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

作者：An Zhang, Yongxiang Liang, Huiping Li, Boyan Zhang, Zuhuan Liu, Qixuan Chang, Han Zhang, Changfei Zhu, Zhigang Geng, Wenguang Zhu, Jie Zeng · 发表于：Nano Letters · 年份：2020 · DOI：10.1021/acs.nanolett.0c03345 · 被引用次数：89 · 研究领域：CO2 Reduction Techniques and Catalysts、Advanced Thermoelectric Materials and Devices、Molecular Junctions and Nanostructures

Probing and understanding the intrinsic active sites of electrocatalysts is crucial to unravel the underlying mechanism of CO 2 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 CO 2 reduction with a high faradaic efficiency of 95% for carbonaceous product. During the CO 2 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 CO 2 electroreduction. This work establishes a fundamental understanding on the mechanism associated with self-reconstruction of heterogeneous catalysts toward CO 2 electroreduction.