Planar defect-driven electrocatalysis of CO2-to-C2H4 conversion
Abstract
The selectivity towards a specific C2+ product, such as ethylene (C2H4), is sensitive to the surface structure of copper (Cu) catalysts in carbon dioxide (CO2) electro-reduction. The fundamental understanding of such sensitivity can guide the development of advanced electrocatalysts, although it remains challenging at the atomic level. In this work, we demonstrated that planar defects, such as stacking faults, could drive the electrocatalysis of CO2-to-C2H4 conversion with higher selectivity and productivity than Cu(100) facets in the intermediate potential region (–0.50 ~ –0.65 V vs. RHE). The unique right bipyramidal Cu nanocrystals containing a combination of (100) facets and a set of parallel planar defects delivered 67% faradaic efficiency (FE) for C2H4 and a partial current density of 217 mA cm–2 at –0.63 V vs. RHE. In contrast, Cu nanocubes with exclusive (100) facets exhibited only 46% FE for C2H4 and a partial current density of 87 mA cm–2 at an identical potential. Both ex situ CO temperature-programmed desorption and in situ Raman spectroscopy analysis implied that the stronger *CO adsorption on planar defect sites facilitates CO generation kinetics, which contributes to a higher surface coverage of *CO and in turn an enhanced reaction rate of C–C coupling towards C2+ products,more »
- Authors:
-
- Univ. of Cincinnati, OH (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Arizona State Univ., Tempe, AZ (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1812505
- Alternate Identifier(s):
- OSTI ID: 1805111
- Report Number(s):
- BNL-221966-2021-JAAM
Journal ID: ISSN 2050-7488
- Grant/Contract Number:
- SC0012704; CBET-2033343; NNCI-ECCS-1542160
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Materials Chemistry. A
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 35; Journal ID: ISSN 2050-7488
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; CO2 electro-reduction; ethylene; planar defects; Cu(100) facet; in situ Raman
Citation Formats
Li, Zhengyuan, Fang, Yanbo, Zhang, Jianfang, Zhang, Tianyu, Jimenez, Juan D., Senanayake, Sanjaya D., Shanov, Vesselin, Yang, Shize, and Wu, Jingjie. Planar defect-driven electrocatalysis of CO2-to-C2H4 conversion. United States: N. p., 2021.
Web. doi:10.1039/d1ta02565a.
Li, Zhengyuan, Fang, Yanbo, Zhang, Jianfang, Zhang, Tianyu, Jimenez, Juan D., Senanayake, Sanjaya D., Shanov, Vesselin, Yang, Shize, & Wu, Jingjie. Planar defect-driven electrocatalysis of CO2-to-C2H4 conversion. United States. https://doi.org/10.1039/d1ta02565a
Li, Zhengyuan, Fang, Yanbo, Zhang, Jianfang, Zhang, Tianyu, Jimenez, Juan D., Senanayake, Sanjaya D., Shanov, Vesselin, Yang, Shize, and Wu, Jingjie. Tue .
"Planar defect-driven electrocatalysis of CO2-to-C2H4 conversion". United States. https://doi.org/10.1039/d1ta02565a. https://www.osti.gov/servlets/purl/1812505.
@article{osti_1812505,
title = {Planar defect-driven electrocatalysis of CO2-to-C2H4 conversion},
author = {Li, Zhengyuan and Fang, Yanbo and Zhang, Jianfang and Zhang, Tianyu and Jimenez, Juan D. and Senanayake, Sanjaya D. and Shanov, Vesselin and Yang, Shize and Wu, Jingjie},
abstractNote = {The selectivity towards a specific C2+ product, such as ethylene (C2H4), is sensitive to the surface structure of copper (Cu) catalysts in carbon dioxide (CO2) electro-reduction. The fundamental understanding of such sensitivity can guide the development of advanced electrocatalysts, although it remains challenging at the atomic level. In this work, we demonstrated that planar defects, such as stacking faults, could drive the electrocatalysis of CO2-to-C2H4 conversion with higher selectivity and productivity than Cu(100) facets in the intermediate potential region (–0.50 ~ –0.65 V vs. RHE). The unique right bipyramidal Cu nanocrystals containing a combination of (100) facets and a set of parallel planar defects delivered 67% faradaic efficiency (FE) for C2H4 and a partial current density of 217 mA cm–2 at –0.63 V vs. RHE. In contrast, Cu nanocubes with exclusive (100) facets exhibited only 46% FE for C2H4 and a partial current density of 87 mA cm–2 at an identical potential. Both ex situ CO temperature-programmed desorption and in situ Raman spectroscopy analysis implied that the stronger *CO adsorption on planar defect sites facilitates CO generation kinetics, which contributes to a higher surface coverage of *CO and in turn an enhanced reaction rate of C–C coupling towards C2+ products, especially C2H4.},
doi = {10.1039/d1ta02565a},
journal = {Journal of Materials Chemistry. A},
number = 35,
volume = 9,
place = {United States},
year = {Tue Jun 15 00:00:00 EDT 2021},
month = {Tue Jun 15 00:00:00 EDT 2021}
}
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