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Atomic-Level Active Sites of Efficient Imidazolate Frameworks-Derived Nickel Catalysts for CO2 Reduction

Abstract

Nickel and nitrogen co-doped carbon (Ni-N-C) has emerged as a promising catalyst for CO2 reduction reaction (CO2RR); however, the chemical nature of its active sites has remained elusive. Herein, we report the exploration of the reactivity and active sites of Ni-N-C for CO2RR. Single atomic Ni coordinated with N confined in the carbon matrix was prepared through thermal activation of chemically Ni-doped zeolitic imidazolate frameworks (ZIF) and directly visualized by aberration-corrected scanning transmission electron microscopy. Electrochemical results show the enhanced intrinsic reactivity and selectivity of Ni−N sites for the reduction of CO2 to CO, delivering a maximum CO Faradaic efficiency of 96% at a low overpotential of 570 mV. Desnity functuional theory (DFT) calculations predict that the edge-located Ni-N2+2 sites with dangling bond-containing carbon atoms is the active site facilitating the dissociation of the C−O bond of *COOH intermediate, while the bulk-hosted Ni−N4 is kinetically inactive. Furthermore, the high capability of the edge-located Ni−N4 being able to thermodynamically suppress the competitive hydrogen evolution is also explained. The proposal of edge-hosed Ni−N2+2 site provides new insight in designing high-efficiency Ni-N-C for CO2 reduction.

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Publication details

The article was received on 13 Aug 2019, accepted on 29 Oct 2019 and first published on 30 Oct 2019


Article type: Communication
DOI: 10.1039/C9TA08862H
J. Mater. Chem. A, 2019, Accepted Manuscript

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    Atomic-Level Active Sites of Efficient Imidazolate Frameworks-Derived Nickel Catalysts for CO2 Reduction

    F. Pan, H. Zhang, Z. Liu, D. A. Cullen, K. Liu, K. L. More, G. Wu, G. Wang and Y. Li, J. Mater. Chem. A, 2019, Accepted Manuscript , DOI: 10.1039/C9TA08862H

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