Density functional theory screening of gas-treatment strategies for stabilization of high energy-density lithium metal anodes
Density functional theory screening of gas-treatment strategies for stabilization of high energy-density lithium metal anodes
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DOI：
10.1016/j.jpowsour.2015.07.027
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发表时间：
2015-05
影响因子：
9.2
通讯作者：
S. Koch;B. Morgan;S. Passerini;G. Teobaldi
中科院分区：
文献类型：
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作者：
S. Koch;B. Morgan;S. Passerini;G. Teobaldi
为了探索分子气体处理新切割的锂箔在高能量密度锂阳极的非电解质钝化中的潜力，密度泛函理论（DFT）已被用于研究分子气体在金属锂表面上的分解。通过DFT几何优化和分子动力学相结合，（N2，O2，CO2）和有害气体（F2，SO2）在Li（bcc）（100），（110）和（111）表面上的相对表面能，功函数，和新兴的电子和弹性性质进行了研究。模拟表明，暴露于不同的分子气体，控制金属Li表面的重构和钝化系统的功函数的实质性变化（高达超过1eV）。与其他考虑的形成金属吸附层的气体相反，SO2处理在形成绝缘钝化层方面最有效，剂量≤1单层。大量的Li →吸附质电荷转移和吸附层弛豫使界面产生明显的弹性硬化，氮处理的吸附层的变化最小。
To explore the potential of molecular gas treatment of freshly cut lithium foils in non-electrolyte-based passivation of high-energy-density Li anodes, density functional theory (DFT) has been used to study the decomposition of molecular gases on metallic lithium surfaces. By combining DFT geometry optimization and Molecular Dynamics, the effects of atmospheric (N2, O2, CO2) and hazardous (F2, SO2) gas decomposition on Li(bcc) (100), (110), and (111) surfaces on relative surface energies, work functions, and emerging electronic and elastic properties are investigated.The simulations suggest that exposure to different molecular gases can be used to induce and control reconstructions of the metal Li surface and substantial changes (up to over 1 eV) in the work function of the passivated system. Contrary to the other considered gases, which form metallic adlayers, SO2treatment emerges as the most effective in creating an insulating passivation layer for dosages ≤1 mono-layer. The substantial Li → adsorbate charge transfer and adlayer relaxation produce marked elastic stiffening of the interface, with the smallest change shown by nitrogen-treated adlayers.