Photocatalytic Formaldehyde Oxidation over Plasmonic Au/TiO 2 under Visible Light: Moisture Indispensability and Light Enhancement

可见光谱 光催化 光化学 甲醛 催化作用 格式化 材料科学 分解 化学 光电子学 有机化学
作者
Xiaobing Zhu,Can Jin,Xiao‐Song Li,Jinglin Liu,Zhiguang Sun,Chuan Shi,Xingguo Li,Ai‐Min Zhu
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:7 (10): 6514-6524 被引量:153
标识
DOI:10.1021/acscatal.7b01658
摘要

With an extension of the absorption band toward visible light, plasmonic photocatalysts directly harvest energy from solar light without compromising the activity, offering a desirable way to address energy and environmental issues. Here we demonstrate photocatalytic oxidation of formaldehyde in air over plasmonic Au/TiO 2 catalyst under visible light in a single-pass continuous flow reactor. Compared to that under dark, a significant enhancement of up to 5 times the reaction rate at 13% RH under visible light is achieved. Au/TiO 2 catalyst exhibits very high activity, a complete conversion of formaldehyde of 83.3% under visible light at 44% RH, but is completely inactive in dry air even under visible light. Also, the plasmonic Au/TiO 2 is efficient for photocatalytic oxidation of formaldehyde under visible light, which is evidenced by a slight difference of conversion between UV light and visible light. To disclose the underlying mechanism, in situ diffuse reflectance infrared Fourier transform (DRIFT) spectra studies are conducted. The contributions of TiO 2 and Au (supported on TiO 2 ), moisture, and visible light are identified. It is ascertained that moisture is indispensable to carbonate decomposition and also accelerates dioxymethylene (DOM) oxidation to formate. Visible light enhances the rate-determining steps of formate oxidation to carbonate and carbonate decomposition. It appropriately illustrates the remarkable difference in activities. On the basis of the spectra experiments, such a pathway of formaldehyde oxidation is proposed, which undergoes four sequential reaction steps ( k 1, k 2, k 3, k 4 ) with reaction conditions dependent on moisture and visible light over Au/TiO 2 catalyst. On the basis of the approximately identical spectra, which indicate the same reaction pathways under visible light or under dark, the insights into the mechanism for photocatalytic oxidation of formaldehyde in air under visible light over Au/TiO 2, are obtained.
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