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

Limvorapitux, Rungmai; Chou, Lien-Yang; Young, Allison P.; Tsung, Chia-Kuang; Nguyen, SonBinh T.

doi:10.1021/acscatal.6b03632

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

Journal Article · Wed Jul 26 00:00:00 EDT 2017 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.6b03632· OSTI ID:1871005

Limvorapitux, Rungmai ^[1]; Chou, Lien-Yang ^[2]; Young, Allison P. ^[3];

^[3];

^[1]

Northwestern Univ., Evanston, IL (United States)
Boston College, Chestnut Hill, MA (United States); ShanghaiTech Univ. (China)
Boston College, Chestnut Hill, MA (United States)

A molecular catalyst, (sal)Mo^VI, 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. Furthermore, 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.

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Research Organization:: Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Defense Threat Reduction Agency (DTRA); National Science Foundation (NSF); Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource; MRSEC program; NSF NSEC program

Grant/Contract Number:: FG02-03ER15457; SC0001329; NNCI-1542205; DMR-1121262; EEC-0647560

OSTI ID:: 1871005

Journal Information:: ACS Catalysis, Vol. 7, Issue 10; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 28 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
tandem reaction
metal−organic framework
in situ H2O2
generation
alkene oxidation
UiO-66
catalysts
crystals
metal nanoparticles
oxidation

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

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