ACS Catalysis
ACS Catalysis
5 years ago

Coupling Molecular and Nanoparticle Catalysts on Single Metal–Organic Framework Microcrystals for the Tandem Reaction of H2O2 Generation and Selective Alkene Oxidation

Coupling Molecular and Nanoparticle Catalysts on Single Metal–Organic Framework Microcrystals for the Tandem Reaction of H2O2 Generation and Selective Alkene Oxidation
Allison P. Young, SonBinh T. Nguyen, Rungmai Limvorapitux, Lien-Yang Chou, Chia-Kuang Tsung
A molecular catalyst, (sal)MoVI, and a heterogeneous catalyst, either Pd or Au nanoparticles (NPs), were integrated into one UiO-66 MOF microcrystal. The resulting dually functionalized catalysts, Pd@UiO-66-(sal)Mo and Au/UiO-66-(sal)Mo, have been utilized for a one-pot tandem reaction of H2O2 generation and selective liquid-phase alkene oxidation. The NPs serve as catalysts for the production of H2O2 from H2 and O2 gases, while the (sal)Mo moieties function as the oxidation catalyst. When the metal NPs are fully encapsulated within the MOF microcrystals, the alkene hydrogenation side reaction is largely suppressed, with a 6-fold decrease in the hydrogenation/oxidation product ratio for 5-bromo-1-cyclooctene favoring the epoxide as the major product. For Au/UiO-66-(sal)Mo, where the two catalysts are in close proximity on the MOF microcrystal, the enhancement in oxidation productivity is increased by 10 times in comparison to the [Au/UiO-66-NH2 + UiO-66-sal(Mo)] physical mixture of the two singly functionalized MOFs.

Publisher URL: http://dx.doi.org/10.1021/acscatal.6b03632

DOI: 10.1021/acscatal.6b03632

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