In-situ construction of Cu–Co4N@CC hierarchical binder-free cathode for advanced and flexible Li–CO2 batteries: Electron structure and mass transfer modulation

Abstract

Li–CO2 batteries with high energy density presents great promising to meet carbon neutrality. Herein, a binder-free cathode is obtained by in-situ growth of ZIF-67-derived Co4N with Cu integration on carbon cloth (CC), which is developed as the advanced catalytic cathode for Li–CO2 batteries. After optimizing the components, the derived Li–CO2 batteries can present a discharge capacity beyond 31 000 mA h g−1 at a current density of 100 mA g−1 as well as an excellent long-term stable cycle life up to 131 cycles at 200 mA g−1. Benefitting from the reorganization of the electronic structure on the Co4N active surface by the introduction of Cu, the reduction of CO2 and the decomposition of discharge products tend to be smoothly, and the assembled batteries exhibit a low overpotential of 1.32 V (Li/Li+) at 100 mA g−1. The superior catalytic performances of Cu–Co4N@CC cathode are well-demonstrated by the combination of experiments and theoretical calculations. Moreover, this binder-free cathode with flexible feature has been proven to be suitable for the development of wearable electronic devices by the assembled flexible Li–CO2 batteries. These findings shed a new light on the expansion of excellent cathode based on non-noble bimetal for advanced and wearable Li–CO2 batteries.