Multi-twinned gold nanoparticles with tensile surface steps for efficient electrocatalytic CO_(2) reduction

作     者：Li-Wei Chen Yu-Chen Hao Jiani Li Linyu Hu Yu Guo Shuai Li Di Liu Zhejiaji Zhu Si-Qian Wu Hui-Zi Huang An-Xiang Yin Bo Wang Ya-Wen Zhang 

作者机构：Ministry of Education Key Laboratory of Cluster ScienceBeijing Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsAdvanced Technology Research Institute(Jinan)School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing National Laboratory for Molecular SciencesState Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China 

出 版 物：《Science China Chemistry》 (中国科学（化学英文版）)

年 卷 期：2022年第65卷第11期

页      面：2188-2196页

核心收录：

学科分类：081705[工学-工业催化] 07[理学] 070205[理学-凝聚态物理] 08[工学] 0817[工学-化学工程与技术] 080501[工学-材料物理与化学] 0805[工学-材料科学与工程（可授工学、理学学位）] 0702[理学-物理学] 

基　　金：the financial support from the National Natural Science Foundation of China(21971012,21922502,and 21971017) the National Key Research and Development Program of China(2020YFB1506300) the Beijing Municipal Natural Science Foundation(JQ20007) the Beijing Institute of Technology Research Fund Program 

主　　题：gold nanoparticles tensile lattice surface steps electrocatalysis CO_(2)reduction 

摘      要：CO_(2) reduction reactions(CO_(2)RR) powered by renewable electricity can directly convert CO_(2) to hydrocarbons and fix the intermittent sustainable energy in portable chemical fuels. It is of great importance to develop advanced catalysts that can boost CO_(2)RR with high activity, selectivity, and efficiency at low overpotentials. Here, we report the solution synthesis using H_(2)O_(2) to modify the surface structures of gold multi-twinned nanoparticles(AuMPs) and create tensile surface steps. Calculations predicted significantly enhanced CO_(2) adsorption and boosted CO_(2)RR capabilities with inhibited hydrogen evolution reaction activity for the tensile surface steps with modified electronic structure. The H_(2)O_(2)-treated AuMPs with surface steps and 3.83% tensile lattices showed much higher activity and selectivity at lower overpotentials for CO_(2)RR than pristine gold *** CO-production current density reached about 98 mA cm^(-2) with a Faradaic efficiency of 95.7% at -0.30 V versus reversible hydrogen electrode in the flow cell, showing a half-cell energy efficiency as high as ~83%. Our strategy represents a rational catalyst design by engineering the surface structures of metal nanoparticles and may find more applicability in future electrocatalysis.