On the mechanism for the reduction of nitrogen monoxide on Rh(111) single-crystal surfaces
On the mechanism for the reduction of nitrogen monoxide on Rh(111) single-crystal surfaces
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DOI：
10.1039/b208091e
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发表时间：
2003-01
影响因子：
3.3
通讯作者：
F. Zaera;C. Gopinath
中科院分区：
文献类型：
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作者：
F. Zaera;C. Gopinath
用同位素标记的分子束进行了等温动力学实验，以表征在Rh(111)单晶表面上一氧化碳还原一氧化氮的表面反应。这里报道的新数据支持先前提出的基本模型，该模型通过在氮原子表面岛的外围形成N-NO中间体来产生氮气。然而，它们也突显了一些额外的微妙的复杂情况。特别是，当从14NO+CO切换到15NO+CO混合物时，少量14N14N的快速脱附表明，反应表面附近的额外吸附物质在促进N-NO中间体的解离中起到了作用。此外，混合14NO+15NO+CO的实验结果表明，先前沉积的14N岛边缘的反应和新的混合14N+15N表面团簇的生长是相结合的。
Isothermal kinetic experiments were carried out with isotopically-labeled molecular beams in order to characterize the surface reactions involved in the reduction of nitrogen monoxide with carbon monoxide on Rh(111) single-crystal surfaces. The new data reported here offers support for the basic model advanced previously where N2 production takes place via the formation of N–NO intermediates at the periphery of atomic nitrogen surface islands. However, they also highlight a few additional subtle complications. In particular, the rapid desorption of a small amount of 14N14N upon switching from 14NO + CO to 15NO + CO mixtures points to the role of additional adsorbates nearby the reaction surface site in facilitating the dissociation of the N–NO intermediates. In addition, the results from experiments with mixed 14NO + 15NO + CO indicate a combination of reactions at the edges of previously deposited 14N islands and the growth of new mixed 14N + 15N surface clusters.