文献类型：期刊文献

英文题名：Modulation of the Reduction Potential of TiO2-x by Fluorination for Efficient and Selective CH4 Generation from CO2 Photoreduction

作者：Xing, Mingyang[1,2,3];Zhou, Yi[1,2];Dong, Chunyang[1,2];Cai, Lejuan[4];Zeng, Lixi[5,6];Shen, Bin[1,2];Pan, Lihan[1,2];Dong, Chencheng[1,2];Chai, Yang[4];Zhang, Jinlong[1,2];Yin, Yadong[3]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Inst Fine Chem, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]Univ Calif Riverside, Dept Chem, Riverside, CA 92521 USA;[4]Hong Kong Polytech Univ, Dept Appl Phys, Kowloon, Hong Kong, Peoples R China;[5]Jinan Univ, Sch Environm, Guangzhou Key Lab Environm Exposure & Hlth, Guangzhou 510632, Guangdong, Peoples R China;[6]Jinan Univ, Guangdong Key Lab Environm Pollut & Hlth, Guangzhou 510632, Guangdong, Peoples R China

年份：2018

卷号：18

期号：6

起止页码：3384

外文期刊名：NANO LETTERS

收录：;EI(收录号：20181905173787);WOS:【SCI-EXPANDED(收录号:WOS:000435524300010)】；

基金：This work was supported by the National Natural Science Foundation of China (21773062, 21577036, 21377038, 21677048, 5171101651, 41522304), State Key Research Development Program of China (2016YFA0204200), the Shanghai Education Development Foundation and Shanghai Municipal Education Commission (16JC1401400), Shanghai Pujiang Program (17PJD011), and the Fundamental Research Funds for the Central Universities (22A201514021). Acknowledgment is also made to the Donors of the American Chemical Society Petroleum Research Fund for partial support of this research (55904-ND10).

语种：英文

外文关键词：Photocatalysis; semiconductors; mesoporous single crystal; fluorination; CO2 photoreduction

摘要：Photocatalytic reduction of CO2 holds great promises for addressing both the environmental and energy issues that are facing the modern society. The major challenge of CO2 photoreduction into fuels such as methane or methanol is the low yield and poor selectivity. Here, we report an effective strategy to enhance the reduction potential of photoexcited electrons by fluorination of mesoporous single crystals of reduced TiO2-x. Density functional theory calculations and photoelectricity tests indicate that the Ti3+ impurity level is upswept by fluorination, owing to the built-in electric field constructed by the substitutional F that replaces surface oxygen vacancies, which leads to the enhanced reduction potential of photoexcited electrons. As a result, the fluorination of the reduced TiO2-x dramatically increases the CH4 production yield by 13 times from 0.125 to 1.63 mu mol/g.h under solar light illumination with the CH4 selectivity being improved from 25.7% to 85.8%. Our finding provides a metal-free strategy for the selective CH4 generation from CO2 photoreduction.