Tunable CO/H<sub>2</sub> ratios of electrochemical reduction of CO<sub>2</sub> through the Zn-Ln dual atomic catalysts.

Liang, Zhong; Song, Lianpeng; Sun, Mingzi; Huang, Bolong; Du, Yaping · Sci Adv · 2021

basic_science · Level V

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Abstract

Electrochemical reduction of CO<sub>2</sub> (CO<sub>2</sub>RR) to value-added liquid fuels is a highly appealing solution for carbon-neutral recycling, especially to syngas (CO/H<sub>2</sub>). 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/H<sub>2</sub> ratios. Moreover, the ZnLa-1/CN electrocatalyst generates the syngas with a ratio of CO/H<sub>2</sub> = 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 H<sub>2</sub>, respectively. This work indicates a promising strategy in the development of atomic catalysts for more controllable CO<sub>2</sub>RR.