Impurity Tolerance of Unsaturated Ni-N-C Active Sites for Practical Electrochemical CO2 Reduction

Josh Leverett; Jodie A. Yuwono; Priyank Kumar; Thanh Tran-Phu; Jiangtao Qu; Julie Cairney; Xichu Wang; Alexandr N. Simonov; Rosalie K. Hocking; Bernt Johannessen; Liming Dai; Rahman Daiyan; Rose Amal

doi:10.1021/acsenergylett.1c02711

Impurity Tolerance of Unsaturated Ni-N-C Active Sites for Practical Electrochemical CO₂Reduction

Josh Leverett
, Jodie A. Yuwono
, Priyank Kumar
, Thanh Tran-Phu
, Jiangtao Qu
, Julie Cairney
, Xichu Wang
, Alexandr N. Simonov
, Rosalie K. Hocking
, Bernt Johannessen
, Liming Dai
, Rahman Daiyan
, Rose Amal

School of Chemistry

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

90 Citations (Scopus)

Abstract

Demonstrating the potential of the electrochemical carbon dioxide reduction reaction (CO2RR) in industrially relevant conditions is a promising route for achieving net-zero emissions through decarbonization. This requires a catalyst system that displays not only high activity and stability but also the capacity to deliver a consistent performance in the presence of waste stream impurities. To explore these opportunities, we investigate the role that the Ni coordination structure plays on the impurity tolerance of highly active single-atom catalysts (SACs) during CO2RR. The as-synthesized materials are highly active for CO2RR to CO, achieving a current density of 470 mA cm-2 and a CO selectivity of 99% in a CO2 electrolyzer. We demonstrate, through high-temperature pyrolysis, that a higher concentration of "unsaturated"Ni-N4-x-Cx sites significantly improves the tolerance to NOx, SOx, volatile organic compounds, and SCN- impurities in aqueous electrolyte, paving the way for SACs capable of CO2RR in industrial conditions.

Original language	English
Pages (from-to)	920-928
Number of pages	9
Journal	ACS Energy Letters
Volume	7
Issue number	3
DOIs	https://doi.org/10.1021/acsenergylett.1c02711
Publication status	Published - 9 Feb 2022

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This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

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10.1021/acsenergylett.1c02711

Cite this

@article{b126aff5e72846f0aac569411419e74c,

title = "Impurity Tolerance of Unsaturated Ni-N-C Active Sites for Practical Electrochemical CO2 Reduction",

abstract = "Demonstrating the potential of the electrochemical carbon dioxide reduction reaction (CO2RR) in industrially relevant conditions is a promising route for achieving net-zero emissions through decarbonization. This requires a catalyst system that displays not only high activity and stability but also the capacity to deliver a consistent performance in the presence of waste stream impurities. To explore these opportunities, we investigate the role that the Ni coordination structure plays on the impurity tolerance of highly active single-atom catalysts (SACs) during CO2RR. The as-synthesized materials are highly active for CO2RR to CO, achieving a current density of 470 mA cm-2 and a CO selectivity of 99\% in a CO2 electrolyzer. We demonstrate, through high-temperature pyrolysis, that a higher concentration of {"}unsaturated{"}Ni-N4-x-Cx sites significantly improves the tolerance to NOx, SOx, volatile organic compounds, and SCN- impurities in aqueous electrolyte, paving the way for SACs capable of CO2RR in industrial conditions. ",

author = "Josh Leverett and Yuwono, \{Jodie A.\} and Priyank Kumar and Thanh Tran-Phu and Jiangtao Qu and Julie Cairney and Xichu Wang and Simonov, \{Alexandr N.\} and Hocking, \{Rosalie K.\} and Bernt Johannessen and Liming Dai and Rahman Daiyan and Rose Amal",

note = "Funding Information: All material and surface characterizations were carried out at Mark Wainwright Analytical Centre (MWAC), UNSW. The work was supported by the Australian Research Council (ARC) Research Hub on Integrated Energy Storage Solutions (IH180100020) and ARC Training Centre for The Global Hydrogen Economy (IC200100023). The authors acknowledge the technical and scientific support from the Microscopy Australia node at UNSW (Electron Microscope Unit) and the University of Sydney. Publisher Copyright: {\textcopyright} 2022 American Chemical Society.",

year = "2022",

month = feb,

day = "9",

doi = "10.1021/acsenergylett.1c02711",

language = "English",

volume = "7",

pages = "920--928",

journal = "ACS Energy Letters",

issn = "2380-8195",

publisher = "American Chemical Society",

number = "3",

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T1 - Impurity Tolerance of Unsaturated Ni-N-C Active Sites for Practical Electrochemical CO2 Reduction

AU - Leverett, Josh

AU - Yuwono, Jodie A.

AU - Kumar, Priyank

AU - Tran-Phu, Thanh

AU - Qu, Jiangtao

AU - Cairney, Julie

AU - Wang, Xichu

AU - Simonov, Alexandr N.

AU - Hocking, Rosalie K.

AU - Johannessen, Bernt

AU - Dai, Liming

AU - Daiyan, Rahman

AU - Amal, Rose

N1 - Funding Information: All material and surface characterizations were carried out at Mark Wainwright Analytical Centre (MWAC), UNSW. The work was supported by the Australian Research Council (ARC) Research Hub on Integrated Energy Storage Solutions (IH180100020) and ARC Training Centre for The Global Hydrogen Economy (IC200100023). The authors acknowledge the technical and scientific support from the Microscopy Australia node at UNSW (Electron Microscope Unit) and the University of Sydney. Publisher Copyright: © 2022 American Chemical Society.

PY - 2022/2/9

Y1 - 2022/2/9

N2 - Demonstrating the potential of the electrochemical carbon dioxide reduction reaction (CO2RR) in industrially relevant conditions is a promising route for achieving net-zero emissions through decarbonization. This requires a catalyst system that displays not only high activity and stability but also the capacity to deliver a consistent performance in the presence of waste stream impurities. To explore these opportunities, we investigate the role that the Ni coordination structure plays on the impurity tolerance of highly active single-atom catalysts (SACs) during CO2RR. The as-synthesized materials are highly active for CO2RR to CO, achieving a current density of 470 mA cm-2 and a CO selectivity of 99% in a CO2 electrolyzer. We demonstrate, through high-temperature pyrolysis, that a higher concentration of "unsaturated"Ni-N4-x-Cx sites significantly improves the tolerance to NOx, SOx, volatile organic compounds, and SCN- impurities in aqueous electrolyte, paving the way for SACs capable of CO2RR in industrial conditions.

AB - Demonstrating the potential of the electrochemical carbon dioxide reduction reaction (CO2RR) in industrially relevant conditions is a promising route for achieving net-zero emissions through decarbonization. This requires a catalyst system that displays not only high activity and stability but also the capacity to deliver a consistent performance in the presence of waste stream impurities. To explore these opportunities, we investigate the role that the Ni coordination structure plays on the impurity tolerance of highly active single-atom catalysts (SACs) during CO2RR. The as-synthesized materials are highly active for CO2RR to CO, achieving a current density of 470 mA cm-2 and a CO selectivity of 99% in a CO2 electrolyzer. We demonstrate, through high-temperature pyrolysis, that a higher concentration of "unsaturated"Ni-N4-x-Cx sites significantly improves the tolerance to NOx, SOx, volatile organic compounds, and SCN- impurities in aqueous electrolyte, paving the way for SACs capable of CO2RR in industrial conditions.

UR - https://www.scopus.com/pages/publications/85125082867

U2 - 10.1021/acsenergylett.1c02711

DO - 10.1021/acsenergylett.1c02711

M3 - Article

AN - SCOPUS:85125082867

SN - 2380-8195

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SP - 920

EP - 928

JO - ACS Energy Letters

JF - ACS Energy Letters

IS - 3

ER -

Impurity Tolerance of Unsaturated Ni-N-C Active Sites for Practical Electrochemical CO₂Reduction

Abstract

UN SDGs

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ARC Training Centre for The Global Hydrogen Economy - UNSW

ARC Centre of Excellence for Electromaterials Science

Cite this

Impurity Tolerance of Unsaturated Ni-N-C Active Sites for Practical Electrochemical CO2 Reduction

Abstract

UN SDGs

Access to Document

Other files and links

Projects

ARC Training Centre for The Global Hydrogen Economy - UNSW

ARC Centre of Excellence for Electromaterials Science

Cite this

Impurity Tolerance of Unsaturated Ni-N-C Active Sites for Practical Electrochemical CO₂Reduction