Single-atom catalysts (SACs) with metal–nitrogen (M–N) sites are one of the most promising electrocatalysts for electrochemical carbon dioxide reduction (ECO₂R). However, challenges in simultaneously enhancing the activity and selectivity greatly limit the efficiency of ECO₂R due to the improper interaction of reactants/intermediates on these catalytic sites. Herein, we report a carbon-based nickel (Ni) cluster catalyst containing both single-atom and cluster sites (NiNx-T, T = 500–800) through a ligandmediated method and realize a highly active and selective electrocatalytic CO₂R process. The catalytic performance can be regulated by the dispersion of Ni–N species via controlling the pyrolysis condition. Benefitting from the synergistic effect of pyrrolicnitrogen coordinated Ni single-atom and cluster sites, NiNx-600 exhibits a satisfying catalytic performance, including a high partial current density of 61.85 mA cm⁻² and a high turnover frequency (TOF) of 7,291 h⁻¹ at −1.2 V vs. RHE, and almost 100% selectivity toward carbon monoxide (CO) production, as well as good stability under 10 h of continuous electrolysis. This work discloses the significant role of regulating the coordination environment of the transition metal sites and the synergistic effect between the isolated single-site and cluster site in enhancing the ECO₂R performance.
| Identifer | oai:union.ndltd.org:DRESDEN/oai:qucosa:de:qucosa:90714 |
| Date | 16 May 2024 |
| Creators | Hao, Qi, Liu, Dong-Xue, Deng, Ruiping, Zhong, Hai-Xia |
| Publisher | Frontiers Media |
| Source Sets | Hochschulschriftenserver (HSSS) der SLUB Dresden |
| Language | English |
| Detected Language | English |
| Type | info:eu-repo/semantics/publishedVersion, doc-type:article, info:eu-repo/semantics/article, doc-type:Text |
| Rights | info:eu-repo/semantics/openAccess |
| Relation | 2296-2646, 837580, 10.3389/fchem.2021.837580, info:eu-repo/grantAgreement/Jilin Province/Science and Technology Development Plan Funding/20200201079JC/, info:eu-repo/grantAgreement/Changchun/Science and Technology Development Plan Funding/19SS010/, info:eu-repo/grantAgreement/Jilin Province/Capital Construction Funds/2020C026-1/ |
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