Recently, the catalysts with metal nanoparticles supported on MOFs have attracted increased interest due to the adjustable structure and function and the high surface area of MOFs. Immobilization of metal nanoparticles on the functional groups of MOF supports has become a particular focus, but it is still a great challenge to synthesize in situ carboxyl-functionalized MOFs. To the best of our knowledge, there has been no report on the in situ construction of free carboxyl groups in the ligand of conventional MOFs for anchoring metal nanoparticles.<br/>We proposed a novel strategy for producing highly dispersed Pd particles on ZIF-8 via the anchoring effect of the carboxyl groups incorporated into the ligand of ZIF-8. The conventional ZIF-8 was firstly functionalized in situ by carboxyl groups incorporated in the ligand of ZIF-8. These carboxyl groups were then occupied via their interaction with cetyltrimethylammonium bromide (CTAB) during the formation of the ZIF-8 framework and subsequently freed by the removal of CTAB. These free carboxyl groups interacted with Pd nanoparticles, guaranteeing the high dispersion of Pd nanoparticles on the FZIF-8. The selective hydrogenation of dienes was selected as a model reaction to demonstrate the advantage of the as-synthesized catalyst because of the importance of this reaction in improving the gasoline quality through removing unstable dienes and preserving the octane number. The as-synthesized Pd nanoparticles supported on the in situ carboxyl-functionalized ZIF-8 showed excellent activity and selectivity for diene hydrogenation due to the high dispersion of Pd nanoparticles and the interaction between the Pd nanoparticles and carboxyl groups. This method opens a new and simple route for greatly improving the dispersion of supported Pd nanoparticles.

Novel strategy for producing highly dispersed Pd particles on ZIF-8 through the occupation and unoccupation of carboxyl groups and its application in selective diene hydrogenation

251st National Meeting (2016)

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