Molecularly Compensated Pre‐Metallation Strategy for Metal‐Ion Batteries and Capacitors. Issue 31 (22nd June 2021)

• Record Type: Journal Article
• Authors: Zou, Kangyu; Song, Zirui; Gao, Xu; Liu, Huanqing; Luo, Zheng; Chen, Jun; Deng, Xinglan; Chen, Libao; Zou, Guoqiang; Hou, Hongshuai; Ji, Xiaobo
• Is Part Of: Angewandte Chemie international edition. Volume 60:Issue 31(2021)
• Page Start: 17070
• Page End: 17079
• Publication Date: 2021-06-22
• Subjects: batteries -- capacitors -- cathode additive -- electrolysis -- organic electrochemistry; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202103569
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: The use of a sacrificial cathode additive as a pre‐metallation method could ensure adequate metal sources for advanced energy storage devices. However, this pre‐metallation technique suffers from the precise regulation of decomposition potential of additive. Herein, a molecularly compensated pre‐metallation (Li/Na/K) strategy has been achieved through Kolbe electrolysis, in which the electrochemical oxidation potential of a metal carboxylate is manipulated by the bonding energy of the oxygen–metal (O–M) moiety. The electron‐donating effect of the substituent and the low charge density of the cation can dramatically weaken the O–M bond strength, further bringing out the reduced potential. Thus, sodium acetate exhibits a superior pre‐sodiation feature for sodium‐ion battery accompanied with a large irreversible specific capacity of 301.8 mAh g −1, remarkably delivering 70.6 % enhanced capacity retention in comparison to the additive‐free system after 100 cycles. This methodology has been extended to construct a high‐performance lithium‐ion battery and a lithium/sodium/potassium‐ion capacitor. Abstract : A molecularly compensated pre‐metallation strategy triggered by Kolbe electrolysis has been successfully achieved for the construction of high‐performance metal‐ion batteries and capacitors. Notably, the electrochemical oxidation potential of the metal carboxylate is modulated by the bonding energy of the oxygen–metal moiety, which is further manipulated by the electronic structure of the substituent and the hardness/softness of metal element.