Observation of Tunneling in the Hydrogenation of Atomic Nitrogen on the Ru(001) Surface to Form NH.
Observation of Tunneling in the Hydrogenation of Atomic Nitrogen on the Ru(001) Surface to Form NH.
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Ru(001) 表面原子氮氢化形成 NH 时隧道效应的观察。
DOI：
10.1021/jz4020585
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发表时间：
2013
期刊：
影响因子：
--
通讯作者：
M. Trenary
中科院分区：
文献类型：
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作者：
I. Waluyo;Yuan Ren;M. Trenary
利用时间依赖反射吸收红外光谱（RAIRS）研究了Ru（001）上NH和ND的生成和解离反应动力学。我们的研究结果表明Ru（001）上的NH和ND的形成和解离遵循一级动力学。在反应温度范围内（NH为320 ~ 390 K， ND为340 ~ 390 K）， NH和ND形成的表观活化能分别为72.2±1.9和87.1±1.8 kJ/mol，而NH和ND在370 ~ 400 K之间的离解反应的表观活化能分别为106.9±4.1和101.8±4.8 kJ/mol。NH生成的表观活化能低于ND生成的表观活化能，以及实验测量的同位素效应与理论结果的比较强烈表明，在高达340 K的温度下，隧道效应已经开始在该反应中发挥作用。
The kinetics of NH and ND formation and dissociation reactions on Ru(001) were studied using time-dependent reflection absorption infrared spectroscopy (RAIRS). Our results indicate that NH and ND formation and dissociation on Ru(001) follow first-order kinetics. In our reaction temperature range (320-390 K for NH and 340-390 K for ND), the apparent activation energies for NH and ND formation were found to be 72.2 ± 1.9 and 87.1 ± 1.8 kJ/mol, respectively, while NH and ND dissociation reactions between 370 and 400 K have apparent activation barriers of 106.9 ± 4.1 and 101.8 ± 4.8 kJ/mol, respectively. The lower apparent activation energy for NH formation than that for ND as well as the comparison between experimentally measured isotope effects with theoretical results strongly indicates that tunneling already starts to play a role in this reaction at a temperature as high as 340 K.