4.8 Article

Ligand centered electrocatalytic efficient CO2 reduction reaction a low overpotential on single-atom Ni regulated molecular catalyst

期刊

NANO RESEARCH
卷 15, 期 7, 页码 5816-5823

出版社

TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-022-4197-6

关键词

single-atom Ni; iron phthalocyanine; molecular catalyst; carbon dioxide reduction reaction; ultra-low overpotential

资金

  1. Alexander von Humboldt Foundation
  2. National Natural Science Foundation of China [21725103]
  3. National Key R&D Program of China [2019YFA0705704]
  4. Strategic Priority Research Program of the Chinese Academy of Sciences [XDA21010210]
  5. Jilin Province Science and Technology Development Plan Funding Project [20200201079JC]
  6. Changchun Science and Technology Development Plan Funding Project [19SS010]
  7. Jilin Province Capital Construction Funds Project [2020C026-1]
  8. K. C. Wong Education Foundation [GJTD-2018-09]

向作者/读者索取更多资源

In this study, an isolated single-atom Ni catalyst regulated strategy was developed to activate and stabilize the iron phthalocyanine molecule (Ni SA@FePc) for a highly efficient CO2RR process at low overpotential. Ni SA@FePc showed significantly enhanced CO2RR performance compared to single-atom Ni catalyst and FePc molecule, thanks to its well-defined and homogenous catalytic centers with unique structures.
Electrochemical CO2 reduction reaction (CO2RR) into value-added chemicals/fuels is crucial for realizing the sustainable carbon cycle while mitigating the energy crisis. However, it is impeded by the relatively high overpotential and low energy efficiency due to the lack of efficient electrocatalysts. Herein, we develop an isolated single-atom Ni catalyst regulated strategy to activate and stabilize the iron phthalocyanine molecule (Ni SA@FePc) toward a highly efficient CO2RR process at low overpotential. The well-defined and homogenous catalytic centers with unique structures confer Ni SA@FePc with a significantly enhanced CO2RR performance compared to single-atom Ni catalyst and FePc molecule and afford the atomic understanding on active sites and catalytic mechanism. As expected, Ni SA@FePc exhibits a high selectivity of more significant Faraday efficiency (>= 95%) over a wide potential range, a high current density of similar to 252 mA.cm(-2) at low overpotential (390 mV), and excellent long-term stability for CO2 RR to CO. X-ray absorption spectroscopy measurement and theoretical calculation indicate the formation of NiN4-O-2-FePc heterogeneous structure for Ni SA@FePc. And CO2 RR prefers to occur at the raised N centers of NiN4-O-2 -FePc heterogeneous structure for Ni SA@FePc, which enables facilitated adsorption of *C001-1 and desorption of CO, and thus accelerated overall reaction kinetics.

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