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Title: Modulation of the reduction potential of TiO2-x by fluorination for efficient and selective CH4 generation from CO2 photoreduction
Authors: Xing, MY
Zhou, Y
Dong, CY
Cai, LJ 
Zeng, LX
Shen, B
Pan, LH
Dong, CC
Chai, Y 
Zhang, JL
Yin, YD
Issue Date: 2018
Source: Nano letters, June 2018, v. 18, no. 6, p. 3384-3390
Abstract: 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.
Keywords: Photocatalysis
Mesoporous single crystal
CO2 photoreduction
Publisher: American Chemical Society
Journal: Nano letters 
ISSN: 1530-6984
EISSN: 1530-6992
DOI: 10.1021/acs.nanolett.8b00197
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