Hydrogen production by photocatalytic steam reforming of methanol on noble metal-modified TiO2

Hydrogen production by photocatalytic steam reforming of methanol on noble metal-modified TiO2
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DOI:
10.1016/j.jcat.2010.05.012
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发表时间:
2010-07-28
影响因子:
7.3
通讯作者:
Selli, Elena
Selli, Elena
中科院分区:
化学1区
文献类型:
--
作者:
Chiarello, Gian Luca;Aguirre, Myriam H.;Selli, Elena

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通过火焰喷雾热解或在TiO2上沉积预制的贵金属纳米粒子,研究了一系列原始或贵金属(Ag、Au、Au-Ag合金和Pt)修饰的TiO2光催化剂在甲醇蒸汽重整中光催化制氢的效果。采用闭式再循环装置,在光催化床上连续进料甲醇/水蒸气。甲醇通过甲醛和甲酸的形成被氧化为二氧化碳。副产物为一氧化碳、甲烷、甲酸甲酯、乙醛和二甲醚。氢以恒定速率析出,随着贵金属的加入,氢的析出速率显著增加,根据其功函数值,铂是最有效的助催化剂,其次是金和银。对入口气体组成的影响进行了系统的调查,提供了有关主要反应路径和工艺优化条件以及CH3OH氧化产物分布的有价值的信息。(C) 2010爱思唯尔公司版权所有。
The photocatalytic production of hydrogen by methanol steam reforming was studied over a series of pristine or noble metal (Ag, Au, Au-Ag alloy and Pt) - modified TiO2 photocatalysts, synthesised by flame spray pyrolysis or by the deposition of preformed noble metal nanoparticles on TiO2. A closed recirculation apparatus was employed, with the photocatalyst bed continuously fed with methanol/water vapours. Methanol underwent oxidation up to CO2 through the formation of formaldehyde and formic acid. Carbon monoxide, methane, methyl formate, acetaldehyde and dimethyl ether were identified as side products. Hydrogen evolved at constant rate, which significantly increased upon noble metal addition, Pt being the most effective co-catalyst, followed by gold and silver, according to their work function values. A systematic investigation into the effects of the inlet gas composition gave valuable information on the prevailing reaction paths and on the conditions of process optimisation, also in terms of distribution of CH3OH oxidation products. (C) 2010 Elsevier Inc. All rights reserved.