负载型钯团簇上氢分子吸附和解离吸附的密度泛函理论

发布时间：2018-10-08 17:10

【摘要】：基于密度泛函理论考察勃姆石(AlOOH)和氧化锆(ZrO_2)负载的钯团簇表面氢分子吸附和解离吸附过程,通过分析一系列不同尺寸的钯团簇上氢吸附能以及氢分子-钯团簇-载体三者之间的电荷转移系统地研究了粒径效应和载体效应。结果表明,顶点位和面位分别是分子吸附和解离吸附的最佳吸附位置。随着钯团簇粒径的上升,氢分子吸附能和解离吸附能都下降,载体-钯团簇-被吸附氢三者之间的电荷转移量和方向也改变。氧化锆载体负载的钯团簇上分子吸附能和解离吸附能均大于勃姆石载体负载的钯团簇,说明载体对氢分子吸附过程有重要影响。
[Abstract]:Based on density functional theory (DFT), the adsorption and dissociation of hydrogen molecules on palladium clusters supported by (AlOOH) and ZrO_2 were investigated. The particle size effect and carrier effect were studied systematically by analyzing the adsorption energy of hydrogen on a series of palladium clusters of different sizes and the charge transfer between hydrogen molecule palladium cluster and carrier. The results show that the vertex and surface positions are the best adsorption sites for molecular adsorption and dissociation adsorption respectively. With the increase of the particle size of palladium cluster, the adsorption energy of hydrogen molecule and dissociation energy decrease, and the charge transfer amount and direction between the carrier, palladium cluster and adsorbed hydrogen also change. The adsorption energy and dissociation energy of zirconia supported palladium clusters are higher than those of bauxite supported palladium clusters, indicating that the carrier has an important influence on the adsorption process of hydrogen molecules.
【作者单位】：化学工程联合国家重点实验室华东理工大学;
【基金】：国家自然科学基金项目(21406063,21576081) 中央高校基本科研业务费项目(WA1514005)~~
【分类号】：O647.3;O641.1

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