Manipulating coordination environment for a high-voltage aqueous copper-chlorine battery

Xiangyong Zhang, Hua Wei, Shizhen Li, Baohui Ren, Jingjing Jiang, Guangmeng Qu, Haiming Lv, Guojin Liang, Guangming Chen, Chunyi Zhi (), Hongfei Li () and Zhuoxin Liu ()
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Xiangyong Zhang: Shenzhen University
Hua Wei: Shenzhen University
Shizhen Li: Shenzhen University
Baohui Ren: Shenzhen University
Jingjing Jiang: Shenzhen University
Guangmeng Qu: Songshan Lake Materials Laboratory
Haiming Lv: Songshan Lake Materials Laboratory
Guojin Liang: City University of Hong Kong
Guangming Chen: Shenzhen University
Chunyi Zhi: Songshan Lake Materials Laboratory
Hongfei Li: Southern University of Science and Technology
Zhuoxin Liu: Shenzhen University

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Aqueous copper-based batteries have many favourable properties and have thus attracted considerable attention, but their application is limited by their low operating voltage originating from the high potential of copper negative electrode (0.34 V vs. standard hydrogen electrode). Herein, we propose a coordination strategy for reducing the intrinsic negative electrode redox potential in aqueous copper-based batteries and thus improving their operating voltage. This is achieved by establishing an appropriate coordination environment through the electrolyte tailoring via Cl− ions. When coordinated with chlorine, the intermediate Cu+ ions in aqueous electrolytes are successfully stabilized and the electrochemical process is decoupled into two separate redox reactions involving Cu2+/Cu+ and Cu+/Cu0; Cu+/Cu0 results in a redox potential approximately 0.3 V lower than that for Cu2+/Cu0. Compared to the coordination with water, the coordination with chlorine also results in higher copper utilization, more rapid redox kinetics, and superior cycle stability. An aqueous copper-chlorine battery, harnessing Cl−/Cl0 redox reaction at the positive electrode, is discovered to have a high discharge voltage of 1.3 V, and retains 77.4% of initial capacity after 10,000 cycles. This work may open up an avenue to boosting the voltage and energy of aqueous copper batteries.

Date: 2023
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DOI: 10.1038/s41467-023-42549-z

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