Kinetics and Dynamics of Photocatalyzed Dissociation of Ethanol on TiO2(110)

Kinetics and Dynamics of Photocatalyzed Dissociation of Ethanol on TiO2(110)
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TiO2(110) 光催化解离乙醇的动力学和动力学

DOI:
10.1063/1674-0068/26/01/1-7
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发表时间:
2013-02
影响因子:
1
通讯作者:
Yang, Xue-ming
Yang, Xue-ming
中科院分区:
化学4区
文献类型:
--
作者:
Mao, Xin-chun;Ren, Ze-feng;Dai, Dong-xu;Yang, Xue-ming

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为了揭示乙醇在TiO 2(110)表面上的光化学性质,分别利用含时和时间分辨飞秒双光子光电子能谱研究了乙醇在TiO 2(110)表面上的光催化分解动力学和动力学。通过监测与乙醇在TiO 2(110)的Ti-5C位上的光催化解离相关的光致激发态的时间演化,已经获得了该表面光催化反应的类分形动力学。在还原的TiO 2(110)上测得的光催化解离速率比在氧化的表面上的快。这归因于还原表面上较大的缺陷密度,这至少在方法学上降低了光催化反应的反应势垒。已经讨论了与用于加速的缺陷电子相关联的可能原因。通过在乙醇/TiO 2(110)界面上进行干涉双脉冲关联,测量了激发态的超快电子动力学.激发态的分析寿命(24 fs)与甲醇/TiO 2(110)上的寿命相似。激发态的出现提供了介导TiO 2衬底与其环境之间的电子转移的通道。因此,研究其超快电子动力学,有助于理解TiO 2的电致变色和光电化学能量转换的微观机理。
the kinetics and dynamics of photocatalyzed dissociation of ethanol on tio2(110) surface have been studied using the time-dependent and time-resolved femtosecond two-photon photoemission spectroscopy respectively, in order to unravel the photochemical properties of ethanol on this prototypical metal oxide surface. by monitoring the time evolution of the photoinduced excited state which is associated with the photocatalyzed dissociation of ethanol on ti-5c sites of tio2(110), the fractal-like kinetics of this surface photocatalytic reaction has been obtained. the measured photocatalytic dissociation rate on reduced tio2(110) is faster than that on the oxidized surface. this is attributed to the larger defect density on the reduced surface which lowers the reaction barrier of the photocatalytic reaction at least methodologically. possible reasons associated with the defect electrons for the acceleration have been discussed. by performing the interferometric two-pulse correlation on ethanol/tio2(110) interface, the ultrafast electron dynamics of the excited state has been measured. the analyzed lifetime (24 fs) of the excited state is similar to that on methanol/tio2(110). the appearance of the excited state provides a channel to mediate the electron transfer between the tio2 substrate and its environment. therefore studying its ultrafast electron dynamics may lead to the understanding of the microscopic mechanism of photocatalysis and photoelectrochemical energy conversion on tio2.
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