Ahmad Sheraz, Din H U, Nguyen Cuong Q, Nguyen Son-Tung, Nguyen C
School of Materials Science and Engineering, Institute of New Energy Material Chemistry, Nankai University, Tianjin 300350, P. R. China.
Computational Science Research Center, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea.
Dalton Trans. 2024 Feb 20;53(8):3785-3796. doi: 10.1039/d3dt03946c.
A significant problem in the area of rechargeable alkali ion battery technologies is the exploration of anode materials with overall high specific capacities and superior physical properties. By using first-principles calculations, we have determined that monolayer TiSiN is precisely such a potential anode candidate. Its demonstrated dynamic, thermal, mechanical, and energetic stabilities make it feasible for experimental realization. An important benefit of the electrode conductivity is that the electronic structure reveals that the pristine system experiences a change from a semiconductor to a metal throughout the entire alkali adsorption process. What's more interesting is that monolayer TiSiN can support up to double-sided 3-layer ad-atoms, resulting in extremely high theoretical capacities for Li, Na, Mg, and K of 1004, 854, 492 and 531 mA h g and low average open-circuit voltages of 0.55, 0.25, 0.55, and -1.3 V, respectively. Alkali diffusion on the surface has been demonstrated to occur extremely quickly, with migration energy barriers for Li, Na, Mg, and K as low as 0.25, 0.14, 0.10, and 0.07 eV, respectively. The results reveal that the migration barrier energy is the lowest for Li and Mg from path-2 and Na and K from path-1. Overall, these findings suggest that monolayer TiSiN is a suitable anode candidate for use in high-performance and low-cost metal-ion batteries.
可充电碱离子电池技术领域的一个重大问题是探索具有整体高比容量和优异物理性能的负极材料。通过第一性原理计算，我们确定单层TiSiN正是这样一种潜在的负极候选材料。其已证明的动态、热、机械和能量稳定性使其在实验上得以实现成为可能。电极导电性的一个重要优点是电子结构表明，在整个碱吸附过程中，原始体系经历了从半导体到金属的转变。更有趣的是，单层TiSiN最多可支持双面3层吸附原子，从而使Li、Na、Mg和K的理论比容量极高，分别为1004、854、492和531 mA h/g，平均开路电压分别低至0.55、0.25、0.55和 -1.3 V。已证明碱在表面的扩散极其迅速，Li、Na、Mg和K的迁移能垒分别低至0.25、0.14、0.10和0.07 eV。结果表明，路径2中Li和Mg以及路径1中Na和K的迁移势垒能量最低。总体而言，这些发现表明单层TiSiN是用于高性能和低成本金属离子电池的合适负极候选材料。
