Aerobic oxidative esterification of primary alcohols over Pd-Au bimetallic catalysts supported on mesoporous silica nanoparticles

Tsai, Chih-Hsiang; Xu, Mengze; Kunal, Pranaw; Trewyn, Brian G.

doi:10.1016/j.cattod.2017.01.046

Aerobic oxidative esterification of primary alcohols over Pd-Au bimetallic catalysts supported on mesoporous silica nanoparticles

Journal Article · Wed Feb 08 00:00:00 EST 2017 · Catalysis Today

DOI:https://doi.org/10.1016/j.cattod.2017.01.046· OSTI ID:1538063

Tsai, Chih-Hsiang ^[1]; Xu, Mengze ^[2]; Kunal, Pranaw ^[2]; Trewyn, Brian G. ^[3]

Iowa State University, Ames, IA (United States); DOE/OSTI
Colorado School of Mines, Golden, CO (United States)
Iowa State University, Ames, IA (United States); Colorado School of Mines, Golden, CO (United States)

Here we have prepared a series of mesoporous silica nanoparticle (MSN) supported Pd-Au bimetallic catalysts using a newly developed sequential impregnation method. These catalysts were fully characterized by various techniques including nitrogen sorption, powder X-ray diffraction, inductively coupled plasma mass spectrometry (ICP-MS), transmission electron microscopy (TEM) and high angle annular dark-field scanning transmission electron microscopy (HADDF-STEM). By using this synthetic approach, we observed metal nanoparticles (NP) with diameters of 1–2 nm homogeneously supported on the MSN. The catalytic performance of these MSN supported metal NPs was tested by aerobic oxidative esterification in a tandem reaction where primary alcohols are oxidized to their corresponding aldehydes and to esters in a subsequent reaction. We determined that Pd NPs are very efficient in the first step of oxidation; however, stagnant in the subsequent oxidation. On the contrary, Au NPs show slow reactivity in converting alcohols to aldehydes, but extraordinarily efficient in the oxidation of aldehydes to esters. By fine tuning the metal ratio, the bimetallic catalyst exhibits better reactivity and selectivity toward a variety of primary alcohols than the corresponding monometallic catalysts. In addition, we also found that the bimetallic Pd-Au@MSN catalysts can be recycled three times without a significant loss in activity.

View Accepted Manuscript (DOE)

Research Organization:: Colorado School of Mines, Golden, CO (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Catalytic Hydrocarbon Functionalization (CCHF); University of Virginia, Charlottesville, VA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: SC0001298

OSTI ID:: 1538063

Alternate ID(s):: OSTI ID: 1496322

Journal Information:: Catalysis Today, Journal Name: Catalysis Today Journal Issue: C Vol. 306; ISSN 0920-5861

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
bimetallic catalysis
mesoporous silica nanoparticles
oxidative esterification
tandem catalysis

Aerobic oxidative esterification of primary alcohols over Pd-Au bimetallic catalysts supported on mesoporous silica nanoparticles

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