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Cited by 532

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Switching the Oxygen Evolution Mechanism on Atomically Dispersed Ru for Enhanced Acidic Reaction Kinetics

Hao, Yixin, Hung, Sung-Fu, Zeng, Wen-Jing, Wang, Ye, Zhang, Chenchen, Kuo, Chun-Han, Wang, Luqi, Zhao, Sheng, Zhang, Ying, Chen, Han-Yi, Peng, Shengjie·2023·Journal of the American Chemical Society

Abstract

Designing stable single-atom electrocatalysts with lower energy barriers is urgent for the acidic oxygen evolution reaction. In particular, the atomic catalysts are highly dependent on the kinetically sluggish acid–base mechanism, limiting the reaction paths of intermediates. Herein, we successfully manipulate the steric localization of Ru single atoms at the Co 3 O 4 surface to improve acidic oxygen evolution by precise control of the anchor sites. The delicate structure design can switch the reaction mechanism from the lattice oxygen mechanism (LOM) to the optimized adsorbate evolution mechanism (AEM). In particular, Ru atoms embedded into cation vacancies reveal an optimized mechanism that activates the proton donor–acceptor function (PDAM), demonstrating a new single-atom catalytic pathway to circumvent the classic scaling relationship. Steric interactions with intermediates at the anchored Ru–O–Co interface played a primary role in optimizing the intermediates’ conformation and reducing the energy barrier. As a comparison, Ru atoms confined to the surface sites exhibit a lattice oxygen mechanism for the oxygen evolution process. As a result, the delicate atom control of the spatial position presents a 100-fold increase in mass activity from 36.96 A g Ru(ads) –1 to 4012.11 A g Ru(anc) –1 at 1.50 V. These findings offer new insights into the precise control of single-atom catalytic behavior.

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Metadata

Authors
Hao, Y., Hung, S.-F., Zeng, W.-J., Wang, Y., Zhang, C., Kuo, C.-H., Wang, L., Zhao, S., Zhang, Y., Chen, H.-Y., & Peng, S.
Venue
Journal of the American Chemical Society
Published
2023-10-23
Volume
145
Issue
43
Pages
23659-23669
ISSN
  • 0002-7863 (ISSN-L)
  • 1520-5126
OpenAlex
W4387871884
Cited by
532
References
1
FWCI
24.90
Type
journal article
Language
en
Open access
closed

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CoChat. (2026). Citation check: Switching the Oxygen Evolution Mechanism on Atomically Dispersed Ru for Enhanced Acidic Reaction Kinetics. https://app.cochat.ai/papers/10.1021/jacs.3c07777
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Hao, Y., Hung, S.-F., Zeng, W.-J., Wang, Y., Zhang, C., Kuo, C.-H., Wang, L., Zhao, S., Zhang, Y., Chen, H.-Y., & Peng, S. (2023). Switching the Oxygen Evolution Mechanism on Atomically Dispersed Ru for Enhanced Acidic Reaction Kinetics. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.3c07777

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