In-Situ Surface Reconstruction of InN Nanosheets for Efficient CO2 Electroreduction into Formate

• Published in: Nano letters 2020-11, Vol.20 (11), p.8229-8235
• Main Authors: Zhang, An, Liang, Yongxiang, Li, Huiping, Zhang, Boyan, Liu, Zuhuan, Chang, Qixuan, Zhang, Han, Zhu, Chang-Fei, Geng, Zhigang, Zhu, Wenguang, Zeng, Jie
• Format: Article
• Language: English
• ISSN: 1530-6984; 1530-6992
• DOI: 10.1021/acs.nanolett.0c03345

Probing and understanding the intrinsic active sites of electrocatalysts is crucial to unravel the underlying mechanism of CO2 electroreduction and provide a prospective for the rational design of high-performance electrocatalysts. However, their structure–activity relationships are not straightforward because electrocatalysts might reconstruct under realistic working conditions. Herein, we employ in-situ measurements to unveil the intrinsic origin of the InN nanosheets which served as an efficient electrocatalyst for CO2 reduction with a high faradaic efficiency of 95% for carbonaceous product. During the CO2 electroreduction, InN nanosheets reconstructed to form the In-rich surface. Density functional theory calculations revealed that the reconstruction of InN led to the redistribution of surface charge that significantly promoted the adsorption of HCOO* intermediates and thus benefited the formation of formate toward CO2 electroreduction. This work establishes a fundamental understanding on the mechanism associated with self-reconstruction of heterogeneous catalysts toward CO2 electroreduction.