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; Xiangping Zhang

doi:10.1038/s41467-020-18143-y

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

Nat Commun. 2020 Aug 28;11(1):4341. doi: 10.1038/s41467-020-18143-y.

Authors

Jiaqi Feng^#^{1

2}, Hongshuai Gao^#¹, Lirong Zheng³, Zhipeng Chen^{4

5}, Shaojuan Zeng¹, Chongyang Jiang^{1

2}, Haifeng Dong¹, Licheng Liu^{4

5}, Suojiang Zhang^{6

7}, Xiangping Zhang^{8

9

10}

Affiliations

¹ Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, 100190, Beijing, P.R. China.
² College of Chemical Engineering, University of Chinese Academy of Science, 100049, Beijing, P.R. China.
³ Beijing Synchrotron Radiation Facility (BSRF), Institute of High Energy Physics, Chinese Academy of Sciences, 100049, Beijing, P.R. China.
⁴ Dalian National Laboratory for Clean Energy, 116023, Dalian, P.R. China.
⁵ Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, 266101, Qingdao, P.R. China.
⁶ Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, 100190, Beijing, P.R. China. sjzhang@ipe.ac.cn.
⁷ College of Chemical Engineering, University of Chinese Academy of Science, 100049, Beijing, P.R. China. sjzhang@ipe.ac.cn.
⁸ Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, 100190, Beijing, P.R. China. xpzhang@ipe.ac.cn.
⁹ College of Chemical Engineering, University of Chinese Academy of Science, 100049, Beijing, P.R. China. xpzhang@ipe.ac.cn.
¹⁰ Dalian National Laboratory for Clean Energy, 116023, Dalian, P.R. China. xpzhang@ipe.ac.cn.

^# Contributed equally.

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 (j_CO) 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 j_CO 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 j_CO 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.