Density functional characterization of N-2 dissociation on the step of ruthenium clusters

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	Density functional characterization of N-2 dissociation on the step of ruthenium clusters
	Cao, Z. X. ; Wan, H. L. ; Zhang, Q. N. ; Zhang QE(张乾二)
刊名	http://dx.doi.org/10.1063/1.1615761
	2003-11-01
关键词	MATRIX INFRARED-SPECTRA AMMONIA-SYNTHESIS MOLECULAR NITROGEN SUPPORTED RUTHENIUM RU(0001) SURFACE ADSORPTION CATALYSTS OSMIUM TEMPERATURES
英文摘要	Mechanisms of N-2 dissociative adsorption on small ruthenium clusters are studied by density functional calculations. The calculations indicate that the step of a ruthenium cluster has high activity for N-2 activation, where an ensemble of five Ru atoms on the stepped surface of clusters is responsible for the active site. Such high activity arises from a strong charge-transfer interaction due to local phase adaptation between the pi* orbital of N-2 and the filled cluster valence orbital over the step region. Results from cluster models with different size show that the activation mechanism and the barrier are sensitive to the structural environment of the step. N-2 dissociation over the step of the 11-atom cluster is a two-step process, where the rate-determining step has a barrier of 22 kcal mol-1. N-2 dissociative adsorption on the stepped surface of 15-atom and 21-atom clusters is a one-step process, and the barrier is similar to7-10 kcal mol-1. Theoretical calculations on the 11-atom Os and Fe cluster models reveal a general activity of the stepped sites for N-2 activation. (C) 2003 American Institute of Physics.
语种	英语
内容类型	期刊论文
源URL	[http://dspace.xmu.edu.cn/handle/2288/61915]
专题	化学化工－已发表论文
推荐引用方式 GB/T 7714	Cao, Z. X.,Wan, H. L.,Zhang, Q. N.,et al. Density functional characterization of N-2 dissociation on the step of ruthenium clusters[J]. http://dx.doi.org/10.1063/1.1615761,2003.
APA	Cao, Z. X.,Wan, H. L.,Zhang, Q. N.,&张乾二.(2003).Density functional characterization of N-2 dissociation on the step of ruthenium clusters.http://dx.doi.org/10.1063/1.1615761.
MLA	Cao, Z. X.,et al."Density functional characterization of N-2 dissociation on the step of ruthenium clusters".http://dx.doi.org/10.1063/1.1615761 (2003).