Photocatalytic reforming of C3-polyols for H2 production Part II. FTIR study on the adsorption and photocatalytic reforming reaction of 2-propanol on Pt/TiO2

被引:47
作者
Gu, Quan [1 ]
Fu, Xianliang [2 ,3 ]
Wang, Xuxu [1 ]
Chen, Shifu [3 ]
Leung, Dennis Y. C. [2 ]
Xie, Xiuqiang [1 ]
机构
[1] Fuzhou Univ, Res Inst Photocatalysis, Fuzhou 350002, Peoples R China
[2] Univ Hong Kong, Dept Mech Engn, Hong Kong, Hong Kong, Peoples R China
[3] Huaibei Normal Univ, Dept Chem, Huaibei 235000, Anhui, Peoples R China
关键词
Photocatalytic reforming; Adsorption; FTIR study; 2-propanol; Pt/TiO2; NANOCRYSTALLINE TIO2 FILMS; VOLATILE ORGANIC-COMPOUNDS; METAL-OXIDE CATALYSTS; PHOTO-KOLBE REACTION; IN-SITU FTIR; DECARBOXYLATIVE ROUTE; HYDROGEN-PRODUCTION; ACETIC-ACID; OXIDATION; METHANOL;
D O I
10.1016/j.apcatb.2011.05.046
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The adsorption behavior and the photocatalytic reforming (PR) process of 2-propanol over Pt (1 wt.%)/TiO2 (PT) photocatalyst have been investigated by Fourier transform infrared (FTIR) spectroscopy. Both the adsorption complexes and the reforming intermediates formed on the PT and the gas-phase were determined and identified by FTIR spectra. The results indicated that the first layer surface of the PT mainly consisted of chemisorbed 2-propanol (Ti-OCH(CH3)(2)) through the condensation of 2-propanol with surface Ti-OH or dissociative adsorption with undercoordinated Ti atoms, while the second layer consisted of physisorbed 2-propanol by interaction with the chemisorbed one or the formed H2O via hydrogen-bond. Under UV irradiation, a rapidly deprotonation of 2-propoxide occurred by the attack of holes (h(+)) and resulted in the formation of acetone, which was then slowly oxidized to acetate and formate species by the hydroxyl radicals ((OH)-O-center dot). The carboxylates finally decarboxylate over the PT to evolve CO2 and CH4 via the photo-Kolbe reaction. According to the results, a reforming mechanism was proposed. The role of the OH groups contained in 2-propanol and its intermediates were found to serve as anchors for their adsorption and to involve the formation of hi transport ways. (C) 2011 Elsevier B.V. All rights reserved.
引用
收藏
页码:689 / 696
页数:8
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