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

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Abstract

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 ∼ 252 mA·cm2 at low overpotential (390 mV), and excellent long-term stability for CO2RR to CO. X-ray absorption spectroscopy measurement and theoretical calculation indicate the formation of NiN4-O2-FePc heterogeneous structure for Ni SA@FePc. And CO2RR prefers to occur at the raised N centers of NiN4-O2-FePc heterogeneous structure for Ni SA@FePc, which enables facilitated adsorption of *COOH and desorption of CO, and thus accelerated overall reaction kinetics.

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Acknowledgments

H. X. Z. acknowledges funding from the Alexander von Humboldt Foundation. This work was supported by the National Natural Science Foundation of China (No. 21725103), National Key R&D Program of China (No. 2019YFA0705704), the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDA21010210), Jilin Province Science and Technology Development Plan Funding Project (No. 20200201079JC), Changchun Science and Technology Development Plan Funding Project (No. 19SS010), Jilin Province Capital Construction Funds Project (No. 2020C026-1), and the K. C. Wong Education Foundation (No. GJTD-2018-09).

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Authors and Affiliations

  1. State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, China

    Jiazhi Wang, Qi Hao, Kai Li & Xinbo Zhang

  2. University of Science and Technology of China, Hefei, 230026, China

    Jiazhi Wang & Xinbo Zhang

  3. Key Laboratory of Automobile Materials, Ministry of Education, Jilin University, Changchun, 130022, China

    Qi Hao

  4. Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, 01062, Germany

    Haixia Zhong

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  1. Jiazhi Wang
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Correspondence to Xinbo Zhang.

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

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Wang, J., Hao, Q., Zhong, H. et al. Ligand centered electrocatalytic efficient CO2 reduction reaction at low overpotential on single-atom Ni regulated molecular catalyst. Nano Res. 15, 5816–5823 (2022). https://doi.org/10.1007/s12274-022-4197-6

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