Promoting CO2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs
Abstract
Electroreduction uses renewable energy to upgrade carbon dioxide to value-added chemicals and fuels. Renewable methane synthesized using such a route stands to be readily deployed using existing infrastructure for the distribution and utilization of natural gas. Here we design a suite of ligand-stabilized metal oxide clusters and find that these modulate carbon dioxide reduction pathways on a copper catalyst, enabling thereby a record activity for methane electroproduction. Density functional theory calculations show adsorbed hydrogen donation from clusters to copper active sites for the *CO hydrogenation pathway towards *CHO. We promote this effect via control over cluster size and composition and demonstrate the effect on metal oxides including cobalt(II), molybdenum(VI), tungsten(VI), nickel(II) and palladium(II) oxides. We report a carbon dioxide-to-methane faradaic efficiency of 60% at a partial current density to methane of 135 milliampere per square centimetre. We showcase operation over 18 h that retains a faradaic efficiency exceeding 55%.
- Authors:
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[1];
[2];
;
[2];
[2];
[2];
[2];
[2];
[2];
[2];
[3];
[3];
[2]
- Univ. of Toronto, ON (Canada); East China University of Science and Technology, Shanghai (China)
- Univ. of Toronto, ON (Canada)
- East China University of Science and Technology, Shanghai (China)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Sponsoring Org.:
- Natural Gas Innovation Fund; USDOE Office of Science (SC); Natural Sciences and Engineering Research Council of Canada (NSERC); Natural Resources Canada; Ontario Research Fund; Canada Foundation for Innovation (CFI); Government of Ontario; China Scholarships Council (CSC)
- OSTI Identifier:
- 1768923
- Alternate Identifier(s):
- OSTI ID: 1771399
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- ENGLISH
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Catalytic mechanisms; Electrocatalysis; Heterogeneous catalysis
Citation Formats
Li, Yuhang, Xu, Aoni, Lum, Yanwei, Wang, Xue, Hung, Sung-Fu, Chen, Bin, Wang, Ziyun, Xu, Yi, Li, Fengwang, Abed, Jehad, Huang, Jianan Erick, Rasouli, Armin Sedighian, Wicks, Joshua, Sagar, Laxmi Kishore, Peng, Tao, Ip, Alexander H., Sinton, David, Jiang, Hao, Li, Chunzhong, and Sargent, Edward H. Promoting CO2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs. United States: N. p., 2020.
Web. doi:10.1038/s41467-020-20004-7.
Li, Yuhang, Xu, Aoni, Lum, Yanwei, Wang, Xue, Hung, Sung-Fu, Chen, Bin, Wang, Ziyun, Xu, Yi, Li, Fengwang, Abed, Jehad, Huang, Jianan Erick, Rasouli, Armin Sedighian, Wicks, Joshua, Sagar, Laxmi Kishore, Peng, Tao, Ip, Alexander H., Sinton, David, Jiang, Hao, Li, Chunzhong, & Sargent, Edward H. Promoting CO2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs. United States. https://doi.org/10.1038/s41467-020-20004-7
Li, Yuhang, Xu, Aoni, Lum, Yanwei, Wang, Xue, Hung, Sung-Fu, Chen, Bin, Wang, Ziyun, Xu, Yi, Li, Fengwang, Abed, Jehad, Huang, Jianan Erick, Rasouli, Armin Sedighian, Wicks, Joshua, Sagar, Laxmi Kishore, Peng, Tao, Ip, Alexander H., Sinton, David, Jiang, Hao, Li, Chunzhong, and Sargent, Edward H. Thu .
"Promoting CO2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs". United States. https://doi.org/10.1038/s41467-020-20004-7. https://www.osti.gov/servlets/purl/1768923.
@article{osti_1768923,
title = {Promoting CO2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs},
author = {Li, Yuhang and Xu, Aoni and Lum, Yanwei and Wang, Xue and Hung, Sung-Fu and Chen, Bin and Wang, Ziyun and Xu, Yi and Li, Fengwang and Abed, Jehad and Huang, Jianan Erick and Rasouli, Armin Sedighian and Wicks, Joshua and Sagar, Laxmi Kishore and Peng, Tao and Ip, Alexander H. and Sinton, David and Jiang, Hao and Li, Chunzhong and Sargent, Edward H.},
abstractNote = {Electroreduction uses renewable energy to upgrade carbon dioxide to value-added chemicals and fuels. Renewable methane synthesized using such a route stands to be readily deployed using existing infrastructure for the distribution and utilization of natural gas. Here we design a suite of ligand-stabilized metal oxide clusters and find that these modulate carbon dioxide reduction pathways on a copper catalyst, enabling thereby a record activity for methane electroproduction. Density functional theory calculations show adsorbed hydrogen donation from clusters to copper active sites for the *CO hydrogenation pathway towards *CHO. We promote this effect via control over cluster size and composition and demonstrate the effect on metal oxides including cobalt(II), molybdenum(VI), tungsten(VI), nickel(II) and palladium(II) oxides. We report a carbon dioxide-to-methane faradaic efficiency of 60% at a partial current density to methane of 135 milliampere per square centimetre. We showcase operation over 18 h that retains a faradaic efficiency exceeding 55%.},
doi = {10.1038/s41467-020-20004-7},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {Thu Dec 03 00:00:00 EST 2020},
month = {Thu Dec 03 00:00:00 EST 2020}
}
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