Fully exposed nickel clusters with electron-rich centers for high-performance electrocatalytic CO2 reduction to CO

Qi Hao; Qi Tang; Hai-Xia Zhong; Jia-Zhi Wang; Dong-Xue Liu; Xin-Bo Zhang

doi:10.1016/j.scib.2022.06.006

Fully exposed nickel clusters with electron-rich centers for high-performance electrocatalytic CO₂ reduction to CO

Sci Bull (Beijing). 2022 Jul 30;67(14):1477-1485. doi: 10.1016/j.scib.2022.06.006. Epub 2022 Jun 7.

Authors

Qi Hao¹, Qi Tang², Hai-Xia Zhong³, Jia-Zhi Wang², Dong-Xue Liu⁴, Xin-Bo Zhang⁵

Affiliations

¹ State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China; Key Laboratory of Automobile Materials (Jilin University), Ministry of Education, School of Materials Science and Engineering, Jilin University, Changchun 130022, China.
² State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China; School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, China.
³ State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China; Center for Advancing Electronics Dresden (CFAED) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden 01062, Germany.
⁴ Key Laboratory of Automobile Materials (Jilin University), Ministry of Education, School of Materials Science and Engineering, Jilin University, Changchun 130022, China.
⁵ State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China; School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, China. Electronic address: xbzhang@ciac.ac.cn.

PMID: 36546191
DOI: 10.1016/j.scib.2022.06.006

Abstract

Single-atom catalysts (SACs) have attracted increasing concerns in electrocatalysis because of their maximal metal atom utilization, distinctive electronic properties, and catalytic performance. However, the isolated single sites are disadvantageous for reactions that require simultaneously activating different reactants/intermediates. Fully exposed metal cluster catalyst (FECC), inheriting the merits of SACs and metallic nanoparticles, can synergistically adsorb and activate reactants/intermediates on their multi-atomic sites, demonstrating great promise in electrocatalytic reactions. Here a facile method to regulate the atomic dispersion of Ni species from cluster to single-atom scale for efficient CO₂ reduction was developed. The obtained Ni FECC exhibits high Faradaic efficiency of CO up to 99%, high CO partial current density of 347.2 mA cm^-2, and robust durability under 20 h electrolysis. Theoretical calculations illuminate that the ensemble of multiple Ni atoms regulated by sulfur atoms accelerates the reaction kinetics and thus improves CO production.

Keywords: Carbon dioxide reduction reaction; Fully exposed metal sites; Industrial current density; Nickel clusters; Sulfur regulation.