Computational Insights into LixOy Formation, Nucleation, and Adsorption on Carbon Nanotube Electrodes in Nonaqueous Li-O2 Batteries.

Content Provider	Semantic Scholar
Author	Yi, Xiaoping Liu, Xunliang Zhang, Peng Dou, Ruifeng Zhou, Wenning
Copyright Year	2020
Abstract	Recent theoretical and experimental studies have shown that the formation of Li2O2, the main discharge product of nonaqueous Li-O2 batteries, is a complex multi-step reaction process. The formation, nucleation and adsorption of LixOy (x ,y = 0, 1, and 2) and (Li2O2)n clusters with n = 1-4 on the surface of CNTs was investigated by periodic density functional theory calculation. The results showed that both Li2O2 and Li2O on CNT electrodes are prefer to be generated by lithiation reaction rather than disproportionation reaction. The free energy profiles demonstrate that the discharge potentials of 2.54V and 1.29V are the threshold values of spontaneous nucleation of (Li2O2)2 and (Li2O)2 on CNT surface, respectively. The electronic structure indicates that Li2O2 is a p-type semiconductor, while Li2O exhibits the properties of an insulator. Interestingly, once Li2O2 molecules condense into large clusters, they will be repelled away from the CNT surface and continue to grow into large-sized Li2O2. Our results provide insights into the full understanding of the electrochemical reaction mechanism and product formation processes of lithium oxides in the cathodes of Li-O2 batteries.
File Format	PDF HTM / HTML
DOI	10.1021/acs.jpclett.9b03757
PubMed reference number	31951140
Journal	Medline
Alternate Webpage(s)	https://s3-eu-west-1.amazonaws.com/pstorage-acs-6854636/21922545/jz9b03757_si_001.pdf
Alternate Webpage(s)	https://doi.org/10.1021/acs.jpclett.9b03757
Journal	The journal of physical chemistry letters
Language	English
Access Restriction	Open
Content Type	Text
Resource Type	Article