Citation: He Ma, Kang Liang, Weizong Wang, Zhengping Ding, Lin Shi, Yurong Ren, Qian Zhao, Shoukun Xu. Enhanced low-temperature performance of Si/C composite anode materials with graphite (1010) surface: Insights from DFT and AIMD simulations[J]. Chinese Chemical Letters, ;2026, 37(7): 111125. doi: 10.1016/j.cclet.2025.111125 shu

Enhanced low-temperature performance of Si/C composite anode materials with graphite (1010) surface: Insights from DFT and AIMD simulations

He Ma ^a ,
Kang Liang ^a ,
Weizong Wang ^a ,
Zhengping Ding ^a ,
Lin Shi ^b ,
Yurong Ren ^{a, *,} ,
Qian Zhao ^{a, *,} ,
Shoukun Xu ^{b, *,}

a.
School of Materials Science and Engineering, Changzhou Key Laboratory of Intelligent Manufacturing and Advanced Technology for Power Battery, Changzhou University, Changzhou 213164, China
b.
School of Computer Science and Artificial Intelligence, Changzhou University, Changzhou 213164, China

ryrchem@cczu.edu.cn

qzhao@cczu.edu.cn

xsk@cczu.edu.cn

Received Date: 3 January 2025
Revised Date: 5 March 2025
Accepted Date: 20 March 2025
Available Online: 20 March 2025

Figures(4)

Silicon/graphite (Si/C) composites, which combine the advantages of Si anodes and commercial graphite anodes, are promising anode materials for high-energy-density lithium-ion batteries (LIBs). Despite experimental and theoretical studies on the electrochemical characteristics of different silicon crystal surfaces, there have been limited investigations on the electrochemical and mechanical properties of Si composite anode materials with different graphite crystal planes, such as the electrode interfaces between Si₍₁₁₁₎ and graphite (0001), as well as amorphous Si and graphite (1010). In this study, models of Si/C anode interfaces for LIBs were constructed to explore the mechanical-electrochemical-low-temperature performance by density functional theory (DFT) calculations and ab initio molecular dynamics (AIMD) simulations. The calculation results indicate that upon Li intercalation into the graphite (1010) surface, the electrical conductivity, electrochemical adsorption, and interfacial mechanical strength of the Si/C composite are significantly enhanced, with a separation work that is 2.3 times higher than that of Si/C on the graphite (0001) surface. More importantly, AIMD simulations at low temperatures reveal that the interface between graphite (1010) and amorphous Si forms a solid electrolyte interphase (SEI) rich in organic components, which significantly improves the Li-diffusion kinetics. This discovery provides new insights for the design and optimization of Si/C anode materials for low-temperature LIBs.
- Lithium-ion battery,
- Silicon/carbon anode,
- Li⁺ diffusion,
- Interface evolution,
- Low-temperature performance
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