Tunable Redox Chemistry and Stability of Radical Intermediates in 2D Covalent Organic Frameworks for High Performance Sodium Ion Batteries

Gu, Shuai; Wu, Shaofei; Cao, Lujie; Li, Minchan; Qin, Ning; Zhu, Jian; Wang, Zhiqiang; Li, Yingzhi; Li, Zhiqiang; Chen, Jingjing; Lu, Zhouguang

2019-06-19

10.1021/jacs.9b03467

Journal of the American Chemical Society   影响因子和分区

0002-7863

Radicals are inevitable intermediates during the charging and discharging of organic redox electrodes. The increase of the reactivity of the radical intermediates is desirable to maximize the capacity and enhance the rate capability but is detrimental to cycling stability. Therefore, it is a great challenge to controllably balance the redox reactivity and stability of radical intermediates to optimize the electrochemical properties with a good combination of high specific capacity, excellent rate capability, and long-term cycle life. Herein, we reported the redox and tunable stability of radical intermediates in covalent organic frameworks (COFs) considered as high capacity and stable anode for sodium-ion batteries. The comprehensive characterizations combined with theoretical simulation confirmed that the redox of C-O center dot and alpha-C radical intermediates play an important role in the sodiation/desodiation process. Specifically, the stacking behavior could be feasibly tuned by the thickness of 2D COFs, essentially determining the redox reactivity and stability of the alpha-C radical intermediates and their contributive capacity. The modulation of reversible redox chemistry and stabilization mechanism of radical intermediates in COFs offers a novel entry to design novel high performance organic electrode materials for energy storage and conversion.

SCI ; EI

英语

ESI高被引

第一 ; 通讯

National Natural Science Foundation of China[21875097]

Chemistry

Chemistry, Multidisciplinary

WOS:000471835600032

AMER CHEMICAL SOC

20192407039679

Anodes ; Charging (batteries) ; Metal ions ; Organic compounds ; Stability

Metallurgy:531.1 ; Secondary Batteries:702.1.2 ; Electron Tubes:714.1 ; Organic Compounds:804.1

Web of Science

Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Guangdong, Peoples R China

Gu, Shuai,Wu, Shaofei,Cao, Lujie,et al. Tunable Redox Chemistry and Stability of Radical Intermediates in 2D Covalent Organic Frameworks for High Performance Sodium Ion Batteries[J]. Journal of the American Chemical Society,2019,141(24):9623-9628.

Gu, Shuai.,Wu, Shaofei.,Cao, Lujie.,Li, Minchan.,Qin, Ning.,...&Lu, Zhouguang.(2019).Tunable Redox Chemistry and Stability of Radical Intermediates in 2D Covalent Organic Frameworks for High Performance Sodium Ion Batteries.Journal of the American Chemical Society,141(24),9623-9628.

Gu, Shuai,et al."Tunable Redox Chemistry and Stability of Radical Intermediates in 2D Covalent Organic Frameworks for High Performance Sodium Ion Batteries".Journal of the American Chemical Society 141.24(2019):9623-9628.