期刊
ACS CATALYSIS
卷 8, 期 8, 页码 7113-7119出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b01014
关键词
CO2; reduction; electrocatalyst; CeO2; copper; oxygen vacancy
资金
- National Key Research and Development Program of China [2017YFA0206901, 2018YFA0209401]
- Natural Science Foundation of China [21688102, 21473038, 21773036]
- the Key Basic Research Program of Science and Technology Commission of Shanghai Municipality [17JC1400100]
- Collaborative Innovation Center of Chemistry for Energy Materials
- Hui-Chun Chin and Tsung-Dao Lee Chinese Undergraduate Research Endowment
- XAFCA beamline of Singapore Synchrotron Light source
The electrocatalytic reduction of CO2 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 CeO2 to optimize the CO2 electrocatalytic reduction to CH4. We carried out theoretical calculations to predict that the single-atomic Cu substitution in CeO2(110) surface can stably enrich up to three oxygen vacancies around each Cu site, yielding a highly effective catalytic center for CO2 adsorption and activation. This theoretical prediction is consistent with our controlled synthesis of the Cu-doped, mesoporous CeO2 nanorods. Structural characterizations indicate that the low concentration (<5%) Cu species in CeO2 nanorods are highly dispersed at single-atomic level with an unconventionally low coordination number similar to 5, suggesting the direct association of 3 oxygen vacancies with each Cu ion on surfaces. This multiple oxygen vacancy-bound, single atomic Cu-substituted CeO2 enables an excellent electrocatalytic selectivity in reducing CO2 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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