Coupling of 0D/1D Grain Boundaries Inducing Extreme Charge Rearrangement/Magnetic Resonance for Ultrabroadband Electromagnetic Wave Absorption

Abstract

Ferrite–carbon composites effectively absorb electromagnetic (EM) waves via coupled mechanisms. However, the dynamic evolution of intrinsic polarization and magnetic loss mechanisms following interfacial coupling has long been overlooked, impeding broadening of the ultra-broadband EM wave absorption performance in heterostructures. Herein, via surface ligand modulation, in situ growth of 0D Fe₃O₄ quantum dots (QDs) on the surface of 1D carbon nanotubes triggers grain boundary coupling. The energy rebalancing effect at the interface induces an extreme charge rearrangement within the Fe₃O₄ QDs. This rearrangement enhances dipole orientation hysteresis and charge accumulation, resulting in charge and interfacial polarization losses. Meanwhile, for subcritical Fe₃O₄ QDs, short-range magnetic resonance and magnetic exchange–triggered magnetic resonance transfer synergistically enhance the magnetic loss. Through charge rearrangement/magnetic resonance induced by 0D/1D grain boundary coupling, an effective bandwidth of nearly 10 GHz is achieved at a minimal thickness of 2 mm, covering the X and Ku bands. This strategy provides an effective paradigm and novel theoretical insights for ultra-broadband electromagnetic wave absorption applications.

Keywords

charge rearrangement / electromagnetic wave absorption / ferrite–carbon matrix composites / grain boundary coupling

References

[1] Y. Shi, Z. Ma, X. Zhang, et al., “Flexible Film Constructed by Asymmetrically-Coordinated La₁N₄Cl₁ Moieties on Interconnected Nitrogen-Doped Graphene Nanocages for High-Efficiency Electromagnetic Wave Absorption,” Advanced Functional Materials 34, no. 16 (2023): 2313483.

[2] Z. He, L. Shi, R. Sun, et al., “Low-Temperature Oxidation Induced Phase Evolution With Gradient Magnetic Heterointerfaces for Superior Electromagnetic Wave Absorption,” Nano-Micro Letters 17 (2024): 7.

[3] J. Huang, L. Hu, L. Wang, et al., “Constructing Pb-O Bonds to Trigger Efficient Cross-Scale Charge Transfer for High-Performance Electromagnetic Wave Absorption and Multicolor Conversion,” Chemical Engineering Journal 504, no. 15 (2025): 159004.

[4] X. Liu, J. Chen, D. Lan, et al., “Synergistic Polarization Effect of Selenium-Deficient Quantum Dots Integrated Carbon Nanotubes for Superior Electromagnetic Wave Absorption,” Composites Communications 56 (2025): 102390.

[5] Y. Zhang, S. Zhang, D. Lan, et al., “Multiple Charge Carriers Manipulation Toward Semiconductive Ceramic Nanocomposites for Corrosion-Resistant Electromagnetic Wave Absorption,” Small 21, no. 20 (2025): 2500581.

[6] F. Hu, P. Ding, F. Wu, et al., “Novel Cable-Like Tin@Carbon Whiskers Derived From the Ti₂SnC MAX Phase for Ultra-Wideband Electromagnetic Wave Absorption,” Carbon Energy 6, no. 12 (2024): e638.

[7] S. Cheng, D. Sheng, S. Mukherjee, et al., “Carbon Nanolayer-Mounted Single Metal Sites Enable Dipole Polarization Loss Under Electromagnetic Field,” Nature Communications 15 (2024): 9077.

[8] Y. Li, Y. Qing, Y. Zhang, and H. Xu, “Simultaneously Tuning Structural Defects and Crystal Phase in Accordion-Like Ti_xO_2x−1 Derived From Ti₃C₂T_x Mxene for Enhanced Electromagnetic Attenuation,” Journal of Advanced Ceramics 12, no. 10 (2023): 1946–1960.

[9] L. Wang, Y. Wang, J. Lu, et al., “Electromagnetic Absorption by Magnetic Oxide Nanomaterials: A Review,” ACS Applied Nano Materials 6, no. 24 (2023): 22611–22634.

[10] Y. Hou, B. Li, J. Chen, et al., “Electromagnetic Wave Absorption Properties of Core Double-Shell Structured α-Fe(Si)@Fe₃O₄@SiO₂ Composites,” Applied Surface Science 615, no. 1 (2023): 156345.

[11] B. Dai, F. Dong, H. Wang, et al., “Fabrication of CuS/Fe₃O₄@Polypyrrole Flower-Like Composites for Excellent Electromagnetic Wave Absorption,” Journal of Colloid and Interface Science 634, no. 15 (2023): 481–494.

[12] S. Wang, Q. Liu, S. Li, F. Huang, and H. Zhang, “Joule-Heating-Driven Synthesis of a Honeycomb-Like Porous Carbon Nanofiber/High Entropy Alloy Composite as an Ultralightweight Electromagnetic Wave Absorber,” ACS Nano 18, no. 6 (2024): 5040–5050.

[13] Y. Shu, T. Zhao, W. Jia, et al., “A Crosslinked Coral-Like Co@CoO/RGO Nanohybrid Structure With Good Electromagnetic Wave Absorption Performance,” Journal of Colloid and Interface Science 642, no. 15 (2023): 393–407.

[14] B. Du, M. Cai, X. Wang, J. Qian, C. He, and A. Shui, “Enhanced Electromagnetic Wave Absorption Property of Binary ZnO/NiCo₂O₄ Composites,” Journal of Advanced Ceramics 10 (2021): 832–842.

[15] Y. Guo, M. Zhang, T. Cheng, et al., “Enhancing Electromagnetic Wave Absorption in Carbon Fiber Using FeS₂ Nanoparticles,” Nano Research 16 (2023): 9591–9601.

[16] Y. Zhou, C. Tang, S. Li, et al., “Quantifying Heterogeneous Interface Effect of Fe₃O₄(111)/C for Enhanced Low-Frequency Electromagnetic Wave Absorption,” Carbon 232, no. 15 (2025): 119792.

[17] M. Lv, H. Wang, H. Xing, et al., “Bimagnetic Co_xNi_100–x Nanocrystals Anchored on MoS₂ Nanosheets for Applications as Microwave Absorption Materials,” ACS Applied Nano Materials 7, no. 20 (2024): 24201–24212.

[18] Z. Tang, L. Xu, C. Xie, et al., “Synthesis of CuCo₂S₄@Expanded Graphite With Crystal/Amorphous Heterointerface and Defects for Electromagnetic Wave Absorption,” Nature Communications 14 (2023): 5951.

[19] J. Huang, L. Wang, B. Wang, et al., “Unraveling the Carbon Dot Bridges in Oxidized Carbon Nanotubes for Efficient Microwave Absorption,” Chemical Engineering Journal 473, no. 1 (2023): 145356.

[20] G. Ma, Y. Liu, K. Zhang, et al., “Shape-Tunable Vanadium Selenide/Reduced Graphene Oxide Composites With Excellent Electromagnetic Wave Absorption Performance,” Carbon 210, no. 15 (2024): 119795.

[21] F. Yan, J. Qian, S. Wang, and J. Zhai, “Progress and Outlook on Lead-Free Ceramics for Energy Storage Applications,” Nano Energy 123 (2024): 109394.

[22] X. Liu, J. Zhou, Y. Xue, and X. Lu, “Structural Engineering of Hierarchical Magnetic/Carbon Nanocomposites via In Situ Growth for High-Efficient Electromagnetic Wave Absorption,” Nano-Micro Letters 16, no. 1 (2024): 174.

[23] A. Azizi, M. Dogan, J. D. Cain, et al., “Frustration and Atomic Ordering in a Monolayer Semiconductor Alloy,” Physical Review Letters 124, no. 9 (2020): 096101.

[24] S. Lee, “Hot Electron-Driven Chemical Reactions: A Review,” Applied Surface Science Advances 16 (2023): 100428.

[25] W. D. Kaplan and Y. Kauffmann, “Structural Order in Liquids Induced by Interfaces With Crystals,” Annual Review of Materials Research 36, no. 1 (2006): 1–48.

[26] J. Chen, Z. Han, C. Sun, et al., “Air-Microwave Simultaneously Induced Carbon Fiber Surface Oxidation and Magnetism Adjustment by CoO_x Nanoparticles Rapid Assembly for Interface Enhancement and Electromagnetic Wave Absorption of Its Composites,” Journal of Colloid and Interface Science 678, no. 15 (2024): 785–794.

[27] W. Mi, Z. Guo, Q. Wang, Y. Yang, and H. Bai, “Charge Ordering in Reactive Sputtered (100) and (111) Oriented Epitaxial Fe₃O₄ Films,” Scripta Materialia 68, no. 12 (2013): 972–975.

[28] L. L. Li, J. Ji, R. Fei, et al., “A Facile Microwave Avenue to Electrochemiluminescent Two-Color Graphene Quantum Dots,” Advanced Functional Materials 22, no. 14 (2012): 2971–2979.

[29] H. Li, S. Ye, J. Guo, et al., “The Design of Room-Temperature-Phosphorescent Carbon Dots and Their Application as a Security Ink,” Journal of Materials Chemistry C 7, no. 34 (2019): 10605–10612.

[30] B. Shi, H. Liang, Z. Xie, Q. Chang, and H. Wu, “Dielectric Loss Enhancement Induced by the Microstructure of CoFe₂O₄ Foam to Realize Broadband Electromagnetic Wave Absorption,” International Journal of Minerals, Metallurgy, and Materials 30, no. 7 (2023): 1388–1397.

[31] R. Guo, Y. Zhang, X. Zhang, H. Yang, and T. Hu, “CoFe₂O₄ Nanosheets Grown In Situ on Nickel Nanowires for Efficient Hydrazine Oxidation-Boosted Hydrogen Production,” Chemical Engineering Journal 491, no. 1 (2024): 152028.

[32] Z. Zhou, E. V. Ushakova, E. Liu, et al., “A Co-Crystallization Induced Surface Modification Strategy With Cyanuric Acid Modulates the Bandgap Emission of Carbon Dots,” Nanoscale 12, no. 20 (2020): 10987–10993.

[33] X. You, H. Ouyang, R. Deng, et al., “Graphene Aerogel Composites With Self-Organized Nanowires-Packed Honeycomb Structure for Highly Efficient Electromagnetic Wave Absorption,” Nano-Micro Letters 17 (2024): 47.

[34] Z. Ma, Y. Shen, X. Zhang, et al., “Enhanced Dielectric Loss Induced by Asymmetrically Coordinated Iron Single-Atoms With Curved Configurations on Turing-Like Surfaces for Electromagnetic Wave Absorption,” Advanced Functional Materials 35, no. 3 (2024): 2413783.

[35] X. Zhang, Y. Shi, J. Xu, et al., “Identification of The Intrinsic Dielectric Properties of Metal Single Atoms for Electromagnetic Wave Absorption,” Nano-Micro Letters 14 (2021): 27.

[36] J. Huang, L. Wang, B. Wang, G. Liu, W. Wang, and C. Ge, “Research Progress on Modulation of Electromagnetic Performance Through Micro-Nanostructure Design,” Journal of Inorganic Materials 39, no. 8 (2024): 853–870.

[37] P. Liu, Y. Li, H. Xu, et al., “Hierarchical Fe-Co@TiO₂ With Incoherent Heterointerfaces and Gradient Magnetic Domains for Electromagnetic Wave Absorption,” ACS Nano 18, no. 1 (2024): 560–570.

[38] J. Huang, L. Wang, G. Liu, et al., “Regulating Heterogeneous Charge Distribution/Magnetic Resonance via Ligand Constraints for Enhanced Electromagnetic Wave Absorption,” Carbon 238, no. 5 (2025): 120244.

[39] L. Peng, Y. Zhang, M. He, et al., “Generation of High-Density Biskyrmions by Electric Current,” npj Quantum Materials 2 (2017): 30.

[40] J. Wang, Z. Wu, C. Yang, et al., “Controllable Regulation of MoS₂ Surface Atomic Exposure for Boosting Interfacial Polarization and Microwave Absorption,” Advanced Functional Materials 34, no. 51 (2024): 2409923.

[41] L. Li, F. Pan, H. Guo, et al., “Tailored Magnetic Spatial Confinement With Enhanced Polarization and Magnetic Response for Electromagnetic Wave Absorption,” Small 20, no. 46 (2024): 2402564.

[42] S. Tang, J. Niu, C. Gu, et al., “VIS-IR Electrochromic Device With Electromagnetic Wave Absorption Function Based on a Fe₃O₄@PANI Composite Material,” Journal of Materials Chemistry C 12, no. 28 (2024): 10621–10634.

[43] L. Li, Z. He, Z. Wang, H. Kang, D. Li, and Q. Fang, “Sustainable Eucommia ulmoides Gum Composites With Outstanding Electromagnetic Wave Absorption Properties,” Composites Communications 48 (2024): 101945.

[44] H. Pan, L. Xu, K. Li, et al., “The Electromagnetic Wave Absorption Composite of Flower-Like Structure NiCo₂O₄ and Fe₃O₄ Derived From Low-Temperature Preparation Method,” Materials Science and Engineering: B 296 (2023): 116714.

[45] J. Guo, Y. Sun, X. Li, et al., “Carbonization Tuned Core-Shell Fe₃O₄@C Nanostructures With Enhanced Electromagnetic Wave Absorption,” Advanced Materials Interfaces 12, no. 13 (2025): 2500075.

[46] Y. Wu, S. Tan, P. Liu, et al., “Controllable Heterogeneous Interfaces and Dielectric Regulation of Hollow Raspberry-Shaped Fe₃O₄@rGO Hybrids for High-Performance Electromagnetic Wave Absorption,” Journal of Materials Science & Technology 151, no. 10 (2023): 10–18.

[47] W. Zhao, M. Zhang, Y. Miao, et al., “Structural Design and Controllable Preparation of SiCNWs@Fe₃O₄@NC Nanocomposites for Electromagnetic Wave Absorption,” International Journal of Minerals, Metallurgy, and Materials 32, no. 3 (2025): 520–533.

[48] H. Wang, R. Zhang, L. Qu, et al., “Design of MXene-Modified Hierarchical Core-Shell Fe₃O₄@Polypyrrole Composites for Electromagnetic Wave Absorption,” Ceramics International 51 (2025): 44702–44714.

[49] M. Li, F. Wei, Q. Chen, et al., “Multidimensional Fe₃O₄@CoNi-CNTs Composite: Synergizing High-Dielectricity and High-Permeability for Enhanced Electromagnetic Wave Absorption,” Ceramics International 51, no. 15 (2025): 21055–21066.

[50] Q. Wei, Y. Huang, L. Dong, et al., “Fe₃O₄ Nanoparticles Embedded into Pyridinic-N-Rich Carbon Nanohoneycomb With Strong dx²-Pz Orbital Hybridization for High-Performance Electromagnetic Wave Absorption,” ACS Applied Materials & Interfaces 16, no. 29 (2024): 38414–38428.

[51] Z. Guo, J. Ren, X. Xu, et al., “Multiphase Co/Ni Metal Nitrides With Heterointerfaces for Enhanced Interfacial Polarization Loss in Electromagnetic Wave Absorption,” Journal of Materials Science & Technology 236, no. 20 (2025): 19–27.

[52] Y. Cheng, X. Liu, J. Ren, et al., “Component-Based Modulation Engineering to Improve Magnetoelectric Coupling for Self-Anticorrosion Broadband Absorption,” Carbon 239, no. 10 (2025): 120325.

[53] S. Zhang, M. Li, G. Chen, et al., “Achieving High Performance Microwave Attenuation by Anchoring Magnetic CoNi Nanoparticles Onto Few-Layer Ti₃C₂T_xMXene,” Journal of Alloys and Compounds 1023, no. 15 (2025): 180015.

[54] L. Xie, R. Liu, X. Jiang, et al., “Carbon Induced Multiple Interfaces and In-Situ Formed Defects in Oxidation of Co Toward Enhancing Microwave Absorption Performances,” Carbon 238, no. 5 (2025): 120272.

RIGHTS & PERMISSIONS

2025 The Author(s). Carbon Energy published by Wenzhou University and John Wiley & Sons Australia, Ltd.