A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction

Jiaqi Feng, Hongshuai Gao, Lirong Zheng, Zhipeng Chen, Shaojuan Zeng, Chongyang Jiang, Haifeng Dong, Licheng Liu, Suojiang Zhang () and Xiangping Zhang ()
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Jiaqi Feng: Chinese Academy of Sciences
Hongshuai Gao: Chinese Academy of Sciences
Lirong Zheng: Chinese Academy of Sciences
Zhipeng Chen: Dalian National Laboratory for Clean Energy
Shaojuan Zeng: Chinese Academy of Sciences
Chongyang Jiang: Chinese Academy of Sciences
Haifeng Dong: Chinese Academy of Sciences
Licheng Liu: Dalian National Laboratory for Clean Energy
Suojiang Zhang: Chinese Academy of Sciences
Xiangping Zhang: Chinese Academy of Sciences

Nature Communications, 2020, vol. 11, issue 1, 1-8

Abstract: Abstract Developing effective catalysts based on earth abundant elements is critical for CO2 electroreduction. However, simultaneously achieving a high Faradaic efficiency (FE) and high current density of CO (jCO) remains a challenge. Herein, we prepare a Mn single-atom catalyst (SAC) with a Mn-N3 site embedded in graphitic carbon nitride. The prepared catalyst exhibits a 98.8% CO FE with a jCO of 14.0 mA cm−2 at a low overpotential of 0.44 V in aqueous electrolyte, outperforming all reported Mn SACs. Moreover, a higher jCO of 29.7 mA cm−2 is obtained in an ionic liquid electrolyte at 0.62 V overpotential. In situ X-ray absorption spectra and density functional theory calculations demonstrate that the remarkable performance of the catalyst is attributed to the Mn-N3 site, which facilitates the formation of the key intermediate COOH* through a lowered free energy barrier.

Date: 2020
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DOI: 10.1038/s41467-020-18143-y

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