Pd-C_(2)N催化丙烷脱氢反应的密度泛函理论研究  

Density functional theory study on Pd-C_(2)N catalytic dehydrogenation of propane

作　　者：赵雅兰 康丽华[1] ZHAO Yalan;KANG Lihua(School of Chemistry and Chemical Engineering,Shihezi University,Shihezi,Xinjiang 832003,China)

机构地区：[1]石河子大学化学化工学院,新疆石河子832003

出　　处：《石河子大学学报（自然科学版）》2022年第5期537-546,共10页Journal of Shihezi University(Natural Science)

基　　金：新疆生产建设兵团博士资金项目(2013BB010)。

摘　　要：丙烷脱氢制丙烯技术由于选择性高,价格相对便宜,是丙烯生产的一种非常有前景的方法。在本研究中,设计出一种Pd-C_(2)N二维单原子催化剂。通过密度泛函理论研究Pd-C_(2)N上丙烷脱氢的反应,所有模拟计算使用B3LYP泛函,对Pd原子使用LAN2DZ赝势,对于C,H,N非金属原子使用6-31g^(**)基组。分析催化剂静电势,态密度及反应物在催化剂上的吸附作用及反应机理。计算研究表明,Pd-C_(2)N催化丙烷脱氢反应路径为先脱甲基上的氢原子,再脱亚甲基上的氢原子从而生成丙烯,能垒为25.09 kcal·mol^(-1)。丙烯在催化剂上将进一步进行脱氢反应,能垒为42.81 kcal·mol^(-1)。Pd-C_(2)N催化剂在丙烷脱氢反应中表现出优异的催化性能,为设计潜在的新型丙烷脱氢潜在的催化剂提供了理论依据。Propane dehydrogenation to propylene is a promising method for propylene production due to its high selectivity and relatively low price.In this study,a two-dimensional monatomic Pd-C_(2)N catalyst was designed.The reaction of propane dehydrogenation on Pd-C_(2)N is studied by density functional theory.All simulation calculations are performed using B3LYP functional,LAN2DZ pseudopotential for Pd atoms,and 6-31g** basis set for C,H,and N nonmetallic atoms.The electrostatic potential,state density,adsorption and reaction mechanism of reactants on catalyst were analyzed.The calculation results show that Pd-C_(2)N catalyzes propane dehydrogenation by dehydrogenation of hydrogen atoms on methyl group and then hydrogen atoms on methylene group to generate propylene,with an energy barrier of 25.09 kcal·mol^(-1).The dehydrogenation of propylene on the catalyst was further carried out with an energy barrier of 42.81 kcal·mol^(-1).Pd-C_(2)N catalyst shows excellent catalytic performance in propane dehydrogenation,which provides a theoretical basis for the design of potential new catalysts for propane dehydrogenation.

关 键 词：丙烷脱氢 Pd-C_(2)N 密度泛函理论 催化性能 

分 类 号：O643.32[理学—物理化学]