Electrochemical Conversion of CO 2 to Syngas with Controllable CO/H 2 Ratios over Co and Ni Single‐Atom Catalysts
Abstract
Abstract The electrochemical CO 2 reduction reaction (CO 2 RR) to yield synthesis gas (syngas, CO and H 2 ) has been considered as a promising method to realize the net reduction in CO 2 emission. However, it is challenging to balance the CO 2 RR activity and the CO/H 2 ratio. To address this issue, nitrogen‐doped carbon supported single‐atom catalysts are designed as electrocatalysts to produce syngas from CO 2 RR. While Co and Ni single‐atom catalysts are selective in producing H 2 and CO, respectively, electrocatalysts containing both Co and Ni show a high syngas evolution (total current >74 mA cm −2 ) with CO/H 2 ratios (0.23–2.26) that are suitable for typical downstream thermochemical reactions. Density functional theory calculations provide insights into the key intermediates on Co and Ni single‐atom configurations for the H 2 and CO evolution. The results present a useful case on how non‐precious transition metal species can maintain high CO 2 RR activity with tunable CO/H 2 ratios.
- Authors:
-
[1];
[3];
[4];
[5];
[4]
- National Synchrotron Radiation Laboratory CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei Anhui 230029 China, Department of Chemical Engineering Columbia University New York NY 10027 USA
- School of Materials Science and Engineering Nanyang Technological University Singapore 639798 Singapore
- Department of Chemical Engineering Columbia University New York NY 10027 USA
- Department of Chemical Engineering Columbia University New York NY 10027 USA, Chemistry Division Brookhaven National Laboratory Upton NY 11973 USA
- Center for Functional Nanomaterials Brookhaven National Laboratory Upton NY 11973 USA
- Department of Physics Florida A&,M University Tallahassee FL 32307 USA
- National Synchrotron Radiation Laboratory CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei Anhui 230029 China
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1581851
- Grant/Contract Number:
- FG02-13ER16381; SC0009476
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition) Journal Volume: 59 Journal Issue: 8; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
He, Qun, Liu, Daobin, Lee, Ji Hoon, Liu, Yumeng, Xie, Zhenhua, Hwang, Sooyeon, Kattel, Shyam, Song, Li, and Chen, Jingguang G. Electrochemical Conversion of CO 2 to Syngas with Controllable CO/H 2 Ratios over Co and Ni Single‐Atom Catalysts. Germany: N. p., 2020.
Web. doi:10.1002/anie.201912719.
He, Qun, Liu, Daobin, Lee, Ji Hoon, Liu, Yumeng, Xie, Zhenhua, Hwang, Sooyeon, Kattel, Shyam, Song, Li, & Chen, Jingguang G. Electrochemical Conversion of CO 2 to Syngas with Controllable CO/H 2 Ratios over Co and Ni Single‐Atom Catalysts. Germany. https://doi.org/10.1002/anie.201912719
He, Qun, Liu, Daobin, Lee, Ji Hoon, Liu, Yumeng, Xie, Zhenhua, Hwang, Sooyeon, Kattel, Shyam, Song, Li, and Chen, Jingguang G. Thu .
"Electrochemical Conversion of CO 2 to Syngas with Controllable CO/H 2 Ratios over Co and Ni Single‐Atom Catalysts". Germany. https://doi.org/10.1002/anie.201912719.
@article{osti_1581851,
title = {Electrochemical Conversion of CO 2 to Syngas with Controllable CO/H 2 Ratios over Co and Ni Single‐Atom Catalysts},
author = {He, Qun and Liu, Daobin and Lee, Ji Hoon and Liu, Yumeng and Xie, Zhenhua and Hwang, Sooyeon and Kattel, Shyam and Song, Li and Chen, Jingguang G.},
abstractNote = {Abstract The electrochemical CO 2 reduction reaction (CO 2 RR) to yield synthesis gas (syngas, CO and H 2 ) has been considered as a promising method to realize the net reduction in CO 2 emission. However, it is challenging to balance the CO 2 RR activity and the CO/H 2 ratio. To address this issue, nitrogen‐doped carbon supported single‐atom catalysts are designed as electrocatalysts to produce syngas from CO 2 RR. While Co and Ni single‐atom catalysts are selective in producing H 2 and CO, respectively, electrocatalysts containing both Co and Ni show a high syngas evolution (total current >74 mA cm −2 ) with CO/H 2 ratios (0.23–2.26) that are suitable for typical downstream thermochemical reactions. Density functional theory calculations provide insights into the key intermediates on Co and Ni single‐atom configurations for the H 2 and CO evolution. The results present a useful case on how non‐precious transition metal species can maintain high CO 2 RR activity with tunable CO/H 2 ratios.},
doi = {10.1002/anie.201912719},
journal = {Angewandte Chemie (International Edition)},
number = 8,
volume = 59,
place = {Germany},
year = {Thu Jan 09 00:00:00 EST 2020},
month = {Thu Jan 09 00:00:00 EST 2020}
}
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