Advantageous Role of Ir0 Supported on TiO2 Nanosheets in Photocatalytic CO2 Reduction to CH4: Fast Electron Transfer and Rich Surface Hydroxyl Groups

Ir-based heterogeneous catalysts for photocatalytic CO2 reduction have rarely been reported and are worthy of investigation. In this work, TiO2 nanosheets with a higher specific surface area and more oxygen vacancies were employed to support Ir metal by impregnation (Imp) and ethylene glycol (EG) re...

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Published inACS applied materials & interfaces Vol. 13; no. 5; pp. 6219 - 6228
Main Authors Tang, Kunlin, Wang, Zhiqiang, Zou, Weixin, Guo, Hongyu, Wu, Yuchao, Pu, Yu, Tong, Qing, Wan, Haiqin, Gu, Xianrui, Dong, Lin, Rong, Junfeng, Chen, Yu-Wen
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LanguageEnglish
Published American Chemical Society 10.02.2021
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Abstract Ir-based heterogeneous catalysts for photocatalytic CO2 reduction have rarely been reported and are worthy of investigation. In this work, TiO2 nanosheets with a higher specific surface area and more oxygen vacancies were employed to support Ir metal by impregnation (Imp) and ethylene glycol (EG) reduction methods. In comparison with Ir/TiO2 (Imp) and TiO2, Ir/TiO2 (EG) exhibited excellent photocatalytic performance toward CO2 reduction, especially for CH4 production on account of the oxygen defect of TiO2 and rich surface hydroxyl groups produced from the interaction between TiO2 nanosheets and metallic Ir. In situ ESR suggested that the oxygen defect was significant for CO2 adsorption/activation. Furthermore, metallic Ir was beneficial for photogenerated electron transfer, surface hydroxyl generation, and adsorption of the CO intermediate, generating more available electrons and reducing agents for CH4 production. In situ CO2 DRIFTS confirmed the key synergistic interaction between the oxygen defect and metallic Ir in the photoreduction from CO2 to CH4.
AbstractList Ir-based heterogeneous catalysts for photocatalytic CO2 reduction have rarely been reported and are worthy of investigation. In this work, TiO2 nanosheets with a higher specific surface area and more oxygen vacancies were employed to support Ir metal by impregnation (Imp) and ethylene glycol (EG) reduction methods. In comparison with Ir/TiO2 (Imp) and TiO2, Ir/TiO2 (EG) exhibited excellent photocatalytic performance toward CO2 reduction, especially for CH4 production on account of the oxygen defect of TiO2 and rich surface hydroxyl groups produced from the interaction between TiO2 nanosheets and metallic Ir. In situ ESR suggested that the oxygen defect was significant for CO2 adsorption/activation. Furthermore, metallic Ir was beneficial for photogenerated electron transfer, surface hydroxyl generation, and adsorption of the CO intermediate, generating more available electrons and reducing agents for CH4 production. In situ CO2 DRIFTS confirmed the key synergistic interaction between the oxygen defect and metallic Ir in the photoreduction from CO2 to CH4.
Ir-based heterogeneous catalysts for photocatalytic CO2 reduction have rarely been reported and are worthy of investigation. In this work, TiO2 nanosheets with a higher specific surface area and more oxygen vacancies were employed to support Ir metal by impregnation (Imp) and ethylene glycol (EG) reduction methods. In comparison with Ir/TiO2 (Imp) and TiO2, Ir/TiO2 (EG) exhibited excellent photocatalytic performance toward CO2 reduction, especially for CH4 production on account of the oxygen defect of TiO2 and rich surface hydroxyl groups produced from the interaction between TiO2 nanosheets and metallic Ir. In situ ESR suggested that the oxygen defect was significant for CO2 adsorption/activation. Furthermore, metallic Ir was beneficial for photogenerated electron transfer, surface hydroxyl generation, and adsorption of the CO intermediate, generating more available electrons and reducing agents for CH4 production. In situ CO2 DRIFTS confirmed the key synergistic interaction between the oxygen defect and metallic Ir in the photoreduction from CO2 to CH4.Ir-based heterogeneous catalysts for photocatalytic CO2 reduction have rarely been reported and are worthy of investigation. In this work, TiO2 nanosheets with a higher specific surface area and more oxygen vacancies were employed to support Ir metal by impregnation (Imp) and ethylene glycol (EG) reduction methods. In comparison with Ir/TiO2 (Imp) and TiO2, Ir/TiO2 (EG) exhibited excellent photocatalytic performance toward CO2 reduction, especially for CH4 production on account of the oxygen defect of TiO2 and rich surface hydroxyl groups produced from the interaction between TiO2 nanosheets and metallic Ir. In situ ESR suggested that the oxygen defect was significant for CO2 adsorption/activation. Furthermore, metallic Ir was beneficial for photogenerated electron transfer, surface hydroxyl generation, and adsorption of the CO intermediate, generating more available electrons and reducing agents for CH4 production. In situ CO2 DRIFTS confirmed the key synergistic interaction between the oxygen defect and metallic Ir in the photoreduction from CO2 to CH4.
Ir-based heterogeneous catalysts for photocatalytic CO₂ reduction have rarely been reported and are worthy of investigation. In this work, TiO₂ nanosheets with a higher specific surface area and more oxygen vacancies were employed to support Ir metal by impregnation (Imp) and ethylene glycol (EG) reduction methods. In comparison with Ir/TiO₂ (Imp) and TiO₂, Ir/TiO₂ (EG) exhibited excellent photocatalytic performance toward CO₂ reduction, especially for CH₄ production on account of the oxygen defect of TiO₂ and rich surface hydroxyl groups produced from the interaction between TiO₂ nanosheets and metallic Ir. In situ ESR suggested that the oxygen defect was significant for CO₂ adsorption/activation. Furthermore, metallic Ir was beneficial for photogenerated electron transfer, surface hydroxyl generation, and adsorption of the CO intermediate, generating more available electrons and reducing agents for CH₄ production. In situ CO₂ DRIFTS confirmed the key synergistic interaction between the oxygen defect and metallic Ir in the photoreduction from CO₂ to CH₄.
Author Zou, Weixin
Tang, Kunlin
Guo, Hongyu
Wu, Yuchao
Gu, Xianrui
Dong, Lin
Chen, Yu-Wen
Wan, Haiqin
Rong, Junfeng
Wang, Zhiqiang
Pu, Yu
Tong, Qing
AuthorAffiliation Department of Chemistry
Department of Chemical Engineering
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, School of Chemistry and Chemical Engineering, Center of Modern Analysis, Jiangsu Key Laboratory of Vehicle Emissions Control
The University of Texas at Austin
Research Institute of Petroleum Processing, Sinopec
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surface hydroxyl
synergistic mechanism
CO2 photoreduction
oxygen defect
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Snippet Ir-based heterogeneous catalysts for photocatalytic CO2 reduction have rarely been reported and are worthy of investigation. In this work, TiO2 nanosheets with...
Ir-based heterogeneous catalysts for photocatalytic CO₂ reduction have rarely been reported and are worthy of investigation. In this work, TiO₂ nanosheets with...
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SubjectTerms adsorption
carbon dioxide
electron transfer
Energy, Environmental, and Catalysis Applications
ethylene glycol
nanosheets
oxygen
photocatalysis
photoreduction
surface area
synergism
Title Advantageous Role of Ir0 Supported on TiO2 Nanosheets in Photocatalytic CO2 Reduction to CH4: Fast Electron Transfer and Rich Surface Hydroxyl Groups
URI http://dx.doi.org/10.1021/acsami.0c19233
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