Design And Synthesis Of Hollow Pd/MOF Microsphere With Double Shells And Properties In The Catalysis Of Hydrogenation

The composites of metal nanoparticles@Metal-organic framework(MNPs@ MOFs)not only have demonstrated many application potentials in catalysis,sensing,gas adsorption/separation,etc,thanks to their structural distinctiveness and property diversity,and they always showed more novel and excellent properties compared to the pristine counterpart.At the present,there are variety of MNPs@MOFs composites have been designed and synthesized,and according to the location,size of metal nanoparticles embedding in the MOFs,and the whole structure morphology,they are briefly classified into four type structures-Distribution type,Core-shell,Yolk-shell and Rattle type.The structural diversity may always lead to the diversity of application value.In this paper,based on the former research,we designed a novel hollow Pd/MOF microsphere with double shells structure named Void@MOF/ MNPs@MOF,and successfully fabricated two kind structures like this named Void@HKUST-1/Pd@ZIF-8 and Void@ZIF-8/Pd@ZIF-8 and studied the catalytic size-selectivity for the hydrogenation of olefins.There are divided into two parts of main research during my graduate career.For the first part,we choose the sulfonated polystyrene spheres(SPS)as the holding template to support the first inner MOFs shell-HKUST-1.Pd nanoparticles can be embedded in the SPS@HKUST-1 to obtain SPS@HKUST-1/Pd,and the growth of ZIF-8 on HKUST-1 shell will be initiated by the coordination of Zn2+ ions to the carboxylate groups on HKUST-1 shell surfaces to achieve the SPS@HKUST-1/Pd@ZIF-8 nanostructure.At the last,removed the template,the final structure,Void@HKUST-1/Pd@ZIF-8,is attained and studied the catalytic size-selectivity for the hydrogenation of olefins.For the second part,based on the first synthesis path,we changed the inner MOFs shell from the HKUST-1 to ZIF-8 successfully,due to the tedious process for fabricated the HKUST-1,and finally,we obtained the more stable Void@ZIF-8/Pd@ZIF-8 microspheres because of the inherent stability of ZIF-8 crystal and studied its catalytic property of the hydrogenation of styrene.