Ultrasmall Cu Nanocrystals Dispersed in Nitrogen-Doped Carbon as Highly Efficient Catalysts for CO2 Electroreduction

Xiangfu Meng; Guoxing Pan; Hongji Liu; Yong Qian; Xingyu Wang; Changlai Wang; Lin Hu; Hui Wang; Qianwang Chen

doi:10.1021/acsami.2c00050

Ultrasmall Cu Nanocrystals Dispersed in Nitrogen-Doped Carbon as Highly Efficient Catalysts for CO₂ Electroreduction

ACS Appl Mater Interfaces. 2022 Apr 20;14(15):17240-17248. doi: 10.1021/acsami.2c00050. Epub 2022 Apr 5.

Authors

Xiangfu Meng^{1

2}, Guoxing Pan³, Hongji Liu^{1

2}, Yong Qian^{1

2}, Xingyu Wang^{1

2}, Changlai Wang^{2

4}, Lin Hu¹, Hui Wang^{1

2}, Qianwang Chen^{1

2}

Affiliations

¹ High Magnetic Field Laboratory, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei, Anhui 230031, P. R. China.
² Hefei National Laboratory for Physical Science at Microscale, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.
³ Institutes of Physical Science and Information Technology, Anhui University, Hefei, Anhui 230601, P. R. China.
⁴ Center of Super-Diamond and Advanced Films (COSDAF), Department of Materials Science and Engineering, City University of Hong Kong, Kowloon, Hong Kong 999077, Hong Kong.

PMID: 35380787
DOI: 10.1021/acsami.2c00050

Abstract

The electroreduction of carbon dioxide (CO₂) to a liquid product is a viable method for establishing an artificial carbon cycle. Unfortunately, most electrocatalysts' low efficiency and instability prevent them from being used in practical applications. In the current study, we developed ultrasmall Cu nanocrystals embedded in nitrogen-doped carbon nanosheets (Cu/NC-NSs) for selective CO₂ electroreduction by adjusting the potential. Cu/NC-NSs had 43.7 and 63.5% Faradaic efficiencies for the synthesis of ethanol and formate with applied potentials of -0.37 and -0.77 V vs reversible hydrogen electrode (RHE) using a flow cell architecture, respectively. Moreover, these Cu/NC-NSs show a steady catalytic performance up to 16 h. Density functional theory (DFT) calculations were performed to investigate the reaction mechanism. Furthermore, the synergistic effect formed by nitrogen-doped carbon and highly dispersed copper atoms led to their excellent performance in CO₂ electroreduction.

Keywords: CO2 electroreduction; Cu nanoparticles; liquid product; nitrogen-doped carbon; synergistic effect.