Graphical Abstract

Microwave absorption materials are prone to degradation in extremely humid and salty environments, and it is still challenging to develop a dense and firm interface to protect microwave absorbers. Herein, a robust FeSiAl@PUA@SiO2 (PUA: acrylic polyurethane) gradient hybrid was prepared through plasma-enhanced chemical vapor deposition (PECVD) to achieve efficient microwave absorption and anti-corrosion properties. The organic/inorganic dual coat of PUA/SiO2 not only facilitated the interface polarization but also effectively reduced the dielectric constant and optimized impedance matching. Owing to the unique hybrid structure, the (PECVD-FeSiAl@PUA)@SiO2 exhibited highly efficient microwave absorbing performance in frequency bands covering almost the entire Ku-bands (12–18 GHz) with a minimum reflection loss (RLmin) of −47 dB with a matching thickness of 2.3 mm. The organic/inorganic dual protection effectively shields against the corrosive medium, as the corrosion potential and the polarization resistance increased from −0.167 to −0.047 V and 8,064 to 16,273 Ω·cm2, respectively. While the corrosion current decreased from 3.04 × 10−6 to 2.16 × 10−6 A/cm2. Hence, the plasma-enhanced densification of PUA created a strong bridge to integrate FeSiAl and organic/inorganic components acquiring dual-function of efficient microwave absorption and anti-corrosion, which opened a promising platform for potential practical absorbers.
Zhang, K. L.; Zhang, J. Y.; Hou, Z. L.; Bi, S.; Zhao, Q. L. Multifunctional broadband microwave absorption of flexible graphene composites. Carbon 2019, 141, 608–617.
Wang, Y. Y.; Zhu, J. L.; Li, N.; Shi, J. F.; Tang, J. H.; Yan, D. X.; Li, Z. M. Carbon aerogel microspheres with in-situ mineralized TiO2 for efficient microwave absorption. Nano Res. 2022, 15, 7723–7730.
Meng, X.; He, L.; Liu, Y. Q.; Yu, Y. S.; Yang, W. W. Carbon-coated defect-rich MnFe2O4/MnO heterojunction for high-performance microwave absorption. Carbon 2022, 194, 207–219.
Hu, Q. M.; Yang, R. L.; Mo, Z. C.; Lu, D. W.; Yang, L. L.; He, Z. F.; Zhu, H.; Tang, Z. K.; Gui, X. C. Nitrogen-doped and Fe-filled CNTs/NiCo2O4 porous sponge with tunable microwave absorption performance. Carbon 2019, 153, 737–744.
Fu, H. H.; Guo, Y.; Yu, J.; Shen, Z.; Zhao, J.; Xie, Y.; Ling, Y.; Ouyang, S.; Li, S. Q.; Zhang, W. Tuning the shell thickness of core–shell α-Fe2O3@SiO2 nanoparticles to promote microwave absorption. Chin. Chem. Lett. 2022, 33, 957–962.
Ren, S. N.; Yu, H. J.; Wang, L.; Huang, Z. K.; Lin, T. F.; Huang, Y. D.; Yang, J.; Hong, Y. C.; Liu, J. Y. State of the art and prospects in metal−organic framework-derived microwave absorption materials. Nano-Micro Lett. 2022, 14, 68.
Arai, K. I.; Tsuya, N.; Ohmori, K.; Yamamoto, T.; Miyazaki, T. Magnetic properties of ribbon-form sendust alloy. J. Magn. Magn. Mater. 1980, 19, 85–87.
Wakiyama, T.; Takahashi, M.; Nishimaki, S.; Shimoda, J. Magnetic properties of Fe-Si-Al single crystals. IEEE Trans. Magn. 1981, 17, 3147–3150.
Wu, Y. P.; Gao, X.; Cheng, J. X.; Wen, W. W.; Wang, Q. B.; Zhu, Z. M. Optimum design for permittivity of dielectric absorbing materials. J. Phys. Conf. Ser. 2021, 1765, 012002.
Qing, Y. C.; Su, J. B.; Wen, Q. L.; Luo, F.; Zhu, D. M.; Zhou, W. C. Enhanced dielectric and electromagnetic interference shielding properties of FeSiAl/Al2O3 ceramics by plasma spraying. J. Alloys Compd. 2015, 651, 259–265.
Duan, Y. P.; Liu, W.; Song, L. L.; Wang, T. M. A discrete structure: FeSiAl/carbon black composite absorption coatings. Mater. Res. Bull. 2017, 88, 41–48.
Zhou, L.; Huang, J. L.; Wang, H. B.; Chen, M.; Dong, Y. L.; Zheng, F. K. FeSiAl/ZnO-filled resin composite coatings with enhanced dielectric and microwave absorption properties. J. Mater. Sci. Mater. Electron. 2019, 30, 1896–1906.
Liu, D.; Wu, C.; Yan, M.; Wang, J. Correlating the microstructure, growth mechanism and magnetic properties of FeSiAl soft magnetic composites fabricated via HNO3 oxidation. Acta Mater. 2018, 146, 294–303.
Liu, W.; Shao, Q. W.; Ji, G. B.; Liang, X. H.; Cheng, Y.; Quan, B.; Du, Y. W. Metal–organic-frameworks derived porous carbon-wrapped Ni composites with optimized impedance matching as excellent lightweight electromagnetic wave absorber. Chem. Eng. J. 2017, 313, 734–744.
Xu, C. Y.; Wang, L.; Li, X.; Qian, X.; Wu, Z. C.; You, W. B.; Pei, K.; Qin, G.; Zeng, Q. W.; Yang, Z. Q. et al. Hierarchical magnetic network constructed by CoFe nanoparticles suspended within “tubes on rods” matrix toward enhanced microwave absorption. Nano-Micro Lett. 2021, 13, 47.
Ma, G. J.; Duan, Y. P.; Liu, Y.; Gao, S. H. Effect of surface modified SiO2 powders on microwave absorbing properties of flaky FeSiAl coatings. J. Mater. Sci. Mater. Electron. 2018, 29, 17405–17415.
Guo, Y.; Zhang, X. Z.; Feng, X. Q.; Jian, X.; Zhang, L.; Deng, L. J. Non-isothermal oxidation kinetics of FeSiAl alloy powder for microwave absorption at high temperature. Compos. B. Eng. 2018, 155, 282–287.
Chen, Y. H.; Huang, Z. H.; Lu, M. M.; Cao, W. Q.; Yuan, J.; Zhang, D. Q.; Cao, M. S. 3D Fe3O4 nanocrystals decorating carbon nanotubes to tune electromagnetic properties and enhance microwave absorption capacity. J. Mater. Chem. A 2015, 3, 12621–12625.
Tian, W.; Li, J. Y.; Liu, Y. F.; Deng, L. J.; Guo, Y.; Jian, X. Large-scale synthesis of fluorine-free carbonyl iron-organic silicon hydrophobic absorbers with long term corrosion protection property. Nano Res. 2022, 15, 9479–9491.
Cao, L.; Jiang, J. T.; Wang, Z. Q.; Gong, Y. X.; Liu, C.; Zhen, L. Electromagnetic properties of flake-shaped Fe-Si alloy particles prepared by ball milling. J. Magn. Magn. Mater. 2014, 368, 295–299.
Guo, Y.; Ali, R.; Zhang, X. Z.; Tian, W.; Zhang, L.; Lu, H. P.; Jian, X.; Xie, J. L.; Deng, L. J. Raman and XPS depth profiling technique to investigate the corrosion behavior of FeSiAl alloy in salt spray environment. J. Alloys Compd. 2020, 834, 155075.
Li, J. Y.; Guo, Y.; Yang, R. Q.; Liu, Z. Y.; Tian, H. X.; Tian, W.; Liu, Y. F.; Jian, X. Achieving ultra-low frequency microwave absorbing properties based on anti-corrosive silica-pinned flake FeSiAl hybrid with full L band absorption. J. Alloys Compd. 2021, 888, 161574.
Zhang, X. Z.; Guo, Y.; Ali, R.; Tian, W.; Liu, Y. F.; Zhang, L.; Wang, X.; Zhang, L. B.; Yin, L. J.; Su, H. et al. Bifunctional carbon-encapsulated FeSiAl hybrid flakes for enhanced microwave absorption properties and analysis of corrosion resistance. J. Alloys Compd. 2020, 828, 154079.
Liu, S.; Qin, S. H.; Jiang, Y.; Song, P. G.; Wang, H. Lightweight high-performance carbon-polymer nanocomposites for electromagnetic interference shielding. Compos. Part A Appl. Sci. Manuf. 2021, 145, 106376.
Chen, K. X.; Liu, M.; Shi, Y. Q.; Wang, H. R.; Fu, L. B.; Feng, Y. Z.; Song, P. A. Multi-hierarchical flexible composites towards superior fire safety and electromagnetic interference shielding. Nano Res. 2022, 15, 9531–9543.
Tang, T. T.; Wang, S. C.; Jiang, Y.; Xu, Z. G.; Chen, Y.; Peng, T. S.; Khan, F.; Feng, J. B.; Song, P. G.; Zhao, Y. Flexible and flame-retarding phosphorylated MXene/polypropylene composites for efficient electromagnetic interference shielding. J. Mater. Sci. Technol. 2022, 111, 66–75.
Chen, K. X.; Feng, Y. Z.; Shi, Y. Q.; Wang, H. R.; Fu, L. B.; Liu, M.; Lv, Y. C.; Yang, F. Q.; Yu, B.; Liu, M. H. et al. Flexible and fire safe sandwich structured composites with superior electromagnetic interference shielding properties. Compos. Part A Appl. Sci. Manuf. 2022, 160, 107070.
Liu, L.; Ma, Z. W.; Zhu, M. H.; Liu, L. N.; Dai, J. F.; Shi, Y. Q.; Gao, J. F.; Dinh, T.; Nguyen, T.; Tang, L. C. et al. Superhydrophobic self-extinguishing cotton fabrics for electromagnetic interference shielding and human motion detection. J. Mater. Sci. Technol. 2023, 132, 59–68.
Maklakov, S. S.; Lagarkov, A. N.; Maklakov, S. A.; Adamovich, Y. A.; Petrov, D. A.; Rozanov, K. N.; Ryzhikov, I. A.; Zarubina, A. Y.; Pokholok, K. V.; Filimonov, D. S. Corrosion-resistive magnetic powder Fe@SiO2 for microwave applications. J. Alloys Compd. 2017, 706, 267–273.
Xue, F.; Jia, D. M.; Li, Y.; Jing, X. L. Facile preparation of a mechanically robust superhydrophobic acrylic polyurethane coating. J. Mater. Chem. A 2015, 3, 13856–13863.
Pan, Y.; Li, J. Y.; Liu, Z. Y.; Yang, R. Q.; Liu, Y. F.; Yin, L. J.; Liu, H. K.; Jian, X. Inorganic/organic bilayer of silica/acrylic polyurethane decorating FeSiAl for enhanced anti-corrosive microwave absorption. Appl. Surf. Sci. 2021, 567, 150829.
Nguyen, B. Q. H.; Shanmugasundaram, A.; Hou, T. F.; Park, J.; Lee, D. W. Realizing the flexible and transparent highly-hydrophobic film through siloxane functionalized polyurethane-acrylate micro-pattern. Chem. Eng. J. 2019, 373, 68–77.
Xu, J. J.; Wang, K.; Zu, S. Z.; Han, B. H.; Wei, Z. X. Hierarchical nanocomposites of polyaniline nanowire arrays on graphene oxide sheets with synergistic effect for energy storage. ACS Nano 2010, 4, 5019–5026.
Liu, P. B.; Gao, S.; Wang, Y.; Huang, Y.; He, W. J.; Huang, W. H.; Luo, J. H. Carbon nanocages with N-doped carbon inner shell and Co/N-doped carbon outer shell as electromagnetic wave absorption materials. Chem. Eng. J. 2020, 381, 122653.
Guo, Y.; Jian, X.; Zhang, L.; Mu, C. H.; Yin, L. J.; Xie, J. L.; Mahmood, N.; Dou, S. X.; Che, R. C.; Deng, L. J. Plasma-induced FeSiAl@Al2O3@SiO2 core–shell structure for exceptional microwave absorption and anti-oxidation at high temperature. Chem. Eng. J. 2020, 384, 123371.
Tian, W.; Zhang, X. Z.; Guo, Y.; Mu, C. H.; Zhou, P. H.; Yin, L. J.; Zhang, L. B.; Zhang, L.; Lu, H. P.; Jian, X. et al. Hybrid silica-carbon bilayers anchoring on FeSiAl surface with bifunctions of enhanced anti-corrosion and microwave absorption. Carbon 2021, 173, 185–193.
Ma, Y. J.; Ye, Y. P.; Wan, H. Q.; Chen, L.; Zhou, H. D.; Chen, J. M. Chemical modification of graphene oxide to reinforce the corrosion protection performance of UV-curable polyurethane acrylate coating. Prog. Org. Coat. 2020, 141, 105547.
Jian, X.; Tian, W.; Li, J. Y.; Deng, L. J.; Zhou, Z. W.; Zhang, L.; Lu, H. P.; Yin, L. J.; Mahmood, N. High-temperature oxidation-resistant ZrN0.4B0.6/SiC nanohybrid for enhanced microwave absorption. ACS Appl. Mater. Interfaces 2019, 11, 15869–15880.
Liu, P. J.; Ng, V. M. H.; Yao, Z. J.; Zhou, J. T.; Lei, Y. M.; Yang, Z. H.; Lv, H. L.; Kong, L. B. Facile synthesis and hierarchical assembly of flowerlike NiO structures with enhanced dielectric and microwave absorption properties. ACS Appl. Mater. Interfaces 2017, 9, 16404–16416.
Yan, L. W.; Hong, C. Q.; Sun, B. Q.; Zhao, G. D.; Cheng, Y. H.; Dong, S.; Zhang, D. Y.; Zhang, X. H. In situ growth of core–sheath heterostructural SiC nanowire arrays on carbon fibers and enhanced electromagnetic wave absorption performance. ACS Appl. Mater. Interfaces 2017, 9, 6320–6331.
Byun, K. M.; Lee, W. J. Deposition characteristics of low dielectric constant SiOF films prepared by ECR PECVD. Met. Mater. 2000, 6, 155–160.
Zhang, J. J.; Li, Z. H.; Qi, X. S.; Gong, X.; Xie, R.; Deng, C. Y.; Zhong, W.; Du, Y. W. Constructing flower-like core@shell MoSe2-based nanocomposites as a novel and high-efficient microwave absorber. Compos. B Eng. 2021, 222, 109067.
Zhou, L.; Gao, L.; Yang, M.; Zhang, B. S.; Wei, G. K. In situ growth of nanocarbon-coated Ni particles by PECVD for enhanced microwave absorption. J. Mater. Sci. Mater. Electron. 2022, 33, 16306–16319.
Li, C.; Qi, X. S.; Gong, X.; Peng, Q.; Chen, Y. L.; Xie, R.; Zhong, W. Magnetic–dielectric synergy and interfacial engineering to design yolk–shell structured CoNi@void@C and CoNi@void@C@MoS2 nanocomposites with tunable and strong wideband microwave absorption. Nano Res. 2022, 15, 6761–6771.
Wang, G. Z.; Gao, Z.; Tang, S. W.; Chen, C. Q.; Duan, F. F.; Zhao, S. C.; Lin, S. W.; Feng, Y. H.; Zhou, L.; Qin, Y. Microwave absorption properties of carbon nanocoils coated with highly controlled magnetic materials by atomic layer deposition. ACS Nano 2012, 6, 11009–11017.
Hou, T. Q.; Jia, Z. R.; Dong, Y. H.; Liu, X. H.; Wu, G. L. Layered 3D structure derived from MXene/magnetic carbon nanotubes for ultra-broadband electromagnetic wave absorption. Chem. Eng. J. 2022, 431, 133919.
Zhang, J. J.; Qi, X. S.; Gong, X.; Peng, Q.; Chen, Y. L.; Xie, R.; Zhong, W. Microstructure optimization of core@shell structured MSe2/FeSe2@MoSe2 (M = Co, Ni) flower-like multicomponent nanocomposites towards high-efficiency microwave absorption. J. Mater. Sci. Technol. 2022, 128, 59–70.
Li, C.; Li, Z. H.; Qi, X. S.; Gong, X.; Chen, Y. L.; Peng, Q.; Deng, C. Y.; Jing, T.; Zhong, W. A generalizable strategy for constructing ultralight three-dimensional hierarchical network heterostructure as high-efficient microwave absorber. J. Colloid Interface Sci. 2022, 605, 13–22.
Yang, P. A.; Huang, Y. X.; Li, R.; Huang, X.; Ruan, H. B.; Shou, M. J.; Li, W. J.; Zhang, Y. X.; Li, N.; Dong, L. C. Optimization of Fe@Ag core–shell nanowires with improved impedance matching and microwave absorption properties. Chem. Eng. J. 2022, 430, 132878.
Han, M. Y.; Zhou, M.; Wu, Y.; Zhao, Y.; Cao, J. M.; Tang, S. L.; Zou, Z. Q.; Ji, G. B. Constructing angular conical FeSiAl/SiO2 composites with corrosion resistance for ultra-broadband microwave absorption. J. Alloys Compd. 2022, 902, 163792.
Zhang, Z. Y.; Zhao, Y. H.; Li, Z. H.; Zhang, L. J.; Liu, Z. X.; Long, Z. K.; Li, Y. J.; Liu, Y.; Fan, R. H.; Sun, K. et al. Synthesis of carbon/SiO2 core–sheath nanofibers with Co-Fe nanoparticles embedded in via electrospinning for high-performance microwave absorption. Adv. Compos. Hybrid Mater. 2022, 5, 513–524.
Ma, Z.; Zhang, Y.; Cao, C. T.; Yuan, J.; Liu, Q. F.; Wang, J. B. Attractive microwave absorption and the impedance match effect in zinc oxide and carbonyl iron composite. Phys. B 2011, 406, 4620–4624.
Meng, X.; Lei, W. J.; Yang, W. W.; Liu, Y. Q.; Yu, Y. S. Fe3O4 nanoparticles coated with ultra-thin carbon layer for polarization-controlled microwave absorption performance. J. Colloid Interface Sci. 2021, 600, 382–389.
Yang, H.-J.; Cao, W.-Q.; Zhang, D.-Q.; Su, T.-J.; Shi, H.-L.; Wang, W.-Z.; Yuan, J.; Cao, M.-S. NiO hierarchical nanorings on SiC: Enhancing relaxation to tune microwave absorption at elevated temperature. ACS Appl. Mater. Interfaces 2015, 7, 7073–7077.
Wang, X. X.; Cao, W. Q.; Cao, M. S.; Yuan, J. Assembling nano-microarchitecture for electromagnetic absorbers and smart devices. Adv. Mater. 2020, 32, 2002112.
Wu, M.; Darboe, A. K.; Qi, X. S.; Xie, R.; Qin, S. J.; Deng, C. Y.; Wu, G. L.; Zhong, W. Optimization, selective and efficient production of CNTs/CoXFe3−XO4 core/shell nanocomposites as outstanding microwave absorbers. J. Mater. Chem. C 2020, 8, 11936–11949.
Ye, Y. W.; Liu, Z. Y.; Liu, W.; Zhang, D. W.; Zhao, H. C.; Wang, L. P.; Li, X. G. Superhydrophobic oligoaniline-containing electroactive silica coating as pre-process coating for corrosion protection of carbon steel. Chem. Eng. J. 2018, 348, 940–951.