论文标题
电池中显式固体接口的DFT建模：方法和挑战
DFT Modelling of Explicit Solid-Solid Interfaces in Batteries: Methods and Challenges
论文作者
论文摘要
数十年来，高能量密度存储设备（如锂电池）中的电极材料特性的密度功能理论（DFT）计算已成为标准实践。相反，可以说，电池中明确界面的DFT建模缺乏普遍采用的方法，并且需要进一步的概念开发。在本文中，我们专注于固体界面，这些界面不仅是在全稳态的电池中，这些界面无处不在。基于液体电解质的电池通常依靠电极表面上的薄而固体钝化膜来起作用。我们使用金属阳极计算来说明显式界面模型对于阐明接触电势，界面的电场以及相对于寄生反应的动力学稳定性至关重要。示例强调了三个关键挑战：（1）大多数电池电极表面的“脏”性质； （2）电压校准和控制； （3）界面结构受动力学而不是热力学控制的事实。为了应对这些挑战，开发新的计算技术并从其他电化学学科中进口见解将是有益的。
Density Functional Theory (DFT) calculations of electrode material properties in high energy density storage devices like lithium batteries have been standard practice for decades. In contrast, DFT modelling of explicit interfaces in batteries arguably lacks universally adopted methodology and needs further conceptual development. In this paper, we focus on solid-solid interfaces, which are ubiquitous not just in all-solid state batteries; liquid-electrolyte-based batteries often rely on thin, solid passivating films on electrode surfaces to function. We use metal anode calculations to illustrate that explicit interface models are critical for elucidating contact potentials, electric fields at interfaces, and kinetic stability with respect to parasitic reactions. The examples emphasize three key challenges: (1) the "dirty" nature of most battery electrode surfaces; (2) voltage calibration and control; and (3) the fact that interfacial structures are governed by kinetics, not thermodynamics. To meet these challenges, developing new computational techniques and importing insights from other electrochemical disciplines will be beneficial.
