科研之友
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摘要
A novel three-dimensional lanthanidemetal-organicframework Nd-PMOF was employed herein to photocatalytically oxidizestyrene to benzaldehyde with 91.4% conversion and 81.2% selectivity.The preparation of this lanthanide MOF not only confirms the possibilitythat lanthanide MOFs can be used for photocatalytic applications butalso presents a new scheme for the photocatalytic oxidation of styrene. @@@ A novelthree-dimensional lanthanide porphyrin-based MOF (Nd-PMOFs)was synthesized by using tetracarboxyphenyl porphyrin as the ligandand the lanthanide Nd as the coordination metal. Its specific crystalstructure information was obtained by single-crystal diffraction withthe space group C2/c and the empiricalformula C72H45N6Nd2O15.25. This new Nd porphyrin-based MOF with an organic frameworkformed by a unique coordination method enables the effective separationof photogenerated electrons and holes under photoluminescence, givingit excellent photocatalytic property which could be verified by thecharacterization data. The photocatalytic performance was examinedby taking tert-butyl hydroperoxide as the oxidantand Nd-PMOFs as the catalyst for photocatalytic oxidation of styreneto benzaldehyde with 91.4% conversion and 81.2% benzaldehyde selectivityunder optimal reactions, which surpasses most of the results reportedin the literature. Several styrenes with other substituents were screenedto explore the general applicability of Nd-PMOF for photocatalysisof styrene, among which Nd-PMOFs also exhibited excellent photocatalyticperformance. This work offers the possibility to apply lanthanideorganometallic frameworks, which are widely used in fluorescent materials,to photocatalysis. In addition, it also provides a new method forthe catalytic generation of benzaldehyde from styrene that is consistentwith the needs of modern green development.
