MXenes are promising cathodes for Li-CO2 batteries owing to their high electrical conductivity and efficient CO2 activation function. However, the effects of adsorption and electronic structures of MXene on the full life cycle of Li-CO2 batteries have been rarely investigated. Here, we employ a coregulation approach to enhance the adsorption-decomposition of lithium carbonate (Li2CO3) by introducing Zn and Cl surface groups onto the Ti3C2 MXene (Zn-Ti3C2Cl2) catalyst. The incorporation of Cl surface groups enhances Li2CO3 adsorption on the MXene catalyst surface, resulting in the formation of small-sized and uniform Li2CO3. Additionally, the introduction of Zn shifts the d-band centers of titanium and promotes CO2 evolution reaction (CO2ER) activity, thereby facilitating the decomposition of discharge products. As a result, the Li-CO2 battery based on the Zn-Ti3C2Cl2 catalyst exhibits an ultralow overpotential (0.72 V) at 200 mA g-1 and stable cycling for up to 1500 h. This work validates the efficacy of promoting reversibility in Li-CO2 batteries by adjusting the adsorption-decomposition process.
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