Binuclear Cu complex catalysis enabling Li-CO2 battery with a high discharge voltage above 3.0 V

Xinyi Sun; Xiaowei Mu; Wei Zheng; Lei Wang; Sixie Yang; Chuanchao Sheng; Hui Pan; Wei Li; Cheng-Hui Li; Ping He; Haoshen Zhou

doi:10.1038/s41467-023-36276-8

Binuclear Cu complex catalysis enabling Li-CO₂ battery with a high discharge voltage above 3.0 V

Nat Commun. 2023 Feb 1;14(1):536. doi: 10.1038/s41467-023-36276-8.

Authors

Xinyi Sun^#¹, Xiaowei Mu^#¹, Wei Zheng², Lei Wang¹, Sixie Yang¹, Chuanchao Sheng¹, Hui Pan¹, Wei Li¹, Cheng-Hui Li², Ping He³, Haoshen Zhou⁴

Affiliations

¹ Center of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid State Microstructures and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, 210093, Nanjing, P. R. China.
² State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing National Laboratory of Microstructures, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, 210093, Nanjing, P. R. China.
³ Center of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid State Microstructures and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, 210093, Nanjing, P. R. China. pinghe@nju.edu.cn.
⁴ Center of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid State Microstructures and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, 210093, Nanjing, P. R. China. hszhou@nju.edu.cn.

^# Contributed equally.

Abstract

Li-CO₂ batteries possess exceptional advantages in using greenhouse gases to provide electrical energy. However, these batteries following Li₂CO₃-product route usually deliver low output voltage (<2.5 V) and energy efficiency. Besides, Li₂CO₃-related parasitic reactions can further degrade battery performance. Herein, we introduce a soluble binuclear copper(I) complex as the liquid catalyst to achieve Li₂C₂O₄ products in Li-CO₂ batteries. The Li-CO₂ battery using the copper(I) complex exhibits a high electromotive voltage up to 3.38 V, an increased output voltage of 3.04 V, and an enlarged discharge capacity of 5846 mAh g^-1. And it shows robust cyclability over 400 cycles with additional help of Ru catalyst. We reveal that the copper(I) complex can easily capture CO₂ to form a bridged Cu(II)-oxalate adduct. Subsequently reduction of the adduct occurs during discharge. This work innovatively increases the output voltage of Li-CO₂ batteries to higher than 3.0 V, paving a promising avenue for the design and regulation of CO₂ conversion reactions.