Regulating the Gibbs Free Energy to Design Aqueous Battery‐Compatible Robust Host

Author:

Lin Jing1,Wang Yanyi1,Chen Minfeng2,Lu Jinlin3,Mi Hongwei14,Chen Jizhang2,He Chuanxin1,Ma Dingtao1,Zhang Peixin14ORCID

Affiliation:

1. College of Chemistry and Environmental Engineering Shenzhen University Shenzhen 518060 P. R. China

2. College of Materials Science and Engineering Nanjing Forestry University Nanjing 210037 P. R. China

3. Research Center for Corrosion and Erosion Process Control of Equipment and Material in Marine Harsh Environment Guangzhou Maritime University Guangzhou 510725 P. R. China

4. Guangdong Flexible Wearable Energy and Tools Engineering Technology Research Center Shenzhen 518060 P. R. China

Abstract

AbstractLow‐cost, high‐voltage‐platform, and high‐capacity MnO2 is the most promising cathode candidate for developing high‐energy‐density aqueous zinc‐ion batteries. However, the Buckets effect of runaway phase transition and irreversible dissolution restricts the electrochemical performance of MnO2. To address this issue, this report presents a bottom‐up targeted assembly concept driven by Gibbs free energy for the design of a robust Ni‐MnO2‐xFx host via Ni2+ pre‐intercalation coupled with fluorine doping. The Gibbs free energy of the host is regulated by the coordination of interlayer reinforcement and interfacial defect repair, which prevents the “layer‐to‐spinel” transition and inhibits dissolution during long‐term cycling. As expected, this cathode provides superior H+/Zn2+ storage performance across a wide temperature range. A capacity of 180.4 mAh g−1 is retained after 1000 cycles at 2 A g−1, a high specific capacity of 293.9 mAh g−1 is retained after 250 cycles at 50 °C and 2 A g−1, and a capacity of 144.5 mAh g−1 is retained after 3000 cycles at 0 °C and 0.5 A g−1. This work provides new insights into the design of stable aqueous battery‐compatible hosts for aqueous zinc‐ion batteries as well as other battery chemistries.

Funder

Shenzhen Science and Technology Innovation Program

National Natural Science Foundation of China

Natural Science Foundation of Guangdong Province

Publisher

Wiley

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