Comparative study of C-H stretch and bend vibrations in methane activation on Ni(100) and Ni(111)
Comparative study of C-H stretch and bend vibrations in methane activation on Ni(100) and Ni(111)
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DOI：
10.1103/physrevlett.94.208303
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发表时间：
2005-05-27
影响因子：
8.6
通讯作者：
Utz, AL
中科院分区：
文献类型：
--
作者：
Juurlink, LBF;Smith, RR;Utz, AL
在清洁的Ni（100）和Ni（111）表面上的状态分辨测量量化了被激发到v=3的nu（4）弯曲振动的CH 4的反应性。与先前数据的比较揭示了3 nu（4）在促进解离化学吸附方面比nu（3）C-H伸缩显著更不有效，即使3 nu（4）包含30%以上的能量。这些结果与气体表面反应性的统计理论相矛盾，为气体表面反应中的振动模式特异性提供了明确的证据，并指出C-H伸缩运动沿着反应路径到解离化学吸附的中心作用。
State-resolved measurements on clean Ni(100) and Ni(111) surfaces quantify the reactivity of CH4 excited to v=3 of the nu(4) bend vibration. A comparison with prior data reveals that 3 nu(4) is significantly less effective than the nu(3) C-H stretch at promoting dissociative chemisorption, even though 3 nu(4) contains 30% more energy. These results contradict statistical theories of gas-surface reactivity, provide clear evidence for vibrational mode specificity in a gas-surface reaction, and point to a central role for C-H stretching motion along the reaction path to dissociative chemisorption.