4.6 Article

Promoting CO2 and H2O activation on O-vacancy regulated In-Ti dual- sites for enhanced CH4 photo-production

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JOURNAL OF ENERGY CHEMISTRY
卷 86, 期 -, 页码 599-608

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ELSEVIER
DOI: 10.1016/j.jechem.2023.07.020

关键词

In single atoms; Oxygen vacancies; CO 2 photoreduction; Water dissociation; Synergetic effect

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This study demonstrates the successful conversion of CO2 to methane using the delicately designed In/TiO2-VO photocatalyst. The relationship between the structure and performance of the photocatalyst is clarified through experimental and theoretical analyses. This work provides a new strategy for the development of effective photocatalysts.
Engineering the specific active sites of photocatalysts for simultaneously promoting CO2 and H2O activa-tion is important to achieve the efficient conversion of CO2 to hydrocarbon with H2O as a proton source under sunlight. Herein, we delicately design the In/TiO2-VO photocatalyst by engineering In single atoms (SAs) and oxygen vacancies (VOs) on porous TiO2. The relation between structure and performance of the photocatalyst is clarified by both experimental and theoretical analyses at the atomic levels. The In/TiO2- VO photocatalyst furnish a high CH4 production rate up to 35.49 lmol g-1 h-1 with a high selectivity of 91.3% under simulated sunlight, while only CO is sluggishly generated on TiO2-VO. The combination of in situ spectroscopic analyses with theoretical calculations reveal that the VO sites accelerate H2O disso-ciation and increase proton feeding for CO2 reduction. Furthermore, the VO regulated In-Ti dual sites enable the formation of a stable adsorption conformation of In-C-O-Ti intermediate, which is responsible for the highly selective reduction of CO2 to CH4. This work demonstrates a new strategy for the develop-ment of effective photocatalysts by coupling metal SA sites with the adjacent metal sites of support to synergistically enhance the activity and selectivity of CO2 photoreduction.(c) 2023 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.

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