物理化学学报Issue(5)：829-835,7.DOI:10.3866/PKU.WHXB201403211
水合Pb（OH）+在高岭石（001）晶面的吸附机理
Adsorption Mechanism of Hydrated Pb(OH)+ on the Kaolinite (001) Surface
摘要
Abstract
The adsorption behavior of Pb(OH)+ on the basal octahedral (001) surface of kaolinite has been investigated using the Perdew-Burke-Ernzerhof generalized gradient approximation (GGA-PBE) of density functional theory with periodic slab models, where the water environment was considered. The coordination geometry, coordination number, preferred adsorption position, and adsorption type were examined, with binding energy estimated. Al the monodentate and bidentate complexes exhibited hemi- directed geometry with coordination numbers of 3-5. Site of“Ou”with“up”hydrogen was more favorable for monodentate complex than site of“Ol”with“lying”hydrogen. Monodentate complexation of“Ou”site with a high binding energy of -182.60 kJ∙mol-1 should be the most preferred adsorption mode, while bidentate complexation on“OuOl”site of single Al center was also probable. The stability of adsorption complex was found closely related to the hydrogen bonding interactions between surface Ol and H in aqua ligands of Pb(II). Mul iken population and density of states analyses showed that coupling of Pb 6p with the antibonding Pb 6s-O 2p states was the primary orbital interaction between Pb(II) and the surface oxygen. Hydrogen complexation occupied a much large proportion in the joint coordination structure of bidentate complex, where bonding state fil ing predominated for the Pb-Ol interaction.关键词
Pb(OH)+/高岭石/化学吸附/密度泛函理论/配位数Key words
Pb(OH)+/Kaolinite/Chemical adsorption/Density functional theory/Coordination number分类
化学化工引用本文复制引用
王娟,夏树伟,于良民..水合Pb（OH）+在高岭石（001）晶面的吸附机理[J].物理化学学报,2014,(5):829-835,7.基金项目
The project was supported by the National Natural Science Foundation of China (20677053) and Natural Science Foundation of Shandong Province, China (ZR2012CQ015).国家自然科学基金(20677053)和山东省自然科学基金(ZR2012CQ015)资助项目 （20677053）
