Binuclear Cu complex catalysis enabling Li-CO<sub>2</sub> battery with a high discharge voltage above 3.0 V.

Sun, Xinyi; Mu, Xiaowei; Zheng, Wei; Wang, Lei; Yang, Sixie; Sheng, Chuanchao; Pan, Hui; Li, Wei et al. · Nat Commun · 2023

basic_science · Level V

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Abstract

Li-CO<sub>2</sub> batteries possess exceptional advantages in using greenhouse gases to provide electrical energy. However, these batteries following Li<sub>2</sub>CO<sub>3</sub>-product route usually deliver low output voltage (<2.5 V) and energy efficiency. Besides, Li<sub>2</sub>CO<sub>3</sub>-related parasitic reactions can further degrade battery performance. Herein, we introduce a soluble binuclear copper(I) complex as the liquid catalyst to achieve Li<sub>2</sub>C<sub>2</sub>O<sub>4</sub> products in Li-CO<sub>2</sub> batteries. The Li-CO<sub>2</sub> 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<sup>-1</sup>. And it shows robust cyclability over 400 cycles with additional help of Ru catalyst. We reveal that the copper(I) complex can easily capture CO<sub>2</sub> 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-CO<sub>2</sub> batteries to higher than 3.0 V, paving a promising avenue for the design and regulation of CO<sub>2</sub> conversion reactions.