Tunable CO/H₂ ratios of electrochemical reduction of CO₂ through the Zn-Ln dual atomic catalysts

Electrochemical reduction of CO₂ (CO₂RR) to value-added liquid fuels is a highly appealing solution for carbon-neutral recycling, especially to syngas (CO/H₂). Current strategies suffer from poor faradaic efficiency (FE), selectivity, and controllability to the ratio of products. In this work, we have synthesized a series of single and dual atomic catalysts on the carbon nitride nanosheets. Adjusting the ratio of La and Zn atomic sites produces syngas with a wide range of CO/H2 ratios. Moreover, the ZnLa-1/CN electrocatalyst generates the syngas with a ratio of CO/H₂ = 0.5 at a wide potential range, and the total FE of CO2RR reaches 80% with good stability. Density functional theory calculations have confirmed that the Zn and La affect electronic structures and determine the formation of CO and H₂, respectively. This work indicates a promising strategy in the development of atomic catalysts for more controllable CO₂RR. © The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science.