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甲醇在TiO2(110)表面光催化氧化的波长相关性
引用本文:王志强,郝群庆,周传耀,戴东旭,杨学明.甲醇在TiO2(110)表面光催化氧化的波长相关性[J].化学物理学报,2015,28(4):459-464.
作者姓名:王志强  郝群庆  周传耀  戴东旭  杨学明
作者单位:中国科学院大连化学物理研究所分子反应动力学国家重点实验室,大连116023,中国科学院大连化学物理研究所分子反应动力学国家重点实验室,大连116023,中国科学院大连化学物理研究所分子反应动力学国家重点实验室,大连116023,中国科学院大连化学物理研究所分子反应动力学国家重点实验室,大连116023,中国科学院大连化学物理研究所分子反应动力学国家重点实验室,大连116023
摘    要:用程序升温脱附谱的方法研究了甲醇在TiO2(110)表面光催化氧化的波长相关性.对于不同波长的激发光,甲醇光催化解离的产物相似,都是在光照的过程中通过O-H键和C-H键的断裂形成甲醛,解离出的氢原子转移到相邻的两配位的桥氧原子(Ob)上形成ObH.但是反应速率与激发光波长强烈相关.在360 nm光照下,甲醇的反应速率是400 nm光照时的4.8倍.这与以前使用时间分辨的飞秒激光吸收光谱测量的结果是一致的,他们认为近带隙激发和过带隙激发产生的电荷相比,前者的复合速率要远快于后者.

关 键 词:二氧化钛,光催化,波长相关性,程序升温脱附谱
收稿时间:2015/7/11 0:00:00

Excitation Wavelength Dependence of Photocatalyzed Oxidation of Methanol on TiO2(110)
Zhi-qiang Wang,Qun-qing Hao,Chuan-yao Zhou,Dong-xu Dai and Xue-ming Yang.Excitation Wavelength Dependence of Photocatalyzed Oxidation of Methanol on TiO2(110)[J].Chinese Journal of Chemical Physics,2015,28(4):459-464.
Authors:Zhi-qiang Wang  Qun-qing Hao  Chuan-yao Zhou  Dong-xu Dai and Xue-ming Yang
Affiliation:State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Science, Dalian 116023, China,State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Science, Dalian 116023, China,State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Science, Dalian 116023, China,State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Science, Dalian 116023, China and State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Science, Dalian 116023, China
Abstract:Post-irradiation temperature-programmed desorption (TPD) has been used to study the photocatalyzed oxidation of methanol on TiO2(110) surface under the irradiation of 360, 380 and 400 nm light. The photocatalytic process initiated by ultraviolet light of different wavelength are similar. Methanol has been photocatalytically converted into formaldehyde, and the released hydrogen atoms transfer to the neighboring twofold coordinated oxygen to form bridging hydroxyls. The reaction rate, however, is strongly wavelength dependent. The reaction rate under 360 nm light irradiation is 4.8 times of that in the case of 400 nm exposure, consistent with a previous femtosecond time-resolved absorption measurement on TiO2 which shows the faster charge carrier recombination in the near-band-gap than the over-band-gap excitation. So far, the underlying factors which govern the excitation wavelength dependence of photocatalytic activity of TiO2 and other photocatalysts remain unclear, and future studies are needed to address this important issue.
Keywords:Titanium dioxide  Photocatalysis  Excitation wavelength dependence  Temperature-programmed desorption
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