Journal
ACS CATALYSIS
Volume 8, Issue 2, Pages 1009-1017Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.7b03473
Keywords
blue titania; solvothermal synthesis; solar to chemical conversions; CO2 reduction; hydrogen generation; degradation of methyl orange
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Funding
- National Key Research and Development Program of China [2016YFB0901600]
- NSF of China [51502331]
- STC of Shanghai [16JC1401700, 16ZR1440400]
- Key Research Program of Chinese Academy of Sciences [QYZDJ-SSW-JSC013, KGZD-EW-T06]
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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 H-2 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 mu mol 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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