Final Report for Department of Energy grant DE-FG02-91ER45455, "Theoretical Study of Reactions at the Electrode-Electrolyte Interface"

[摘要] In this project, reaction rates were predicted by numerical methods, in a collaboration with Argonne National Laboratory . Emphasis is on electron transfer and transport involving ions known to be important in enhancing stress corrosion cracking in light water reactors and on electron transfer at oxide surfaces. In the latter part of the grant period we placed increased emphasis on development and use of self consistent tight binding methods for this kind of study. We showed that by careful fitting of results from first principles plane wave calculations,we could model surfaces and interfaces oxides and metals using these methods. We obtained results for the titanium/titanium oxide interface in this way and completed a model of the ruthenium dioxide surface using our innovative self consistent tight binding molecular dynamics methods. We completed development of a description of liquid water within the self consistent tight binding context and studied the rutile water 110 interface to determine if it is hydroxylated. A self consistent tight binding study of titanium metal surfaces demonstrated the usefulness of this method for metals. In collaboration with the Argonne group, we extended the tight binding calculations on rutile titania to the anatase form and made the first calculations of the relative stability of anatase and rutile as a function of crystallite size. We completed studies of small anatase particles in water using the method and found significant distortions of nanoparticle crystallite shapes as a consequence of interactions with the water.

[发布日期] 2009-05-19

[学科分类] 材料科学（综合）

[关键词] ANL;ELECTRON TRANSFER;MOLECULAR DYNAMICS METHOD;OXIDES;REACTION KINETICS;RUTHENIUM;RUTILE;STABILITY;STRESS CORROSION;TITANIUM;TRANSPORT;WATER Corrosion;electron transfer;passivation