PdZn intermetallic compound stabilized on ZnO/nitrogendecorated carbon hollow spheres for catalytic semihydrogenation of alkynols  

作　　者：Chunlin Ye Xujian Chen Shasha Li Binbin Feng Yanghe Fu Fumin Zhang De-Li Chen Weidong Zhu 

机构地区：[1]Key Laboratory of the Ministry of Education for Advanced Catalysis Materials,Institute of Physical Chemistry,Zhejiang Normal University,Jinhua 321004,China

出　　处：《Nano Research》2022年第4期3090-3098,共9页纳米研究（英文版）

基　　金：We thank the financial supports from the National Natural Science Foundation of China(No.21576243);the Natural Science Foundation of Zhejiang Province(Nos.LY18B060006,LY17B060001,and LY21B030003).

摘　　要：Enhancing the selectivity of noble metal catalysts through electronic modulation is important for academic research and chemical industrial processes.Herein,we report a facile sacrificial template strategy for the synthesis of PdZn intermetallic compound(3-4 nm)highly distributed in ZnO/nitrogen-decorated carbon hollow spheres(PdZn-ZnO/NCHS)to optimize the selectivity of Pd catalysts,which involves carbonization of a core-shell structured polystyrene(PS)@ZIF-8 precursor in an inert atmosphere,impregnation Pd precursor,and subsequent H2 reduction treatment.Due to the unique structural and compositional features,the developed PdZn-ZnO/NCHS delivers an excellent catalytic performance for the semihydrogenation of 2-methyl-3-butyn-2-ol(MBY)to 2-methyl-3-buten-2-ol(MBE)with high activity(>99%),high selectivity(96%),and good recyclability,outperforming the analog Pd on ZnO(Pd/ZnO)as well as the supported Pd nanoparticles(Pd/C and Pd/NC).Density functional theory(DFT)calculations reveal that the presence of Znδ+species in PdZn-ZnO/NCHS alters the adsorption modes of reactant and product,leading to a decrease of the adsorption strength and an enhancement of the energy barrier for overhydrogenation,which results in a kinetic favor for the selective transformation of MBY to MBE.In addition,PdZn-ZnO/NCHS was also very effective for the partial hydrogenation of dehydrolinalool to hydrolinalool.

关 键 词：PdZn intermetallic compound semihydrogenation of alkynol MOF-derived N-decorated carbon hollow sphere density functional theory(DFT) 

分 类 号：O64[理学—物理化学]