First-principles Study on NO Adsorption and Dissociation on O-Predosed Ir(100)

doi:10.7503/cjcu20120704

Abstract

Abstract:

Adsorption and dissociation of NO on O-predosed Ir(100) and the effect of co-adsorbed oxygen on the selectivity of possible products N₂, N₂O and NO₂ were investigated via first-principles density functional theory(DFT) and periodic slab model. The adsorption structures of the initial, transition and final states involved in the NO dissociation process were optimized, and the potential energy profile for each step was obtained. The results show that the most stable site for NO adsorption on O-predosed Ir(100) is the bridge site, while the top site is less stable. There are two dissociation paths for NO adsorbed on the bridge and top sites, one is direct dissociation, and the other is that NO firstly diffuses from bridge site to horizontal hollow site, followed by dissociation into N and O atoms. Similar as the decomposition mechanism on clean Ir(100), the latter is favored over the former and is the primary path for NO dissociation. The predosed O atoms inhibit the dissociation of NO at the bridge and top sites in different degrees, leading to the competition of NO dissociation on both sites. N₂ is still the predominant product, and N₂O and NO₂ are unlikely to be produced on O-predosed Ir(100), well consistent with the experimental observation. Compared with clean Ir(100), the predosed O atoms on the surface have almost no impact on the formation of N₂ at low N/O coverage, while promote the N₂ formation at high N/O coverage.

Key words: First-principle, NO dissociation, N₂ formation, Ir(100) surface, O-Predosed surface

CLC Number:

O641

TrendMD:

HE Chao-Zheng, WANG Hui, HUAI Li-Yuan, LIU Jing-Yao. First-principles Study on NO Adsorption and Dissociation on O-Predosed Ir(100)[J]. Chem. J. Chinese Universities, 2013, 34(4): 946.

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