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Cited by 382

The DOI matches its Crossref record; 59 of the 59 references it cites were found in a registry or an index.

Lattice-Hydride Mechanism in Electrocatalytic CO2 Reduction by Structurally Precise Copper-Hydride Nanoclusters

Tang, Qing, Lee, Yongjin, Li, Dai-Ying, Choi, Woojun, Liu, C. W., Lee, Dongil, Jiang, De-en·2017·Journal of the American Chemical Society
DOI 10.1021/jacs.7b05591
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Abstract

Copper electrocatalysts can reduce CO 2 to hydrocarbons at high overpotentials. However, a mechanistic understanding of CO 2 reduction on nanostructured Cu catalysts has been lacking. Herein we show that the structurally precise ligand-protected Cu-hydride nanoclusters, such as Cu 32 H 20 L 12 (L is a dithiophosphate ligand), offer unique selectivity for electrocatalytic CO 2 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 CO 2 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 CO 2 reduction on the Cu 32 H 20 L 12 cluster demonstrate that HCOOH is indeed the main product at low overpotential, while H 2 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 CO 2 reduction by copper-hydride nanoclusters and other metal nanoclusters that contain hydrides.

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Metadata

Authors
Tang, Q., Lee, Y., Li, D.-Y., Choi, W., Liu, C. W., Lee, D., & Jiang, D.-E.
Venue
Journal of the American Chemical Society
Publisher
American Chemical Society (ACS)
Published
2017-07-06
Volume
139
Issue
28
Pages
9728-9736
ISSN
  • 0002-7863 (ISSN-L)
  • 1520-5126
DOI
10.1021/jacs.7b05591
OpenAlex
W2670129164
Cited by
382
References
59
FWCI
7.12
Type
journal article
Language
en
Open access
closed

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