水分子在立方ZrO2(110)面吸附与解离的密度泛函理论研究  

Density Functional Theory Study of H_2O Adsorption and Decomposition on Cubic ZrO_2(110) Surface

作　　者：杨亚丽[1] 陆春海[2] 黄娟 李奕[1] 陈文凯[1] 

机构地区：[1]福州大学化学系,福建福州350108 [2]中国工程物理研究院,四川绵阳621900 [3]新干县第二中学,江西新干331300

出　　处：《催化学报》2009年第4期328-334,共7页

基　　金：福建省高等学校新世纪优秀人才计划(HX2006-103);福建省教育厅科技项目(JA08019);福建省自然科学基金(U0650012)

摘　　要：采用密度泛函理论中的广义梯度近似(GGA)的PW91方法结合周期性平板模型,研究了H2O,OH和O在立方ZrO2(110)面上不同吸附位的吸附.结果表明,在bridge位H2O以垂直底物平面氢原子向上模式吸附在立方ZrO2(110)面时发生解离形成表面羟基,吸附能为150.5 kJ/mol.而在top位H2O以垂直底物平面氢原子向下模式吸附为物理吸附,吸附能为14.8 kJ/mol.OH和O在立方ZrO2(110)面的最佳吸附位是top位,其吸附能分别为241.5和209.1 kJ/mol.同时分析了Mulliken布居、态密度和伸缩振动频率.The adsorption of H2O,OH,and O on the different sites of cubic ZrO2（110） surface has been studied with a periodic slab model by PW91 approach of GGA within the framework of density functional theory.The results showed that H2O molecule adsorption on cubic ZrO2（110） surface is dissociation adsorption when the adsorption model is bridge（H-up）,and these H2O molecules form surface hydroxyl groups.The adsorption energy is 150.5 kJ/mol.The top（H-down） adsorption model is physical adsorption with an adsorption energy of 14.8 kJ/mol.The top site was found to be the most stable adsorption site for OH and O,and the calculated adsorption energy is 241.5 and 209.1 kJ/mol,respectively.The Mulliken population,the density of states,and the stretch vibrational frequencies have also been analyzed.

关 键 词：水 二氧化锆 密度泛函理论 吸附 解离 

分 类 号：O647.31[理学—物理化学]