物理化学学报 >> 2004, Vol. 20 >> Issue (07): 755-758.doi: 10.3866/PKU.WHXB20040718

研究简报 上一篇    下一篇

无氧条件下Pt/TiO2光催化重整降解一乙醇胺水溶液制氢

吴玉琪;吕功煊;李树本   

  1. 中国科学院兰州化学物理研究所,羰基合成与选择氧化国家重点实验室,兰州　730000
  • 收稿日期:2003-12-16 修回日期:2004-02-16 发布日期:2004-07-15
  • 通讯作者: 吕功煊 E-mail:gxlu@ns.lzb.ac.cn

Hydrogen Production by Pt/TiO2 Anaerobic Photocatalytic Reforming Degradation of Aqueous Monoethanolamine

Wu Yu-Qi;Lü Gong-Xuan;Li Shu-Ben   

  1. State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou　730000
  • Received:2003-12-16 Revised:2004-02-16 Published:2004-07-15
  • Contact: Lü Gong-Xuan E-mail:gxlu@ns.lzb.ac.cn

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摘要： 以一乙醇胺（以下简称乙醇胺）为电子给体,在无氧条件下进行了Pt/TiO2光催化重整制氢的研究.详细讨论了诸多因素如催化剂表面Pt化学状态、Pt担载量、溶液pH值、乙醇胺溶液浓度等对产氢效率的影响,并用XRD、HNMR、XPS等进行了深入表征,探讨了Pt/TiO2光催化重整降解乙醇胺和产氢的反应, 实验表明,利用所制备的光催化剂, 可实现在消除水中有机污染物的同时制取氢气的目标.催化剂表面的Pt以Pt0的化学状态存在, 有利于析氢；溶液pH值和浓度的变化对产生速率也有一定的影响.同时发现Pt/TiO2光催化重整乙醇胺制氢反应的最佳条件是:Pt的最佳担载量约为0.5％～1.0％；乙醇胺溶液最佳浓度约为0.05 mol•L－1；最佳溶液pH值范围为4～10；氨基取代的羰基类化合物是其主要中间产物.

关键词: 光催化重整, 降解, 乙醇胺, Pt/TiO2, 制氢

Abstract: The production of hydrogen by anaerobic photocatalytic reforming degradation of aqueous monoethanolamine (ethanolamine, shortened form in the following text)solution has been investigated using a Pt/TiO2 catalyst. The effect of many factors such as ethanolamine concentration, catalyst surface chemical state, and pH of systems on the photocatalytic production of hydrogen have been studied in detail. The catalyst and the products were characterized using HNMR, XRD and XPS techniques; the possible reaction mechanism was discussed. The hydrogen production was achieved simultaneously with the photocatalytic reforming degradation of aqueous ethanolamine solution. It was showed that the aim of both producing hydrogen and photocatalytic reforming degradation of aqueous organic pollutant could be achieved using a Pt/TiO2 catalyst. The Pt particles were identified as existed in Pt0 state on the TiO2. The pH and the ethanolamine concentration affect the hydrogen production rate significantly. At the same time, it was found that the optimum concentration of ethanolamine, pH value and Pt loading is 0.05 mol•L－1, 4～10 and 0.5％～1.0％ respectively. And the amino substituted carbonyl compounds was the main intermediates.

Key words: Photocatalytic reforming, Degradation, Monoethanolamine, Pt/TiO2, H2 production