Anionic redox reaction in layered NaCr2/3Ti1/3S2 through electron holes formation and dimerization of S–S

Tian Wang, Guo-Xi Ren, Zulipiya Shadike, Ji-Li Yue, Ming-Hui Cao, Jie-Nan Zhang, Ming-Wei Chen, Xiao-Qing Yang, Seong-Min Bak, Paul Northrup, Pan Liu (), Xiao-Song Liu () and Zheng-Wen Fu ()
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Tian Wang: Fudan University
Guo-Xi Ren: Chinese Academy of Science
Zulipiya Shadike: Brookhaven National Laboratory
Ji-Li Yue: Nanjing University of Science and Technology
Ming-Hui Cao: Fudan University
Jie-Nan Zhang: Chinese Academy of Sciences
Ming-Wei Chen: Shanghai Jiao Tong University
Xiao-Qing Yang: Brookhaven National Laboratory
Seong-Min Bak: Brookhaven National Laboratory
Paul Northrup: Stony Brook University
Pan Liu: Shanghai Jiao Tong University
Xiao-Song Liu: Chinese Academy of Science
Zheng-Wen Fu: Fudan University

Nature Communications, 2019, vol. 10, issue 1, 1-12

Abstract: Abstract The use of anion redox reactions is gaining interest for increasing rechargeable capacities in alkaline ion batteries. Although anion redox coupling of S2− and (S2)2− 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-NaCr2/3Ti1/3S2 cathode that delivers a high reversible capacity of ~186 mAh g−1 (0.95 Na) based on the cation and anion redox process. Various charge compensation mechanisms of the sulfur anionic redox process in layered NaCr2/3Ti1/3S2, 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 (S2)n− species with shortened S–S distances is obtained. These results provide valuable information for the development of materials based on the anionic redox reaction.

Date: 2019
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DOI: 10.1038/s41467-019-12310-6

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