Atomically dispersed Cu‐Zn tandem catalyst for efficient electrocatalytic reduction of CO2 to alcohols

Abstract Electrochemical carbon dioxide reduction reaction (CO 2 RR) is one of the most prospective strategies to achieve carbon neutrality. Multi‐carbon compound (C 2+ ) products have higher commercial value and wider applications, among which ethanol is a widely used chemical feedstock and high energy density fuel. Here, we prepared nitrogen‐doped carbon nanofibers containing copper‐zinc double atoms using the electrospinning technique and controlled the content of both metal atoms by varying the calcination temperature. This catalyst exhibited ultra‐high selectivity for ethanol at low potentials. Ethanol selectivity at −0.3 V versus RHE was more than 60% with the total alcohol selectivity of over 80%. Meanwhile, we explored the ethanol production pathway by combining density‐functional theory (DFT) and ATR‐FTIR spectroscopy, and found that OCCO* intermediates were most abundant for the optimal ratio of Cu to Zn atoms, lowering the energetic barriers to ethanol formation, and thus improving the selectivity of ethanol production.