摘要
采用量子化学的密度泛函理论方法,探讨了H2S、HS和S在立方ZrO2(110)面上不同吸附位的吸附情况。构型优化的结果表明:在bridge位H2S以垂直底物平面H原子向上、垂直底物平面H原子向下、平行底物平面和hollow位H2S平行底物平面模式吸附在ZrO2(110)面发生解离吸附。SH和S的最佳吸附位分别为桥位和顶位。Mulliken布局和态密度分析显示S原子的p轨道与Zr原子的d轨道发生相互作用。通过计算解离反应的能垒,表明H2S分子在立方ZrO2(110)面发生两步解离。
The adsorption of H2S, HS and S on the different sites of cubic ZrO2 （110） surface has been studies by density functional theory calculation with GGA-PW91 method. The results of geometry optimization indicate that the stable structures of dissociative adsorption are H2S molecules adsorbed on bridge sites and parallel on the hollow site. SH and S were found to prefer bridge sites and top sites, respectively. The analysis of Mulliken population and density of states indicates that p orbital in sulfur interacted with d orbital in zirconium. Complete linear synchronous transit （LST） and quadratic synchronous transit （QST） methods were used to search the transition state for dissociation reaction. The results reveal that H2S dissociated on ZrO2 （110） surface and formed hydroxyl and sulfhydryl groups.
出处
《无机化学学报》
SCIE
CAS
CSCD
北大核心
2009年第8期1457-1463,共7页
Chinese Journal of Inorganic Chemistry
基金
福建省高等学校新世纪优秀人才计划(No.HX2006-103)
福建省教育厅科技项目(No.JA08019)
煤燃烧国家重点实验室开放基金(No.FSKLCC0814)资助
关键词
硫化氢
二氧化锆
密度泛函理论
吸附
解离
H2S
ZrO2
density functional theory
adsorption
decomposition
