Production of C2/C3 Oxygenates from Planar Copper Nitride-Derived Mesoporous Copper via Electrochemical Reduction of CO2
Abstract
Electrochemical reduction of CO2 provides an opportunity to produce fuels and chemicals in a carbon-neutral manner, assuming that CO2 can be captured from the atmosphere. To do so requires efficient, selective, and stable catalysts. In this study, we report a highly mesoporous metallic Cu catalyst prepared by electrochemical reduction of thermally nitrided Cu foil. Under aqueous saturated CO2 reduction conditions, the Cu3N-derived Cu electrocatalyst produces virtually no CH4, very little CO, and exhibits a faradaic efficiency of 68% in C2+ products (C2H4, C2H5OH, and C3H7OH) at a current density of ~18.5 mA cm–2 and a cathode potential of -1.0 V versus the reversible hydrogen electrode. Under these conditions, the catalyst produces more oxygenated products than hydrocarbons. We show that surface roughness is a good descriptor of catalytic performance. The roughest surface reached 98% CO utilization efficiency for C2+ product formation from CO2 reduction and the ratio of oxygenated to hydrocarbon products correlates with the degree of surface roughness. These effects of surface roughness are attributed to the high population of undercoordinated sites as well as a high pH environment within the mesopores and adjacent to the surface of the catalyst.
- Authors:
-
[2];
[3];
[2];
[3]
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis (JCAP)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis (JCAP; Univ. of California, Berkeley, CA (United States); Shanghai Jiao Tong Univ. (China)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis (JCAP), Chemical Sciences Division
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1609119
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 32; Journal Issue: 7; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Layers; Electrodes; Surface roughness; Catalysts; Electrolytes
Citation Formats
Ebaid, Mohamed, Jiang, Kun, Zhang, Zemin, Drisdell, Walter S., Bell, Alexis T., and Cooper, Jason K. Production of C2/C3 Oxygenates from Planar Copper Nitride-Derived Mesoporous Copper via Electrochemical Reduction of CO2. United States: N. p., 2020.
Web. doi:10.1021/acs.chemmater.0c00761.
Ebaid, Mohamed, Jiang, Kun, Zhang, Zemin, Drisdell, Walter S., Bell, Alexis T., & Cooper, Jason K. Production of C2/C3 Oxygenates from Planar Copper Nitride-Derived Mesoporous Copper via Electrochemical Reduction of CO2. United States. https://doi.org/10.1021/acs.chemmater.0c00761
Ebaid, Mohamed, Jiang, Kun, Zhang, Zemin, Drisdell, Walter S., Bell, Alexis T., and Cooper, Jason K. Tue .
"Production of C2/C3 Oxygenates from Planar Copper Nitride-Derived Mesoporous Copper via Electrochemical Reduction of CO2". United States. https://doi.org/10.1021/acs.chemmater.0c00761. https://www.osti.gov/servlets/purl/1609119.
@article{osti_1609119,
title = {Production of C2/C3 Oxygenates from Planar Copper Nitride-Derived Mesoporous Copper via Electrochemical Reduction of CO2},
author = {Ebaid, Mohamed and Jiang, Kun and Zhang, Zemin and Drisdell, Walter S. and Bell, Alexis T. and Cooper, Jason K.},
abstractNote = {Electrochemical reduction of CO2 provides an opportunity to produce fuels and chemicals in a carbon-neutral manner, assuming that CO2 can be captured from the atmosphere. To do so requires efficient, selective, and stable catalysts. In this study, we report a highly mesoporous metallic Cu catalyst prepared by electrochemical reduction of thermally nitrided Cu foil. Under aqueous saturated CO2 reduction conditions, the Cu3N-derived Cu electrocatalyst produces virtually no CH4, very little CO, and exhibits a faradaic efficiency of 68% in C2+ products (C2H4, C2H5OH, and C3H7OH) at a current density of ~18.5 mA cm–2 and a cathode potential of -1.0 V versus the reversible hydrogen electrode. Under these conditions, the catalyst produces more oxygenated products than hydrocarbons. We show that surface roughness is a good descriptor of catalytic performance. The roughest surface reached 98% CO utilization efficiency for C2+ product formation from CO2 reduction and the ratio of oxygenated to hydrocarbon products correlates with the degree of surface roughness. These effects of surface roughness are attributed to the high population of undercoordinated sites as well as a high pH environment within the mesopores and adjacent to the surface of the catalyst.},
doi = {10.1021/acs.chemmater.0c00761},
journal = {Chemistry of Materials},
number = 7,
volume = 32,
place = {United States},
year = {Tue Mar 03 00:00:00 EST 2020},
month = {Tue Mar 03 00:00:00 EST 2020}
}
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