TRANSITION-METAL BONDING FUNCTIONS AND THEIR APPLICATION IN ADSORPTIONS AND CATALYTIC REACTIONS 1 THEORETICAL-MODEL

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	TRANSITION-METAL BONDING FUNCTIONS AND THEIR APPLICATION IN ADSORPTIONS AND CATALYTIC REACTIONS 1 THEORETICAL-MODEL
	HUANG, KH ; Huang KH(黄开辉)
刊名	http://dx.doi.org/10.1016/0304-5102(91)85127-N
	1991
关键词	HYDROGEN CHEMISORPTION BINDING-ENERGY CLUSTER-MODEL SURFACES CO NICKEL PHOTOEMISSION NI SPECTROSCOPY MOLECULES
英文摘要	A new method has been proposed for rapidly and chemically-intuitively giving correct information on the relative abilities or relative data (binding energy, bond structure, bond strength, vibration frequencies of surface species, etc.) of chemisorptions, dissociation and reactions on various transition metals, and the effects caused by the Metal-Promoter (or -Support) Interactions. In order to achieve this purpose, the LCAO method is first used to derive the wave function of the mono-transition-metal atom, represented by the combination of molecular orbital (M.O.) bands, where each M.O. is described as the linear combination of s and d orbitals. Second, based on various electronic spectra before and after adsorption, we assume that the adsorption and reaction occur chiefly on the valence band around the Fermi level. The valence band consists of three M.O. Groups (MOGs): the vacant MOG at the bottom of the s band, the vacant or fractional half-occupied MOG of the d band and the occupied MOG at the top of the occupied band near the Fermi level, denoted as PSI-(Mi, Vs), PSI-(Mi, Vd) and PSI-(Mi, d(occ)), respectively. Assuming that the M.O.'s energy distribution is even, the concept of mean energy and mean chemisorption binding energy is employed, and the three MOGs can be simplified as three representative M.O.s. According to the principle of Bloch energy band formation, the concept of d-s band overlap and the probability theory, some simple formulas with the parameters of metal band structure such as the width of the d band, the atomic orbital effective exponents and the total electron number of the s and d orbitals have been derived to calculate coefficients of the s and d orbitals of the three representative M.O.s. The interaction between metal and absorbate is characterized by bonding functions which depend on three factors: the overlap integral between the wave function of three representative M.O.s and the adsorbate, the thermodynamic potential and the ability of electron transfer. The bonding functions D,A,B and AB have been proposed to characterize the bonds involved in metal electron donation, metal electron acceptance, d electron back-donation and sigma-pi coordination, respectively. Our model involves intuitive chemical localized bonds and represents the delocalized effects of energy bands. Its advantages (relatively realistic, intuition, rapidity, convenience and practice) and drawbacks (the inability to obtain the absolute amounts of surface bond strength, electron charge distribution and detailed energy levels) were discussed in comparison with the EHMO, CNDO, X-alpha-SW, LDF, GVB and EMT methods.
语种	英语
出版者	J MOL CATAL
内容类型	期刊论文
源URL	[http://dspace.xmu.edu.cn/handle/2288/88612]
专题	化学化工－已发表论文
推荐引用方式 GB/T 7714	HUANG, KH,Huang KH. TRANSITION-METAL BONDING FUNCTIONS AND THEIR APPLICATION IN ADSORPTIONS AND CATALYTIC REACTIONS 1 THEORETICAL-MODEL[J]. http://dx.doi.org/10.1016/0304-5102(91)85127-N,1991.
APA	HUANG, KH,&黄开辉.(1991).TRANSITION-METAL BONDING FUNCTIONS AND THEIR APPLICATION IN ADSORPTIONS AND CATALYTIC REACTIONS 1 THEORETICAL-MODEL.http://dx.doi.org/10.1016/0304-5102(91)85127-N.
MLA	HUANG, KH,et al."TRANSITION-METAL BONDING FUNCTIONS AND THEIR APPLICATION IN ADSORPTIONS AND CATALYTIC REACTIONS 1 THEORETICAL-MODEL".http://dx.doi.org/10.1016/0304-5102(91)85127-N (1991).