Materials Science

Structural regulation and interface design of high speciflc energy silicon-based anode

  • SHI Liyi ,
  • XU Yuefeng
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  • Center for Nanoscience and Technology Research, Shanghai University, Shanghai 200444, China

Received date: 2025-08-28

  Online published: 2025-11-12

Abstract

Silicon-based anode materials, as a highly potential candidate for the next-generation anode, exhibit a theoretical specific capacity of up to 4 200 mAh$\cdot$g$^{-1}$, significantly surpassing the current commercial graphite anode materials (with a specific capacity of only 372 mAh$\cdot$g$^{-1})$. However, inherent challenges such as poor intrinsic conductivity, severe volumetric expansion, and parasitic surface reactions critically impair their cycling stability and high-rate performance. Especially, t. he unstable solid electrolyte interphase (SEI) on silicon surfaces exacerbates internal polarization, accelerates capacity degradation, and significantly limited cycle life, which have become bottlenecks restricting the commercial application of silicon-based anodes. This review systematically addresses these limitations through structural engineering and interface modification strategies, presenting novel approaches for constructing high-capacity silicon-based anodes and anticipating future research directions. This discourse systematically outlines the design principles and construction methodologies for high-energy-density silicon-based anodes. Through rigorous exploration of material science and structural engineering, this review also demonstrate novel materials, innovative techniques, and advanced protocals on silicon anodes to resolve existing limitations, enhancing the development of silicon-based anodes toward enhanced rate capability, prolonged cycle life, superior safety performance, and broader temperature range.

Cite this article

SHI Liyi , XU Yuefeng . Structural regulation and interface design of high speciflc energy silicon-based anode[J]. Journal of Shanghai University, 2025 , 31(5) : 797 -812 . DOI: 10.12066/j.issn.1007-2861.2707

References

[1] Deng Y, Feng X, Qian Z, et al. Silicon anode modification strategies in solid-state lithium-ion batteries [J]. Materials Horizons, 2025, 12(15): 5513-5538.
[2] Li J, Wang F, Xue L, et al. Research progress on the structure design of nano-silicon anode for high-energy lithium-ion battery [J]. Applied Energy, 2025, 390(23): 125820.
[3] Xu M, Xu C, Sun S, et al. Synergistic multi-carbon strategy enabling Li storage performance of micron-Si anode for flexible lithium ion micro-capacitors [J]. Carbon, 2025, 241(11): 120386.
[4] Jia T, Zhong G, Lv Y, et al. Prelithiation strategies for silicon-based anode in high energy density lithium-ion battery [J]. Green Energy & Environment, 2023, 8(5): 1325-1340.
[5] Wu S, Wu H, Kong X, et al. In-situ construction of dual-coated silicon/carbon composite anode for fast-charging Li-ion batteries [J]. Chemical Engineering Journal, 2024, 502(24): 158032.
[6] Kim M, Moon H, Kim S, et al. Tunable solvation structures for fast charging of micron-Si anodes in energy-dense lithium-ion batteries [J]. Chemical Engineering Journal, 2025, 511(9): 162079.
[7] Yang Z, Trask S E, Wu X, et al. Efiect of Si content on extreme fast charging behavior in silicon-graphite composite anodes [J]. Batteries, 2023, 9(2): 138-150.
[8] Zhu X, Feng W, Huang Y. Improving electrochemical performance of silicon anode through building "soft-hard" double-layer coating [J]. Green Energy & Environment, 2025, 10(3): 609- 618.
[9] Li X, Zhang Z, Gong L, et al. Modelling and analysis of the volume change behaviors of Li-ion batteries with silicon-graphene composite electrodes [J]. Chemical Engineering Journal, 2023, 470(20): 144188.
[10] Han M, Lin Z, Ji X, et al. Growth of flexible and porous surface layers of vertical graphene sheets for accommodating huge volume change of silicon in lithium-ion battery anodes [J]. Materials Today Energy, 2020, 17(3): 100445.
[11] Liu J, Ma R, Zheng W, et al. Cross-linking network of soft-rigid dual chains to effectively suppress volume change of silicon anode [J]. The Journal of Physical Chemistry Letters, 2022, 13(33): 7712-7721.
[12] Ma W, Wu H, Long T, et al. Bamboo inspired silicon anodes with ultrahigh initial coulombic efficiency and high capacity for the Li-ion batteries [J]. Small, 2023, 20(14): 2308109.
[13] Wang J, Gao C, Yang Z, et al. Carbon-coated mesoporous silicon shell-encapsulated silicon nano-grains for high performance lithium-ion batteries anode [J]. Carbon, 2022, 192(7): 277-284.
[14] Cai Y, Liu C, Yu Z, et al. Slidable and highly ionic conductive polymer binder for highperformance Si anodes in lithium-ion batteries [J]. Advanced Science, 2022, 10(6): 2205590.
[15] Jin Y, Zhu B, Lu Z, et al. Challenges and recent progress in the development of Si anodes for lithium-ion battery [J]. Advanced Energy Materials, 2017, 7(23): 1700715.
[16] Chen X, Wang B, Ye Y, et al. Design of electrodes and electrolytes for silicon-based anode lithium-ion batteries [J]. Energy & Environmental Materials, 2024, 8(2): e12838.
[17] Dong Z, Gu H, Du W, et al. Si/Ti3SiC2 composite anode with enhanced elastic modulus and high electronic conductivity for lithium-ion batteries [J]. Journal of Power Sources, 2019, 431(22): 55-62.
[18] Yao J, Zhu G, Huang J, et al. Si/graphite@C composite fabricated by electrostatic self-assembly and following thermal treatment as an anode material for lithium-ion battery [J]. Molecules, 2024, 29(17): 4108.
[19] Liu Y, Su Z, Wang Y, et al. Fabrication of high-performance silicon anode materials for lithium-ion batteries by the impurity compensation doping method [J]. Journal of Solid State Electrochemistry, 2023, 27(4): 969-976.
[20] Ma Y, Wu F, Chen N, et al. Reversing the dendrite growth direction and eliminating the concentration polarization via an internal electric field for stable lithium metal anodes [J]. Chemical Science, 2022, 13(32): 9277-9284.
[21] Zhang R, Xiao Z, Lin Z, et al. Unraveling the fundamental mechanism of interface conductive network influence on the fast-charging performance of SiO-based anode for lithium-ion batteries [J]. Nano-Micro Letters, 2024, 16: 43.
[22] Wang Y, Yang X, Yuan Y, et al. N-rich solid electrolyte interface constructed in situ via a binder strategy for highly stable silicon anode [J]. Advanced Functional Materials, 2023, 33(34): 2301716.
[23] Seo J Y, Kim S, Kim J H, et al. Mechanical shutdown of battery separators: silicon anode failure [J]. Nature Communications, 2024, 15(1): 10134.
[24] Cheng Z, Chen W, Zhang Y, et al. Enhanced cycleability of micron-size silicon anode by in situ polymerized polymer electrolyte [J]. Advanced Functional Materials, 2024, 34(48): 2408145.
[25] Gan C, Ye X, Zhang S, et al. Current density induced growth of Li15Si4 alloy in silicon-carbon anodes during first lithiation process [J]. Journal of Energy Storage, 2021, 41(9): 102930.
[26] Qu Y, Hou C, Tian H, et al. The structural design and electrochemical performances of tetrahedral encapsulated silicon and reduced graphene oxide-polydopamine film composites for anode materials [J]. Journal of Energy Storage, 2025, 119(15): 116404.
[27] Li Z, Hu T, Yang J, et al. In situ constructing of rigid-soft coupling solid-electrolyte interphase on silicon electrode toward high-performance lithium ion batteries [J]. Small, 2023, 20(8): 2305991.
[28] Köbbing L, Latz A, Horstmann B . Voltage hysteresis of silicon nanoparticles: chemomechanical particle-SEI model [J]. Advanced Functional Materials, 2023, 34(7): 2308818.
[29] Quan L, Su Q, Lei H, et al. Integrated prelithiation and SEI engineering for high-performance silicon anodes in lithium-ion batteries [J]. National Science Review, 2025, 12(7): nwaf084.
[30] Mu T, Sun Y, Wang C, et al. Long-life silicon anodes by conformal molecular-deposited polyurea interface for lithium ion batteries [J]. Nano Energy, 2022, 103(13): 107829.
[31] Huang W, Wang Y, Lv L, et al. 1-Hydroxyethylidene-1, 1-diphosphonic acid: a multifunctional interface modifler for eliminating HF in silicon anode [J]. Energy Storage Materials, 2021, 42(9): 493-501.
[32] Li A M, Wang Z, Pollard T P, et al. High voltage electrolytes for lithium-ion batteries with micro-sized silicon anodes [J]. Nature Communications, 2024, 15(1): 1206.
[33] Wang L, Lu J J, Li S Y, et al. Controllable interface engineering for the preparation of high rate silicon anode [J]. Advanced Functional Materials, 2024, 34(40): 2403574.
[34] Zhang S S. Unveiling electrochemical properties of silicon for stable cycling performance of silicon anode materials [J]. Journal of The Electrochemical Society, 2024, 171(7): 070518.
[35] Wu F, Dong Y, Su Y, et al. Benchmarking the effect of particle size on silicon anode materials for lithium-ion batteries [J]. Small, 2023, 19(42): 2301301.
[36] Huang L, Wang J, Hu Y, et al. Low-cost silicon cutting waste reused as a high-power-density silicon-based anode [J]. RSC Advances, 2024, 14(47): 34823-34832.
[37] Shen L, Sun K, Xi F, et al. Conversion of photovoltaic waste silicon into amorphous silicon nanowire anodes [J]. Energy & Environmental Science, 2025, 18(9): 4348-4361.
[38] Luo Y, Guo S, Gao Z, et al. Ethanol-controlled release strategy induced local solvation polymerization of silicates for high-performance nano-silicon anode [J]. Journal of Colloid and Interface Science, 2025, 689(13): 137224.
[39] Qin G, Jia Z, Sun S, et al. Carbon-coated Si nanosheets as anode materials for highperformance lithium-ion batteries [J]. ACS Applied Nano Materials, 2024, 7(7): 7595-7604.
[40] Wan N, Wang L, Li S Y, et al. Engineering high-rate anode materials via montmorillonite-derived silicon nanosheets [J]. Small, 2025: 2412705.
[41] Mados E, Harpak N, Levi G, et al. Synthesis and electrochemical performance of siliconnanowire alloy anodes [J]. RSC Advances, 2021, 11(43): 26586-26593.
[42] Wu H, Du N, Shi X, et al. Rational design of three-dimensional macroporous silicon as high performance Li-ion battery anodes with long cycle life [J]. Journal of Power Sources, 2016, 331(31): 76-81.
[43] Song J, Kou L, Wang Y, et al. A three-dimensional porous Si/SiOx decorated by nitrogendoped carbon as anode materials for lithium-ion batteries [J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2023, 673(17): 131821.
[44] Li Z, Liang Z, Ma Z, et al. Boosting the anode performance of the porous Si coated with polydopamine and cross-linked with sodium alginate [J]. Journal of Alloys and Compounds, 2024, 971(2): 172738.
[45] Yang D, Lv T, Song J, et al. Enabling stable high lithium storage of Si anode via synergistic effects of nanosized Fe3C and partially graphitized porous carbon [J]. Chemical Engineering Journal, 2024, 496(17): 153844.
[46] Li Z, Li D, Sun X, et al. Ion-conductive and mechanically robust chitosan-based network binder for silicon/graphite anode [J]. Journal of Energy Storage, 2024, 93(18): 112264.
[47] Li C, Wang J, Wang X, et al. Regulating the mechano-electrochemistry of graphite-silicon hybrid anode through layered electrode structure design [J]. Journal of Energy Chemistry, 2025, 104(5): 176-184.
[48] Zhao J, Wang B, Zhan Z, et al. Boron-doped three-dimensional porous carbon framework/carbon shell encapsulated silicon composites for high-performance lithium-ion battery anodes [J]. Journal of Colloid and Interface Science, 2024, 664(12): 790-800.
[49] Lee Y, Naikwade M, Lee S W. Interface engineering of styrenic polymer grafted porous micro-silicon/polyaniline composite for enhanced lithium storage anode materials [J]. Polymers, 2024, 16(24): 3544.
[50] Cheng Z, Lin H, Liu Y, et al. A stress-buffering hierarchically porous silicon/carbon composite for high-energy lithium-ion batteries [J]. Advanced Functional Materials, 2025: 2505207.
[51] Xu W, Sun Z, Tang C, et al. Biomimetics-driven design of micron-sized SiO composites for high-performance lithium-ion batteries [J]. Advanced Functional Materials, 2025, 35(25): 2422743.
[52] Hernandha R F H, Umesh B, Patra J, et al. Double nitrogenation layer formed using nitric oxide for enhancing Li+ storage performance, cycling stability, and safety of Si electrodes [J]. Advanced Science, 2024, 11(25): 2310062.
[53] Li W, Xu S, Zhong C, et al. A LiF-pie-structured interphase for silicon anodes [J]. Nano-Micro Letters, 2025, 17(1): 322.
[54] Ma H, Zhao B, Han Z, et al. Integrating robust SEI on recycled micro-sized silicon scrap for stable lithium ion battery [J]. Chemical Engineering Journal, 2025, 507(5): 160149.
[55] Dou F, Weng Y, Wang Q, et al. In situ imaging analysis of the inhibition effect of functional coating on the volume expansion of silicon anodes [J]. Chemical Engineering Journal, 2021, 417(15): 128122.
[56] Wang Q, Zhu M, Chen G, et al. High-performance microsized Si anodes for lithium-ion batteries: insights into the polymer conflguration conversion mechanism [J]. Advanced Materials, 2022, 34(16): 2109658.
[57] Cheng H, Liu Y, Cheng Z, et al. Ti3C2Tx MXene wrapped, carbon-coated porous Si sheets for improved lithium storage performance [J]. Chinese Chemical Letters, 2024, 35(2): 108923.
[58] Zhang Y, Wu B, Bi J, et al. Facilitating prelithiation of silicon carbon anode by localized high-concentration electrolyte for high-rate and long-cycle lithium storage [J]. Carbon Energy, 2024, 6(6): e480.
[59] Sun D, Li J, Nie H. Incorporation of lithium oxide into silicon anode via magnetron cosputtering to optimize structural stability and cycling performance [J]. Ionics, 2024, 31(1): 177-188.
[60] Chen C, Chen G, Nevar A, et al. Enhancing performance of silicon/graphene composites by transition lattice interfaces constructed using plasma [J]. Surfaces and Interfaces, 2024, 50(7): 104468.
[61] Han Z, Maitarad P, Yodsin N, et al. Catalysis-induced highly-stable interface on porous silicon for high-rate lithium-ion batteries [J]. Nano-Micro Letters, 2025, 17(1): 200.
[62] Cheng Z, Lin H, Liu Y, et al. Enabling the transport dynamics and interfacial stability of porous si anode via rigid and flexible carbon encapsulation for high-energy lithium storage [J]. Small, 2024, 20(52): 2407560.
[63] Zou X, Li M, Li H, et al. Three-dimensional CNTs boosting the conductive conflnement structure of silicon/carbon anodes in lithium-ion batteries [J]. Chemical Engineering Journal, 2024, 498(19): 155573.
[64] Fan X, Cai T, Wang S, et al. Carbon nanotube-reinforced dual carbon stress-buffering for highly stable silicon anode material in lithium-ion battery [J]. Small, 2023, 19(30): 2300431.
[65] Guan X, Zhang Y, Kinloch I A, et al. "Nanoskeleton" Si-SiOx/C anodes toward highly stable lithium-ion batteries [J]. ACS Applied Materials & Interfaces, 2025, 17(7): 10580-10592.
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