Combined Computational and Experimental Study of Li Exchange Reaction at the Surface of Spinel LiMn2O4 as a Rechargeable Li-Ion Battery Cathode
Combined Computational and Experimental Study of Li Exchange Reaction at the Surface of Spinel LiMn2O4 as a Rechargeable Li-Ion Battery Cathode
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DOI：
10.1021/jp509232m
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发表时间：
2014-11
影响因子：
3.7
通讯作者：
M. Nakayama;H. Taki;Tomoaki Nakamura;Satoshi Tokuda;R. Jalem;T. Kasuga
中科院分区：
文献类型：
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作者：
M. Nakayama;H. Taki;Tomoaki Nakamura;Satoshi Tokuda;R. Jalem;T. Kasuga
锂锰氧化物（LiMn 2 O 4）被认为是可再充电锂离子电池的有吸引力的正极，特别是用于电动车辆的电源，因此迫切需要改善其充放电动力学。在当前的文件中，锂离子交换反应的动力学在LiMn 2 O 4阴极和非水液体电解质之间的界面处使用实验和计算技术进行了研究。电化学交流阻抗测量显示对应于界面Li离子交换的两个峰，并且根据吸附原子模型[布鲁斯，P.G.;赛义迪河，巴西-地Y. J. Electroanal。1992，322，93]。为了更深入地了解后一个过程，从电极表面脱锂使用密度泛函理论（DFT）进行了模拟，并将DFT结果与交流阻抗行为对电位的依赖性进行了比较。我们得出结论，化学势格拉德…
Lithium manganese oxide (LiMn2O4) is regarded as an attractive positive electrode for rechargeable Li-ion batteries, in particular for the power source of electric vehicles, and there is thus an urgent need to improve its charge–discharge kinetics. In the current paper, the kinetics of a Li-ion exchange reaction at the interface between a LiMn2O4 cathode and nonaqueous liquid electrolytes is studied using experimental and computational techniques. Electrochemical ac impedance measurements showed two semicircles corresponding to the interfacial Li-ion exchange, and they are ascribed to the desolvation and lattice incorporation processes according to the adatom model [Bruce, P. G.; Saidi, M. Y. J. Electroanal. Chem. 1992, 322, 93]. To gain deeper insight into the latter process, delithiation from the electrode surface was simulated using density functional theory (DFT), and the DFT results were compared to the dependence of the ac impedance behavior on potential. We conclude that the chemical potential grad...