Fast charging is desirable for the global use of full electric vehicles (EVs); however, it faces challenges based on Li kinetics. A structural design based on the electrostatic repulsion (ER) between cations over the full charging process is proposed herein to facilitate the fast Li kinetics of LiMO ( = transition metal) layered oxides in lithium-ion batteries (LIBs). This process is divided into two steps under the Li kinetic mechanism, in which LiO is a transition state upon migration. First, changing the O3- to O2-type layered cathodes causes the expansion of the LiO slab and elimination of the ER between Li and M ions in the hidden space based on the edge-shared mode for the Li-abundant region. Second, expanding the LiO space to release the stressed environment provides easy accommodation of Li ions through the ionic radius of the dopants in the Li-deficient region. Using unified atomistic calculations of density functional theory and kinetic Monte Carlo simulations, the systematic design flow can be understood in terms of the structural parameters, site energetics for the kinetic barrier, and statistical transitions based on various Co-based LiMO models. Our concrete understanding of local-to-macroscopic structural scales suggests a generalized direction for facilitating fast Li kinetics for realizing fast-charging LIBs.

中文翻译：

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促进层状氧化物阴极中快速锂动力学的统一设计流程


快速充电对于全球使用纯电动汽车 (EV) 来说是可取的；然而，它面临着基于锂动力学的挑战。本文提出了一种基于整个充电过程中阳离子之间的静电斥力（ER）的结构设计，以促进锂离子电池（LIB）中LiMO（=过渡金属）层状氧化物的快速Li动力学。在Li动力学机制下，这个过程分为两个步骤，其中LiO是迁移时的过渡态。首先，将 O3 型层状阴极改为 O2 型层状阴极会导致 Li2O 板的膨胀，并基于富锂区域的边缘共享模式消除隐藏空间中 Li 和 M 离子之间的 ER。其次，扩大Li2O空间以释放应力环境，可以通过缺锂区域中掺杂剂的离子半径轻松容纳锂离子。使用密度泛函理论和动力学蒙特卡罗模拟的统一原子计算，可以根据结构参数、动力学势垒的位点能量学以及基于各种钴基LiMO模型的统计转变来理解系统设计流程。我们对局部到宏观结构尺度的具体理解提出了促进快速锂动力学以实现快速充电锂离子电池的通用方向。