Interfacial Synthesis of Polyaniline/Graphene Oxide Composites for Tunable Electromagnetic Wave Absorption

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This study successfully achieved the controlled composite of polyaniline (PANI) on the surface of graphene oxide (GO) nanosheets using a one-pot interfacial synthesis method. It efficiently exfoliated the expanded layer structure of GO nanosheets and formed a three-dimensional interpenetrating network structure. This structural feature together with the interaction between PANI and GO significantly enhanced the electromagnetic loss capability of the composite material. When the PANI/GO molar ratio was optimized to 3:1, the reflection loss (RL) of the composite reached − 48 dB, and the effective absorption bandwidth (RL ≤ -10 dB) extended to 4.8 GHz. By constructing multiphase heterogeneous interface, the composite achieved ideal impedance matching characteristics and multiple polarization relaxation mechanisms, which were verified by measured input impedance curves and Cole-Cole semicircular curves. When the sample thickness was adjusted within the range of 2.2-5.0 mm, its effective absorption bandwidth could reach 11 GHz (5–16 GHz), demonstrating excellent broadband wave absorption performance. This study provides a reference for designing novel electromagnetic functional composite materials with multi-heterogeneous and hierarchical structures. The tunable nanostructure of the PANI/GO composite prepared via interfacial synthesis holds promise in providing solutions in the development of electromagnetic wave absorption technology. Graphene Oxide Polyaniline Interfacial Synthesis Electromagnetic Wave Absorption Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Figure 8 Figure 9 1. Introduction With the exponential expansion of information technology, environmental electromagnetic radiation pollution has emerged as a critical challenge threatening biological health, electronic equipment stability, and military information security [ 1 ]. Traditional magnetic loss-based absorbing materials (such as ferrites, magnetic metals, and their alloy systems) are limited by their inherent high density, narrow bandwidth response, and susceptibility to chemical environments [ 2 – 4 ], rendering them difficult to meet the urgent demand for "lightweight, broadband, strong loss" abs orbing materials in modern electronic systems [ 5 – 6 ]. Carbon-based electromagnetic wave (EMW) absorption materials have shown significant practical value in the field of electromagnetic absorption due to their low density, tunable conductivity, and outstanding corrosion resistance [ 7 – 10 ]. As a representative carbon material, graphene, leveraging its distinctive topological structure characterized by low density, high specific surface area, and superior electrical/thermal conductivity, has become a pivotal system in electromagnetic functional material research over the past decade [ 10 – 13 ]. However, the inherent high conductivity of graphene causes a severe impedance mismatch between its surface impedance and free space impedance, thereby resulting in significant reflection of incident electromagnetic waves. This limitation significantly deters the EMW absorption performance of graphene materials [ 14 ]. Current research primarily focuses on designing graphene-based heterogeneous composite systems to improve their electromagnetic response characteristics. Prevalent strategies include integrating graphene with dielectric or magnetic materials [ 15 – 16 ]. Compared to magnetic components, polyaniline (PANI) exhibits notable advantages in terms of material density, dielectric loss efficiency, and impedance matching characteristics [ 17 ]. The molecular-scale integration of PANI with graphene facilitates the synergistic utilization of the polarization relaxation effect of PANI and the conductive loss mechanism of graphene, thereby achieving broadband strong absorption characteristics [ 17 ]. For example, Chen et al. [ 18 ] synthesized graphene/PANI hybrids via in-situ intercalation polymerization, attaining a minimum reflection loss (RL min ) of -36.9 dB at a thickness of 3.5 mm. Liu et al. [ 19 ] developed a series of graphene/PANI/NiFe 2 O 4 nanocomposites with a RL min of -50.5 dB. Wang et al. [ 20 ] designed a hierarchical structure of graphene/Fe 3 O 4 @SiO 2 /PANI composite, achieving a RL min of -40.7 dB and an effective absorption bandwidth (EAB) of 5.8 GHz. However, in the aforementioned experiments, the polymerization of PANI on graphene sheets exhibited disordered arrangement, limiting the formation of an effective conductive network [ 11 , 21 ]. Presently, mechanically stirred assisted chemical oxidation polymerization remains the dominant process for PANI synthesis, yet it poses significant challenges in the control of PANI nanostructures [ 22 – 24 ]. In contrast, the interfacial synthesis method [ 25 – 26 ] utilizes the liquid-liquid interface as the reaction site, enabling the large-scale preparation of nanofiber structures without the necessity for templating agents or surfactants. Interfacial synthesis involves introducing an organic solvent and an aqueous solution to form a two-phase system with an interface, thereby confining the contact range between the initiator and reactants to the two-phase interface. At the interface, monomers and oxidizers interact, initiating the continuous growth of the polymer [ 27 ]. In this work, by controlling interfacial conditions, nanostructured PANI in different morphologies were composited with graphene oxide (GO) nanosheets and used as EMW absorption material. The integration of PANI and GO not only created numerous heterointerfaces to enhance interfacial polarization, but also established an effective conduction loss mechanism, synergistically improving the EMW absorption performance. Furthermore, the effects of interfacial synthesis on the EMW absorption properties were systematically discussed. 2. Experimental Section 2.1. Materials Graphene Oxide (GO) was laboratory-synthesized via an improved Hummers method [ 28 ]. Aniline (AN, AR) ammonium persulfate ((NH 4 ) 2 S 2 O 8 , APS, AR), hydrochloric acid (HCl, 1 mol/L), Chloroform (CHCl 3 , AR) were supplied by East China Chemical Industry Co., Ltd. Absolute ethanol (C 2 H 6 O, AR) was bought from Sinopharm Chemical Reagent Co., Ltd. All chemical reagents were used directly without further purification unless mentioned. 2.2. Preparation of PANI/GO Composites A series of PANI/GO composites were prepared via interfacial synthesis in this experiment, as shown in Fig. 1 . In the first step, 0.09 g of aniline monomer was dissolved in 10 mL of chloroform and stirred in an ice bath for 20 minutes to prepare solution A. Simultaneously, 0.03 g of GO and 0.91 g of APS were sequentially added to 10 mL of deionized water. Then, HCl solution (1 mol/L, 0.1 mL) was added dropwise, followed by ultrasonic dispersion for 5 minutes and stirring in ice bath for 20 minutes to obtain solution B. The mixed solutions of A and B underwent interfacial synthesis process in a 0–4°C environment. Upon completion of the reaction, the product was collected by centrifugation at 8000 rpm for 2 minutes, washed alternately with absolute ethanol and deionized water to remove unreacted monomers, and finally subjected to vacuum drying oven for 12 hours to yield the PANI/GO composite. To systematically study the influence of synthesis parameters on the composites, two sets of comparative experiments were designed: (1) Maintaining a fixed feed ratio of GO to aniline monomer at 1:1, the effect of reaction time on the product was examined at different time intervals (12 h, 24 h, 36 h), with the products labeled as T-1-12, T-1-24, T-1-36 respectively; (2) With the reaction time held constant at 36 h, the influence of varying GO to aniline molar ratios (1:2, 1:3, and 1:4) on the products was evaluated, labeled as T-2-36, T-3-36, T-4-36 respectively. 2.3. Characterization The microstructures of the samples were characterized by scanning electron microscopy (SEM). The phase structure of the samples was examined by X-ray pattern diffraction (XRD) (D8 ADVANCE, Bruker, Germany) using Cu Kα radiation. The surface composition and chemical states of the samples were analyzed using X-ray photoelectron spectroscopy (XPS). The molecular structure and chemical bonds were analyzed using a PE Spectrum One Fourier Transform Infrared Spectrometer (FTIR spectrometer) and an InVia Quotation confocal laser Raman spectrometer). The electromagnetic absorption characteristics of the samples were characterized using a vector network analyzer (VNA, model 3671D, CECS Instruments Co. Ltd) based on the air coaxial method. The measured sample was mixed with a paraffin matrix at a ratio of 20 wt% to form a uniform slurry. Subsequently, it was pressed into shape using a precision mold (inner diameter 3.04 mm and outer diameter 7.00 mm) to prepare standard coaxial ring-shaped specimens. 3. Results and Discussion 3.1. Structure and Morphology of PANI/GO Composites As shown in Fig. 2 a and Fig. S1 a, the crystal structures of GO, PANI, and PANI/GO composites prepared under different conditions were analyzed by XRD. The XRD pattern of GO displayed a sharp (001) crystal plane diffraction peak at 2θ = 11°, reflecting its well-ordered layered structure [ 26 ]. In contrast, there was no corresponding diffraction peak for GO in the T-3-36 composite while it showed diffraction peaks near 2θ = 19.8° and 25.1°, which may be attributed to the (020) and (200) crystal planes of PANI, respectively. The observed peak positions are consistent with those of PANI, confirming the successful synthesis of PANI and the effective exfoliation of GO nanosheets in the composite [ 28 – 29 ]. The other samples obtained under different reaction conditions (Fig. S1 a) also revealed that all composites prepared by adjusting the reaction time (12, 24, and 36 h) and feed ratio (GO/aniline from 1:2 to 1:4) exhibited the similar diffraction features of PANI in the range of 15°-30° [ 30 ]. It indicated that PANI molecular chains achieved ordered arrangement on the GO surface through π-π conjugation interactions [ 31 ]. FTIR spectra were used to analyze the functional group composition and molecular structure The FTIR spectrum of GO (Fig. 2 b) clearly showed its typical oxygen-containing functional group structure. The broad absorption peak at 3400 cm⁻¹ is attributed to the stretching vibration of surface hydroxyl groups (-OH) [ 31 ]. The peaks observed at 1405 cm⁻¹, 1700 cm⁻¹, and 1215 cm⁻¹ corresponded to the C-O deformation vibration of carboxyl groups, the C = O stretching vibration of carboxyl -COOH, and the asymmetric stretching vibration of epoxy groups (C-O-C), respectively [ 32 ]. Additionally, the weak absorption peak at 1615 cm⁻¹ is usually related to the H-O-H bending vibration of adsorbed water [ 33 ]. The FTIR spectra of the PANI/GO composites (Fig. 2 b and Fig. S1 b) clearly revealed the successful loading of PANI and its interaction with GO. The appearance of new peaks at 1474 cm⁻¹ and 1554 cm⁻¹ directly confirmed the successful synthesis of PANI with a benzenoid-quinoid alternating structure in the composite [ 34 ]. Compared with the typical spectrum of pure PANI, the composites showed characteristic absorption bands at 1114 cm⁻¹ (in-plane bending vibration of benzenoid ring C-H) and 1297 cm⁻¹ (C-N stretching), indicating that PANI was successfully loaded onto the GO surface [ 25 , 34 ]. The structural evolution and interfacial interactions were studied using Raman spectroscopy. As shown in Fig. S1 c, the pristine GO exhibited two characteristic double peaks at 1346 cm⁻¹ (D band) and 1587 cm⁻¹ (G band), indicating the presence of moderate structural defects within the material [ 35 ]. In comparison, the distinct peaks of PANI were located at 1324 cm⁻¹ (benzene ring C-C breathing vibration) and 1579 cm⁻¹ (quinoid structure C = C stretching vibration). For the PANI/GO (T-3-36) composite, the D and G bands were observed to shift to 1352 cm⁻¹ and 1593 cm⁻¹, respectively. This shift substantiated that PANI molecular chains facilitate interfacial charge redistribution on the GO surface through π-π conjugation, which was accompanied by the breakage of sp² domain and the formation of local defect [ 36 ]. These newly generated defects may serve as effective polarization relaxation centers [ 34 ], thereby enhancing the electromagnetic wave loss capability of the composite. X-ray photoelectron spectroscopy (XPS) was further used to examine the surface chemical properties and elemental composition of T-3-36. As shown in Fig. 2 c, four characteristic peaks observed in PANI/GO composite were ascribed to the spectra of C 1s, O 1s, N 1s, and S 2p [ 34 – 36 ]. Among them, the S 2p signal stemmed from the reaction residual of APS. Analysis of the C 1s fine spectrum further revealed the surface chemical composition characteristics of the material. As shown in Fig. 2 d, the spectrum can be deconvoluted into four main characteristic peaks. The peak at 284.8 eV was attributed to sp² hybridized carbon (C-C), which constituted the three-dimensional conductive framework of the composite and provided necessary electron transport pathways for electromagnetic energy dissipation [ 34 ]. The C-N characteristic peak observed at 285.6 eV confirmed the successful introduction of PANI molecular chains. This signal may originate from covalent bonding formed between PANI and GO. Such interfacial interactions facilitated the generation of interface polarization effects [ 35 ]. The characteristic peak at 286.6 eV corresponded to the C-O bond, indicating that some partially reduced hydroxyl and epoxy groups were retained in the composite. Furthermore, the C = O peak at 287.2 eV arose from the carbonyl and carboxyl structures inherent in the GO nanosheets. These strongly electronegative groups can effectively promote the dipole polarization relaxation process [ 36 ]. The presence of these polar functional groups not only improved the impedance matching characteristics of the material but also acts as dipole centers to enhance polarization loss [ 24 ]. Figure 2 e presented the characteristic spectrum of N 1s, where the three peaks are deconvoluted. The peak at 398.9 eV was assigned to imine nitrogen (= N-). The prominent peak at 400.8 eV corresponded to protonated amine nitrogen (-N⁺H-). The significant presence of the protonated amine nitrogen main peak clearly indicates that the PANI chains were in a conductive doped state [ 31 ]. The peak at 401.4 eV originated from nitrogen oxides (N-O), which may result from slight oxidation of PANI during synthesis or storage [ 37 ]. Additonally, the formation of N-O structures further confirmed the successful doping of the conductive polymer, thereby facilitating electron migration through effective pathways [ 39 ].. As shown in Fig. 2 f, three characteristic peaks corresponding to oxygen species in different chemical environments are observed in the spectrum. The three peaks of O 1s spectrum were attributed to the C-O, C = O, and -OH bonds, located at 531.1, 532.0 and 533.2 eV, respectively [ 34 , 39 , 42 ]. The material contains abundant polar bonds such as C-N, C = O, and C-O, which played a crucial role in its performance. These diverse covalent bonds not only effectively suppress phase separation but also enhance the structural stability of the nanocomposite [ 40 ]. In the presence of an electromagnetic field, these polar bonds functioned as microscopic dipoles, inducing significant dipole polarization relaxation. Meanwhile, the heterogeneous interface formed between PANI and GO induced interface polarization, collectively constituting multiple polarization mechanisms [ 41 ]. The highly conductive network within the material also provided efficient paths for interfacial charge transfer, which was beneficial for the enhancement of the electromagnetic wave absorption performance. SEM was used to systematically study the effects of reaction time and feed ratio on the microscopic morphology of PANI/GO composites (Fig. 3 ). Initially, with the GO/aniline feed ratio fixed at 1:1, the effect of reaction time on the structural evolution was investigated. As the reaction time increased from 12 to 36 hours, distinct morphological transformations of PANI on GO sheets were observed. At12 hours, the PANI growth began as randomly distributed island-like protrusions. By 24 hours, these structures evolved into closely packed sphere-like formations, eventually transitioning into a relatively smooth and more ordered nanostructure at 36 hours, This progression indicated that prolonged reaction time favors the controlled and regular growth of PANI. Subsequently, with the optimal reaction time of 36 hours, the influence of GO/aniline ratio was investigated. A feed ratio of 1:2 yielded several rod-like PANI nanostructures with length of about 800 nm and diameter of about 350 nm featuring surface protrusions. Upon increasing the feed ratio to 1:3, the PANI nanorods with smoother morphology turned thinner and these nanorods interconnected, forming a continuous and well-defined three-dimensional network structure. However, when the feed ratio was further increased to 1:4, excessive aniline polymerization occurred, leading to disordered accumulation of the product and destruction of the cross-linked network. Therefore, when the reaction time was 36 hours and the GO/aniline feed ratio was 1:3, the prepared PANI/GO composite exhibited the most regular structure and optimal cross-linking in its network morphology. 3.2. EMW Absorption Performance of PANI/GO Composites Based on transmission line theory, the EMW absorption performance of PANI/GO composites were quantitatively evaluated through systematic characterization of complex permittivity (ε r = ε' - jε'') and complex permeability (µ r = µ' - jµ''). Among them, the real parts of permittivity (ε') and permeability (µ') represented the material's ability to store electric and magnetic field energy, respectively, while the imaginary parts (ε'', µ'') reflected the dissipation efficiency of electromagnetic energy [ 41 ]. The effect of interfacial reaction time on the composite’s performance was initially studied. As shown in Fig. S2, the ε' values of T-1-12, T-1-24, and T-1-36 exhibited significant frequency dispersion characteristics across the 2–18 GHz range. The material's ability to store electric field energy generally decreased with increasing frequency, indicating a strong frequency-dependent polarization response. The ε'' and tan δₑ of the series samples also showed similar trends. Subsequently, the impact of feed ratio on composite’s performance was investigated. As shown in Fig. 4 , the ε' values of T-2-36, T-3-36, and T-4-36 also show strong frequency dependence with increasing frequency, exhibiting a decreasing trend, indicating strong dispersion characteristics of the composites. The variation trend of ε'' values (Fig. 4 b) further corroborated the presence of multiple relaxation mechanisms, corresponding to the synergistic effect of interface polarization and dipole orientation polarization [ 34 , 43 ]. Regarding the magnetic properties, the permeability values of the PANI/GO series samples (Figs. 4 d- 4 e) remain unchanged (µ' ≈ 1 and µ'' ≈ 0) acro frequency range, confirming that the composite behaved as a typical dielectric material. Generally, EMW absorption capability is evaluated by the effective absorption bandwidth (EAB) and reflection loss (RL). Based on transmission line theory and electromagnetic parameters, the RL value of the absorber can be calculated using the following two equations: $$\:RL\left(dB\right)=20l\text{g}\left|\frac{{Z}_{in}-{Z}_{0}}{{Z}_{in}+{Z}_{0}}\right|$$ 1 $$\:{Z}_{in}={Z}_{0}\sqrt{\frac{{\mu\:}_{r}}{{\epsilon\:}_{r}}}tanℎ\left(j\frac{2\pi\:fd}{c}\sqrt{{\mu\:}_{r}{\epsilon\:}_{r}}\right)$$ 2 where Z₀ is free space impedance, Z in is input impedance of the absorber, f is microwave frequency, d is absorber thickness, and c is speed of light. If the RL value is less than − 10 dB, it means 90% of the incident microwave energy is lost. As shown in Fig. S3, the minimum reflection loss (RL min ) of PANI and GO were − 13.8 dB and − 11.4 dB, respectively, consistent with literature reports [ 48 , 50 ]. In contrast, the RL min of the composite T-1-12 demonstrated markedly superior performance compared to the above single-component samples, reaching − 28.2 dB. As shown in Fig. S3, the RL curve of T-1-36 exhibited favorable wave absorption characteristics, with the effective absorption bandwidth covering the 4–18 GHz frequency range at the thickness of 1.9-5.0 mm. With prolonged reaction time, the composite's RL values progressively increased, accompanied by a rise in the maximum effective bandwidth (EAB max ) from 2.2 GHz to 4.2 GHz, indicating a gradual improvement in the overall EMW absorption performance of the composites. With the optimal reaction time of 36 hours, the influence of GO/aniline ratio on the EMW performance was further examined. As shown in Fig. 5 , the three samples T-2-36, T-3-36, and T-4-36 all exhibit favorable wave absorption characteristics, with their EAB covering the 4–18 GHz frequency range at different thickness. Specifically, the RL min of T-2-36 and T-4-36 were measured at -42.2 dB and − 46.0 dB, respectively, accompanied by EAB max of 3.2 GHz and 3.8 GHz. In comparison, the comprehensive performance of T-3-36 was more excellent, with its RL min further decreasing to -48.0 dB and its EAB max increasing to 4.6 GHz. Overall, as the aniline addition amount increased, the EMW absorption performance of the composite firstly enhanced and then declined, with T-3-36 exhibiting the optimal comprehensive performance among all samples. To assess the performance advantages of the as-prepared composites, a comparative analysis was conducted with the reported PANI and graphene-based materials, as shown in Fig. 6 . Notably, the T-3-36 demonstrated outstanding comprehensive performance among two-component composites [ 48 – 50 , 52 ]. For example, tannic acid-doped PANI/GO composites synthesized via in-situ polymerization method exhibited a RL min of -24.1 dB at 14.2 GHz [ 52 ], while PANI/reduce GO reached − 40 dB at 10.2 GHz with a 3.5 GHz [ 53 ]. Although PANI-AFG with RL min of -51.5 dB and EAB max of 4 GHz [ 21 ] was prepared, it required complex synthesis involving hard-to-obtain AFG. Furthermore, compared to the PANI/GO/NiFe 2 O 4 ternary composite (RL min = -50.5 dB, EAB max = 5.3 GHz) [ 19 ], the performance of T-3-36 was only slightly lower but was obtained without introducing magnetic components. It demonstrated that the interfacial engineering strategy achieved comparable performance with significantly higher efficiency and cost-effectiveness. To further explore the loss mechanism, Cole-Cole diagrams were analyzed. As shown in Fig. 7 , the presence of multiple nearly semicircular arcs in the diagrams confirmed the existence of Debye relaxation processes, serving as a primary contributor to dielectric loss. The Cole-Cole diagrams of PANI/GO materials revealed a distinct evolution in relaxation behavior. Figure 7 a (T-1-12) showed a single broadened semicircle, indicating a wide distribution of relaxation times, which may arise from interface polarization or non-uniform distribution of molecular dipole distribution. As the reaction conditions changed, Fig. 7 b (T-1-24) and Fig. 7 c (T-1-36) began to exhibit a double semicircle structure, indicating dual relaxation characteristics in the high and low frequency regions. The overall characteristics of Figs. 7 a-c indicate that the material was dominated by a non-uniform structure under the corresponding preparation conditions, accompanied by significant interface polarization. In contrast, the samples corresponding to Figs. 7 d-f exhibit more complex multiple relaxation behaviors. Multiple overlapping semicircles can be observed in Fig. 7 d (T-2-36) and Fig. 7 f (T-4-36), indicating the existence of multiple competing polarization loss processes inside the material. Moreover, the sharp rise in the imaginary part value in the low frequency region in Fig. 7 e (T-3-36) can be attributed to the obvious space charge accumulation effect at the interface. These complex Cole-Cole diagrams in Figs. 7 d-f implied that highly complex or diverse multiphase structures are formed inside the material, and their interface effects and polarization mechanisms were more sophisticated than those observed in the samples in Figs. 7 a-c. The input impedance (Z in ) is a key parameter for characterizing the ability to allow EMW to enter the absorber. The ratio of Z in to the free space impedance (Z 0 ) (Z = |Z in /Z 0 |) directly reflects the impedance matching characteristic of the material. The Z in values were shown in Fig. S5a.The reaction time significantly impacted the impedance matching performance of the composite. When the reaction time increased from 12 hours to 36 hours, the impedance matching capability improved significantly. The curves of T-1-12 and T-1-24 exceeded 1, with both low and high frequency regions deviating significantly from the ideal matching line, indicating severe impedance mismatch with free space This resulted in high reflection of incident EMW. In contrast, T-1-36 performed better than T-1-12 and T-1-24, confirming that sufficient reaction time is crucial for forming a microstructure with superior impedance matching. Among these samples, T-3-36 exhibited the closest normalized input impedance to the ideal matching condition under ‌characteristic thickness‌, While T-2-36 and T-4-36 remained generally close to the ideal value, indicating moderate impedance matching‌ and ‌partial surface reflection‌. For excellent EMW absorption materials, achieving a ‌balance between impedance matching and attenuation characteristics‌ is crucial, as this combination determines the material's effectiveness as a ‌high-performance microwave absorber‌. The attenuation characteristics of the material are also crucial for evaluating EMW absorption capability. The formula for the attenuation constant (α) is as follows: $$\:\alpha\:=2\pi\:fc{\epsilon\:}^{"}{\mu\:}^{"}-{\epsilon\:}^{{\prime\:}}{\mu\:}^{{\prime\:}}+\sqrt{\left({\epsilon\:}^{{\prime\:}}{\mu\:}^{"}+{\epsilon\:}^{"}{\mu\:}^{{\prime\:}}\right)+{\left({\epsilon\:}^{"}{\mu\:}^{"}-{\epsilon\:}^{{\prime\:}}{\mu\:}^{{\prime\:}}\right)}^{2}}$$ 3 The attenuation constant characterizes the attenuation rate of EMW in the material, directly reflecting the material's ability to dissipate electromagnetic energy. As shown in Fig. S5b, the α values of all samples almost increase with frequency, conforming to the typical dispersion behavior of dielectric materials. The effect of interfacial reaction time on the attenuation ability of the composite was initially studied. As the time increased from 12 hours to 36 hours, the attenuation performance of samples T-1-12 T-1-24, and T-1-36 progressively improved. The α value of T-1-12 was always below 80, indicating limited loss capability, while T-1-24 exhibited higher α value than T-1-12, though the maximum value did not exceed 100. Notably, T-1-36 demonstrated α values exceeding 100 in the 12–18 GHz high frequency region. The longer the interfacial reaction time, the stronger the attenuation ability of the composite. Subsequently, the impact of the GO/aniline feed ratio on the composite’s performance was investigated. Under the same reaction time, T-2-36 and T-4-36 exhibited stronger intrinsic loss capability, with their α values significantly higher than those of T-1-12, T-1-24, and T-1-36 samples. Especially, T-3-36 exhibited the most pronounced intrinsic loss, significantly outperforming all other samples across the entire frequency band, reaching a peak of about 280 at 18 GHz. The exceptional attenuation performance enabled the composite to achieve superior Joule heat conversion efficiency [ 39 ], demonstrating outstanding electromagnetic energy to thermal energy conversion capability. These results indicate that optimizing reaction time and feed ratio allowed for precise control of the microstructure of the composite, thereby effectively tailoring its attenuation characteristics. The high attenuation constant of the material originated from the synergistic effect of multiple loss mechanisms. The conjugated molecular chains of PANI contributed to conductive loss [ 30 ]. The defect sites in GO induced interface polarization relaxation [ 42 ]. The charge accumulation at heterogeneous interfaces triggered tunneling effects [ 34 ]. The ‌hierarchical structure‌ formed by ‌layered GO‌ and ‌rod-like PANI‌ facilitated ‌multiple reflections and scattering‌ of EMW, further amplifying energy attenuation. When incident EMW penetrated the composite, they undergo ‌repeated reflections‌ between the ‌layered GO‌ and ‌rod-like PANI‌, resulting in ‌progressive wave attenuation‌. In addition to defect polarization relaxation and dipole polarization relaxation, charge migration contributed to charge redistribution at the PANI/GO interface [34,45]. Under an electromagnetic field, such polarization generated dielectric relaxation, which further facilitated electromagnetic energy dissipation [46]. The material system contained a variety of polarization relaxation processes: defects at the edges of GO sheets promoted electron transition polarization [43–44], the dynamic transformation of the quinone-benzenamine structure in PANI chains triggered dipole reorientation [30], and the spatial charge distribution at the PANI/GO heterogeneous interface induced interface polarization [29]. These multiscale relaxation mechanisms collectively enhanced the dielectric loss performance of the material, which was verified by Cole-Cole fitting of the dielectric spectra [34]. The excellent EMW absorption performance of the composite was attributed to the synergistic optimization of attenuation capability and impedance matching, achieving efficient absorption and dissipation of EMW. As discussed above, the EMW absorption mechanism of the PANI/GO composite was shown in Fig. 8 . It involved multi-physics field coupling processes. Incident electromagnetic waves were partially reflected at the material interface, and the remaining energy entered the absorber interior through the impedance matching layer. Therefore, the three-dimensional network constructed by PANI nanorods and GO nanosheets allowed incident EMW to undergo multiple reflections, prolonging the electromagnetic wave path and enhancing energy dissipation, combined with the high conductivity of PANI to cause significant Joule heating effect [ 47 ]. Secondly, the intrinsic dipole moment of the benzenoid-quinoid structure in PANI molecular chains and the local polarization of carboxyl groups at the GO edges produced relaxation response under the drive of alternating electromagnetic fields [ 30 ]. Thirdly, the difference in conductivity between PANI and GO and the dielectric constant difference induced the formation of a space charge accumulation layer at the heterogeneous interface, generating a strong interface polarization electric field [ 34 ]. The model design was illustrated in Fig. 9 a, which depicted the sample and perfect electrical conductor (PEC). Figures 9 b-d illustrated the three-dimensional radar cross section (3D RCS), which showed the reflected output of the three samples across the full range of detection angles. T-3-36 owned the weakest wave scattering signal, indicating a better microwave absorption capacity compared to the other samples (GO and PANI). Figure 9 e provided a visual comparison of the RCS values of different samples at various angles. It is evident that T-3-36 exhibits superior performance compared to the other samples with RCS values below − 15 dBm 2 for the majority of angles. In conclusion, the RCS results indicate that T-3-36 has the potential for practical application. 4. Conclusions In summary, PANI/GO composites were successfully through interfacial synthesis. The structure-performance relationship between their nanostructures and electromagnetic wave absorption properties was systematically revealed. Experiments showed that when the reaction time was optimized to 36 h and the feed molar ratio of aniline to GO was adjusted to 3:1, the obtained PANI/GO composite exhibited optimal EMW absorption characteristics with a RL min of -48 dB and an EAB of 4.8 GHz. The excellent EMW absorption performance originated from the successful exfoliation of GO and the construction of three-dimensional network of the composite. The synergistic interaction between PANI and GO introduced significant dipole and interface polarization effects and constituted an efficient conductive network, thereby achieving efficient dissipation of electromagnetic energy through the synergy of dielectric relaxation and conductive loss. This work provides an alternative way for the advancement of EMW absorption composites with multi-heterogeneous and hierarchical structures. Declarations Declaration of competing interest The authors declare the following financial interests/personal relationships which may be considered as potential competing interests. Liang Li reports financial support was provided by National Natural Science Foundation of China, If there are other authors, they declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. Author Contribution L. Tang conceived the main research and wrote the main manuscript text. T. Li, H. Huang, and X. Yu completed data organization and management. Y. Yu participated in the entire process of data collection and literature review, while J. Ji was responsible for obtaining funding and completing the simulation calculations. L. Li has completed the final draft of the manuscript. All authors have reviewed the manuscript. Acknowledgments This work has been supported by National Natural Science Foundation of China (No. U24A20554), Guizhou Provincial Science and Technology Major Special Project ([2024]012), and Key R&D Plan of Hubei Province (2023BAB100). Data Availability All data supporting the findings of this study can be found in the paper and its supplementary information. Detailed data can be found in the supplementary materials, along with the original references used in this study. References Y. Huang, H. Zhang, G. Zeng, Z. Li, D. Zhang, H. Zhu, R. Xie, L. Zheng, J. Zhu, The Microwave Absorption Properties of Carbon-Encapsulated Nickel Nanoparticles/Silicone Resin Flexible Absorbing Material. J. Alloy Compd. 682 , 138–143 (2016). https://doi.org/10.1016/j.jallcom.2016.04.289 J.L. Gunjakar, A.M. More, K.V. Gurav, C.D. Lokhande, Chemical Synthesis of Spinel Nickel Ferrite (NiFe₂O₄) Nanosheets. Appl. Surf. Sci. 254 (18), 5844–5848 (2008). https://doi.org/10.1016/j.apsusc.2008.03.065 Q. Liu, X. 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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-8247974","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":565810511,"identity":"f45fb2aa-e234-4c82-897d-763db46c7526","order_by":0,"name":"Long Tang","email":"","orcid":"","institution":"Wuhan Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Long","middleName":"","lastName":"Tang","suffix":""},{"id":565810512,"identity":"2a99ba5c-554e-4c78-87f5-0728859d5629","order_by":1,"name":"Tianhao Li","email":"","orcid":"","institution":"Shenzhen Polytechnic 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composite.\u003c/p\u003e","description":"","filename":"image1.png","url":"https://assets-eu.researchsquare.com/files/rs-8247974/v1/98c10f528d34fa6c54a45cd7.png"},{"id":100356881,"identity":"d2e04a5b-513e-4778-bc0f-7ea80561cd1b","added_by":"auto","created_at":"2026-01-16 07:17:53","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":217427,"visible":true,"origin":"","legend":"\u003cp\u003e(a) XRD patterns of GO, PANI, T-3-36, (b) FTIR spectra of GO, PANI, T-3-36, (c) XPS spectra of T-3-36, elements spectra of (d) C 1s, (e) N 1s, and (f) O 1s.\u003c/p\u003e","description":"","filename":"image2.png","url":"https://assets-eu.researchsquare.com/files/rs-8247974/v1/c11d5d85f5fe2e023a3ca9f5.png"},{"id":99832980,"identity":"469e0cc9-d62c-4988-966a-e31d9a8d7432","added_by":"auto","created_at":"2026-01-08 17:59:47","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":669192,"visible":true,"origin":"","legend":"\u003cp\u003eSEM images of (a)T-1-12, (b) T-1-24, (c) T-1-36, (d) T-2-36, (e) T-3-36, and (f) T-4-36.\u003c/p\u003e","description":"","filename":"image3.png","url":"https://assets-eu.researchsquare.com/files/rs-8247974/v1/29140cb141312cdc482256a2.png"},{"id":100357002,"identity":"327cc11e-329d-4441-8e29-0b8999c733aa","added_by":"auto","created_at":"2026-01-16 07:18:15","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":169287,"visible":true,"origin":"","legend":"\u003cp\u003eElectromagnetic parameters of T-2-36, T-3-36, and T-4-36: (a) e′, (b) e′′, (c) tande, (d) m′, (e) m′′, and (f) tandm.\u003c/p\u003e","description":"","filename":"image4.png","url":"https://assets-eu.researchsquare.com/files/rs-8247974/v1/b0056ab73dcfe43f317d5ce8.png"},{"id":100356914,"identity":"d6d27bf1-3f5d-4853-a9f7-945fe437ef20","added_by":"auto","created_at":"2026-01-16 07:17:57","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":410607,"visible":true,"origin":"","legend":"\u003cp\u003e3D RL values (a,b,c) and RL values (d,e,f) of T-2-36, T-3-36, and T-4-36.\u003c/p\u003e","description":"","filename":"image5.png","url":"https://assets-eu.researchsquare.com/files/rs-8247974/v1/0db46f9eb61237139ad3dbcd.png"},{"id":100356994,"identity":"1d9f4594-5e77-4a54-83d2-85b45b5f26b0","added_by":"auto","created_at":"2026-01-16 07:18:14","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":81265,"visible":true,"origin":"","legend":"\u003cp\u003eComparison with other electromagnetic wave absorption materials based on GO and PANI.\u003c/p\u003e","description":"","filename":"image6.png","url":"https://assets-eu.researchsquare.com/files/rs-8247974/v1/498b20fe56988d032a697fb6.png"},{"id":100356367,"identity":"693dcdd8-8be4-43ac-9c06-bf121bc80645","added_by":"auto","created_at":"2026-01-16 07:05:54","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":88586,"visible":true,"origin":"","legend":"\u003cp\u003eCole-Cole plots of (a)T-1-12, (b) T-1-24, (c) T-1-36, (d) T-2-36, (e) T-3-36, (f) T-4-36.\u003c/p\u003e","description":"","filename":"image7.png","url":"https://assets-eu.researchsquare.com/files/rs-8247974/v1/21a8d80d20fc2627253bdce1.png"},{"id":99832986,"identity":"f4392300-bf23-4ae4-92df-392e9b87bc97","added_by":"auto","created_at":"2026-01-08 17:59:48","extension":"png","order_by":8,"title":"Figure 8","display":"","copyAsset":false,"role":"figure","size":1490946,"visible":true,"origin":"","legend":"\u003cp\u003eIllustration of EMW absorption mechanisms for the PANI/GO composite.\u003c/p\u003e","description":"","filename":"image8.png","url":"https://assets-eu.researchsquare.com/files/rs-8247974/v1/f48968986725657058ddbaf3.png"},{"id":99832987,"identity":"37282813-d53f-4585-9df1-3c73c5110213","added_by":"auto","created_at":"2026-01-08 17:59:48","extension":"png","order_by":9,"title":"Figure 9","display":"","copyAsset":false,"role":"figure","size":311480,"visible":true,"origin":"","legend":"\u003cp\u003e(a) CST simulation model. CST simulation results of PEC substrate covered with (b) GO, (c) PANI, (d) T-3-36. (e) The simulated RCS values at different scattering angles.\u003c/p\u003e","description":"","filename":"image9.png","url":"https://assets-eu.researchsquare.com/files/rs-8247974/v1/4f1ff360611c0189e92ebec9.png"},{"id":104739531,"identity":"1f0d32de-fe07-4d2c-830c-bd6670899c84","added_by":"auto","created_at":"2026-03-16 16:08:43","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":3205690,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-8247974/v1/22e023d4-3e35-4016-b0cc-4f2ef0292f2b.pdf"},{"id":99832989,"identity":"8ac89a75-64fe-41a5-83eb-3309b9e76add","added_by":"auto","created_at":"2026-01-08 17:59:48","extension":"doc","order_by":0,"title":"","display":"","copyAsset":false,"role":"supplement","size":7258112,"visible":true,"origin":"","legend":"","description":"","filename":"20251124.doc1.doc","url":"https://assets-eu.researchsquare.com/files/rs-8247974/v1/270f80bb1700f524e9c775fa.doc"}],"financialInterests":"No competing interests reported.","formattedTitle":"Interfacial Synthesis of Polyaniline/Graphene Oxide Composites for Tunable Electromagnetic Wave Absorption","fulltext":[{"header":"1. Introduction","content":"\u003cp\u003eWith the exponential expansion of information technology, environmental electromagnetic radiation pollution has emerged as a critical challenge threatening biological health, electronic equipment stability, and military information security [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e]. Traditional magnetic loss-based absorbing materials (such as ferrites, magnetic metals, and their alloy systems) are limited by their inherent high density, narrow bandwidth response, and susceptibility to chemical environments [\u003cspan additionalcitationids=\"CR3\" citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e], rendering them difficult to meet the urgent demand for \"lightweight, broadband, strong loss\" abs orbing materials in modern electronic systems [\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eCarbon-based electromagnetic wave (EMW) absorption materials have shown significant practical value in the field of electromagnetic absorption due to their low density, tunable conductivity, and outstanding corrosion resistance [\u003cspan additionalcitationids=\"CR8 CR9\" citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e]. As a representative carbon material, graphene, leveraging its distinctive topological structure characterized by low density, high specific surface area, and superior electrical/thermal conductivity, has become a pivotal system in electromagnetic functional material research over the past decade [\u003cspan additionalcitationids=\"CR11 CR12\" citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e]. However, the inherent high conductivity of graphene causes a severe impedance mismatch between its surface impedance and free space impedance, thereby resulting in significant reflection of incident electromagnetic waves. This limitation significantly deters the EMW absorption performance of graphene materials [\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eCurrent research primarily focuses on designing graphene-based heterogeneous composite systems to improve their electromagnetic response characteristics. Prevalent strategies include integrating graphene with dielectric or magnetic materials [\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e]. Compared to magnetic components, polyaniline (PANI) exhibits notable advantages in terms of material density, dielectric loss efficiency, and impedance matching characteristics [\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e]. The molecular-scale integration of PANI with graphene facilitates the synergistic utilization of the polarization relaxation effect of PANI and the conductive loss mechanism of graphene, thereby achieving broadband strong absorption characteristics [\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e]. For example, Chen et al. [\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e] synthesized graphene/PANI hybrids via in-situ intercalation polymerization, attaining a minimum reflection loss (RL\u003csub\u003emin\u003c/sub\u003e) of -36.9 dB at a thickness of 3.5 mm. Liu et al. [\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e] developed a series of graphene/PANI/NiFe\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e nanocomposites with a RL\u003csub\u003emin\u003c/sub\u003e of -50.5 dB. Wang et al. [\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e] designed a hierarchical structure of graphene/Fe\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e@SiO\u003csub\u003e2\u003c/sub\u003e/PANI composite, achieving a RL\u003csub\u003emin\u003c/sub\u003e of -40.7 dB and an effective absorption bandwidth (EAB) of 5.8 GHz. However, in the aforementioned experiments, the polymerization of PANI on graphene sheets exhibited disordered arrangement, limiting the formation of an effective conductive network [\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e, \u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e]. Presently, mechanically stirred assisted chemical oxidation polymerization remains the dominant process for PANI synthesis, yet it poses significant challenges in the control of PANI nanostructures [\u003cspan additionalcitationids=\"CR23\" citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eIn contrast, the interfacial synthesis method [\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e] utilizes the liquid-liquid interface as the reaction site, enabling the large-scale preparation of nanofiber structures without the necessity for templating agents or surfactants. Interfacial synthesis involves introducing an organic solvent and an aqueous solution to form a two-phase system with an interface, thereby confining the contact range between the initiator and reactants to the two-phase interface. At the interface, monomers and oxidizers interact, initiating the continuous growth of the polymer [\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e]. In this work, by controlling interfacial conditions, nanostructured PANI in different morphologies were composited with graphene oxide (GO) nanosheets and used as EMW absorption material. The integration of PANI and GO not only created numerous heterointerfaces to enhance interfacial polarization, but also established an effective conduction loss mechanism, synergistically improving the EMW absorption performance. Furthermore, the effects of interfacial synthesis on the EMW absorption properties were systematically discussed.\u003c/p\u003e"},{"header":"2. Experimental Section","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003e2.1. Materials\u003c/h2\u003e \u003cp\u003eGraphene Oxide (GO) was laboratory-synthesized via an improved Hummers method [\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e]. Aniline (AN, AR) ammonium persulfate ((NH\u003csub\u003e4\u003c/sub\u003e)\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e8\u003c/sub\u003e, APS, AR), hydrochloric acid (HCl, 1 mol/L), Chloroform (CHCl\u003csub\u003e3\u003c/sub\u003e, AR) were supplied by East China Chemical Industry Co., Ltd. Absolute ethanol (C\u003csub\u003e2\u003c/sub\u003eH\u003csub\u003e6\u003c/sub\u003eO, AR) was bought from Sinopharm Chemical Reagent Co., Ltd. All chemical reagents were used directly without further purification unless mentioned.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec4\" class=\"Section2\"\u003e \u003ch2\u003e2.2. Preparation of PANI/GO Composites\u003c/h2\u003e \u003cp\u003eA series of PANI/GO composites were prepared via interfacial synthesis in this experiment, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. In the first step, 0.09 g of aniline monomer was dissolved in 10 mL of chloroform and stirred in an ice bath for 20 minutes to prepare solution A. Simultaneously, 0.03 g of GO and 0.91 g of APS were sequentially added to 10 mL of deionized water. Then, HCl solution (1 mol/L, 0.1 mL) was added dropwise, followed by ultrasonic dispersion for 5 minutes and stirring in ice bath for 20 minutes to obtain solution B. The mixed solutions of A and B underwent interfacial synthesis process in a 0\u0026ndash;4\u0026deg;C environment. Upon completion of the reaction, the product was collected by centrifugation at 8000 rpm for 2 minutes, washed alternately with absolute ethanol and deionized water to remove unreacted monomers, and finally subjected to vacuum drying oven for 12 hours to yield the PANI/GO composite.\u003c/p\u003e \u003cp\u003eTo systematically study the influence of synthesis parameters on the composites, two sets of comparative experiments were designed: (1) Maintaining a fixed feed ratio of GO to aniline monomer at 1:1, the effect of reaction time on the product was examined at different time intervals (12 h, 24 h, 36 h), with the products labeled as T-1-12, T-1-24, T-1-36 respectively; (2) With the reaction time held constant at 36 h, the influence of varying GO to aniline molar ratios (1:2, 1:3, and 1:4) on the products was evaluated, labeled as T-2-36, T-3-36, T-4-36 respectively.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec5\" class=\"Section2\"\u003e \u003ch2\u003e2.3. Characterization\u003c/h2\u003e \u003cp\u003eThe microstructures of the samples were characterized by scanning electron microscopy (SEM). The phase structure of the samples was examined by X-ray pattern diffraction (XRD) (D8 ADVANCE, Bruker, Germany) using Cu Kα radiation. The surface composition and chemical states of the samples were analyzed using X-ray photoelectron spectroscopy (XPS). The molecular structure and chemical bonds were analyzed using a PE Spectrum One Fourier Transform Infrared Spectrometer (FTIR spectrometer) and an InVia Quotation confocal laser Raman spectrometer). The electromagnetic absorption characteristics of the samples were characterized using a vector network analyzer (VNA, model 3671D, CECS Instruments Co. Ltd) based on the air coaxial method. The measured sample was mixed with a paraffin matrix at a ratio of 20 wt% to form a uniform slurry. Subsequently, it was pressed into shape using a precision mold (inner diameter 3.04 mm and outer diameter 7.00 mm) to prepare standard coaxial ring-shaped specimens.\u003c/p\u003e \u003c/div\u003e"},{"header":"3. Results and Discussion","content":"\u003cdiv id=\"Sec7\" class=\"Section2\"\u003e \u003ch2\u003e3.1. Structure and Morphology of PANI/GO Composites\u003c/h2\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eAs shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea and Fig. \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003ea, the crystal structures of GO, PANI, and PANI/GO composites prepared under different conditions were analyzed by XRD. The XRD pattern of GO displayed a sharp (001) crystal plane diffraction peak at 2θ\u0026thinsp;=\u0026thinsp;11\u0026deg;, reflecting its well-ordered layered structure [\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e]. In contrast, there was no corresponding diffraction peak for GO in the T-3-36 composite while it showed diffraction peaks near 2θ\u0026thinsp;=\u0026thinsp;19.8\u0026deg; and 25.1\u0026deg;, which may be attributed to the (020) and (200) crystal planes of PANI, respectively. The observed peak positions are consistent with those of PANI, confirming the successful synthesis of PANI and the effective exfoliation of GO nanosheets in the composite [\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e]. The other samples obtained under different reaction conditions (Fig.\u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003ea) also revealed that all composites prepared by adjusting the reaction time (12, 24, and 36 h) and feed ratio (GO/aniline from 1:2 to 1:4) exhibited the similar diffraction features of PANI in the range of 15\u0026deg;-30\u0026deg; [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. It indicated that PANI molecular chains achieved ordered arrangement on the GO surface through π-π conjugation interactions [\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eFTIR spectra were used to analyze the functional group composition and molecular structure The FTIR spectrum of GO (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb) clearly showed its typical oxygen-containing functional group structure. The broad absorption peak at 3400 cm⁻\u0026sup1; is attributed to the stretching vibration of surface hydroxyl groups (-OH) [\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e]. The peaks observed at 1405 cm⁻\u0026sup1;, 1700 cm⁻\u0026sup1;, and 1215 cm⁻\u0026sup1; corresponded to the C-O deformation vibration of carboxyl groups, the C\u0026thinsp;=\u0026thinsp;O stretching vibration of carboxyl -COOH, and the asymmetric stretching vibration of epoxy groups (C-O-C), respectively [\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e]. Additionally, the weak absorption peak at 1615 cm⁻\u0026sup1; is usually related to the H-O-H bending vibration of adsorbed water [\u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e]. The FTIR spectra of the PANI/GO composites (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb and Fig. \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003eb) clearly revealed the successful loading of PANI and its interaction with GO. The appearance of new peaks at 1474 cm⁻\u0026sup1; and 1554 cm⁻\u0026sup1; directly confirmed the successful synthesis of PANI with a benzenoid-quinoid alternating structure in the composite [\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e]. Compared with the typical spectrum of pure PANI, the composites showed characteristic absorption bands at 1114 cm⁻\u0026sup1; (in-plane bending vibration of benzenoid ring C-H) and 1297 cm⁻\u0026sup1; (C-N stretching), indicating that PANI was successfully loaded onto the GO surface [\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e, \u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e]. The structural evolution and interfacial interactions were studied using Raman spectroscopy. As shown in Fig. \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003ec, the pristine GO exhibited two characteristic double peaks at 1346 cm⁻\u0026sup1; (D band) and 1587 cm⁻\u0026sup1; (G band), indicating the presence of moderate structural defects within the material [\u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e]. In comparison, the distinct peaks of PANI were located at 1324 cm⁻\u0026sup1; (benzene ring C-C breathing vibration) and 1579 cm⁻\u0026sup1; (quinoid structure C\u0026thinsp;=\u0026thinsp;C stretching vibration). For the PANI/GO (T-3-36) composite, the D and G bands were observed to shift to 1352 cm⁻\u0026sup1; and 1593 cm⁻\u0026sup1;, respectively. This shift substantiated that PANI molecular chains facilitate interfacial charge redistribution on the GO surface through π-π conjugation, which was accompanied by the breakage of sp\u0026sup2; domain and the formation of local defect [\u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e]. These newly generated defects may serve as effective polarization relaxation centers [\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e], thereby enhancing the electromagnetic wave loss capability of the composite. X-ray photoelectron spectroscopy (XPS) was further used to examine the surface chemical properties and elemental composition of T-3-36. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec, four characteristic peaks observed in PANI/GO composite were ascribed to the spectra of C 1s, O 1s, N 1s, and S 2p [\u003cspan additionalcitationids=\"CR35\" citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e]. Among them, the S 2p signal stemmed from the reaction residual of APS. Analysis of the C 1s fine spectrum further revealed the surface chemical composition characteristics of the material. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed, the spectrum can be deconvoluted into four main characteristic peaks. The peak at 284.8 eV was attributed to sp\u0026sup2; hybridized carbon (C-C), which constituted the three-dimensional conductive framework of the composite and provided necessary electron transport pathways for electromagnetic energy dissipation [\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e]. The C-N characteristic peak observed at 285.6 eV confirmed the successful introduction of PANI molecular chains. This signal may originate from covalent bonding formed between PANI and GO. Such interfacial interactions facilitated the generation of interface polarization effects [\u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e]. The characteristic peak at 286.6 eV corresponded to the C-O bond, indicating that some partially reduced hydroxyl and epoxy groups were retained in the composite. Furthermore, the C\u0026thinsp;=\u0026thinsp;O peak at 287.2 eV arose from the carbonyl and carboxyl structures inherent in the GO nanosheets. These strongly electronegative groups can effectively promote the dipole polarization relaxation process [\u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e]. The presence of these polar functional groups not only improved the impedance matching characteristics of the material but also acts as dipole centers to enhance polarization loss [\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e]. Figure\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ee presented the characteristic spectrum of N 1s, where the three peaks are deconvoluted. The peak at 398.9 eV was assigned to imine nitrogen (=\u0026thinsp;N-). The prominent peak at 400.8 eV corresponded to protonated amine nitrogen (-N⁺H-). The significant presence of the protonated amine nitrogen main peak clearly indicates that the PANI chains were in a conductive doped state [\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e]. The peak at 401.4 eV originated from nitrogen oxides (N-O), which may result from slight oxidation of PANI during synthesis or storage [\u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e]. Additonally, the formation of N-O structures further confirmed the successful doping of the conductive polymer, thereby facilitating electron migration through effective pathways [\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e].. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ef, three characteristic peaks corresponding to oxygen species in different chemical environments are observed in the spectrum. The three peaks of O 1s spectrum were attributed to the C-O, C\u0026thinsp;=\u0026thinsp;O, and -OH bonds, located at 531.1, 532.0 and 533.2 eV, respectively [\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e, \u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e, \u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eThe material contains abundant polar bonds such as C-N, C\u0026thinsp;=\u0026thinsp;O, and C-O, which played a crucial role in its performance. These diverse covalent bonds not only effectively suppress phase separation but also enhance the structural stability of the nanocomposite [\u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e40\u003c/span\u003e]. In the presence of an electromagnetic field, these polar bonds functioned as microscopic dipoles, inducing significant dipole polarization relaxation. Meanwhile, the heterogeneous interface formed between PANI and GO induced interface polarization, collectively constituting multiple polarization mechanisms [\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e]. The highly conductive network within the material also provided efficient paths for interfacial charge transfer, which was beneficial for the enhancement of the electromagnetic wave absorption performance.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eSEM was used to systematically study the effects of reaction time and feed ratio on the microscopic morphology of PANI/GO composites (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e). Initially, with the GO/aniline feed ratio fixed at 1:1, the effect of reaction time on the structural evolution was investigated. As the reaction time increased from 12 to 36 hours, distinct morphological transformations of PANI on GO sheets were observed. At12 hours, the PANI growth began as randomly distributed island-like protrusions. By 24 hours, these structures evolved into closely packed sphere-like formations, eventually transitioning into a relatively smooth and more ordered nanostructure at 36 hours, This progression indicated that prolonged reaction time favors the controlled and regular growth of PANI. Subsequently, with the optimal reaction time of 36 hours, the influence of GO/aniline ratio was investigated. A feed ratio of 1:2 yielded several rod-like PANI nanostructures with length of about 800 nm and diameter of about 350 nm featuring surface protrusions. Upon increasing the feed ratio to 1:3, the PANI nanorods with smoother morphology turned thinner and these nanorods interconnected, forming a continuous and well-defined three-dimensional network structure. However, when the feed ratio was further increased to 1:4, excessive aniline polymerization occurred, leading to disordered accumulation of the product and destruction of the cross-linked network. Therefore, when the reaction time was 36 hours and the GO/aniline feed ratio was 1:3, the prepared PANI/GO composite exhibited the most regular structure and optimal cross-linking in its network morphology.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec8\" class=\"Section2\"\u003e \u003ch2\u003e3.2. EMW Absorption Performance of PANI/GO Composites\u003c/h2\u003e \u003cp\u003eBased on transmission line theory, the EMW absorption performance of PANI/GO composites were quantitatively evaluated through systematic characterization of complex permittivity (ε\u003csub\u003er\u003c/sub\u003e\u0026thinsp;=\u0026thinsp;ε' - jε'') and complex permeability (\u0026micro;\u003csub\u003er\u003c/sub\u003e\u0026thinsp;=\u0026thinsp;\u0026micro;' - j\u0026micro;''). Among them, the real parts of permittivity (ε') and permeability (\u0026micro;') represented the material's ability to store electric and magnetic field energy, respectively, while the imaginary parts (ε'', \u0026micro;'') reflected the dissipation efficiency of electromagnetic energy [\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eThe effect of interfacial reaction time on the composite\u0026rsquo;s performance was initially studied. As shown in Fig. S2, the ε' values of T-1-12, T-1-24, and T-1-36 exhibited significant frequency dispersion characteristics across the 2\u0026ndash;18 GHz range. The material's ability to store electric field energy generally decreased with increasing frequency, indicating a strong frequency-dependent polarization response. The ε'' and tan δₑ of the series samples also showed similar trends. Subsequently, the impact of feed ratio on composite\u0026rsquo;s performance was investigated. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e, the ε' values of T-2-36, T-3-36, and T-4-36 also show strong frequency dependence with increasing frequency, exhibiting a decreasing trend, indicating strong dispersion characteristics of the composites. The variation trend of ε'' values (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb) further corroborated the presence of multiple relaxation mechanisms, corresponding to the synergistic effect of interface polarization and dipole orientation polarization [\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e, \u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e43\u003c/span\u003e]. Regarding the magnetic properties, the permeability values of the PANI/GO series samples (Figs.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed-\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ee) remain unchanged (\u0026micro;' \u0026asymp; 1 and \u0026micro;'' \u0026asymp; 0) acro frequency range, confirming that the composite behaved as a typical dielectric material.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eGenerally, EMW absorption capability is evaluated by the effective absorption bandwidth (EAB) and reflection loss (RL). Based on transmission line theory and electromagnetic parameters, the RL value of the absorber can be calculated using the following two equations:\u003cdiv id=\"Equ1\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equ1\" name=\"EquationSource\"\u003e\n$$\\:RL\\left(dB\\right)=20l\\text{g}\\left|\\frac{{Z}_{in}-{Z}_{0}}{{Z}_{in}+{Z}_{0}}\\right|$$\u003c/div\u003e\u003cdiv class=\"EquationNumber\"\u003e1\u003c/div\u003e\u003c/div\u003e\u003cdiv id=\"Equ2\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equ2\" name=\"EquationSource\"\u003e\n$$\\:{Z}_{in}={Z}_{0}\\sqrt{\\frac{{\\mu\\:}_{r}}{{\\epsilon\\:}_{r}}}tanℎ\\left(j\\frac{2\\pi\\:fd}{c}\\sqrt{{\\mu\\:}_{r}{\\epsilon\\:}_{r}}\\right)$$\u003c/div\u003e\u003cdiv class=\"EquationNumber\"\u003e2\u003c/div\u003e\u003c/div\u003e\u003c/p\u003e \u003cp\u003ewhere Z₀ is free space impedance, Z\u003csub\u003ein\u003c/sub\u003e is input impedance of the absorber, f is microwave frequency, d is absorber thickness, and c is speed of light. If the RL value is less than \u0026minus;\u0026thinsp;10 dB, it means 90% of the incident microwave energy is lost.\u003c/p\u003e \u003cp\u003eAs shown in Fig. S3, the minimum reflection loss (RL\u003csub\u003emin\u003c/sub\u003e) of PANI and GO were \u0026minus;\u0026thinsp;13.8 dB and \u0026minus;\u0026thinsp;11.4 dB, respectively, consistent with literature reports [\u003cspan citationid=\"CR48\" class=\"CitationRef\"\u003e48\u003c/span\u003e, \u003cspan citationid=\"CR50\" class=\"CitationRef\"\u003e50\u003c/span\u003e]. In contrast, the RL\u003csub\u003emin\u003c/sub\u003e of the composite T-1-12 demonstrated markedly superior performance compared to the above single-component samples, reaching \u0026minus;\u0026thinsp;28.2 dB. As shown in Fig. S3, the RL curve of T-1-36 exhibited favorable wave absorption characteristics, with the effective absorption bandwidth covering the 4\u0026ndash;18 GHz frequency range at the thickness of 1.9-5.0 mm. With prolonged reaction time, the composite's RL values progressively increased, accompanied by a rise in the maximum effective bandwidth (EAB\u003csub\u003emax\u003c/sub\u003e) from 2.2 GHz to 4.2 GHz, indicating a gradual improvement in the overall EMW absorption performance of the composites.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eWith the optimal reaction time of 36 hours, the influence of GO/aniline ratio on the EMW performance was further examined. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e, the three samples T-2-36, T-3-36, and T-4-36 all exhibit favorable wave absorption characteristics, with their EAB covering the 4\u0026ndash;18 GHz frequency range at different thickness. Specifically, the RL\u003csub\u003emin\u003c/sub\u003e of T-2-36 and T-4-36 were measured at -42.2 dB and \u0026minus;\u0026thinsp;46.0 dB, respectively, accompanied by EAB\u003csub\u003emax\u003c/sub\u003e of 3.2 GHz and 3.8 GHz. In comparison, the comprehensive performance of T-3-36 was more excellent, with its RL\u003csub\u003emin\u003c/sub\u003e further decreasing to -48.0 dB and its EAB\u003csub\u003emax\u003c/sub\u003e increasing to 4.6 GHz. Overall, as the aniline addition amount increased, the EMW absorption performance of the composite firstly enhanced and then declined, with T-3-36 exhibiting the optimal comprehensive performance among all samples. To assess the performance advantages of the as-prepared composites, a comparative analysis was conducted with the reported PANI and graphene-based materials, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e. Notably, the T-3-36 demonstrated outstanding comprehensive performance among two-component composites [\u003cspan additionalcitationids=\"CR49\" citationid=\"CR48\" class=\"CitationRef\"\u003e48\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR50\" class=\"CitationRef\"\u003e50\u003c/span\u003e, \u003cspan citationid=\"CR52\" class=\"CitationRef\"\u003e52\u003c/span\u003e]. For example, tannic acid-doped PANI/GO composites synthesized via in-situ polymerization method exhibited a RL\u003csub\u003emin\u003c/sub\u003e of -24.1 dB at 14.2 GHz [\u003cspan citationid=\"CR52\" class=\"CitationRef\"\u003e52\u003c/span\u003e], while PANI/reduce GO reached \u0026minus;\u0026thinsp;40 dB at 10.2 GHz with a 3.5 GHz [\u003cspan citationid=\"CR53\" class=\"CitationRef\"\u003e53\u003c/span\u003e]. Although PANI-AFG with RL\u003csub\u003emin\u003c/sub\u003e of -51.5 dB and EAB\u003csub\u003emax\u003c/sub\u003e of 4 GHz [\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e] was prepared, it required complex synthesis involving hard-to-obtain AFG. Furthermore, compared to the PANI/GO/NiFe\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e ternary composite (RL\u003csub\u003emin\u003c/sub\u003e = -50.5 dB, EAB\u003csub\u003emax\u003c/sub\u003e = 5.3 GHz) [\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e], the performance of T-3-36 was only slightly lower but was obtained without introducing magnetic components. It demonstrated that the interfacial engineering strategy achieved comparable performance with significantly higher efficiency and cost-effectiveness.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eTo further explore the loss mechanism, Cole-Cole diagrams were analyzed. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003e, the presence of multiple nearly semicircular arcs in the diagrams confirmed the existence of Debye relaxation processes, serving as a primary contributor to dielectric loss. The Cole-Cole diagrams of PANI/GO materials revealed a distinct evolution in relaxation behavior. Figure\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ea (T-1-12) showed a single broadened semicircle, indicating a wide distribution of relaxation times, which may arise from interface polarization or non-uniform distribution of molecular dipole distribution. As the reaction conditions changed, Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003eb (T-1-24) and Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ec (T-1-36) began to exhibit a double semicircle structure, indicating dual relaxation characteristics in the high and low frequency regions.\u003c/p\u003e \u003cp\u003eThe overall characteristics of Figs.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ea-c indicate that the material was dominated by a non-uniform structure under the corresponding preparation conditions, accompanied by significant interface polarization. In contrast, the samples corresponding to Figs.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ed-f exhibit more complex multiple relaxation behaviors. Multiple overlapping semicircles can be observed in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ed (T-2-36) and Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ef (T-4-36), indicating the existence of multiple competing polarization loss processes inside the material. Moreover, the sharp rise in the imaginary part value in the low frequency region in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ee (T-3-36) can be attributed to the obvious space charge accumulation effect at the interface. These complex Cole-Cole diagrams in Figs.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ed-f implied that highly complex or diverse multiphase structures are formed inside the material, and their interface effects and polarization mechanisms were more sophisticated than those observed in the samples in Figs.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ea-c.\u003c/p\u003e \u003cp\u003eThe input impedance (Z\u003csub\u003ein\u003c/sub\u003e) is a key parameter for characterizing the ability to allow EMW to enter the absorber. The ratio of Z\u003csub\u003ein\u003c/sub\u003e to the free space impedance (Z\u003csub\u003e0\u003c/sub\u003e) (Z = |Z\u003csub\u003ein\u003c/sub\u003e/Z\u003csub\u003e0\u003c/sub\u003e|) directly reflects the impedance matching characteristic of the material. The Z\u003csub\u003ein\u003c/sub\u003e values were shown in Fig. S5a.The reaction time significantly impacted the impedance matching performance of the composite. When the reaction time increased from 12 hours to 36 hours, the impedance matching capability improved significantly. The curves of T-1-12 and T-1-24 exceeded 1, with both low and high frequency regions deviating significantly from the ideal matching line, indicating severe impedance mismatch with free space This resulted in high reflection of incident EMW. In contrast, T-1-36 performed better than T-1-12 and T-1-24, confirming that sufficient reaction time is crucial for forming a microstructure with superior impedance matching. Among these samples, T-3-36 exhibited the closest normalized input impedance to the ideal matching condition under \u0026zwnj;characteristic thickness\u0026zwnj;, While T-2-36 and T-4-36 remained generally close to the ideal value, indicating moderate impedance matching\u0026zwnj; and \u0026zwnj;partial surface reflection\u0026zwnj;. For excellent EMW absorption materials, achieving a \u0026zwnj;balance between impedance matching and attenuation characteristics\u0026zwnj; is crucial, as this combination determines the material's effectiveness as a \u0026zwnj;high-performance microwave absorber\u0026zwnj;.\u003c/p\u003e \u003cp\u003eThe attenuation characteristics of the material are also crucial for evaluating EMW absorption capability. The formula for the attenuation constant (α) is as follows:\u003cdiv id=\"Equ3\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equ3\" name=\"EquationSource\"\u003e\n$$\\:\\alpha\\:=2\\pi\\:fc{\\epsilon\\:}^{\u0026quot;}{\\mu\\:}^{\u0026quot;}-{\\epsilon\\:}^{{\\prime\\:}}{\\mu\\:}^{{\\prime\\:}}+\\sqrt{\\left({\\epsilon\\:}^{{\\prime\\:}}{\\mu\\:}^{\u0026quot;}+{\\epsilon\\:}^{\u0026quot;}{\\mu\\:}^{{\\prime\\:}}\\right)+{\\left({\\epsilon\\:}^{\u0026quot;}{\\mu\\:}^{\u0026quot;}-{\\epsilon\\:}^{{\\prime\\:}}{\\mu\\:}^{{\\prime\\:}}\\right)}^{2}}$$\u003c/div\u003e\u003cdiv class=\"EquationNumber\"\u003e3\u003c/div\u003e\u003c/div\u003e\u003c/p\u003e \u003cp\u003eThe attenuation constant characterizes the attenuation rate of EMW in the material, directly reflecting the material's ability to dissipate electromagnetic energy. As shown in Fig. S5b, the α values of all samples almost increase with frequency, conforming to the typical dispersion behavior of dielectric materials. The effect of interfacial reaction time on the attenuation ability of the composite was initially studied. As the time increased from 12 hours to 36 hours, the attenuation performance of samples T-1-12 T-1-24, and T-1-36 progressively improved. The α value of T-1-12 was always below 80, indicating limited loss capability, while T-1-24 exhibited higher α value than T-1-12, though the maximum value did not exceed 100. Notably, T-1-36 demonstrated α values exceeding 100 in the 12\u0026ndash;18 GHz high frequency region. The longer the interfacial reaction time, the stronger the attenuation ability of the composite. Subsequently, the impact of the GO/aniline feed ratio on the composite\u0026rsquo;s performance was investigated. Under the same reaction time, T-2-36 and T-4-36 exhibited stronger intrinsic loss capability, with their α values significantly higher than those of T-1-12, T-1-24, and T-1-36 samples. Especially, T-3-36 exhibited the most pronounced intrinsic loss, significantly outperforming all other samples across the entire frequency band, reaching a peak of about 280 at 18 GHz. The exceptional attenuation performance enabled the composite to achieve superior Joule heat conversion efficiency [\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e], demonstrating outstanding electromagnetic energy to thermal energy conversion capability. These results indicate that optimizing reaction time and feed ratio allowed for precise control of the microstructure of the composite, thereby effectively tailoring its attenuation characteristics. The high attenuation constant of the material originated from the synergistic effect of multiple loss mechanisms. The conjugated molecular chains of PANI contributed to conductive loss [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. The defect sites in GO induced interface polarization relaxation [\u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e]. The charge accumulation at heterogeneous interfaces triggered tunneling effects [\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e]. The \u0026zwnj;hierarchical structure\u0026zwnj; formed by \u0026zwnj;layered GO\u0026zwnj; and \u0026zwnj;rod-like PANI\u0026zwnj; facilitated \u0026zwnj;multiple reflections and scattering\u0026zwnj; of EMW, further amplifying energy attenuation. When incident EMW penetrated the composite, they undergo \u0026zwnj;repeated reflections\u0026zwnj; between the \u0026zwnj;layered GO\u0026zwnj; and \u0026zwnj;rod-like PANI\u0026zwnj;, resulting in \u0026zwnj;progressive wave attenuation\u0026zwnj;. In addition to defect polarization relaxation and dipole polarization relaxation, charge migration contributed to charge redistribution at the PANI/GO interface [34,45]. Under an electromagnetic field, such polarization generated dielectric relaxation, which further facilitated electromagnetic energy dissipation [46]. The material system contained a variety of polarization relaxation processes: defects at the edges of GO sheets promoted electron transition polarization [43\u0026ndash;44], the dynamic transformation of the quinone-benzenamine structure in PANI chains triggered dipole reorientation [30], and the spatial charge distribution at the PANI/GO heterogeneous interface induced interface polarization [29]. These multiscale relaxation mechanisms collectively enhanced the dielectric loss performance of the material, which was verified by Cole-Cole fitting of the dielectric spectra [34]. The excellent EMW absorption performance of the composite was attributed to the synergistic optimization of attenuation capability and impedance matching, achieving efficient absorption and dissipation of EMW.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003col\u003e \u003cspan\u003e \u003cli\u003e \u003cp\u003eAs discussed above, the EMW absorption mechanism of the PANI/GO composite was shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig8\" class=\"InternalRef\"\u003e8\u003c/span\u003e. It involved multi-physics field coupling processes. Incident electromagnetic waves were partially reflected at the material interface, and the remaining energy entered the absorber interior through the impedance matching layer. Therefore, the three-dimensional network constructed by PANI nanorods and GO nanosheets allowed incident EMW to undergo multiple reflections, prolonging the electromagnetic wave path and enhancing energy dissipation, combined with the high conductivity of PANI to cause significant Joule heating effect [\u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e47\u003c/span\u003e]. Secondly, the intrinsic dipole moment of the benzenoid-quinoid structure in PANI molecular chains and the local polarization of carboxyl groups at the GO edges produced relaxation response under the drive of alternating electromagnetic fields [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. Thirdly, the difference in conductivity between PANI and GO and the dielectric constant difference induced the formation of a space charge accumulation layer at the heterogeneous interface, generating a strong interface polarization electric field [\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e].\u003c/p\u003e \u003c/li\u003e \u003c/span\u003e \u003c/ol\u003e \u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe model design was illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig9\" class=\"InternalRef\"\u003e9\u003c/span\u003ea, which depicted the sample and perfect electrical conductor (PEC). Figures\u0026nbsp;\u003cspan refid=\"Fig9\" class=\"InternalRef\"\u003e9\u003c/span\u003eb-d illustrated the three-dimensional radar cross section (3D RCS), which showed the reflected output of the three samples across the full range of detection angles. T-3-36 owned the weakest wave scattering signal, indicating a better microwave absorption capacity compared to the other samples (GO and PANI). Figure\u0026nbsp;\u003cspan refid=\"Fig9\" class=\"InternalRef\"\u003e9\u003c/span\u003ee provided a visual comparison of the RCS values of different samples at various angles. It is evident that T-3-36 exhibits superior performance compared to the other samples with RCS values below \u0026minus;\u0026thinsp;15 dBm\u003csup\u003e2\u003c/sup\u003e for the majority of angles. In conclusion, the RCS results indicate that T-3-36 has the potential for practical application.\u003c/p\u003e \u003c/div\u003e"},{"header":"4. Conclusions","content":"\u003cp\u003eIn summary, PANI/GO composites were successfully through interfacial synthesis. The structure-performance relationship between their nanostructures and electromagnetic wave absorption properties was systematically revealed. Experiments showed that when the reaction time was optimized to 36 h and the feed molar ratio of aniline to GO was adjusted to 3:1, the obtained PANI/GO composite exhibited optimal EMW absorption characteristics with a RL\u003csub\u003emin\u003c/sub\u003e of -48 dB and an EAB of 4.8 GHz. The excellent EMW absorption performance originated from the successful exfoliation of GO and the construction of three-dimensional network of the composite. The synergistic interaction between PANI and GO introduced significant dipole and interface polarization effects and constituted an efficient conductive network, thereby achieving efficient dissipation of electromagnetic energy through the synergy of dielectric relaxation and conductive loss. This work provides an alternative way for the advancement of EMW absorption composites with multi-heterogeneous and hierarchical structures.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e \u003ch2\u003eDeclaration of competing interest\u003c/h2\u003e \u003cp\u003eThe authors declare the following financial interests/personal relationships which may be considered as potential competing interests. Liang Li reports financial support was provided by National Natural Science Foundation of China, If there are other authors, they declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.\u003c/p\u003e \u003c/p\u003e\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eL. Tang conceived the main research and wrote the main manuscript text. T. Li, H. Huang, and X. Yu completed data organization and management. Y. Yu participated in the entire process of data collection and literature review, while J. Ji was responsible for obtaining funding and completing the simulation calculations. L. Li has completed the final draft of the manuscript. All authors have reviewed the manuscript.\u003c/p\u003e\u003ch2\u003eAcknowledgments\u003c/h2\u003e \u003cp\u003eThis work has been supported by National Natural Science Foundation of China (No. U24A20554), Guizhou Provincial Science and Technology Major Special Project ([2024]012), and Key R\u0026amp;D Plan of Hubei Province (2023BAB100).\u003c/p\u003e\u003ch2\u003eData Availability\u003c/h2\u003e\u003cp\u003eAll data supporting the findings of this study can be found in the paper and its supplementary information. Detailed data can be found in the supplementary materials, along with the original references used in this study.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eY. Huang, H. Zhang, G. Zeng, Z. Li, D. 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Lai, Preparation of Polyaniline/Graphene Composites and Their Electromagnetic Wave Absorption Performance., M.S. Thesis, Nanjing University of Science and Technology, 2018\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":true,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true},"keywords":"Graphene Oxide, Polyaniline, Interfacial Synthesis, Electromagnetic Wave Absorption","lastPublishedDoi":"10.21203/rs.3.rs-8247974/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-8247974/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eConventional methods for preparing polyaniline/graphene composites often suffer from issues such as insufficient intermolecular crosslinking and uncontrollable morphological microstructure, leading to long-standing application limitations in the field of electromagnetic wave absorption. This study successfully achieved the controlled composite of polyaniline (PANI) on the surface of graphene oxide (GO) nanosheets using a one-pot interfacial synthesis method. It efficiently exfoliated the expanded layer structure of GO nanosheets and formed a three-dimensional interpenetrating network structure. This structural feature together with the interaction between PANI and GO significantly enhanced the electromagnetic loss capability of the composite material. When the PANI/GO molar ratio was optimized to 3:1, the reflection loss (RL) of the composite reached \u0026minus;\u0026thinsp;48 dB, and the effective absorption bandwidth (RL \u0026le; -10 dB) extended to 4.8 GHz. By constructing multiphase heterogeneous interface, the composite achieved ideal impedance matching characteristics and multiple polarization relaxation mechanisms, which were verified by measured input impedance curves and Cole-Cole semicircular curves. When the sample thickness was adjusted within the range of 2.2-5.0 mm, its effective absorption bandwidth could reach 11 GHz (5\u0026ndash;16 GHz), demonstrating excellent broadband wave absorption performance. This study provides a reference for designing novel electromagnetic functional composite materials with multi-heterogeneous and hierarchical structures. The tunable nanostructure of the PANI/GO composite prepared via interfacial synthesis holds promise in providing solutions in the development of electromagnetic wave absorption technology.\u003c/p\u003e","manuscriptTitle":"Interfacial Synthesis of Polyaniline/Graphene Oxide Composites for Tunable Electromagnetic Wave Absorption","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2026-01-08 17:59:43","doi":"10.21203/rs.3.rs-8247974/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"a1a062af-efcf-42b5-bc84-2c499ef1fdc7","owner":[],"postedDate":"January 8th, 2026","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[],"tags":[],"updatedAt":"2026-03-16T16:04:26+00:00","versionOfRecord":{"articleIdentity":"rs-8247974","link":"https://doi.org/10.1007/s10854-026-16895-9","journal":{"identity":"journal-of-materials-science-materials-in-electronics","isVorOnly":false,"title":"Journal of Materials Science: Materials in Electronics"},"publishedOn":"2026-03-12 15:58:38","publishedOnDateReadable":"March 12th, 2026"},"versionCreatedAt":"2026-01-08 17:59:43","video":"","vorDoi":"10.1007/s10854-026-16895-9","vorDoiUrl":"https://doi.org/10.1007/s10854-026-16895-9","workflowStages":[]},"version":"v1","identity":"rs-8247974","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-8247974","identity":"rs-8247974","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}

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