Understanding the Origin of Selective Reduction of CO2 to CO on Single-Atom Nickel Catalyst.

Shi He; Dong Ji; Junwei Zhang; Peter Novello; Xueqian Li; Qiang Zhang; Xixiang Zhang; Jie Liu

doi:10.1021/acs.jpcb.9b09730

Understanding the Origin of Selective Reduction of CO2 to CO on Single-Atom Nickel Catalyst.

Shi He, Dong Ji, Junwei Zhang, Peter Novello, Xueqian Li, Qiang Zhang, Xixiang Zhang, Jie Liu

Research output: Contribution to journal › Article › peer-review

23 Scopus citations

Abstract

Electrochemical reduction of CO2 to CO offers a promising strategy for regulating the global carbon cycle and providing feedstock for the chemical industry. Understanding the origin that determines the faradaic efficiency (FE) of reduction of CO2 to CO is critical for developing a highly efficient electrocatalyst. Here, by constructing a single-atom Ni catalyst on nitrogen-doped winged carbon nanofiber (NiSA-NWC), we find that the single-atom Ni catalyst possesses the maximum CO FE of over 95% at -1.6 V vs Ag/AgCl, which is about 30% higher than the standard Ni nanoparticles on the same support. The Tafel analysis reveals that the single-atom Ni catalyst has a preferred reduction of CO2 to CO and a slower rate for the hydrogen evolution reaction. We propose that the domination of singular Ni1+ electronic states and limited hydrogen atom adsorption sites on the single-atom Ni catalyst lead to the observed high FE for CO2 reduction to CO.

Original language	English (US)
Pages (from-to)	511-518
Number of pages	8
Journal	The journal of physical chemistry. B
Volume	124
Issue number	3
DOIs	https://doi.org/10.1021/acs.jpcb.9b09730
State	Published - Dec 27 2019

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: This research is partially supported by the National Science Foundation (CHE-1565657) and the Army Research Office(Award W911NF-15-1-0320). S.H. was supported by fellowships from Department of Chemistry at Duke University. The authors also acknowledge the support by the Duke University Shared Materials Instrumentation Facility (SMIF), a member of the North Carolina Research Triangle Nanotechnology Network (RTNN), which is supported by the National Science Foundation (Grant ECCS-1542015) as part of the National Nanotechnology Coordinated Infrastructure (NNCI).

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title = "Understanding the Origin of Selective Reduction of CO2 to CO on Single-Atom Nickel Catalyst.",

abstract = "Electrochemical reduction of CO2 to CO offers a promising strategy for regulating the global carbon cycle and providing feedstock for the chemical industry. Understanding the origin that determines the faradaic efficiency (FE) of reduction of CO2 to CO is critical for developing a highly efficient electrocatalyst. Here, by constructing a single-atom Ni catalyst on nitrogen-doped winged carbon nanofiber (NiSA-NWC), we find that the single-atom Ni catalyst possesses the maximum CO FE of over 95% at -1.6 V vs Ag/AgCl, which is about 30% higher than the standard Ni nanoparticles on the same support. The Tafel analysis reveals that the single-atom Ni catalyst has a preferred reduction of CO2 to CO and a slower rate for the hydrogen evolution reaction. We propose that the domination of singular Ni1+ electronic states and limited hydrogen atom adsorption sites on the single-atom Ni catalyst lead to the observed high FE for CO2 reduction to CO.",

author = "Shi He and Dong Ji and Junwei Zhang and Peter Novello and Xueqian Li and Qiang Zhang and Xixiang Zhang and Jie Liu",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: This research is partially supported by the National Science Foundation (CHE-1565657) and the Army Research Office(Award W911NF-15-1-0320). S.H. was supported by fellowships from Department of Chemistry at Duke University. The authors also acknowledge the support by the Duke University Shared Materials Instrumentation Facility (SMIF), a member of the North Carolina Research Triangle Nanotechnology Network (RTNN), which is supported by the National Science Foundation (Grant ECCS-1542015) as part of the National Nanotechnology Coordinated Infrastructure (NNCI).",

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AU - He, Shi

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AU - Zhang, Qiang

AU - Zhang, Xixiang

AU - Liu, Jie

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: This research is partially supported by the National Science Foundation (CHE-1565657) and the Army Research Office(Award W911NF-15-1-0320). S.H. was supported by fellowships from Department of Chemistry at Duke University. The authors also acknowledge the support by the Duke University Shared Materials Instrumentation Facility (SMIF), a member of the North Carolina Research Triangle Nanotechnology Network (RTNN), which is supported by the National Science Foundation (Grant ECCS-1542015) as part of the National Nanotechnology Coordinated Infrastructure (NNCI).

PY - 2019/12/27

Y1 - 2019/12/27

N2 - Electrochemical reduction of CO2 to CO offers a promising strategy for regulating the global carbon cycle and providing feedstock for the chemical industry. Understanding the origin that determines the faradaic efficiency (FE) of reduction of CO2 to CO is critical for developing a highly efficient electrocatalyst. Here, by constructing a single-atom Ni catalyst on nitrogen-doped winged carbon nanofiber (NiSA-NWC), we find that the single-atom Ni catalyst possesses the maximum CO FE of over 95% at -1.6 V vs Ag/AgCl, which is about 30% higher than the standard Ni nanoparticles on the same support. The Tafel analysis reveals that the single-atom Ni catalyst has a preferred reduction of CO2 to CO and a slower rate for the hydrogen evolution reaction. We propose that the domination of singular Ni1+ electronic states and limited hydrogen atom adsorption sites on the single-atom Ni catalyst lead to the observed high FE for CO2 reduction to CO.

AB - Electrochemical reduction of CO2 to CO offers a promising strategy for regulating the global carbon cycle and providing feedstock for the chemical industry. Understanding the origin that determines the faradaic efficiency (FE) of reduction of CO2 to CO is critical for developing a highly efficient electrocatalyst. Here, by constructing a single-atom Ni catalyst on nitrogen-doped winged carbon nanofiber (NiSA-NWC), we find that the single-atom Ni catalyst possesses the maximum CO FE of over 95% at -1.6 V vs Ag/AgCl, which is about 30% higher than the standard Ni nanoparticles on the same support. The Tafel analysis reveals that the single-atom Ni catalyst has a preferred reduction of CO2 to CO and a slower rate for the hydrogen evolution reaction. We propose that the domination of singular Ni1+ electronic states and limited hydrogen atom adsorption sites on the single-atom Ni catalyst lead to the observed high FE for CO2 reduction to CO.

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Understanding the Origin of Selective Reduction of CO2 to CO on Single-Atom Nickel Catalyst.

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