The high-rate ethanol electrosynthesis from CO is challenging due to the low selectivity and poor activity, which requires the competition with other reduction products and H . Here, the electrochemical reconstruction of Cs Cu Cl perovskite to form surface Cl-bonded, low-coordinated Cs modified Cu(200) nanocubes (CuClCs), is demonstrated. Density functional theory calculations reveal that the CuClCs structure possesses low Bader charges and a large coordination capacity; and thus, can promote the CO -to-ethanol pathway via stabilizing C-O bond in oxygenate intermediates. The CuClCs catalyst exhibits outstanding partial current densities for producing ethanol (up to 2124 ± 54 mA cm ) as one of the highest reported values in the electrochemical CO or CO reduction. This work suggests an attractive strategy with surface alkali-metal cations for ampere-level CO -to-ethanol electrosynthesis.
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