Yin Yinghui, Zhao Ruijie, Deng Yue, Franco Alejandro A
Laboratoire de Réactivité et Chimie des Solides (LRCS), Université de Picardie Jules Verne and CNRS, UMR 7314 , 33 rue St. Leu, 80039 Amiens, France.
Réseau sur le Stockage Electrochimique de l'Energie (RS2E), CNRS FR3459 , 80039 Amiens, France.
J Phys Chem Lett. 2017 Feb 2;8(3):599-604. doi: 10.1021/acs.jpclett.6b02732. Epub 2017 Jan 19.
We simulated the discharge process of Li-O batteries and the growth of LiO thin films at the mesoscale with a novel kinetic Monte Carlo model, which combined a stochastic description of mass transport and detailed elementary reaction kinetics. The simulation results show that the ordering of the LiO thin film is determined by the interplay between diffusion and reaction kinetics. Due to the fast reaction kinetics on the catalyst, the LiO formed in the presence of catalyst (cat-CNF) shows a low degree of ordering and is more likely to be amorphous. Moreover, the mobility of the LiO ion pair, which depends largely on the nature of the electrolyte, also impacts the homogeneity of the compactness of the LiO thin film. These results are of high importance for understanding the role of the catalyst and reaction kinetics in Li-O batteries.
我们使用一种新颖的动力学蒙特卡罗模型，在中尺度上模拟了锂氧电池的放电过程以及LiO薄膜的生长，该模型结合了质量传输的随机描述和详细的基元反应动力学。模拟结果表明，LiO薄膜的有序性由扩散和反应动力学之间的相互作用决定。由于催化剂上的快速反应动力学，在催化剂（cat-CNF）存在下形成的LiO显示出低程度的有序性，并且更可能是无定形的。此外，LiO离子对的迁移率在很大程度上取决于电解质的性质，这也影响了LiO薄膜致密性的均匀性。这些结果对于理解催化剂和反应动力学在锂氧电池中的作用非常重要。
