. References A. Iqbal, P. Sambyal, C.M. Koo, 2D MXenes for electromagnetic shielding: a review, Adv. Funct. Mater. 30 (47) (2020) 2000883. Z.H. Zeng, F.Z. Jiang, Y. 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Zhang, Enhanced microwave absorption of biomass carbon/nickel/polypropylene (C/Ni/PPy) ternary composites through the synergistic effects, J. Alloys Compd. 890 (2022) 161801. Scheme Scheme 1 and 2 are available in the Supplementary Files section. Additional Declarations No competing interests reported. Supplementary Files Scheme1and2.docx Cite Share Download PDF Status: Under Review Version 1 posted Reviewers invited by journal 02 Apr, 2026 Editor assigned by journal 12 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-8832982","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":616641639,"identity":"6e55f8d1-b67b-4799-9a62-9db5d6b1a4cb","order_by":0,"name":"lei 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17:08:55","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-8832982/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-8832982/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":106441105,"identity":"dd9a850e-17ab-42b1-ab05-65f96d4f6bbb","added_by":"auto","created_at":"2026-04-08 14:43:29","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":116165,"visible":true,"origin":"","legend":"\u003cp\u003eFT-IR spectra of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS, FPPU, HA, HA-FWPU\u003c/p\u003e","description":"","filename":"1.png","url":"https://assets-eu.researchsquare.com/files/rs-8832982/v1/41b5df732f1a72c94b9e9d98.png"},{"id":106441098,"identity":"48918623-bb61-45c3-b9c3-99d1fad1c956","added_by":"auto","created_at":"2026-04-08 14:43:27","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":682156,"visible":true,"origin":"","legend":"\u003cp\u003e2-1 The TEM image of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e nanoparticles ,(a)Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e ,(b) Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS\u003c/p\u003e\n\u003cp\u003e2-2 Effect of dispersion experiment\u003c/p\u003e","description":"","filename":"2.png","url":"https://assets-eu.researchsquare.com/files/rs-8832982/v1/9ac54cec17ae47989e99f541.png"},{"id":106441198,"identity":"7c0577a0-1271-48f4-8570-044cd36c6404","added_by":"auto","created_at":"2026-04-08 14:43:42","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":119716,"visible":true,"origin":"","legend":"\u003cp\u003eStability test chart of HA-FWPU emulsion with different Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e additions\u003c/p\u003e","description":"","filename":"3.png","url":"https://assets-eu.researchsquare.com/files/rs-8832982/v1/d0ff1212dbb748f587fc7449.png"},{"id":106441197,"identity":"00218a81-8e9b-4532-9042-fea8db308816","added_by":"auto","created_at":"2026-04-08 14:43:41","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":117629,"visible":true,"origin":"","legend":"\u003cp\u003eParticle size diagram of HA-FWPU emulsion with different Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e additions\u003c/p\u003e","description":"","filename":"4.png","url":"https://assets-eu.researchsquare.com/files/rs-8832982/v1/6e193224cf6a66bc80c7b167.png"},{"id":106441099,"identity":"6be33fc5-3d93-4e58-a197-0de9db168667","added_by":"auto","created_at":"2026-04-08 14:43:27","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":371172,"visible":true,"origin":"","legend":"\u003cp\u003eThe SEM image of HA-FWPU film cross section\u003c/p\u003e","description":"","filename":"5.png","url":"https://assets-eu.researchsquare.com/files/rs-8832982/v1/007a977d082b09304583d21a.png"},{"id":106441200,"identity":"5483da90-460d-4e9e-aad6-b27351befaf2","added_by":"auto","created_at":"2026-04-08 14:43:43","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":115756,"visible":true,"origin":"","legend":"\u003cp\u003eXRD patterns of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4,\u003c/sub\u003e Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS and HA-FWPU\u003c/p\u003e","description":"","filename":"6.png","url":"https://assets-eu.researchsquare.com/files/rs-8832982/v1/2b827d6ed42713058b7c46ce.png"},{"id":106441104,"identity":"2ce8de2a-bb84-4a8c-a618-2621a0fc4668","added_by":"auto","created_at":"2026-04-08 14:43:29","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":111663,"visible":true,"origin":"","legend":"\u003cp\u003e7-1 Stress-strain diagram of HA-FWPU film with different Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e additions\u003c/p\u003e\n\u003cp\u003e7-2 Tensile strength of HA-FWPU film with different Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e additions\u003c/p\u003e\n\u003cp\u003e\u003cimg width=\"313\" height=\"231\" 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K14+J/is/R8k/wBwp/P82FFFFYHqhXo/wg/5jP8AvQ/yavOK9H+EH/MZ/wB6H+TV1YP+IeDxH/uXzR6TRRRXqnwIUUUUAeQfFT/kcYf+vFP/AEOSuOrsfip/yOMP/Xin/oclcdXkYr+Kz9FyL/cKfz/NhRRRXOeuFegfCL/kIav/ANcof5vXn9egfCL/AJCGr/8AXKH+b104T+KeHxF/uL9V+Z6hRRRXrH5+FFFFAHkfxW/5Gu2/68l/9DauLrtPit/yNdt/15L/AOhtXF15GK/is/RMg/3CHz/NhRRRXOewFd78I/8AkM6t/wBe8X/oT1wVd78I/wDkM6t/17xf+hPXThP4qPE4h/3GXqvzPU6KKK9Y/PgooooA8p+LTv8A29pyh3C/ZnOFYgZ3CuFy3/PST/v43+Ndz8Wv+Rh07/r1f/0MVw1eXipyVVpM+9yLD0p4KMpRTd30XcMt/wA9JP8Av43+NGW/56Sf9/G/xoorm9pPuex9UofyL7kGW/56Sf8Afxv8a7j4TO//AAkV+pdyv2UHBYkZ31w9dv8ACf8A5GW+/wCvQf8AoYrows5Oqk2ePnuHpQwMpRgk9Oi7o9ZrD8a/8iRrX/XlL/6Ca3Kw/Gv/ACJGtf8AXlL/AOgmvVPghngP/kQ9C/68ov8A0EUUeA/+RD0L/ryi/wDQRRQAeLVgv9EurRbjTvOi2SNDeuPKb5shZBnIU4//AF1znga2/wCJ608lr4c0+QQsqwaTIHeUZXJfBxtHGPc1d8d2kdvEZ4vDH9rfbpIo7sxH52VWBUEdSOOvbjNVPBVpGviJprXwVJoUS27K88pwXJZcKB3HBP4UID0CiiigAorjPFfiS9ttc0Kz05gltPqcdvcy937lB7ep/D1rC1LxzqMM2qanFMRBp+sxWC2+BteLGHz/ALRPOe2BQB6hXD/GH/kntz/13h/9DFY+o+OdRhl1TU45iINP1mOwW3wNrxYw+f8AaJ5z2wK1/jCQPh5dE9BPD/6GKAO1g/1Ef+6P5VJWBpHjTw9qtxBY2GrW0906/LGrctgZOPwFb9AHi3xI/wCR6uv+uEX8jXMV0/xI/wCR6uv+uEX8jXMV4+J/is/SMk/3Cn8/zYUUUVgeoFek/CH/AFGsf9dY/wD0E15tXpPwh/1Gsf8AXWP/ANBNdWD/AInyPA4k/wBz/wC3l+p6PRRRXqnwQUUUUAeM/Ev/AJHib/r2i/8AZq5Wuq+Jf/I8Tf8AXtF/7NXK14+J/is/R8k/3Cn8/wA2FFFFYHqhXo/wg/5jP+9D/Jq84r0f4Qf8xn/eh/k1dWD/AIh4PEf+5fNHpNFFFeqfAhRRRQB5B8VP+Rxh/wCvFP8A0OSuOrsfip/yOMP/AF4p/wChyVx1eRiv4rP0XIv9wp/P82FFFFc564V6B8Iv+Qhq/wD1yh/m9ef16B8Iv+Qhq/8A1yh/m9dOE/inh8Rf7i/VfmeoUUUV6x+fhRRRQB5H8Vv+Rrtv+vJf/Q2ri67T4rf8jXbf9eS/+htXF15GK/is/RMg/wBwh8/zYUUUVznsBXe/CP8A5DOrf9e8X/oT1wVd78I/+Qzq3/XvF/6E9dOE/io8TiH/AHGXqvzPU6KKK9Y/PgooooA8o+LX/Iw6d/16v/6GK4au5+LX/Iw6d/16v/6GK4avJxf8Vn6Fw/8A7hH1f5hRRRXMe0Fdv8J/+Rlvv+vQf+hiuIrt/hP/AMjLff8AXoP/AEMV0YT+KjxuIP8AcJ/L80es1h+Nf+RI1r/ryl/9BNblYfjX/kSNa/68pf8A0E165+eDPAf/ACIehf8AXlF/6CKKPAf/ACIehf8AXlF/6CKKAJfFq3b+HbgWMl5HINpY2Shp9mfmCA8bsVyngux1Kx8XsmoS+ILhRZlhLfODCNzKVAx/FjgjsQa6XxvbzXHhmYQresUkjkcWJAn2qwJ2Z71wU4v7mDQ459P8Rz6Xb3E1wTdxlpvL2YTft5yHJwDzigD12iobTzPsUHn583y135/vY5/WpqAOH1v4YaZqOqWN5aBoDHe/abkNNI3mgkkhRuwpJPUYp978PVur27QXCLp95qEeozJt+cOo5QdsMcHPbmu1ooA4q8+HqXV7doLhBp95qMeozJtO/eo5QdsMcHPbmo/jDz8PbrP/AD3h/wDQxXc1w/xh/wCSe3P/AF3h/wDQxQB1Fho2mWnlT2unWcMwUYkjgVWGR6gVoVHB/qI/90fyqSgDxb4kf8j1df8AXCL+RrmK6f4kf8j1df8AXCL+RrmK8fE/xWfpGSf7hT+f5sKKKKwPUCvSfhD/AKjWP+usf/oJrzavSfhD/qNY/wCusf8A6Ca6sH/E+R4HEn+5/wDby/U9Hooor1T4IKKKKAPGfiX/AMjxN/17Rf8As1crXVfEv/keJv8Ar2i/9mrla8fE/wAVn6Pkn+4U/n+bCiiisD1Qr0f4Qf8AMZ/3of5NXnFej/CD/mM/70P8mrqwf8Q8HiP/AHL5o9Jooor1T4EKKKKAPIPip/yOMP8A14p/6HJXHV2PxU/5HGH/AK8U/wDQ5K46vIxX8Vn6LkX+4U/n+bCiiiuc9cK9A+EX/IQ1f/rlD/N68/r0D4Rf8hDV/wDrlD/N66cJ/FPD4i/3F+q/M9Qooor1j8/CiiigDyP4rf8AI123/Xkv/obVxddp8Vv+Rrtv+vJf/Q2ri68jFfxWfomQf7hD5/mwooornPYCu9+Ef/IZ1b/r3i/9CeuCrvfhH/yGdW/694v/AEJ66cJ/FR4nEP8AuMvVfmep0UUV6x+fBRRRQB5R8Wv+Rh07/r1f/wBDFcNXc/Fr/kYdO/69X/8AQxXDV5OL/is/QuH/APcI+r/MKKKK5j2grt/hP/yMt9/16D/0MVxFdv8ACf8A5GW+/wCvQf8AoYrown8VHjcQf7hP5fmj1msPxr/yJGtf9eUv/oJrcrD8a/8AIka1/wBeUv8A6Ca9c/PBngP/AJEPQv8Aryi/9BFFHgP/AJEPQv8Aryi/9BFFAEXj+4mtfCNzJbz3sL741LWK5mKlwCE9CR3rl/AE0UniciO78Vzn7M5xrK4jHzL93/a/pXZ+LLm5tPDtxLaSTQsMB5oIvNkiQn5mVe5A/wAe1ct8PdVa+1OaOy1zVNYshGTK97bFBC+RgKx6k88e1CA9CooooAKKKKACuH+MP/JPbn/rvD/6GK7iuG+MQz8PLoA4zNDz/wADFAHawf6iP/dH8qkrI8NaTc6PpfkXeqXWpOzbxLcYyoIHyjHb/GtegDxb4kf8j1df9cIv5GuYrp/iR/yPV1/1wi/ka5ivHxP8Vn6Rkn+4U/n+bCiiisD1Ar0n4Q/6jWP+usf/AKCa82r0n4Q/6jWP+usf/oJrqwf8T5HgcSf7n/28v1PR6KKK9U+CCiiigDxn4l/8jxN/17Rf+zVytdV8S/8AkeJv+vaL/wBmrla8fE/xWfo+Sf7hT+f5sKKKKwPVCvR/hB/zGf8Aeh/k1ecV6P8ACD/mM/70P8mrqwf8Q8HiP/cvmj0miiivVPgQooooA8g+Kn/I4w/9eKf+hyVx1dj8VP8AkcYf+vFP/Q5K46vIxX8Vn6LkX+4U/n+bCiiiuc9cK9A+EX/IQ1f/AK5Q/wA3rz+vQPhF/wAhDV/+uUP83rpwn8U8PiL/AHF+q/M9Qooor1j8/CiiigDyP4rf8jXbf9eS/wDobVxddp8Vv+Rrtv8AryX/ANDauLryMV/FZ+iZB/uEPn+bCiiiuc9gK734R/8AIZ1b/r3i/wDQnrgq734R/wDIZ1b/AK94v/Qnrpwn8VHicQ/7jL1X5nqdFFFesfnwUUUUAeUfFr/kYdO/69X/APQxXDV3Pxa/5GHTv+vV/wD0MVw1eTi/4rP0Lh//AHCPq/zCiiiuY9oK7f4T/wDIy33/AF6D/wBDFcRXb/Cf/kZb7/r0H/oYrown8VHjcQf7hP5fmj1msPxr/wAiRrX/AF5S/wDoJrcrD8a/8iRrX/XlL/6Ca9c/PBngP/kQ9C/68ov/AEEUUeA/+RD0L/ryi/8AQRRQBlazpuq6x4nuYNM8YS6eYo0Js4rYSbAR1JPTPpS+HrDUtL8U/ZdU8T3WpObZmW3ltfKUjK/OrDhsdMdRmqPimHxVLqmqW+i6Lb3VlchMzvceU6uEA+UhgePWrPhT/hJv7Ytodd0a2sbSC3kEUkM3mlmJXhjuJ6DNAHcUUUUAFFQm8tluham4hFwRuERcbyPXHWla6gW4W3aaMTMMiMsNxH060AS1w/xh/wCSe3P/AF3h/wDQxXZm6gW4W3aaMTMMiMsNxH061xnxh/5J7c/9d4f/AEMUAdpB/qI/90fyqSo4P9RH/uj+VSUAeLfEj/kerr/rhF/I1zFdP8SP+R6uv+uEX8jXMV4+J/is/SMk/wBwp/P82FFFFYHqBXpPwh/1Gsf9dY//AEE15tXpPwh/1Gsf9dY//QTXVg/4nyPA4k/3P/t5fqej0UUV6p8EFFFFAHjPxL/5Hib/AK9ov/Zq5Wuq+Jf/ACPE3/XtF/7NXK14+J/is/R8k/3Cn8/zYUUUVgeqFej/AAg/5jP+9D/Jq84r0f4Qf8xn/eh/k1dWD/iHg8R/7l80ek0UUV6p8CFFFFAHkHxU/wCRxh/68U/9Dkrjq7H4qf8AI4w/9eKf+hyVx1eRiv4rP0XIv9wp/P8ANhRRRXOeuFegfCL/AJCGr/8AXKH+b15/XoHwi/5CGr/9cof5vXThP4p4fEX+4v1X5nqFFFFesfn4UUUUAeR/Fb/ka7b/AK8l/wDQ2ri67T4rf8jXbf8AXkv/AKG1cXXkYr+Kz9EyD/cIfP8ANhRRRXOewFd78I/+Qzq3/XvF/wChPXBV3vwj/wCQzq3/AF7xf+hPXThP4qPE4h/3GXqvzPU6KKK9Y/PgooooA8o+LX/Iw6d/16v/AOhiuGrufi1/yMOnf9er/wDoYrhq8nF/xWfoXD/+4R9X+YUUUVzHtBXb/Cf/AJGW+/69B/6GK4iu3+E//Iy33/XoP/QxXRhP4qPG4g/3Cfy/NHrNYfjX/kSNa/68pf8A0E1uVh+Nf+RI1r/ryl/9BNeufngzwH/yIehf9eUX/oIoo8B/8iHoX/XlF/6CKKAN+iiigAooooA4HxJ4Y0678X6TPZLHb3tvdC9vrzfhhGOikk9WOAB2APauS1e7u/s/iC8+b7dF4mhWJv4lCjCge2OPxr0W4+Hvh671o6rc2kkt6ZRMZGnc5YHI4zjAwOK0JvDOlz6kb6S2BmMqTMNx2NIowrlehYDvQB5Vq93d/Z/EF5lvt0PiaFYm/iAXhQPbHH412XxiJHw8uiBk+dDx/wADFdHN4Z0ufUjfSWwMxlWdhuOxpFGFcr0LAd6534w/8k9uf+u8P/oYoAuaB4m13UL+C1vvCl1YW7Kd1y86sq4HHHXnp+NdZUcH+oj/AN0fyqSgDxb4kf8AI9XX/XCL+RrmK6f4kf8AI9XX/XCL+RrmK8fE/wAVn6Rkn+4U/n+bCiiisD1Ar0n4Q/6jWP8ArrH/AOgmvNq9J+EP+o1j/rrH/wCgmurB/wAT5HgcSf7n/wBvL9T0eiiivVPggooooA8Z+Jf/ACPE3/XtF/7NXK11XxL/AOR4m/69ov8A2auVrx8T/FZ+j5J/uFP5/mwooorA9UK9H+EH/MZ/3of5NXnFej/CD/mM/wC9D/Jq6sH/ABDweI/9y+aPSaKKK9U+BCiiigDyD4qf8jjD/wBeKf8AoclcdXY/FT/kcYf+vFP/AEOSuOryMV/FZ+i5F/uFP5/mwooornPXCvQPhF/yENX/AOuUP83rz+vQPhF/yENX/wCuUP8AN66cJ/FPD4i/3F+q/M9Qooor1j8/CiiigDyP4rf8jXbf9eS/+htXF12nxW/5Gu2/68l/9DauLryMV/FZ+iZB/uEPn+bCiiiuc9gK734R/wDIZ1b/AK94v/Qnrgq734R/8hnVv+veL/0J66cJ/FR4nEP+4y9V+Z6nRRRXrH58FFFFAHlHxa/5GHTv+vV//QxXDV3Pxa/5GHTv+vV//QxXDV5OL/is/QuH/wDcI+r/ADCiiiuY9oK7f4T/APIy33/XoP8A0MVxFdv8J/8AkZb7/r0H/oYrown8VHjcQf7hP5fmj1msPxr/AMiRrX/XlL/6Ca3Kw/Gv/Ika1/15S/8AoJr1z88GeA/+RD0L/ryi/wDQRRR4D/5EPQv+vKL/ANBFFAG/RRRQAUUUUAFFFFABXD/GH/kntz/13h/9DFdxXDfGE4+Ht0T/AM94f/QxQB2sH+oj/wB0fyqSqmm31rqFkktlcwXMYAUvDIHAOOmR3q3QB4t8SP8Akerr/rhF/I1zFdP8SP8Akerr/rhF/I1zFePif4rP0jJP9wp/P82FFFFYHqBXpPwh/wBRrH/XWP8A9BNebV6T8If9RrH/AF1j/wDQTXVg/wCJ8jwOJP8Ac/8At5fqej0UUV6p8EFFFFAHjPxL/wCR4m/69ov/AGauVrqviX/yPE3/AF7Rf+zVytePif4rP0fJP9wp/P8ANhRRRWB6oV6P8IP+Yz/vQ/yavOK9H+EH/MZ/3of5NXVg/wCIeDxH/uXzR6TRRRXqnwIUUUUAeQfFT/kcYf8ArxT/ANDkrjq7H4qf8jjD/wBeKf8AoclcdXkYr+Kz9FyL/cKfz/NhRRRXOeuFegfCL/kIav8A9cof5vXn9egfCL/kIav/ANcof5vXThP4p4fEX+4v1X5nqFFFFesfn4UUUUAeR/Fb/ka7b/ryX/0Nq4uu0+K3/I123/Xkv/obVxdeRiv4rP0TIP8AcIfP82FFFFc57AV3vwj/AOQzq3/XvF/6E9cFXe/CP/kM6t/17xf+hPXThP4qPE4h/wBxl6r8z1OiiivWPz4KKKKAPKPi1/yMOnf9er/+hiuGrufi1/yMOnf9er/+hiuGrycX/FZ+hcP/AO4R9X+YUUUVzHtBXb/Cf/kZb7/r0H/oYriK7f4T/wDIy33/AF6D/wBDFdGE/io8biD/AHCfy/NHrNYfjX/kSNa/68pf/QTW5WH41/5EjWv+vKX/ANBNeufngzwH/wAiHoX/AF5Rf+giijwH/wAiHoX/AF5Rf+giigDfooooAKKKKACiiigArhvjEAfh5dA9DPD/AOhiu5rh/jD/AMk9uf8ArvD/AOhigDqNF0fT9FsFg0y0htYn+dliXALEDk/lWhUcH+oj/wB0fyqSgDxb4kf8j1df9cIv5GuYrp/iR/yPV1/1wi/ka5ivHxP8Vn6Rkn+4U/n+bCiiisD1Ar0n4Q/6jWP+usf/AKCa82r0n4Q/6jWP+usf/oJrqwf8T5HgcSf7n/28v1PR6KKK9U+CCiiigDxn4l/8jxN/17Rf+zVytdV8S/8AkeJv+vaL/wBmrla8fE/xWfo+Sf7hT+f5sKKKKwPVCvR/hB/zGf8Aeh/k1ecV6P8ACD/mM/70P8mrqwf8Q8HiP/cvmj0miiivVPgQooooA8g+Kn/I4w/9eKf+hyVx1dj8VP8AkcYf+vFP/Q5K46vIxX8Vn6LkX+4U/n+bCiiiuc9cK9A+EX/IQ1f/AK5Q/wA3rz+vQPhF/wAhDV/+uUP83rpwn8U8PiL/AHF+q/M9Qooor1j8/CiiigDyP4rf8jXbf9eS/wDobVxddp8Vv+Rrtv8AryX/ANDauLryMV/FZ+iZB/uEPn+bCiiiuc9gK734R/8AIZ1b/r3i/wDQnrgq734R/wDIZ1b/AK94v/Qnrpwn8VHicQ/7jL1X5nqdFFFesfnwUUUUAeUfFr/kYdO/69X/APQxXDV3Pxa/5GHTv+vV/wD0MVw1eTi/4rP0Lh//AHCPq/zCiiiuY9oK7f4T/wDIy33/AF6D/wBDFcRXb/Cf/kZb7/r0H/oYrown8VHjcQf7hP5fmj1msPxr/wAiRrX/AF5S/wDoJrcrD8a/8iRrX/XlL/6Ca9c/PBngP/kQ9C/68ov/AEEUUeA/+RD0L/ryi/8AQRRQBv0UUUAFFFFABRRRQBhT+MdLt9Re0keTEdylpJMF/dpM4yqE+vv0GRWJ8Yf+Se3P/XeH/wBDFchqukXpXXdKCOb278RxTwrjlo2ywcewGcntivSfGnhtvFfhqfS0uRbPIyOshXcAVYHp+FAG1B/qI/8AdH8qkrgh4X8eKoA8aw4AwP8AiXpS/wDCM+Pf+h2h/wDBfHQByXxI/wCR6uv+uEX8jXMV3eo/CrxHq1815feKYZbh1Cl/sYGQOnAOKq/8KZ1n/oZIf/AT/wCvXBWws5zck0fW5dn2Hw2GhRnGV12t39TjqK7H/hTOs/8AQyQ/+An/ANej/hTOs/8AQyw/+An/ANes/qVTujs/1nwn8svuX+Zx1ek/CH/Uax/11j/9BNY//CmdZ/6GWH/wE/8Ar1paR8OvFehLMumeLoYRMQZP9CVskcDrW2Hw0qc+ZnmZtnVDG4f2VNNO6etv8z02iuD/AOEZ8e/9DtD/AOC+Oj/hGfHv/Q7Q/wDgvjrtPmTvKK4P/hGfHv8A0O0P/gvjo/4Rnx7/ANDtD/4L46AOV+Jf/I8Tf9e0X/s1crXeal8LPEmr3pvL/wAVQyzlQhf7GBwM44B9zVX/AIUzrP8A0MkP/gJ/9euCthZzm5Jo+sy7PsPhcNCjOMrrtbv6nG0V2X/CmdZ/6GSH/wABP/r0f8KZ1n/oZIf/AAE/+vWf1Kp3R2/6z4T+WX3L/M42vR/hB/zGf96H+TVlf8KZ1n/oZIf/AAE/+vWjpHw48V6F539meLYYfOwZP9CVs4zjr9TW1DDSpz5mzzc2zqhjMP7KmmndPW3+Z6bRXB/8Iz49/wCh2h/8F8dH/CM+Pf8Aodof/BfHXafMHeUVwf8AwjPj3/odof8AwXx0f8Iz49/6HaH/AMF8dAHOfFT/AJHGH/rxT/0OSuOrvdU+F/iXWrwXWo+K4ZplQRhvsQX5QSQMA+pNVP8AhTOs/wDQyQ/+An/164K2FnUm5Jn1eW57h8Lho0Zxd1fa3dvucbRXZf8ACmdZ/wChkh/8BP8A69H/AApnWf8AoZIf/AT/AOvWf1Kp3R3f6z4T+WX3L/M42vQPhF/yENX/AOuUP83qj/wpnWf+hkh/8BP/AK9X9J+G3inQpJn03xZDC0wAc/YlbIGcdfqa2oYadOfM2edmud0MZhnSpxad1vb/ADPT6K4P/hGfHv8A0O0P/gvjo/4Rnx7/ANDtD/4L467T5c7yiuD/AOEZ8e/9DtD/AOC+Oj/hGfHv/Q7Q/wDgvjoA5/4rf8jXbf8AXkv/AKG1cXXfar8MPE2t3S3Oo+K4ZpkTy1b7EFwuSccH1Jqn/wAKZ1n/AKGSH/wE/wDr1w1sLOpNyTPqsszzD4TDRozi21fa3e/c42iuy/4UzrP/AEMkP/gJ/wDXo/4UzrP/AEMkP/gJ/wDXrL6lU7o7/wDWfCfyy+5f5nG13vwj/wCQzq3/AF7xf+hPVT/hTOs/9DJD/wCAn/16vaT8NPFGhTSy6b4shheZQrn7ErZAzjr9TWtDDTpz5mzzs0zuhjMM6NOLTdt7f5nqFFcH/wAIz49/6HaH/wAF8dH/AAjPj3/odof/AAXx13Hy53lFcH/wjPj3/odof/BfHR/wjPj3/odof/BfHQBifFr/AJGHTv8Ar1f/ANDFcNXf6t8MvE+uXEc+peK4ZpI1KIfsSrgE57GqX/CmdZ/6GSH/AMBP/r1w18NOpPmTPqcrzzD4TDKjOLbV9rd/U42iuy/4UzrP/QyQ/wDgJ/8AXo/4UzrP/QyQ/wDgJ/8AXrL6lU7o9D/WfCfyy+5f5nG12/wn/wCRlvv+vQf+hiov+FM6z/0MkP8A4Cf/AF6u6V8MvE+h3L3GneK4YZZE2M32INkZzjk1rQw06c1Js8/NM8w+Lw0qMItN23t39T1GsPxr/wAiRrX/AF5S/wDoJrn/APhGfHv/AEO0P/gvjqG98G+NtQsp7S68ZwyQToY5F+wINykYIyK7j5Y6PwH/AMiHoX/XlF/6CKKv6Dpf9i6DY6b5vm/ZIEh34xu2jGcUUAaFFFFABRRRQAUUUUAJtG7dgZ6ZpaKKACvIPEUs40rx4Y5MKl9BtO9ty8p93H1P616/TPJjOf3ac9flHNAHGeNdSvLSCG/0tnaHRZY57mONhiRSMMp5zwhz+PtUvjLVZLvwZrRgtZltjYmWC8DrtkJAI2gHcDz6dq67yowCNi4PXjrS+WhTZtXb6Y4oA4LUNBur7wJJdwJHFqUMMVxavA7fvBGoYBvUn5gfrTNCW9n8US+Zaypp+u20Wo7Hz/o7IRuQ+hbKn8TXoIUKMAAAdhRigDznw3pVzqniPVbiK6MMVjrkzthmLSoUA8vGcbMnP8qseCRI/gnTIuXvoLi4LI5JdXBlxuzz/d6+1d6qKmdqqueuBihY0V2ZUUM3UgcmgDgfh1LfPekTNK0R0u2afeSf9ILPuzn+LHX8K9Apqqq52qBk5OB1NOoAK4jW728i+IjW0E0pgOhyTGETFFDh8b8euOK7eq8ljayzmeS2haYrsMjICxX0z6e1AHCWeo6vdfCqw/s65nk1ia0M4lOZHO05OT/tYC/jXTaR4ot9Z07TbmC2upEv4gxeKMskR6MrMOhByK1YdPtLbHkWsMWF2DZGFwvpx29qdb2dvaQmG2gihiJJ2RoFXnrwKAPP/BsGo+I/Bx8+7vY5mS4WK+W8csX8x1AIz/CAuKp6VrusNd6JeTfayl1E+kXUTOxVbtM4lx/wE5P1r0y2tYLOLyrWCOGPOdsahRn6CnCGIYxGnDFx8o4Y9T9eT+dAHn+owaxd+MdS0nSNRnhkisbV4ZJJ22xHf8zFedxKjGO+au6dc3M2p+M4Jbm4IgnjWBTK37sGMH5eeMn0rsVtLdLprlYIhOw2tKEG4j0J60hsrY3P2k28RnwB5mwbsDpzQBz+nXNwfiNq9o1xK9vHZW7pEzZVCS+SB74FdPUK2luly1wkESzuMNIEG5h6E9amoAK8w1zxLrFpp/jB4Ly4DWF7DHbSAJiFW25GCOfvH1r0+subw1pFxHdxzWMTpeOJLhTnErDoT69KAMbxX4luNAuNOliYNZQzouoEjJEb5UHPscE/hUvi7xElt4e1ldOuZI9Qs7VplZYmwuACCGI2nqK2ptGsLm1ubae2WSC6wZkckh8ADn8h+VPn0yzudMOnzwK9oUEZibOCvp9KAOP1K61oeDZdYsrm+jubVYpmhk2ETooDSEYHAYMf++e1Jo/iG8v/ABNdWH2qd7TUYor7TJSACsOf3g6evTPYiu3S1hjtFtljXyFTywh5G3GMfTFMisbaF4nigjRoYvJjIX7qcfKPbgflQBxGi33iHUtfvlgupHtbTWJoJzJs2LbhAQq8ZLbjwfzq54N1K/1XwnpF3d3kslzNcyrI5CjcAXABAHQbR+VdRZaZZ6c9w1nAsTXEhlmK5+dz1Y+9NtdHsbLeLW2SIOzMVXIALfeIHQZ9qAMjwudQXU9XjutTN/ZrKv2Z5NgcHH7z7oHyhuB9DXSVm6T4d0rQmmbSrCG1M2PMMYwWxnGfzNaVABXL+O9SvNMstKksZ5Inm1S3gkCYy6MSGXn1rqKqX+mWeppEt7AsywyCWMNn5XHRh7igDmtC1y7bWPFP22WV4bG4jSCFsfIGQHAx1yT707wx4tL6LdjX5dt9p901tcmOJjuycowUDOCpHbtW8mhadHcy3CWqrLNKs0jgkF3Xox56ipYdLs7fUbi/ht0S7uQomlHVwOmfpQByUWrX99441awjub02YjtWhMW1RB5isSxyM44HH8qyNV8Qa7pLavaG8uJbnSbtL7O1R51g2MqeO3IyOa9Eh0uzt9Rnv4oFW6uAFllGcuB0B+lPksbaZ5XkgjdpovJkJXJdOflPtyfzoA5DXdXvUfw/PZ3d0sGqX+NiBQxhMZKgZHHQH8aj0+/8QW3iXwzp2s3WJri1uXuo4wu1ypGzJA6gEZxxmuvudJsrtrVp7ZHNoweDP/LMgYyPwp13ptpfTQTXMCvLbktFJyGQkYOCOeRQByviC/1Cw0ayv7e7uz5N6v2nYUbEJlKkspGWGMAY+tdpWdJ4f0ubUIr2Syia5iQIj46KDkDHQ4PIz0rRoAKxfGGo3OkeEtTv7JwlxbQNIhZQwyPatqqmp6bb6vps9jeqXt512SKGK5HpkUAc1pXiG/u/GVtp80uLVtHW8cNEFJkLAE59MGp9E8XreaxrNnqBht0tAtzA+4Ya2YfeJ9iDn0yK0T4X043f2nbMJ/sn2LeJWB8nOdv/ANfrUz6BYPq8GpmJvtcEJgRwxAKHqCOh/GgDntY8WSR+JNMi0+787Tbq0nlZraNZWZkIA2nn1OfpVXV9b8QaVq15pP2yOW5uLAT6Y/kKPMlQ4eMjuTwfYV1suiWU2r22pNGwurVGjiIYgKrfeGOnNTz6fa3N7bXc0KvcWu7yXPVNww2PqKAOL1DxjezfD2XxFpk6qVhgADRhgJS4EgP0zj6il1DxB4hsY7cy7Yop9aitIJJIQHmt3HJK9jnoePpXTXPhnS7rQ20d7bbYM24xIxUE7t/Uc/e5qxqWj2mrWcdteIXSJ1ljYMQyOpyrAjkEUAYfibxO3h/TtUla5gFwA32NJiEGRGGP+9yenU8Ct3Rbw6holjdtIsjT26SMy9CSoJx+NNutFsr2xmtLuETxTKyyeZyxyME57HHpVq1torO1itrdAkUKBEUdgBgUAS0UUUAFFFFABRRRQAUUUUAFFFFABRRRQAUUUUAFFFFABRRRQAUUUUAFFFFABRRRQAUUUUAFFFFABRRRQAUUVT1iIT6NexG4Nt5kDp54P+rypG78OtAE0V5bTuUhuIpGU4Ko4JBqavMvD17qOh69o+heKtIiE8QaLTtStvuSYQgq31H05xx3rS0jxtqN54n0zTbqG2UX0dxvER3iF4ycBZAcPwBnHQ0Ad3RXmNp8QddmttOuWi08pc6u2mFNjg+z5zxj0qS5+IGs2mi6jKY7KS7sNYGnltjBJEPQ4zkH8TQB6NNPFbxmSeRI0H8TsAPzNPVgyhlIIIyCO9eYeLvEF5eaF4z0LUlgeTT4IpY5okKhlcg4IJOCPrV9PFupxyDStGshcTafp1tMY9pJnLgZXOcKAvf1oA9BopqMXjVipUkA4PUU6gAooooAKKKKACiiigAooooAKKKKACiiigAooooAKKKKACiiigAooooAKKKKACiiigAooooAKKKKACiiigAooooAKKKKACiiigAooooAKKKKACiiigAooooAKKKKACiiigAooooAKgvLSG/sprS5TfDOhjkXOMqRgip6KAMuLw9ZRzwSuJZjbKVt1lkLiEEYO3PfHGTk4rP07wFoelXFlNZwTRyWJk8g+e52B/vDBPTnpXSUUAc3H4C0SKCCFIpxHBd/bYx5zfLN/e/zxWP4u8DGXRJoNBtnkuLvUI7y58yfAJBJZsk8E+1d5RQBgy+DtJurXUI7iGVjqZVrtmlO+Tb91Sw7DHQUkvgvSJb61vDFMtxbQiASRzshkjHRXwfmH1rfooAQAAAAYA6CloooAKKKKACiiigAooooAKKKKACiiigAooooAKKKKACiiigAooooAKKKKACiiigD/9k=\"/\u003e7-3 Elongation at break of HA-FWPU film with different Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e additions\u003c/p\u003e","description":"","filename":"7.png","url":"https://assets-eu.researchsquare.com/files/rs-8832982/v1/5b7c05f5e3072f420b3ae290.png"},{"id":106441172,"identity":"f11dbd4b-5624-49db-b672-161d720c748c","added_by":"auto","created_at":"2026-04-08 14:43:36","extension":"png","order_by":8,"title":"Figure 8","display":"","copyAsset":false,"role":"figure","size":102084,"visible":true,"origin":"","legend":"\u003cp\u003e8-2 Hysteresis loop diagram of HA-FWPU with different Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e additions\u003c/p\u003e\n\u003cp\u003e8-1 Hysteresis loop diagram of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e and Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS\u003c/p\u003e\n\u003cp\u003e\u003cimg width=\"381\" height=\"294\" 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14:43:43","extension":"png","order_by":9,"title":"Figure 9","display":"","copyAsset":false,"role":"figure","size":140724,"visible":true,"origin":"","legend":"\u003cp\u003eTG curves of HA-FWPU film with different Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS additions\u003c/p\u003e","description":"","filename":"9.png","url":"https://assets-eu.researchsquare.com/files/rs-8832982/v1/76ae848b17a7f956c3d483c4.png"},{"id":106724208,"identity":"15094d6b-ab44-4809-adc3-53d4fed63a6a","added_by":"auto","created_at":"2026-04-12 18:26:41","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2434669,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-8832982/v1/f3d5fe74-660c-4300-8b89-1e8cb59fcdb2.pdf"},{"id":106441186,"identity":"95eac09a-518b-4335-9775-e29f490c3e76","added_by":"auto","created_at":"2026-04-08 14:43:36","extension":"docx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":1564590,"visible":true,"origin":"","legend":"","description":"","filename":"Scheme1and2.docx","url":"https://assets-eu.researchsquare.com/files/rs-8832982/v1/eb21dd6508c70a7d796218f0.docx"}],"financialInterests":"No competing interests reported.","formattedTitle":"Fabrication and Characterization of Humic Acid-Modified Fe 3 O 4 /Waterborne Polyurethane Nanocomposite Emulsions","fulltext":[{"header":"1. Introduction","content":"\u003cp\u003eWaterborne polyurethane (WPU) has emerged as an environmentally benign alternative to solvent-based polyurethanes, employing water as the dispersion medium to significantly reduce volatile organic compounds (VOCS)\u003csup\u003e[\u003cspan additionalcitationids=\"CR2 CR3 CR4\" citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e]\u003c/sup\u003e. Owing to its low toxicity, biocompatibility, and versatile processability, WPU is widely utilized in coatings, adhesives, textile finishing, and biomedical applications\u003csup\u003e[\u003cspan additionalcitationids=\"CR7 CR8 CR9 CR10\" citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e]\u003c/sup\u003e. However, its practical deployment is often constrained by inherent limitations such as poor water resistance, moderate mechanical strength, and limited functionality\u003csup\u003e[\u003cspan additionalcitationids=\"CR13 CR14\" citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e]\u003c/sup\u003e. To address these shortcomings, researchers have explored various modification strategies, including the incorporation of organic and inorganic fillers, to enhance the comprehensive performance and expand the application scope of WPU\u003csup\u003e[\u003cspan additionalcitationids=\"CR17 CR18 CR19\" citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eAmong inorganic modifiers, magnetic Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e nanoparticles have attracted considerable attention due to their superparamagnetic behavior, high surface area, and unique electronic properties\u003csup\u003e[\u003cspan additionalcitationids=\"CR22\" citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e]\u003c/sup\u003e. These features make them promising candidates for developing polymer composites with tailored electromagnetic characteristics, suitable for electromagnetic interference (EMI) shielding, wave-absorbing materials, and sensors\u003csup\u003e[\u003cspan additionalcitationids=\"CR25\" citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e]\u003c/sup\u003e. Nevertheless, the high density, strong aggregation tendency, and lack of surface functional groups of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e nanoparticles often lead to poor dispersion and phase separation within polymer matrices, compromising the stability and performance of the resulting composites\u003csup\u003e[\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e]\u003c/sup\u003e. Therefore, improving the interfacial compatibility between Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e and the WPU matrix remains a critical challenge.\u003c/p\u003e \u003cp\u003eHumic acid (HA), a natural macromolecule derived from lignite, is rich in reactive functional groups such as carboxyl (-COOH), hydroxyl (-OH), and aromatic rings\u003csup\u003e[\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e]\u003c/sup\u003e. Its incorporation into polymer systems can enhance emulsion stability, mechanical reinforcement, and thermal resistance, while offering a cost-effective and sustainable modification pathway\u003csup\u003e[\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e]\u003c/sup\u003e. Previous studies have demonstrated that HA can act as a cross-linking agent and stabilizer in WPU systems, improving both colloidal and mechanical properties\u003csup\u003e[\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eIn this study, we propose a synergistic modification strategy to fabricate high-performance HA-FWPU magnetic nanocomposite emulsions. Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e nanoparticles were first surface-functionalized with IPTS to introduce reactive isocyanate groups, enabling covalent integration into the WPU network during prepolymerization. Simultaneously, HA was incorporated as a hydrophilic cross-linker to enhance emulsion stability and interfacial adhesion. The effects of HA and surface-modified Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e on the emulsion properties, film morphology, mechanical performance, thermal stability, and magnetic behavior were systematically investigated. The optimized composite exhibited significantly enhanced mechanical strength and magnetic responsiveness, demonstrating its potential as a multifunctional material for advanced applications.\u003c/p\u003e"},{"header":"2. Experimental","content":"\u003cp\u003e2.1 Materials\u0026nbsp;\u003c/p\u003e\n\u003cp\u003ePolycaprolactone diol (PCL, Mₙ= 1000 g/mol) was supplied by Jining Baiyi Chemical Co., Ltd. (China). Isophorone diisocyanate (IPDI, 99%) was obtained from Bayer AG. Dibutyltin dilaurate (DBTDL, 95%), triethylamine (TEA, 99%), N-methyl-2-pyrrolidone (NMP, 99%), trimethylolpropane (TMP, 98%), 2,2-bis(hydroxymethyl)propionic acid (DMPA, 98%), and (3-isocyanatopropyl)triethoxysilane (IPTS, 95%) were purchased from Shanghai Macklin Biochemical Co., Ltd. Ferric chloride hexahydrate (FeCl\u003csub\u003e3\u003c/sub\u003e\u0026bull;6H\u003csub\u003e2\u003c/sub\u003eO, 99%), ferrous chloride tetrahydrate (FeCl\u003csub\u003e2\u003c/sub\u003e\u0026bull;4H\u003csub\u003e2\u003c/sub\u003eO, 99%), ammonia solution (25-28%), nitric acid (HNO\u003csub\u003e3\u003c/sub\u003e, 65-68%), hydrochloric acid (HCl, 36-38%), sodium hydroxide (NaOH, 96%), potassium hydroxide (KOH, 85%), and ethanol (99.7%) were provided by Tianjin Comio Chemical Reagent Co., Ltd. Lignite was sourced from Yunnan province. All chemicals were used as received without further purification. Deionized water was used throughout the experiments.\u003c/p\u003e\n\u003cp\u003e2.2 Methods\u003c/p\u003e\n\u003cp\u003e2.2.1 Synthesis of\u0026nbsp;Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e nanoparticles\u003c/p\u003e\n\u003cp\u003eFe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e nanoparticles were synthesized via a co-precipitation method\u003csup\u003e[31]\u003c/sup\u003e. Briefly, FeCl\u003csub\u003e2\u003c/sub\u003e\u0026bull;4H\u003csub\u003e2\u003c/sub\u003eO and\u0026nbsp;FeCl\u003csub\u003e3\u003c/sub\u003e\u0026bull;6H\u003csub\u003e2\u003c/sub\u003eO(molar ratio 1:2) were dissolved in 100 mL deionized water under vigorous stirring. The solution was heated to 80\u0026deg;C under nitrogen atmosphere, followed by the dropwise addition of ammonia solution to adjust the pH to 9. The reaction was maintained at 80\u0026deg;C for 60 min. The resulting black precipitate was separated magnetically, washed repeatedly with ethanol and deionized water, and dried under vacuum at 40 \u0026deg;C for 12 h.\u003c/p\u003e\n\u003cp\u003e2.2.2 Surface modification of\u0026nbsp;Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e with IPTS\u003c/p\u003e\n\u003cp\u003eThe as-synthesized\u0026nbsp;Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e powder (1.5 g) was dispersed in 100 mL toluene via ultrasonication for 30 min. IPTS (6.5 mL) was then added under nitrogen protection. The mixture was refluxed at 130 \u0026deg;C for 60 h with continuous stirring. After cooling to room temperature, the modified nanoparticles (denoted as Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS) were magnetically separated, washed with toluene and acetone, and dried under vacuum at 40\u0026nbsp;\u0026deg;C\u0026nbsp;for 12 h.\u003c/p\u003e\n\u003cp\u003e2.2.3 Extraction of humic acid\u003c/p\u003e\n\u003cp\u003eHA was extracted from lignite using an alkaline dissolution-acid precipitation protocol\u003csup\u003e[32]\u003c/sup\u003e. Briefly, 10 g of nitric acid-oxidized coal powder (120 mesh) was mixed with 100 mL of a 2 wt% mixed alkali solution (KOH:NaOH = 1:1) and stirred at 80 \u0026deg;C for 50 min. The mixture was filtered, and the filtrate was centrifuged at 8000 rpm for 5 min. The supernatant was acidified to pH 3 using HCl, leading to HA precipitation. The precipitate was collected, washed to neutrality, and dried at 50 \u0026deg;C under vacuum for 24 h.\u003c/p\u003e\n\u003cp\u003e2.2.4 Preparation of HA-FWPU nanocomposite emulsions\u003c/p\u003e\n\u003cp\u003eThe HA-FWPU emulsions were synthesized via a prepolymer emulsification method.\u0026nbsp;Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS (varying amounts: 0, 0.5, 1.0, 2.0, and 4.0 wt% relative to total solids) was dispersed in 2 mL NMP via ultrasonication for 15 min. The dispersion was transferred to a three-necked flask equipped with a mechanical stirrer, condenser, and nitrogen inlet. PCL (15.01 g, 15.01 mmol), IPDI (7.48 g, 33.6 mmol), DMPA (1.0 g, 7.46 mmol), and 2-3 drops of DBTDL catalyst were added sequentially. The reaction was carried out at 80 \u0026deg;C for 2 h under nitrogen. HA (0.3g, predetermined as the optimal content based on prior optimization\u003csup\u003e[33]\u003c/sup\u003e) was then added, and the reaction continued for another 1 h. The temperature was lowered to 40 \u0026deg;C, and TEA (0.9 g, 8.91 mmol) was added for neutralization. After 30 min, deionized water was added under high-speed stirring to emulsify the prepolymer, yielding an emulsion with 25% solid content. The resulting emulsions were designated as HA-FWPU0, HA-FWPU1, HA-FWPU2, HA-FWPU3, and HA-FWPU4, corresponding to\u0026nbsp;Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS loadings of 0, 0.5, 1.0, 2.0, and 4.0 wt%, respectively.\u003c/p\u003e\n\u003cp\u003eTable 1 \u0026nbsp;Table of different HA-FWPU emulsion formulas\u003c/p\u003e\n\u003cdiv align=\"\"\u003e\n \u003ctable border=\"1\" cellspacing=\"0\" cellpadding=\"0\" width=\"570\"\u003e\n \u003ctbody\u003e\n \u003ctr\u003e\n \u003ctd rowspan=\"2\" style=\"width: 83px;\"\u003e\n \u003cp\u003eSample\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd colspan=\"6\" valign=\"top\" style=\"width: 378px;\"\u003e\n \u003cp\u003eraw material /（g/mmol）\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd rowspan=\"2\" style=\"width: 109px;\"\u003e\n \u003cp\u003e\u003cem\u003ew\u003c/em\u003e(Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e)/%\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 71px;\"\u003e\n \u003cp\u003eIPDI\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 76px;\"\u003e\n \u003cp\u003ePCL\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003eDMPA\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003eTMP\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003eTEA\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 61px;\"\u003e\n \u003cp\u003eHA\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 83px;\"\u003e\n \u003cp\u003eHA-FWPU0\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 71px;\"\u003e\n \u003cp\u003e7.48/33.6\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 76px;\"\u003e\n \u003cp\u003e15.01/15.01\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e1.0/7.46\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e0.2/1.49\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e0.9/8.91\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 61px;\"\u003e\n \u003cp\u003e0.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 109px;\"\u003e\n \u003cp\u003e0\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 83px;\"\u003e\n \u003cp\u003eHA-FWPU1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 71px;\"\u003e\n \u003cp\u003e7.48/33.6\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 76px;\"\u003e\n \u003cp\u003e15.01/15.01\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e1.0/7.46\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e0.2/1.49\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e0.9/8.91\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 61px;\"\u003e\n \u003cp\u003e0.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 109px;\"\u003e\n \u003cp\u003e0.5\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 83px;\"\u003e\n \u003cp\u003eHA-FWPU2\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 71px;\"\u003e\n \u003cp\u003e7.48/33.6\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 76px;\"\u003e\n \u003cp\u003e15.01/15.01\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e1.0/7.46\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e0.2/1.49\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e0.9/8.91\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 61px;\"\u003e\n \u003cp\u003e0.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 109px;\"\u003e\n \u003cp\u003e1.0\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 83px;\"\u003e\n \u003cp\u003eHA-FWPU3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 71px;\"\u003e\n \u003cp\u003e7.48/33.6\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 76px;\"\u003e\n \u003cp\u003e15.01/15.01\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e1.0/7.46\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e0.2/1.49\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e0.9/8.91\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 61px;\"\u003e\n \u003cp\u003e0.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 109px;\"\u003e\n \u003cp\u003e2.0\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 83px;\"\u003e\n \u003cp\u003eHA-FWPU4\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 71px;\"\u003e\n \u003cp\u003e7.48/33.6\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 76px;\"\u003e\n \u003cp\u003e15.01/15.01\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e1.0/7.46\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e0.2/1.49\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 57px;\"\u003e\n \u003cp\u003e0.9/8.91\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 61px;\"\u003e\n \u003cp\u003e0.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 109px;\"\u003e\n \u003cp\u003e4.0\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003c/tbody\u003e\n \u003c/table\u003e\n\u003c/div\u003e\n\u003cp\u003e2.2.5 Film preparation\u003c/p\u003e\n\u003cp\u003eThe emulsions were cast onto polytetrafluoroethylene plates and dried at room temperature for 5 days, followed by vacuum drying at 50 \u0026deg;C for 24 h. The films were peeled off and stored in a desiccator for further characterization.\u003c/p\u003e\n\u003cp\u003e2.3 Characterization\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eThe morphologies of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e and Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS were characterized by scanning electron microscopy (SEM, S4800, Rigaku, Japan) and transmission electron microscopy (TEM, JEM-F200, JEOL, Japan).\u0026nbsp;The FT-IR test was characterized by a Fourier infrared spectrometer (VECTOR-22, Bruker, Germany). The stability of the HA-FWPU emulsion was characterized by a stability tester (Turbiscan Lab, Formulaction, France). The emulsion particle size was characterized by a dynamic laser light scattering instrument (Zetasizer Nano-ZS, Malver, UK). The crystal structures of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e, Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS and HA-FWPU films were characterized by X-ray powder diffraction (XRD, CARY 800, Thermo Fisher). The mechanical properties of the HA-FWPU film are characterized by a universal testing machine (XWW-20B, Chengde Jinjian Testing Instrument Co., Ltd., China), the sensor is 500N, and the tensile speed is 20 mm/min. The thermal stability of the film was characterized by a thermogravimetric differential thermal analyzer (Q500, TA Corporation, USA), with a heating rate of 10 \u0026deg;C/min and a temperature range of 25 ~ 600 \u0026deg;C. The magnetic properties of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e and HA-FWPU films were characterized by a vibrating sample magnetometer (VSM, 7304, LAKE-SHORE, USA).\u003c/p\u003e"},{"header":"3. Results and discussion","content":"\u003cp\u003e3.1 FI-IR analysis\u003c/p\u003e\n\u003cp\u003eFig. 1. shows the FT-IR spectra of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS, FPPU, HA, and HA-FWPU。Among them, Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS is used to represent IPTS modified Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e, and FPPU is used to represent the prepolymer formed by introducing only Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e without adding HA. In the Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS spectrum, the peak at 576 cm\u003csup\u003e-1\u003c/sup\u003e was attributed to the stretching vibration of the Fe-O bond. The characteristic absorption peak of Si-O-Si can be clearly observed at 1055 cm\u003csup\u003e-1\u003c/sup\u003e. The strong absorption peak observed at 2270 cm\u003csup\u003e-1\u003c/sup\u003e was the characteristic peak of the -NCO group. C-H stretching vibration absorption peaks on -CH\u003csub\u003e3\u003c/sub\u003e and -CH\u003csub\u003e2\u003c/sub\u003e- and stretching vibration peaks of N-H bonds on amino groups were observed at 2930 cm\u003csup\u003e-1\u003c/sup\u003e and 3329 cm\u003csup\u003e-1\u003c/sup\u003e, respectively\u003csup\u003e[34]\u003c/sup\u003e.\u0026nbsp;The above analysis shows that Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e has been successfully modified using IPTS. In the FPPU spectrum, in addition to some characteristic peaks of the WPU prepolymer, the stretching vibration peaks of Fe-O bonds were also observed at 576cm\u003csup\u003e-1\u003c/sup\u003e, which indicates that Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e has been introduced into the aqueous polyurethane system. In addition, a characteristic peak of -NCO was also observed at 2270 cm\u003csup\u003e-1\u003c/sup\u003e, which indicates that there was still unreacted -NCO in the FPPU.\u0026nbsp;In the HA spectrum, the broad peak at 3700 ~ 3200cm\u003csup\u003e-1\u003c/sup\u003e was due to the stretching vibration of the phenolic hydroxyl group, and the in-plane bending vibration peak of the hydroxyl group was observed at 1370 cm\u003csup\u003e-1\u003c/sup\u003e.The C-C stretching vibration peak of benzene ring skeleton appeared at 1600 cm\u003csup\u003e-1\u003c/sup\u003e, an in-plane bending vibration peak of C-H was observed at 1240 cm\u003csup\u003e-1\u003c/sup\u003e, the peak at 1710 cm\u003csup\u003e-1\u003c/sup\u003e was due to the stretching vibration of the C=O double bond of -COOH. Finally, in the HA-FWPU spectrum, the strong peak at 576 cm\u003csup\u003e-1\u003c/sup\u003e was attributed to the stretching vibration of the Fe-O bond. In addition, the -NCO characteristic peak at 2270 cm\u003csup\u003e-1\u003c/sup\u003e disappeared, it indicates that -NCO from the IPTS and the reactive monomer has been completely reacted by -OH in humic acid. In summary, HA-FWPU magnetic nanocomposites have been successfully prepared.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e3.2 TEM analysis of surface modified Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e\u003c/p\u003e\n\u003cp\u003eFig. 2-1 shows the TEM image of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e and Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS nanoparticles. It can be seen from the figure that the agglomeration of pure Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e was more serious, but after the surface modification of IPTS, the agglomeration phenomenon between the particles weakens, which also proves that IPTS has been successfully modified on the surface of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e. Fig.2-2 was the effect of the dispersibility experiment of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e and Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS nanoparticles in ethanol solution.\u0026nbsp;The modification effect of IPTS can be seen intuitively from the figure, which greatly improves the dispersion of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e nanoparticles in organic systems.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e3.3 HA-FWPU emulsion properties\u003c/p\u003e\n\u003cp\u003e3.3.1 Emulsion stability analysis\u003c/p\u003e\n\u003cp\u003eThe TSI value reflects the degree of stability of the emulsion. The smaller the TSI value, the better the emulsion stability. When the TSI value exceeds 1, the emulsion stability was poor\u003csup\u003e[35]\u003c/sup\u003e.\u0026nbsp;It can be seen from Fig.3. that compared with WPU, the TSI of HA-FWPU0 modified with HA was decreased by 43.4%, and the stability of the emulsion was significantly improved. It can be seen that the introduction of HA improves the stability of WPU emulsion.\u0026nbsp;In addition, with the introduction of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e and the continuous increase of the amount, the TSI index of HA-FWPU emulsion also showed an increasing trend, and the stability of the emulsion gradually decreased. When Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u0026nbsp;\u003c/sub\u003ewas added in a small amount, the TSI index of HA-FWPU emulsion was less than 1, and the emulsion still has good stability. This was attributed to the reactive group -NCO grafted on the surface of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS particles, which reacts with -OH in the system to graft onto the WPU matrix, emulsifies with WPU, and disperses uniformly. However, when the Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e addition amount exceeds 2%, the TSI index of the HA-FWPU emulsion will all exceed 1, and the stability of the prepared emulsion was poor. This was due to the fact that agglomeration is easy to occur when the amount of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e introduced was too large, and it was easy to separate from the WPU system under the effect of gravity, which eventually leads to poor emulsion stability\u003csup\u003e[36]\u003c/sup\u003e.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e3.3.2 \u0026nbsp;Emulsion particle size analysis\u003c/p\u003e\n\u003cp\u003eFig. 4. was \u0026nbsp; particle size distribution diagram of a series of HA-FWPU emulsions corresponding to different Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e additions. It can be seen from the figure that the particle size distribution index of each emulsion shows a continuously increasing trend with the increase of the Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e addition amount, but all remain within a small value. This shows that the particle size distribution of each emulsion was narrow and the particle size of the emulsion is relatively uniform. This was due to the introduction of HA increased the -COOH content in the prepolymer, making it easier to emulsify and disperse. In addition, as the amount of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e added increases, the average particle size of the emulsion also increases. This was due to the increasing amount of nano Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e added, which will increase its agglomeration effect, and eventually lead to a slight increase in particle size of HA-FWPU emulsion.\u003c/p\u003e\n\u003cp\u003e3.4 HA-FWPU films properties\u003c/p\u003e\n\u003cp\u003e3.4.1 SEM analysis\u003c/p\u003e\n\u003cp\u003eFig. 5 shows the SEM micrographs of the fractured sections of the HA-FWPU film samples. Among them, (a), (b), (c), and (d) represent cross-sectional TEM images of HA-FWPU0, HA-FWPU1, HA-FWPU3, and HA-FWPU4 adhesive films, respectively. It can be seen from the figure that the cross-section of the HA-WPU0 film shown in Fig. 5 (a) is relatively flat, and no nanoparticles are present. Fig.5 (b), Fig.5 (c), and Fig.5 (d) the film cross sections were interspersed with many white particles, and the white particles are Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e nanoparticles grafted onto the WPU matrix through chemical bonding. Among them, the distribution of white particles in Fig.5 (b) and Fig.5 (c) is relatively uniform, the agglomeration phenomenon is not obvious, and Fig.5 (c) has a lot more white particles than Fig.5 (b). In Fig.5(d), obvious agglomeration of nanoparticles appears. The reason for this phenomenon was that as the amount of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e nanoparticles added continues to increase, the number of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e nanoparticles present in the section of the film increases. However, when the addition amount exceeds the optimal addition amount (2.0%), the agglomeration of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e nanoparticles was severe, which eventually leads to uneven distribution in the cross section. \u0026nbsp;\u003c/p\u003e\n\u003cp\u003e3.4.2 XRD analysis\u003c/p\u003e\n\u003cp\u003eFig. 6 shows the XRD patterns of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e, Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS and HA-FWPU.\u0026nbsp;Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e and Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS all show diffraction peaks at 2\u0026theta; = 30.2, 35.3, 43.2, 53.6, 57.2, and 62.7. These correspond to the (220), (311), (400), (511), and (440) crystal planes in the Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e cubic lattice, respectively. This shows that the prepared Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e has a magnetite spinel structure\u003csup\u003e[37]\u003c/sup\u003e, and the modification of IPTS does not change the crystal structure of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e.\u0026nbsp;A new broad absorption peak appears at 2\u0026theta; = 19.8 in HA-FWPU, which was due to the orderly arrangement of the hard segments of HA-FWPU polymer.\u0026nbsp;In addition, a diffraction peak appears at the same position as Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e, indicating that Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e has been introduced into the WPU system. However, the peak intensities were weakened and some of the peak positions are not obvious. This was because Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS was added in a small amount and the broad absorption peak at 2\u0026theta; = 19.8 also has a certain masking effect on other peaks.\u003c/p\u003e\n\u003cp\u003e3.4.3 Mechanical performance analysis\u003c/p\u003e\n\u003cp\u003eIt can be seen from Fig. 7-1 that the introduction of nano Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e has a certain degree of influence on the mechanical properties of HA-FWPU film. The specific performance was that with the increasing amount of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u0026nbsp;\u003c/sub\u003eadded, the tensile strength of HA-FWPU film shows a trend of first increase and then decrease, while the elongation at break decreases.\u0026nbsp;As shown in Fig.7-2 and 7-3, where the Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e addition amount is 0% (mass fraction, the same applies hereinafter), the minimum tensile strength of the HA-FWPU film is 13.72Mpa and the maximum elongation at break is 1001.02 %；When the added amount of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e is 2.0%, the tensile strength of HA-FWPU3 film reaches a maximum of 23.01Mpa and the elongation at break is 671.37%. The change in the tensile strength of the above HA-FWPU film can be attributed to the following two points :(1) Nano-Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e surface modified by IPTS in polyurethane matrix through strong interfacial force (covalent bond) formed between them, so that it achieves good dispersion in the polyurethane body, the addition of nano-Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e Improve the tensile strength of Waterborne polyurethane materials. (2) When the amount of nano Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e introducedwas too large, its large density and nano effect will cause agglomeration, affect its interaction with the polymer, and deteriorate compatibility. When the agglomeration of nanoparticles was severe, fracture stress points will be generated, which will seriously affect the mechanical properties of the polymer and eventually lead to a decrease in tensile strength\u003csup\u003e[38]\u003c/sup\u003e.\u0026nbsp;In addition, with the continuous increase of the amount of nano Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e introduced, the breaking elongation of waterborne polyurethane has decreased, and the minimum was 614.83% of HA-FWPU4 (4.0%) film. This effect may be related to the rigidity of the inorganic nanomaterial itself, so the plasticity of the polyurethane material was suppressed to a certain extent, resulting in a continuous decrease in elongation at break.\u003c/p\u003e\n\u003cp\u003e3.4.4 VSM analysis\u003c/p\u003e\n\u003cp\u003eFig. 8-1 shows the hysteresis loops of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e and Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS.\u0026nbsp;It can be seen from the Figure that with the increase of the magnetic field, the magnetization increases continuously until it reaches the saturation magnetization (Ms). The coercivity (Hc) of both is zero, indicating that the prepared nanoparticles are superparamagnetic\u003csup\u003e[39]\u003c/sup\u003e. The maximum saturation magnetization of pure Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u0026nbsp;\u003c/sub\u003ewas 62 emu/g, while the maximum saturation magnetization of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e modified by IPTS decreased to 41 emu/g, which further indicates that Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS has been successfully obtained.\u0026nbsp;Fig. 8-2 shows the hysteresis loops of HA-FWPU with different Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e additions. As shown in figure, HA-FWPU with different Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e additions has excellent magnetic properties. With the increase of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS, the saturation magnetization of HA-FWPU also increases.\u0026nbsp;When Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS was added in an amount of 2.0%, the saturation magnetization can reach 6.01 emu/g , indicating that the prepared magnetic composite material has excellent magnetic properties.\u003c/p\u003e\n\u003cp\u003e3.4.5 Thermogravimetric analysis\u003c/p\u003e\n\u003cp\u003eTable 2 TG data of HA-FWPU film with different Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS additions\u003c/p\u003e\n\u003ctable border=\"1\" cellspacing=\"0\" cellpadding=\"0\" class=\"fr-table-selection-hover\"\u003e\n \u003ctbody\u003e\n \u003ctr\u003e\n \u003ctd rowspan=\"2\" style=\"width: 122px;\"\u003e\n \u003cp\u003eSample\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd colspan=\"3\" style=\"width: 489px;\"\u003e\n \u003cp\u003eDecomposition temperature /\u003cem\u003e℃\u003c/em\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd style=\"width: 150px;\"\u003e\n \u003cp\u003eT\u003csub\u003e10%\u003c/sub\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 189px;\"\u003e\n \u003cp\u003eT\u003csub\u003e50%\u003c/sub\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 151px;\"\u003e\n \u003cp\u003eT\u003csub\u003e90%\u003c/sub\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd style=\"width: 122px;\"\u003e\n \u003cp\u003eHA-FWPU0\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 150px;\"\u003e\n \u003cp\u003e279.65\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 189px;\"\u003e\n \u003cp\u003e313.06\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 151px;\"\u003e\n \u003cp\u003e349.13\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd style=\"width: 122px;\"\u003e\n \u003cp\u003eHA-FWPU1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 150px;\"\u003e\n \u003cp\u003e282.04\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 189px;\"\u003e\n \u003cp\u003e322.25\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 151px;\"\u003e\n \u003cp\u003e356.01\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd style=\"width: 122px;\"\u003e\n \u003cp\u003eHA-FWPU2\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 150px;\"\u003e\n \u003cp\u003e287.89\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 189px;\"\u003e\n \u003cp\u003e324.70\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 151px;\"\u003e\n \u003cp\u003e362.13\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd style=\"width: 122px;\"\u003e\n \u003cp\u003eHA-FWPU3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 150px;\"\u003e\n \u003cp\u003e284.75\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 189px;\"\u003e\n \u003cp\u003e324.08\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 151px;\"\u003e\n \u003cp\u003e361.32\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd style=\"width: 122px;\"\u003e\n \u003cp\u003eHA-FWPU4\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 150px;\"\u003e\n \u003cp\u003e285.71\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 189px;\"\u003e\n \u003cp\u003e341.2\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd style=\"width: 151px;\"\u003e\n \u003cp\u003e367.94\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003c/tbody\u003e\n\u003c/table\u003e\n\u003cp\u003eThermogravimetry was used to characterize the thermal stability of HA-FWPU film. It can be known from FIG. 9 that the thermal decomposition processes of the respective HA-FWPU films before and after the introduction of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e are similar, and they all consist of three weightless stages. Before 200℃, the moisture and organic solvents are volatile and lost, then the decomposition of the hard part of the polymer, and finally the decomposition of the soft part\u003csup\u003e[40]\u003c/sup\u003e.\u0026nbsp;The decomposition temperature of HA-FWPU film (HA-FWPU1~ 4) with Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS was higher than that of HA-FWPU film (HA-FWPU0) without Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS.\u0026nbsp;On the one hand, the introduction of nano Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e increases the crosslink density of the polymer. on the other hand, Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e itself also has good thermal stability. This can also explain that when the temperature reaches 800℃, the adhesive film has not been decomposed 100% (the remaining part was the introduced Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e).\u0026nbsp;According to Table 2, when the weight loss rate was 50%, the corresponding thermal decomposition temperatures of HA-FWPU0 and HA-FWPU4 are 313.06℃and 341.2℃, respectively, an increase of 10%, This shows that the introduction of nano Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e has improved the thermal stability of waterborne polyurethane to a certain extent.\u003c/p\u003e"},{"header":"4. Conclusion","content":"\u003cp\u003eA novel humic acid-modified Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e/waterborne polyurethane (HA-FWPU) magnetic nanocomposite emulsion was successfully developed through a dual-modification strategy. Surface functionalization of Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e with IPTS improved its dispersibility and covalent integration into the WPU matrix, while HA acted as an effective cross-linker and emulsion stabilizer. The optimized composite (2.0 wt% Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e-IPTS) exhibited a tensile strength of 23.01 MPa, a 67.7% improvement over the unmodified film, along with a saturation magnetization of 6.01 emu/g. The emulsion demonstrated good colloidal stability, and the films showed enhanced thermal resistance. This work provides a sustainable and effective approach to designing multifunctional WPU-based nanocomposites with potential applications in electromagnetic shielding, sensors, functional coatings, and beyond.\u003c/p\u003e "},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eCRediT authorship contribution statement\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eLei Lin: Writing-original draft, Formal analysis, Data curation. Xiaofen Zhao: Writing- original draft, Methodology, Investigation, Formal analysis. Zemin He: Formal analysis, Data curation. Xiangbo Feng: Visualization. Yuzhen Zhao: Writing - review \u0026amp; editing, Writing-original draft, Funding acquisition. Zongcheng Miao: Writing-review \u0026amp; editing, Writing-original draft, Supervision.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eDeclaration of competing interest\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe authors have no competing financial interests or personal relationships that might be construed as influencing the work reported herein.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAcknowledgments\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThis work was sponsored by the National Natural Science Founda-tion of China (52306165), the Scientific and Technical Innovation demonstration project for social development of Xi\u0026rsquo;an Municipal Bureau of Science and Technology (2024JH-CXSF-0020), the Key R\u0026amp;D Program Project of Xianyang (L2023-ZDYF-QYCX-029), Xi Jing University Research Fund (XJ240211) and the Youth Innovation Team of Shaanxi Universities (23JP186).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eData availability\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eData will be made available on request.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003eA. 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Alloys Compd. 890 (2022) 161801. \u003c/li\u003e\n\u003c/ol\u003e"},{"header":"Scheme","content":"\u003cp\u003eScheme 1 and 2 are available in the Supplementary Files section.\u003c/p\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":false,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"polymer-bulletin","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"pobu","sideBox":"Learn more about [Polymer Bulletin](http://link.springer.com/journal/289)","snPcode":"289","submissionUrl":"https://submission.nature.com/new-submission/289/3","title":"Polymer Bulletin","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"Waterborne polyurethane, Organic-inorganic modification, Humic acid, Fe3O4, Nanocomposite, Magnetic properties","lastPublishedDoi":"10.21203/rs.3.rs-8832982/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-8832982/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eHumic acid (HA)-modified Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e/waterborne polyurethane (HA-FWPU) nanocomposite emulsions were successfully fabricated via a dual-modification strategy. Isophorone diisocyanate (IPDI), polycaprolactone diol (PCL-1000), and 2,2-bis(hydroxymethyl)propionic acid (DMPA) served as the primary reactants, while HA and nano-Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e were incorporated as functional modifiers. The optimal modifier content was systematically determined. Comprehensive characterization revealed that HA significantly reduced the average emulsion particle size and improved colloidal stability. Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e nanoparticles were surface-functionalized with (3-isocyanatopropyl)triethoxysilane (IPTS) to enhance compatibility and dispersibility within the polyurethane matrix. The incorporation of nano-Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e not only improved the mechanical properties and thermal stability of the films but also imparted notable electrical conductivity and magnetic responsiveness. At an optimal Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e loading of 2.0 wt%, the HA-FWPU3 film exhibited a tensile strength of 23.01 MPa\u0026mdash;a 67.7% increase over the unmodified counterpart and a saturation magnetization of 6.01 emu/g. This work presents a feasible approach to designing multifunctional waterborne polyurethane composites for potential applications in electromagnetic shielding, sensors, and functional coatings.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e","manuscriptTitle":"Fabrication and Characterization of Humic Acid-Modified Fe 3 O 4 /Waterborne Polyurethane Nanocomposite Emulsions","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2026-04-08 14:43:01","doi":"10.21203/rs.3.rs-8832982/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"reviewersInvited","content":"","date":"2026-04-02T08:47:13+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2026-02-12T14:15:59+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2026-02-12T14:13:10+00:00","index":"","fulltext":""},{"type":"submitted","content":"Polymer Bulletin","date":"2026-02-09T16:55:50+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"polymer-bulletin","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"pobu","sideBox":"Learn more about [Polymer Bulletin](http://link.springer.com/journal/289)","snPcode":"289","submissionUrl":"https://submission.nature.com/new-submission/289/3","title":"Polymer Bulletin","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"7d48c14b-815d-4ec1-990e-89c4a6585453","owner":[],"postedDate":"April 8th, 2026","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[],"tags":[],"updatedAt":"2026-04-08T14:43:02+00:00","versionOfRecord":[],"versionCreatedAt":"2026-04-08 14:43:01","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-8832982","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-8832982","identity":"rs-8832982","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}