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Electrochemical CO2 conversion into value-added chemicals is a promising technology to solve the greenhouse effect and recycle chemical energy. However, the electrochemical CO2 reduction reaction (e-CO2RR) is seriously compromised by weak CO2 adsorption and a rough CO2 activation process based on the chemical inertness of the CO2 molecule and the formed fragile metal–C/O bond. In this paper, we designed and fabricated Au particles embedded in ZrO2. The configuration of Au particles being of positive charge and ZrO2 with negative charge is induced and generated by metal–support interactions (MSIs). As a result, Au/ZrO2@C presents a big difference in the CO2 conversion compared with the known work, affording a formate yield of 112.5 μmol·cm−2·h−1 at −1.1 V vs. reversible hydrogen electrode (RHE), and a max formate Faradaic efficiency of up to 94.1% at −0.9 V vs. RHE. This superior performance was attributed to the activated Au–ZrO2 interface to form the Auδ+ species. Both in-situ Fourier transform infrared (FTIR) spectroscopy and theoretical calculations show that the MSIs configuration can be inclined to the *OCO intermediate generation on Auδ+ species activating CO2 molecules and then accelerate the formation of the *OCHO intermediate in e-CO2RR, thereby favoring the CO2 conversion to formate.
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