Pd(111),Pd(100)及Pd(110)表面H2和O2直接合成H2O2的密度泛函理论研究

催化学报 , 2013, 34(5): 1002-1012. doi: 10.1016/S1872-2067(12)60537-3

Pd(111),Pd(100)及Pd(110)表面H2和O2直接合成H2O2的密度泛函理论研究

田鹏飞 ^1, , 欧阳李科 ^2, , 徐新潮 ^3, , 徐晶 ^4, , 韩一帆 ^5,

1.华东理工大学化学工程联合国家重点实验室,上海200237

2.华东理工大学化学工程联合国家重点实验室,上海200237

3.华东理工大学化学工程联合国家重点实验室,上海200237

4.华东理工大学化学工程联合国家重点实验室,上海200237

5.华东理工大学化学工程联合国家重点实验室,上海200237

基金项目: the National Natural Science Foundation of China(21176071,21106041) 国家自然科学基金(21176071,21106041)

关键词：钯 , 过氧化氢 , 氢气 , 氧气 , 直接合成 , 密度泛函理论

Density functional theory study of direct synthesis of H2O2 from H2 and O2 on Pd(111), Pd(100), and Pd(110) surfaces

TIAN Pengfei ^1, , OUYANG Like ^2, , XU Xinchao ^3, , XU Jing ^4, , HAN Yi-Fan ^5,

1.华东理工大学化学工程联合国家重点实验室,上海200237

2.华东理工大学化学工程联合国家重点实验室,上海200237

3.华东理工大学化学工程联合国家重点实验室,上海200237

4.华东理工大学化学工程联合国家重点实验室,上海200237

5.华东理工大学化学工程联合国家重点实验室,上海200237

Keywords： Palladium , Hydrogen peroxide , Hydrogen , Oxygen , Direct synthesis , Density functional theory

采用周期性密度泛函理论研究了H2和O2在Pd(111),Pd(100)及Pd(110)表面上直接合成H2O2的反应机理,对反应的主要基元步骤进行了计算和分析.结果表明,Pd(111)表面对H2O2直接合成的催化选择性最好,表面原子密度较低的Pd(100)表面和Pd(110)表面上含有O-O键的表面物种解离严重,不利于H2O2的生成.H2O2的选择性与含有O-O键表面物种的O-O键能和表面物种的结合能有关.含有O-O键的表面物种在表面的结合能越大,越容易发生解离,不利于形成H2O2.

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