A Nitrogen-Doped Carbon Catalyst for Electrochemical CO2 Conversion to CO with High Selectivity and Current Density

Huei Ru Molly Jhong; Claire E. Tornow; Bretislav Smid; Andrew A. Gewirth; Stephen M. Lyth; Paul J.A. Kenis

doi:10.1002/cssc.201600843

A Nitrogen-Doped Carbon Catalyst for Electrochemical CO₂ Conversion to CO with High Selectivity and Current Density

Huei Ru Molly Jhong, Claire E. Tornow, Bretislav Smid, Andrew A. Gewirth, Stephen M. Lyth, Paul J.A. Kenis

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

102 Citations (Scopus)

Abstract

We report characterization of a non-precious metal-free catalyst for the electrochemical reduction of CO₂ to CO; namely, a pyrolyzed carbon nitride and multiwall carbon nanotube composite. This catalyst exhibits a high selectivity for production of CO over H₂ (approximately 98 % CO and 2 % H₂), as well as high activity in an electrochemical flow cell. The CO partial current density at intermediate cathode potentials (V=−1.46 V vs. Ag/AgCl) is up to 3.5× higher than state-of-the-art Ag nanoparticle-based catalysts, and the maximum current density is 90 mA cm⁻². The mass activity and energy efficiency (up to 48 %) were also higher than the Ag nanoparticle reference. Moving away from precious metal catalysts without sacrificing activity or selectivity may significantly enhance the prospects of electrochemical CO₂ reduction as an approach to reduce atmospheric CO₂ emissions or as a method for load-leveling in relation to the use of intermittent renewable energy sources.

Original language	English
Pages (from-to)	1094-1099
Number of pages	6
Journal	ChemSusChem
Volume	10
Issue number	6
DOIs	https://doi.org/10.1002/cssc.201600843
Publication status	Published - Mar 22 2017

All Science Journal Classification (ASJC) codes

Environmental Chemistry
Chemical Engineering(all)
Materials Science(all)
Energy(all)

UN SDGs

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

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10.1002/cssc.201600843

Cite this

@article{53a01267b67c4a38b5885f1bcab8cdda,

title = "A Nitrogen-Doped Carbon Catalyst for Electrochemical CO2 Conversion to CO with High Selectivity and Current Density",

abstract = "We report characterization of a non-precious metal-free catalyst for the electrochemical reduction of CO2 to CO; namely, a pyrolyzed carbon nitride and multiwall carbon nanotube composite. This catalyst exhibits a high selectivity for production of CO over H2 (approximately 98 % CO and 2 % H2), as well as high activity in an electrochemical flow cell. The CO partial current density at intermediate cathode potentials (V=−1.46 V vs. Ag/AgCl) is up to 3.5× higher than state-of-the-art Ag nanoparticle-based catalysts, and the maximum current density is 90 mA cm−2. The mass activity and energy efficiency (up to 48 %) were also higher than the Ag nanoparticle reference. Moving away from precious metal catalysts without sacrificing activity or selectivity may significantly enhance the prospects of electrochemical CO2 reduction as an approach to reduce atmospheric CO2 emissions or as a method for load-leveling in relation to the use of intermittent renewable energy sources.",

author = "Jhong, {Huei Ru Molly} and Tornow, {Claire E.} and Bretislav Smid and Gewirth, {Andrew A.} and Lyth, {Stephen M.} and Kenis, {Paul J.A.}",

note = "Funding Information: We gratefully acknowledge financial support from the Department of Energy (DE-FG02005ER46260), the Department of Energy through an STTR grant to Dioxide Materials and UIUC (DE-SC0004453), and the National Science Foundation (CTS 05-47617). The International Institute of Carbon Neutral Energy Research (WPI-I2CNER), sponsored by the World Premier International Research Center Initiative (WPI), MEXT, Japan. The authors are grateful for support from the Progress 100 program of Kyushu University, supported by MEXT, Japan. We also acknowledge Yohan Kim for assistance in electrochemical testing, Richard Haasch, from the Frederick Seitz Materials Research Laboratory Central Facilities for assistance with XPS, Scott Robinson from the Beckman Institute for assistance with SEM imaging, and Steven R Caliari, Sumit Verma, and Byoungsu Kim for stimulating discussions. Publisher Copyright: {\textcopyright} 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim",

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T1 - A Nitrogen-Doped Carbon Catalyst for Electrochemical CO2 Conversion to CO with High Selectivity and Current Density

AU - Jhong, Huei Ru Molly

AU - Tornow, Claire E.

AU - Smid, Bretislav

AU - Gewirth, Andrew A.

AU - Lyth, Stephen M.

AU - Kenis, Paul J.A.

N1 - Funding Information: We gratefully acknowledge financial support from the Department of Energy (DE-FG02005ER46260), the Department of Energy through an STTR grant to Dioxide Materials and UIUC (DE-SC0004453), and the National Science Foundation (CTS 05-47617). The International Institute of Carbon Neutral Energy Research (WPI-I2CNER), sponsored by the World Premier International Research Center Initiative (WPI), MEXT, Japan. The authors are grateful for support from the Progress 100 program of Kyushu University, supported by MEXT, Japan. We also acknowledge Yohan Kim for assistance in electrochemical testing, Richard Haasch, from the Frederick Seitz Materials Research Laboratory Central Facilities for assistance with XPS, Scott Robinson from the Beckman Institute for assistance with SEM imaging, and Steven R Caliari, Sumit Verma, and Byoungsu Kim for stimulating discussions. Publisher Copyright: © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

PY - 2017/3/22

Y1 - 2017/3/22

N2 - We report characterization of a non-precious metal-free catalyst for the electrochemical reduction of CO2 to CO; namely, a pyrolyzed carbon nitride and multiwall carbon nanotube composite. This catalyst exhibits a high selectivity for production of CO over H2 (approximately 98 % CO and 2 % H2), as well as high activity in an electrochemical flow cell. The CO partial current density at intermediate cathode potentials (V=−1.46 V vs. Ag/AgCl) is up to 3.5× higher than state-of-the-art Ag nanoparticle-based catalysts, and the maximum current density is 90 mA cm−2. The mass activity and energy efficiency (up to 48 %) were also higher than the Ag nanoparticle reference. Moving away from precious metal catalysts without sacrificing activity or selectivity may significantly enhance the prospects of electrochemical CO2 reduction as an approach to reduce atmospheric CO2 emissions or as a method for load-leveling in relation to the use of intermittent renewable energy sources.

AB - We report characterization of a non-precious metal-free catalyst for the electrochemical reduction of CO2 to CO; namely, a pyrolyzed carbon nitride and multiwall carbon nanotube composite. This catalyst exhibits a high selectivity for production of CO over H2 (approximately 98 % CO and 2 % H2), as well as high activity in an electrochemical flow cell. The CO partial current density at intermediate cathode potentials (V=−1.46 V vs. Ag/AgCl) is up to 3.5× higher than state-of-the-art Ag nanoparticle-based catalysts, and the maximum current density is 90 mA cm−2. The mass activity and energy efficiency (up to 48 %) were also higher than the Ag nanoparticle reference. Moving away from precious metal catalysts without sacrificing activity or selectivity may significantly enhance the prospects of electrochemical CO2 reduction as an approach to reduce atmospheric CO2 emissions or as a method for load-leveling in relation to the use of intermittent renewable energy sources.

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