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Single-Atomic Cu with Multiple Oxygen Vacancies on Ceria for Electrocatalytic CO2 Reduction to CH4

Wang, Yifei, Chen, Zheng, Han, Peng, Du, Yonghua, Gu, Zhengxiang, Xu, Xin, Zheng, Gengfeng·2018·ACS Catalysis

Abstract

The electrocatalytic reduction of CO 2 into value-added chemicals such as hydrocarbons has the potential for supplying fuel energy and reducing environmental hazards, while the accurate tuning of electrocatalysts at the ultimate single-atomic level remains extremely challenging. In this work, we demonstrate an atomic design of multiple oxygen vacancy-bound, single-atomic Cu-substituted CeO 2 to optimize the CO 2 electrocatalytic reduction to CH 4 . We carried out theoretical calculations to predict that the single-atomic Cu substitution in CeO 2 (110) surface can stably enrich up to three oxygen vacancies around each Cu site, yielding a highly effective catalytic center for CO 2 adsorption and activation. This theoretical prediction is consistent with our controlled synthesis of the Cu-doped, mesoporous CeO 2 nanorods. Structural characterizations indicate that the low concentration (<5%) Cu species in CeO 2 nanorods are highly dispersed at single-atomic level with an unconventionally low coordination number ∼5, suggesting the direct association of 3 oxygen vacancies with each Cu ion on surfaces. This multiple oxygen vacancy-bound, single atomic Cu-substituted CeO 2 enables an excellent electrocatalytic selectivity in reducing CO 2 to methane with a faradaic efficiency as high as 58%, suggesting strong capabilities of rational design of electrocatalyst active centers for boosting activity and selectivity.

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Metadata

Authors
Wang, Y., Chen, Z., Han, P., Du, Y., Gu, Z., Xu, X., & Zheng, G.
Venue
ACS Catalysis
Published
2018-06-22
Volume
8
Issue
8
Pages
7113-7119
ISSN
2155-5435 (ISSN-L)
OpenAlex
W2809213534
Cited by
682
References
8
FWCI
14.70
Type
journal article
Language
en
Open access
closed

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