Anionic redox reaction in layered NaCr<sub>2/3</sub>Ti<sub>1/3</sub>S<sub>2</sub> through electron holes formation and dimerization of S-S.

Wang, Tian; Ren, Guo-Xi; Shadike, Zulipiya; Yue, Ji-Li; Cao, Ming-Hui; Zhang, Jie-Nan; Chen, Ming-Wei; Yang, Xiao-Qing et al. · Nat Commun · 2019

basic_science · Level V

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Abstract

The use of anion redox reactions is gaining interest for increasing rechargeable capacities in alkaline ion batteries. Although anion redox coupling of S<sup>2-</sup> and (S<sub>2</sub>)<sup>2-</sup> through dimerization of S-S in sulfides have been studied and reported, an anion redox process through electron hole formation has not been investigated to the best of our knowledge. Here, we report an O3-NaCr<sub>2/3</sub>Ti<sub>1/3</sub>S<sub>2</sub> cathode that delivers a high reversible capacity of ~186 mAh g<sup>-1</sup> (0.95 Na) based on the cation and anion redox process. Various charge compensation mechanisms of the sulfur anionic redox process in layered NaCr<sub>2/3</sub>Ti<sub>1/3</sub>S<sub>2</sub>, which occur through the formation of disulfide-like species, the precipitation of elemental sulfur, S-S dimerization, and especially through the formation of electron holes, are investigated. Direct structural evidence for formation of electron holes and (S<sub>2</sub>)<sup>n-</sup> species with shortened S-S distances is obtained. These results provide valuable information for the development of materials based on the anionic redox reaction.