Modeling Reactions on the Solid-Liquid Interface With Next Generation Extended Lagrangian Quantum-Based Molecular Dynamics
Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室）；University of Illinois Urbana-Champaign（伊利诺伊大学厄巴纳-香槟分校）
Rae A. Corrigan Grove, Kevin G. Kleiner, Joshua Finkelstein, Ivana Matanovic, Michael E. Wall, Travis E. Jones, Anders M. N. Niklasson, Christian F. A. Negre
We present a series of simulations of the oxygen reduction reaction (ORR) using a novel framework for atomistic simulations of surface catalysis under electrochemical bias. The framework makes use of quantum-mechanical extended Lagrangian Born-Oppenheimer molecular dynamics (XL-BOMD) simulations, which provide the speed and accuracy required for explicit atomistic treatment of both electrode and electrolyte. Simulations of solvated O$_2$ near nitrogen-doped graphene (NG) were performed to gain insight into the ORR, and different mechanisms were observed, depending on the applied bias. Under higher bias the ORR occurred by an outer-sphere mechanism, without adsorption of O$_2$ to NG. In this mechanism, electron transfer between the catalyst and the O$_2$ was mediated by the solvent. Under lower bias the ORR occurred by an inner-sphere mechanism involving adsorption of O$_2$ to NG, leading to direct electron transfer. Our extensive, all-atom quantum-mechanical molecular dynamics simulations also show clear differences between the kinetics of the ORR on this ideally polarizable electrode and commonly used kinetic theories, leading to new insights regarding mechanistic changes with varied overpotentials. Combining quantum accuracy with explicit solvation and electrostatic potential bias, XL-BOMD opens a route to predictive, atomistic insight into electrocatalytic processes, as demonstrated with the ORR.
Emerging Oscillating Reactions at the Insulator/Semiconductor Solid/Solid Interface via Proton Implantation
大多数振荡反应（OR）发生在溶液中。很少有现有的基于固体的OR发生在固体/气体上（例如，氧化或腐蚀）或固/液界面，或在与金属或离子导体相邻的全固体界面（例如，电解或电解）。本文报道了一种新型的全固态OR，它发生在绝缘体（非晶SiO $_2$）/半导体（Si）界面，界面点缺陷作为振荡物种。该OR是H. Schmalzried et al.和J. Janek et al.几十年前。我们使用质子注入作为振荡的驱动力，并采用常见的半导体器件表征技术来监测原位振荡。该方法不仅克服了固体中反应检测的困难，而且能够准确测量界面带电点缺陷的振荡超低浓度（$10^{10}\sim10^{11}$ cm $^{-2}$）。我们提出了一个机制，为报告PDC-OR的基础上，通过识别的界面反应的选择器模型。
Gas-solid Reaction Dynamics on Li$_6$PS$_5$Cl Surfaces: A Case Study of the Influence of CO$_2$ and CO$_2$/O$_2$ Atmospheres Using AIMD and MLFF Simulations
Coupled reaction and diffusion governing interface evolution in solid-state batteries
Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University（哈佛大学约翰·A·保罗森工程与应用科学学院）；Robert Bosch LLC Research and Technology Center（罗伯特·博世有限公司研究与技术中心）
Inward-growth plating of lithium driven by solid-solution based alloy phase for highly reversible lithium metal anode
锂金属电池（LMB）是用于高能量密度能量存储的重要装置，但是Li金属阳极与电解质高度反应并形成不受控制的枝晶，其可引起不期望的寄生反应，从而降低循环稳定性并引起安全问题。尽管在部分解决这些问题方面取得了显著进展，但Li金属仍然在电极/电解质界面处电镀，在该界面处总是发生寄生反应和枝晶形成。在这里，我们展示了向内生长电镀锂到金属箔，同时避免表面沉积，这是由可逆的固溶体基合金相变驱动。固溶体合金相的锂化促进了在表面处新产生的Li原子下沉到箔中，而可逆的合金相变伴随着脱锂期间的脱合金反应，其从箔内部提取Li原子。得到的无枝晶Li阳极产生99.5 ± 0.2%的增强的库仑效率，可逆容量为1660 mA h $g^{-1}$（3.3 mA h cm $^{-2}$）。
Identification of Solid-Electrolyte Interphase Species by Joint Characterization of Li-ion Battery Chemistry by Mass Spectrometry and Electro-Chemical Reaction Networks
Bakar Institute of Digital Materials for the Planet, University of California at Berkeley（加州大学伯克利分校巴克数字材料星球研究所）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；Department of Materials Science and Engineering, University of California at Berkeley（加州大学伯克利分校材料科学与工程系）；Université de Rouen Normandie, INSA Rouen Normandie, Université de Caen Normandie, ENSICAEN, CNRS, Institut CARMeN UMR 6064（鲁昂诺曼底大学、鲁昂国立应用科学学院、卡昂诺曼底大学、ENSICAEN、法国国家科学研究中心CARMeN联合研究所）；TotalEnergies OneTech, TotalEnergies Research & Technology Gonfreville（道达尔能源OneTech、道达尔能源贡夫勒维尔研究与技术部）；Saft, Corporate Research（萨博公司企业研究部）；International Joint Laboratory-Complex Matrices Molecular Characterization (iC2MC)（国际联合实验室-复杂基体分子表征）；TotalEnergies OneTech Belgium（道达尔能源OneTech比利时）；TotalEnergies EP Research & Technology（道达尔能源勘探与生产研究与技术部）；Universite de Pau et des Pays de l’Adour, CNRS, IPREM（波城与阿杜尔地区大学、法国国家科学研究中心IPREM）
