Switching CO 2 Electroreduction toward Ethanol by Delocalization State-Tuned Bond Cleavage

The electrochemical CO2 reduction reaction by copper-based catalysts features a promising approach to generate value-added multicarbon (C2+) products. However, due to the unfavored formation of oxygenate intermediates on the catalyst surface, the selectivity of C2+ alcohols like ethanol remains unsatisfactory compared to that of ethylene. The bifurcation point (i.e., the CH2═CHO* intermediate adsorbed on Cu via a Cu–O–C linkage) is critical to the C2+ product selectivity, whereas the subsequent cleavage of the Cu–O or the O–C bond determines the ethanol or ethylene pathway. Inspired by the hard–soft acid–base theory, in this work, we demonstrate an electron delocalization tuning strategy of the Cu catalyst by…

• NN
  National Natural Science Foundation of China

  Awards: U23A20552, 22025502, 22175022, 22222901
• SA
  Science and Technology Commission of Shanghai Municipality

  Award: 21DZ1206800