从头算分子动力学模拟Pd团簇负载UiO-66材料结构及稳定性  

Ab initio Molecular Dynamics Simulations on the Structures and Stabilities of Pd Clusters Encapsulated UiO-66 Materials

作　　者：陈德利[1] 杨鹏勇 武胜男[1] 何思慧[2] 王芳芳[2] 

机构地区：[1]浙江师范大学先进催化材料教育部重点实验室 [2]浙江师范大学化学与生命科学学院,金华321004

出　　处：《高等学校化学学报》2017年第7期1210-1215,共6页Chemical Journal of Chinese Universities

基　　金：浙江省自然科学基金(批准号:LQ14B030001);国家自然科学基金(批准号:21403198;21303165)资助~~

摘　　要：采用从头算分子动力学模拟与密度泛函理论相结合的方法,计算模拟了不同尺寸的Pdn(n=1~32)金属团簇在UiO-66孔道中的稳定构型,并对金属团簇与材料骨架之间的作用方式、结合能及骨架形变能等进行了讨论.采用Bader电荷分析方法对该体系的电荷转移情况进行了计算分析.结果表明,Pdn团簇稳定负载于UiO-66材料的四面体笼中,且均呈堆积型构型.当Pd原子个数为28时体系的热力学稳定性最好,这与金属团簇和有机配体的成键方式相关,是金属团簇内部结合能和骨架形变能综合作用的结果.In order to understand the structuresand electronic properties of Pdn @ UiO-66 （n = 1-32） at atomic level, ab initio molecular dynamics simulations combined with density functional theory was used to search thermodynamically stable structures. And then the bonding characteristics between the metal cluster and the framework, binding energies, deformation energies of the framework, as well as the charge transfer between the metal cluster and the framework were analyzed. The modeling show that the Pdn clusters were confined in the small cage, i.e., the tetrahedral cage of the UiO-66, and Pd2s @ UiO-66 was found to be the thermodynamically most stable composite with the number of Pd atoms up to 32, which is a result of the interplay of the binding energy for the metal cluster and the deformation energy of the framework. The calculations indicate that the results can be successfully used to locate stable structures for metal nanoparticle （MNP） encapsulated mechanism using MNP

关 键 词：UiO-66 钯金属团簇 从头算分子动力学 密度泛函理论 电荷转移 

分 类 号：O641[理学—物理化学]