Planar defect-driven electrocatalysis of CO2-to-C2H4 conversion

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 rem...

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Bibliographic Details
Published in:Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2021-09, Vol.9 (35), p.19932-19939
Main Authors: Li, Zhengyuan, Fang, Yanbo, Zhang, Jianfang, Zhang, Tianyu, Jimenez, Juan D, Senanayake, Sanjaya D, Shanov, Vesselin, Yang, Shize, Wu, Jingjie
Format: Article
Language:English
Subjects:
Carbon dioxide
Carbon monoxide
Catalysis
Catalysts
CO2 electro-reduction
Conversion
Copper
Cu facet
Current density
Defects
Electrocatalysis
Electrocatalysts
ethylene
in situ Raman
MATERIALS SCIENCE
Nanocrystals
planar defects
Raman spectroscopy
Selectivity
Stacking faults
Surface structure
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Summary: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. Here 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.
ISSN:2050-7488
2050-7496
DOI:10.1039/d1ta02565a