Understanding the effect of host structure of nitrogen doped ultrananocrystalline diamond electrode on electrochemical carbon dioxide reduction

Namal Wanninayake; Qianxiang Ai; Ruixin Zhou; Md Ariful Hoque; Sidney Herrell; Marcelo I. Guzman; Chad Risko; Doo Young Kim

doi:10.1016/j.carbon.2019.10.022

Understanding the effect of host structure of nitrogen doped ultrananocrystalline diamond electrode on electrochemical carbon dioxide reduction

Namal Wanninayake, Qianxiang Ai, Ruixin Zhou, Md Ariful Hoque, Sidney Herrell, Marcelo I. Guzman, Chad Risko, Doo Young Kim

Chemistry

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

34 Scopus citations

Abstract

Despite recent literature reporting the remarkable electrochemical CO₂ reduction reaction (CO2RR) performance of nitrogen-doped graphitic carbon materials (sp²-carbon) and nitrogen-doped diamond materials (sp³-carbon), no systematic studies have been conducted on the catalytic activities of hybrid carbon nanomaterials between diamond and graphitic extremes. In this study, nitrogen-doped ultra-nanocrystalline diamond thin films were prepared by a microwave-assisted chemical vapor deposition technique. The ratio of sp²-carbon phase to sp³-carbon phase was controlled by varying growth conditions. Our results confirm that nitrogen-doped sp²-carbon (graphitic) rich electrodes have better selectivity for the CO2RR products over the nitrogen-doped sp³-carbon rich electrodes, indicating that the host structure of nitrogen dopants is crucial for the catalytic activity. Nitrogen-doped sp²-carbon electrodes present Faradaic efficiency for CO production up to 82% with excellent activity and selectivity. The vital role of the host structure and the potential catalytic sites were detailed by density functional theory (DFT) calculations.

Original language	English
Pages (from-to)	408-419
Number of pages	12
Journal	Carbon
Volume	157
DOIs	https://doi.org/10.1016/j.carbon.2019.10.022
State	Published - Feb 2020

Bibliographical note

Funding Information:
N.W. and D.Y.K. appreciate the support from National Science Foundation under Cooperative Agreement No. 1355438 and Kentucky Science & Engineering Foundation grant (KSEF-3884-RDE-020). M.I.G. thanks research funding from NSF CAREER award (CHE-1255290). R.Z. acknowledges support from the University of Kentucky by a Research Challenge Trust Fund Fellowship. C.R. and Q.A. acknowledge the Research Corporation for Science Advancement (RCSA) Cottrell Scholars program (Award No. 24432) for funding the computational work. Supercomputing resources on the Lipscomb High Performance Computing Cluster were provided by the University of Kentucky Information Technology Department and the Center for Computational Sciences (CCS). The purchase of a new XPS system recently installed at the University of Kentucky was supported by the fund from the NSF EPSCoR grant (grant no. 0814194). The authors thank Prof. Y.T. Cheng, Rosemary Calabro and Dr. Yan Zhang for access to and their assistance on the XPS measurements; Dr. Justin Mobley, Prof. Anne-Frances Miller and Alexis Eugene to their cooperation on NMR measurements; Dr. Dali Qian and Dr. Nicolas Briot to their support on SEM and TEM measurements; Steven maynard for his assistance on building customized flow cell reactor and Prof. Thomas Jaramillo at Stanford University for his helpful suggestions regarding the flow cell design and electrochemical experiments.

Funding Information:
N.W. and D.Y.K. appreciate the support from National Science Foundation under Cooperative Agreement No. 1355438 and Kentucky Science & Engineering Foundation grant ( KSEF-3884-RDE-020 ). M.I.G. thanks research funding from NSF CAREER award ( CHE-1255290 ). R.Z. acknowledges support from the University of Kentucky by a Research Challenge Trust Fund Fellowship. C.R. and Q.A. acknowledge the Research Corporation for Science Advancement (RCSA) Cottrell Scholars program (Award No. 24432 ) for funding the computational work. Supercomputing resources on the Lipscomb High Performance Computing Cluster were provided by the University of Kentucky Information Technology Department and the Center for Computational Sciences (CCS). The purchase of a new XPS system recently installed at the University of Kentucky was supported by the fund from the NSF EPSCoR grant (grant no. 0814194 ). The authors thank Prof. Y.T. Cheng, Rosemary Calabro and Dr. Yan Zhang for access to and their assistance on the XPS measurements; Dr. Justin Mobley, Prof. Anne-Frances Miller and Alexis Eugene to their cooperation on NMR measurements; Dr. Dali Qian and Dr. Nicolas Briot to their support on SEM and TEM measurements; Steven maynard for his assistance on building customized flow cell reactor and Prof. Thomas Jaramillo at Stanford University for his helpful suggestions regarding the flow cell design and electrochemical experiments. Appendix A

Publisher Copyright:
© 2019 Elsevier Ltd

ASJC Scopus subject areas

Chemistry (all)
Materials Science (all)

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10.1016/j.carbon.2019.10.022

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@article{260f7d5041e445dbb32fd2d39f7cc19a,

title = "Understanding the effect of host structure of nitrogen doped ultrananocrystalline diamond electrode on electrochemical carbon dioxide reduction",

abstract = "Despite recent literature reporting the remarkable electrochemical CO2 reduction reaction (CO2RR) performance of nitrogen-doped graphitic carbon materials (sp2-carbon) and nitrogen-doped diamond materials (sp3-carbon), no systematic studies have been conducted on the catalytic activities of hybrid carbon nanomaterials between diamond and graphitic extremes. In this study, nitrogen-doped ultra-nanocrystalline diamond thin films were prepared by a microwave-assisted chemical vapor deposition technique. The ratio of sp2-carbon phase to sp3-carbon phase was controlled by varying growth conditions. Our results confirm that nitrogen-doped sp2-carbon (graphitic) rich electrodes have better selectivity for the CO2RR products over the nitrogen-doped sp3-carbon rich electrodes, indicating that the host structure of nitrogen dopants is crucial for the catalytic activity. Nitrogen-doped sp2-carbon electrodes present Faradaic efficiency for CO production up to 82% with excellent activity and selectivity. The vital role of the host structure and the potential catalytic sites were detailed by density functional theory (DFT) calculations.",

author = "Namal Wanninayake and Qianxiang Ai and Ruixin Zhou and Hoque, {Md Ariful} and Sidney Herrell and Guzman, {Marcelo I.} and Chad Risko and Kim, {Doo Young}",

note = "Funding Information: N.W. and D.Y.K. appreciate the support from National Science Foundation under Cooperative Agreement No. 1355438 and Kentucky Science & Engineering Foundation grant (KSEF-3884-RDE-020). M.I.G. thanks research funding from NSF CAREER award (CHE-1255290). R.Z. acknowledges support from the University of Kentucky by a Research Challenge Trust Fund Fellowship. C.R. and Q.A. acknowledge the Research Corporation for Science Advancement (RCSA) Cottrell Scholars program (Award No. 24432) for funding the computational work. Supercomputing resources on the Lipscomb High Performance Computing Cluster were provided by the University of Kentucky Information Technology Department and the Center for Computational Sciences (CCS). The purchase of a new XPS system recently installed at the University of Kentucky was supported by the fund from the NSF EPSCoR grant (grant no. 0814194). The authors thank Prof. Y.T. Cheng, Rosemary Calabro and Dr. Yan Zhang for access to and their assistance on the XPS measurements; Dr. Justin Mobley, Prof. Anne-Frances Miller and Alexis Eugene to their cooperation on NMR measurements; Dr. Dali Qian and Dr. Nicolas Briot to their support on SEM and TEM measurements; Steven maynard for his assistance on building customized flow cell reactor and Prof. Thomas Jaramillo at Stanford University for his helpful suggestions regarding the flow cell design and electrochemical experiments. Funding Information: N.W. and D.Y.K. appreciate the support from National Science Foundation under Cooperative Agreement No. 1355438 and Kentucky Science & Engineering Foundation grant ( KSEF-3884-RDE-020 ). M.I.G. thanks research funding from NSF CAREER award ( CHE-1255290 ). R.Z. acknowledges support from the University of Kentucky by a Research Challenge Trust Fund Fellowship. C.R. and Q.A. acknowledge the Research Corporation for Science Advancement (RCSA) Cottrell Scholars program (Award No. 24432 ) for funding the computational work. Supercomputing resources on the Lipscomb High Performance Computing Cluster were provided by the University of Kentucky Information Technology Department and the Center for Computational Sciences (CCS). The purchase of a new XPS system recently installed at the University of Kentucky was supported by the fund from the NSF EPSCoR grant (grant no. 0814194 ). The authors thank Prof. Y.T. Cheng, Rosemary Calabro and Dr. Yan Zhang for access to and their assistance on the XPS measurements; Dr. Justin Mobley, Prof. Anne-Frances Miller and Alexis Eugene to their cooperation on NMR measurements; Dr. Dali Qian and Dr. Nicolas Briot to their support on SEM and TEM measurements; Steven maynard for his assistance on building customized flow cell reactor and Prof. Thomas Jaramillo at Stanford University for his helpful suggestions regarding the flow cell design and electrochemical experiments. Appendix A Publisher Copyright: {\textcopyright} 2019 Elsevier Ltd",

year = "2020",

month = feb,

doi = "10.1016/j.carbon.2019.10.022",

language = "English",

volume = "157",

pages = "408--419",

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T1 - Understanding the effect of host structure of nitrogen doped ultrananocrystalline diamond electrode on electrochemical carbon dioxide reduction

AU - Wanninayake, Namal

AU - Ai, Qianxiang

AU - Zhou, Ruixin

AU - Hoque, Md Ariful

AU - Herrell, Sidney

AU - Guzman, Marcelo I.

AU - Risko, Chad

AU - Kim, Doo Young

N1 - Funding Information: N.W. and D.Y.K. appreciate the support from National Science Foundation under Cooperative Agreement No. 1355438 and Kentucky Science & Engineering Foundation grant (KSEF-3884-RDE-020). M.I.G. thanks research funding from NSF CAREER award (CHE-1255290). R.Z. acknowledges support from the University of Kentucky by a Research Challenge Trust Fund Fellowship. C.R. and Q.A. acknowledge the Research Corporation for Science Advancement (RCSA) Cottrell Scholars program (Award No. 24432) for funding the computational work. Supercomputing resources on the Lipscomb High Performance Computing Cluster were provided by the University of Kentucky Information Technology Department and the Center for Computational Sciences (CCS). The purchase of a new XPS system recently installed at the University of Kentucky was supported by the fund from the NSF EPSCoR grant (grant no. 0814194). The authors thank Prof. Y.T. Cheng, Rosemary Calabro and Dr. Yan Zhang for access to and their assistance on the XPS measurements; Dr. Justin Mobley, Prof. Anne-Frances Miller and Alexis Eugene to their cooperation on NMR measurements; Dr. Dali Qian and Dr. Nicolas Briot to their support on SEM and TEM measurements; Steven maynard for his assistance on building customized flow cell reactor and Prof. Thomas Jaramillo at Stanford University for his helpful suggestions regarding the flow cell design and electrochemical experiments. Funding Information: N.W. and D.Y.K. appreciate the support from National Science Foundation under Cooperative Agreement No. 1355438 and Kentucky Science & Engineering Foundation grant ( KSEF-3884-RDE-020 ). M.I.G. thanks research funding from NSF CAREER award ( CHE-1255290 ). R.Z. acknowledges support from the University of Kentucky by a Research Challenge Trust Fund Fellowship. C.R. and Q.A. acknowledge the Research Corporation for Science Advancement (RCSA) Cottrell Scholars program (Award No. 24432 ) for funding the computational work. Supercomputing resources on the Lipscomb High Performance Computing Cluster were provided by the University of Kentucky Information Technology Department and the Center for Computational Sciences (CCS). The purchase of a new XPS system recently installed at the University of Kentucky was supported by the fund from the NSF EPSCoR grant (grant no. 0814194 ). The authors thank Prof. Y.T. Cheng, Rosemary Calabro and Dr. Yan Zhang for access to and their assistance on the XPS measurements; Dr. Justin Mobley, Prof. Anne-Frances Miller and Alexis Eugene to their cooperation on NMR measurements; Dr. Dali Qian and Dr. Nicolas Briot to their support on SEM and TEM measurements; Steven maynard for his assistance on building customized flow cell reactor and Prof. Thomas Jaramillo at Stanford University for his helpful suggestions regarding the flow cell design and electrochemical experiments. Appendix A Publisher Copyright: © 2019 Elsevier Ltd

PY - 2020/2

Y1 - 2020/2

N2 - Despite recent literature reporting the remarkable electrochemical CO2 reduction reaction (CO2RR) performance of nitrogen-doped graphitic carbon materials (sp2-carbon) and nitrogen-doped diamond materials (sp3-carbon), no systematic studies have been conducted on the catalytic activities of hybrid carbon nanomaterials between diamond and graphitic extremes. In this study, nitrogen-doped ultra-nanocrystalline diamond thin films were prepared by a microwave-assisted chemical vapor deposition technique. The ratio of sp2-carbon phase to sp3-carbon phase was controlled by varying growth conditions. Our results confirm that nitrogen-doped sp2-carbon (graphitic) rich electrodes have better selectivity for the CO2RR products over the nitrogen-doped sp3-carbon rich electrodes, indicating that the host structure of nitrogen dopants is crucial for the catalytic activity. Nitrogen-doped sp2-carbon electrodes present Faradaic efficiency for CO production up to 82% with excellent activity and selectivity. The vital role of the host structure and the potential catalytic sites were detailed by density functional theory (DFT) calculations.

AB - Despite recent literature reporting the remarkable electrochemical CO2 reduction reaction (CO2RR) performance of nitrogen-doped graphitic carbon materials (sp2-carbon) and nitrogen-doped diamond materials (sp3-carbon), no systematic studies have been conducted on the catalytic activities of hybrid carbon nanomaterials between diamond and graphitic extremes. In this study, nitrogen-doped ultra-nanocrystalline diamond thin films were prepared by a microwave-assisted chemical vapor deposition technique. The ratio of sp2-carbon phase to sp3-carbon phase was controlled by varying growth conditions. Our results confirm that nitrogen-doped sp2-carbon (graphitic) rich electrodes have better selectivity for the CO2RR products over the nitrogen-doped sp3-carbon rich electrodes, indicating that the host structure of nitrogen dopants is crucial for the catalytic activity. Nitrogen-doped sp2-carbon electrodes present Faradaic efficiency for CO production up to 82% with excellent activity and selectivity. The vital role of the host structure and the potential catalytic sites were detailed by density functional theory (DFT) calculations.

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Understanding the effect of host structure of nitrogen doped ultrananocrystalline diamond electrode on electrochemical carbon dioxide reduction

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