物理化学学报 >> 2013, Vol. 29 >> Issue (08): 1778-1784.doi: 10.3866/PKU.WHXB201305302

催化和表面科学 上一篇    下一篇

基于曙红Y氧化性猝灭的高活性和高稳定的可见光催化产氢催化剂

李波1,2, 吕功煊1   

  1. 1 中国科学院大学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;
    2 中国科学院大学, 北京 100049
  • 收稿日期:2013-04-16 修回日期:2013-05-29 发布日期:2013-07-09
  • 通讯作者: 吕功煊 E-mail:gxlu@lzb.ac.cn
  • 基金资助:

    国家自然科学基金(21173242); 国家重点基础研究发展规划项目(973) (2009CB22003)和国家高技术研究发展计划项目(863) (2012AA051501)资助

Highly Active and Stable Catalyst for Visible Light Hydrogen Production Based on Oxidative Quenching of Eosin Y

LI Bo1,2, LÜ Gong Xuan1   

  1. 1 Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Tianshui Zhong Road 18, Lanzhou 730000, P. R. China;
    2 University of Chinese Academy of Sciences, Beijing 100049, P. R. China
  • Received:2013-04-16 Revised:2013-05-29 Published:2013-07-09
  • Contact: Lü Gong Xuan E-mail:gxlu@lzb.ac.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (21173242), National Key Basic Research Program of China (973) (2009CB22003), and National High Technology Research and Development Program of China (863) (2012AA051501).

摘要:

以曙红Y(EY)敏化Pt/TiO2(EY-Pt/TiO2)光催化产氢体系为模型, 研究了电子传递剂甲基紫精(MV2+)的加入对该体系产氢活性和稳定性的影响, 并通过紫外-可见光(UV-Vis)吸收光谱、荧光光谱和光电化学表征手段对MV2+的作用机制进行了研究. 结果表明, 当以三乙醇胺(TEOA)为电子给体时, MV2+可使EY激发态发生氧化性和还原性淬灭, 有效降低了不稳定中间体EY3-·的形成和积累, 促进了电子由染料分子向产氢活性位点的有效传递, 从而提高了产氢体系的活性和稳定性. 两种敏化体系瞬态光电流以及产氢活性受EY浓度影响的差异进一步证明, MV2+作为电子传递剂有效提高了光生电子的传递和利用效率.

关键词: 甲基紫精, 活性, 稳定性, 产氢, 光催化

Abstract:

The effects and mechanism of methyl viologen (MV2+) on photocatalytic hydrogen production over an active, stable catalyst sensitized by Eosin Y (EY) under visible light were studied by UV-Vis absorption, fluorescence spectroscopies and photoelectric experiments. The results showed that MV2+ increased the efficiency of electron transfer from excited states of EY to the surface of Pt/TiO2 and suppressed accumulation of unstable intermediate EY3-· by an oxidative and reductive quenching mechanism. MV2+ also improved the activity and stability of photocatalytic hydrogen production by an EY-sensitized Pt/TiO2 system with triethanolamine (TEOA) as an electron donor. The effects of transient photocurrent and concentration of EY on the hydrogen production activity of dye-sensitized systems with and without MV2+ provided further evidence that MV2+ acted as an electron transfer agent to effectively improve photoinduced electron transfer and utilization efficiency.

Key words: Methyl violet, Activity, Stability, Hydrogen production, Photocatalysis

MSC2000: 

  • O643