Journal of the American Chemical Society, volume 139, issue 28, pages 9728-9736
Lattice-Hydride Mechanism in Electrocatalytic CO2 Reduction by Structurally Precise Copper-Hydride Nanoclusters
1
Department
of Chemistry, University of California, Riverside, California 92521, United States
|
2
Department
of Chemistry, Yonsei University, Seoul 03722, South Korea
|
Publication type: Journal Article
Publication date: 2017-07-06
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor: 15
ISSN: 00027863, 15205126
General Chemistry
Catalysis
Biochemistry
Colloid and Surface Chemistry
Abstract
Copper electrocatalysts can reduce CO2 to hydrocarbons at high overpotentials. However, a mechanistic understanding of CO2 reduction on nanostructured Cu catalysts has been lacking. Herein we show that the structurally precise ligand-protected Cu-hydride nanoclusters, such as Cu32H20L12 (L is a dithiophosphate ligand), offer unique selectivity for electrocatalytic CO2 reduction at low overpotentials. Our density functional theory (DFT) calculations predict that the presence of the negatively charged hydrides in the copper cluster plays a critical role in determining the selectivity of the reduction product, yielding HCOOH over CO with a lower overpotential. The HCOOH formation proceeds via the lattice-hydride mechanism: first, surface hydrides reduce CO2 to HCOOH product, and then the hydride vacancies are readily regenerated by the electrochemical proton reduction. DFT calculations further predict that hydrogen evolution is less competitive than HCOOH formation at the low overpotential. Confirming the predictions, electrochemical tests of CO2 reduction on the Cu32H20L12 cluster demonstrate that HCOOH is indeed the main product at low overpotential, while H2 production dominates at higher overpotential. The unique selectivity afforded by the lattice-hydride mechanism opens the door for further fundamental and applied studies of electrocatalytic CO2 reduction by copper-hydride nanoclusters and other metal nanoclusters that contain hydrides.
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Tang Q. et al. Lattice-Hydride Mechanism in Electrocatalytic CO2 Reduction by Structurally Precise Copper-Hydride Nanoclusters // Journal of the American Chemical Society. 2017. Vol. 139. No. 28. pp. 9728-9736.
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Tang Q., Lee C., Li D., Choi W., Liu C. W., Lee D., Jiang D. Lattice-Hydride Mechanism in Electrocatalytic CO2 Reduction by Structurally Precise Copper-Hydride Nanoclusters // Journal of the American Chemical Society. 2017. Vol. 139. No. 28. pp. 9728-9736.
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TY - JOUR
DO - 10.1021/jacs.7b05591
UR - https://doi.org/10.1021%2Fjacs.7b05591
TI - Lattice-Hydride Mechanism in Electrocatalytic CO2 Reduction by Structurally Precise Copper-Hydride Nanoclusters
T2 - Journal of the American Chemical Society
AU - Li, Dai-Ying
AU - Liu, C. W.
AU - Jiang, Deen
AU - Tang, Qing
AU - Lee, Chongmok
AU - Choi, Woojun
AU - Lee, Dongil
PY - 2017
DA - 2017/07/06 00:00:00
PB - American Chemical Society (ACS)
SP - 9728-9736
IS - 28
VL - 139
SN - 0002-7863
SN - 1520-5126
ER -
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@article{2017_Tang,
author = {Dai-Ying Li and C. W. Liu and Deen Jiang and Qing Tang and Chongmok Lee and Woojun Choi and Dongil Lee},
title = {Lattice-Hydride Mechanism in Electrocatalytic CO2 Reduction by Structurally Precise Copper-Hydride Nanoclusters},
journal = {Journal of the American Chemical Society},
year = {2017},
volume = {139},
publisher = {American Chemical Society (ACS)},
month = {jul},
url = {https://doi.org/10.1021%2Fjacs.7b05591},
number = {28},
pages = {9728--9736},
doi = {10.1021/jacs.7b05591}
}
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Tang, Qing, et al. “Lattice-Hydride Mechanism in Electrocatalytic CO2 Reduction by Structurally Precise Copper-Hydride Nanoclusters.” Journal of the American Chemical Society, vol. 139, no. 28, Jul. 2017, pp. 9728-9736. https://doi.org/10.1021%2Fjacs.7b05591.
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