Short-Lived Reactive Intermediate in the Decomposition of Formate on NiO(111) Surface Observed by Picosecond Temperature Jump
Short-Lived Reactive Intermediate in the Decomposition of Formate on NiO(111) Surface Observed by Picosecond Temperature Jump
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通过皮秒温跃观测到 NiO(111) 表面甲酸盐分解中的短寿命反应中间体
DOI：
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发表时间：
1998
期刊：
影响因子：
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通讯作者：
C. Hirose
中科院分区：
文献类型：
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作者：
A. Bandara;J. Kubota;K. Onda;A. Wada;S. Kano;K. Domen;C. Hirose
不稳定的中间体是化学反应中不可缺少的成分，但由于缺乏检测短寿命和分数生成物种的技术，它们在固体表面的识别受到阻碍。我们成功地确定了在热分解反应中的中间体，利用皮秒温度跳变的激光脉冲的照射和观察的和频发生光谱。我们证实了甲酸盐在NiO（111）表面上的分解是由稳定的双齿甲酸盐转化为不稳定的单齿甲酸盐，这是反应中间体，并且发现两种物种在分解前处于平衡状态。
Unstable intermediates are indispensable ingredients of chemical reactions, but their identification at solid surfaces has been hampered by the lack of techniques to detect short-lived and fractionally generated species. We succeeded in identifying the intermediate in a thermal decomposition reaction by utilizing the picosecond temperature jump induced by the irradiation of laser pulses and the observation by sum-frequency generation spectroscopy. We verified that the decomposition of formate on the NiO(111) surface is preceded by the transformation of stable bidentate formate to unstable monodentate formate, which is the reactive intermediate, and two species are found to be in equilibrium before decomposition.