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Research Article

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

Jiazhi Wang1,2, Qi Hao1,3, Haixia Zhong4, Kai Li1, Xinbo Zhang1,2( )
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
University of Science and Technology of China, Hefei 230026, China
Key Laboratory of Automobile Materials, Ministry of Education, Jilin University, Changchun 130022, China
Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden 01062, Germany
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Graphical Abstract

Interface-rich Au-doped PdBi one-dimensional (1D) alloy nanochains have been achieved using an “active auxiliary” strategy via a one-step liquid route. The PdBiAu alloy nanochains as multifunctional oxygen reduction reaction (ORR) catalysts boost the power density and durability of a direct methanol fuel cell device.

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·cm−2 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.

Keywords

single-atom Niiron phthalocyaninemolecular catalystcarbon dioxide reduction reactionultra-low overpotential

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Nano Research
Volume 15 Issue 7,
July 2022
Pages 5816-5823
DOI: 10.1007/s12274-022-4197-6
Cite this article:
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 Research, 2022, 15(7): 5816-5823. https://doi.org/10.1007/s12274-022-4197-6
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Received: 09 January 2022
Revised: 24 January 2022
Accepted: 25 January 2022
Published: 18 April 2022
© Tsinghua University Press 2022
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