文献类型：期刊文献

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

作者：Yin, Guoheng[1,2];Huang, Xieyi[1];Chen, Tianyuan[3];Zhao, Wei[1];Bi, Qingyuan[1];Xu, Jing[3];Han, Yifan[3];Huang, Fuqiang[1,4,5]

机构：[1]Chinese Acad Sci, Shanghai Inst Ceram, State Key Lab High Performance Ceram & Superfine, Shanghai 200050, Peoples R China;[2]Univ Chinese Acad Sci, Beijing 100049, Peoples R China;[3]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[4]Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China;[5]Peking Univ, Coll Chem & Mol Engn, State Key Lab Rare Earth Mat Chem & Applicat, Beijing 100871, Peoples R China

年份：2018

卷号：8

期号：2

起止页码：1009

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20180604775555);WOS:【SCI-EXPANDED(收录号:WOS:000424735000034)】；

基金：This work was financially supported by the National Key Research and Development Program of China (Grant no. 2016YFB0901600), the NSF of China (Grant no. 51502331), the STC of Shanghai (Grants no. 16JC1401700 and 16ZR1440400), and the Key Research Program of Chinese Academy of Sciences (Grants no. QYZDJ-SSW-JSC013 and KGZD-EW-T06).

语种：英文

外文关键词：blue titania; solvothermal synthesis; solar to chemical conversions; CO2 reduction; hydrogen generation; degradation of methyl orange

摘要：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.