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Hydrogenated Blue Titania for Efficient Solar to Chemical Conversions: Preparation, Characterization, and Reaction Mechanism of CO2 Reduction

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† State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, People’s Republic of China
‡ University of Chinese Academy of Sciences, Beijing 100049, People’s Republic of China
§ State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
∥ Beijing National Laboratory for Molecular Sciences and State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, People’s Republic of China
*E-mail for Q.B.: [email protected]
*E-mail for Y.H.: [email protected]
*E-mail for F.H.: [email protected]
Cite this: ACS Catal. 2018, 8, 2, 1009–1017
Publication Date (Web):December 21, 2017
https://doi.org/10.1021/acscatal.7b03473
Copyright © 2017 American Chemical Society
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Here we report a facile low-temperature solvothermal method by using Li-dissolved ethanediamine to prepare uniform hydrogenated blue H-TiO2–x with wide spectrum response. H-TiO2–x possesses a distinct crystalline core–amorphous shell structure (TiO2@TiO2–x) with numerous oxygen vacancies and doped H in the amorphous shell. Efficient solar to chemical energy conversions, likely photocatalytic reduction of CO2, degradation of contaminants, and H2 generation from water splitting can be achieved over this blue titania. Notably, the optimized H-TiO2–x(200) shows high activity of CH4 formation at a rate of 16.2 μmol g–1 h–1 and a selectivity of 79% under full solar irradiation. The kinetic isotope effects measurements reveal that the cleavage of the C═O bond from CO2 rather than the O–H bond from H2O is the rate-determining step in CH4 formation. Meanwhile, in situ diffuse reflectance infrared Fourier transform spectroscopy shows the existence of the key intermediate CO2– species. The formation of intermediate CO2– indicates that the defective surface of H-TiO2–x can efficiently accelerate the adsorption and chemical activation of the extremely stable CO2 molecule, which makes the single-electron reduction of CO2 to CO2– easier.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acscatal.7b03473.

  • Full spectroscopic data and TEM images for all samples, photographs, comparison of photocatalytic activities of CO2 reduction over TiO2-based catalysts, O2 formation of CO2 photoreduction over H-TiO2–x, cycling tests, and isotope tracer analyses (PDF)

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Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

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