Reactive force-field simulation and experimental validation of cyclic defects in silicon anodes for lithium-ion batteries

IF 7.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY
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Abstract

Silicon anodes for lithium-ion batteries offer high theoretical capacity but face practical challenges of capacity fading due to significant volumetric changes during charge-discharge cycles. To reveal the underlying mechanisms, we employ reactive force fields (ReaxFFs) in molecular dynamics simulations to conduct atomic analyses of lithiation and delithiation cycles of silicon particles with three diameters. Our simulations demonstrate a volumetric expansion exceeding 280%, primarily along the ⟨110⟩ direction, with an inward movement of the interface between lithiated and unlithiated regions. We introduce a metric, “geometric defect,” derived from the centroid deviation of neighboring atoms, to evaluate the structural integrity of the silicon anode. Geometric defect state of charge curves show a 5% capacity fade due to silicon loss after the initial cycle. Experimental validation confirms a capacity loss exceeding 40% after the first cycle, attributed to internal defects within silicon particles, aligning well with our simulation results.

Abstract Image

锂离子电池硅阳极循环缺陷的反应力场模拟和实验验证
锂离子电池的硅阳极具有很高的理论容量,但在充放电循环过程中,由于体积发生显著变化,因此面临容量衰减的实际挑战。为了揭示其深层机理,我们在分子动力学模拟中采用了反应力场(ReaxFFs),对三种直径的硅颗粒的锂化和脱锂循环进行了原子分析。我们的模拟结果表明,硅颗粒的体积膨胀超过 280%,主要沿⟨110⟩方向膨胀,石化和非石化区域的界面向内移动。我们从相邻原子的中心偏差中引入 "几何缺陷 "指标,以评估硅阳极的结构完整性。几何缺陷电荷状态曲线显示,在初始循环后,由于硅损耗,容量会下降 5%。实验验证证实,在第一个周期后,由于硅颗粒内部缺陷造成的容量损失超过 40%,这与我们的模拟结果非常吻合。
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来源期刊
Cell Reports Physical Science
Cell Reports Physical Science Energy-Energy (all)
CiteScore
11.40
自引率
2.20%
发文量
388
审稿时长
62 days
期刊介绍: Cell Reports Physical Science, a premium open-access journal from Cell Press, features high-quality, cutting-edge research spanning the physical sciences. It serves as an open forum fostering collaboration among physical scientists while championing open science principles. Published works must signify significant advancements in fundamental insight or technological applications within fields such as chemistry, physics, materials science, energy science, engineering, and related interdisciplinary studies. In addition to longer articles, the journal considers impactful short-form reports and short reviews covering recent literature in emerging fields. Continually adapting to the evolving open science landscape, the journal reviews its policies to align with community consensus and best practices.
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