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Surface basicity regulation for stabilizing Li2C2O4 towards lower overpotential Li–CO2 batteries at high current density

Qian Liu, Huyi Yu, Zhaoyang Qin, Xincheng Liang, Yupu Wei, Mengke Hou, Huan Wen, Kedi Yang, Shibin Yin*

https://doi.org/10.1016/j.cjsc.2026.101147

Li−CO2 batteries; Surface basicity; Li2C2O4; Overpotential; High current density

ABSTRACT

Compared with Li2CO3, the intermediate product Li2C2O4 is relatively thermodynamically unstable, leading to a tendency to decompose at lower charge potentials below 3.8 V. However, during high-current-density cycling, Li2C2O4 is vulnerable to undergoing self-decomposition to form insulating Li2CO3. Herein, a surface basicity regulation strategy is proposed to stabilize Li2C2O4 under high-current conditions through constructing a Cu2O-Cu7Te4 heterostructure catalyst. Experimental results and theoretical calculations demonstrate that an increase in surface basicity of Cu7Te4 after the introduction of Cu2O, thus increasing the transfer of electrons from Te to O in Li2C2O4. The adsorption energy of Li2C2O4 on the Cu2O-Cu7Te4 surface is further increased, enabling stable Li2C2O4 electrochemistry, thus reducing the overpotential of Li-CO2 batteries. As a result, the Cu2O-Cu7Te4 cathode shows a low overpotential (1.62 V) and great cyclic stability (340 cycles) at a high current density of 2000 mA g−1. This work elucidates the crucial role of regulating the Surface basicity of the catalyst in stabilizing Li2C2O4 at high current density, thereby reducing the overpotential of Li-CO2 batteries.


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