The nature of transition-metal-oxide surfaces

化学吸附 化学 过渡金属 化学物理 氧化物 电子结构 金属 电子组态 晶体缺陷 结晶学 人口 Crystal(编程语言) 无机化学 计算化学 离子 物理化学 催化作用 吸附 人口学 有机化学 程序设计语言 社会学 生物化学 计算机科学
作者
Victor E. Henrich
出处
期刊:Progress in Surface Science [Elsevier BV]
卷期号:14 (2): 175-199 被引量:105
标识
DOI:10.1016/0079-6816(83)90002-3
摘要

The surfaces of the 3d-transition-metal oxides form a rich and important system in which to study the effects of atomic geometry, ligand coordination and d-orbital population on surface electronic structure and chemisorption. This article considers the properties of those surfaces in terms of the types of surface structures that can exist, including steps and point defects, and their relation to the experimental data that is available for well characterized, single-crystal surfaces. The electronic structure of nearly perfect surfaces is very similar to that of the bulk for many of the oxides that have been studied; atoms at step sites also appear to have properties similar to those of atoms on terraces. Point defects are often associated with surfaces 0 vacancies and attendant transfer of electrons to adjacent metal cations. Those cations are poorly screened from each other, and the excess charge is presumably shared between two or more cations having reduced ligand coordination. Point defects are generally more active for chemisorption than are perfect surfaces, however for Ti2O3 and V2O3, whose cations have 3d1 and 3d2 electronic configurations respectively, the cleaved (047) surface is more active than are surfaces having a high density of defects. The chemisorption behavior of both nearly perfect and defect surfaces of 3d-transition-metal oxides varies widely from one material to another, and it is suggestive to correlate this with cation d-orbital population. However, too few oxides have yet been studied to draw any firm conclusions. Additional theoretical work on perfect surfaces, defects and chemisorption is also necessary in order to gain a more complete understanding of transition-metal-oxide surfaces.
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