Controlling Catalytic Properties of Pd Nanoclusters through Their Chemical Environment at the Atomic Level Using Isoreticular Metal–Organic Frameworks

Li, Xinle; Goh, Tian Wei; Li, Lei; Xiao, Chaoxian; Guo, Zhiyong; Zeng, Xiao Cheng; Huang, Wenyu

doi:10.1021/acscatal.6b00397

Controlling Catalytic Properties of Pd Nanoclusters through Their Chemical Environment at the Atomic Level Using Isoreticular Metal–Organic Frameworks

Journal Article · Tue Apr 12 00:00:00 EDT 2016 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.6b00397· OSTI ID:1255289

Li, Xinle ^[1]; Goh, Tian Wei ^[1]; Li, Lei ^[2]; Xiao, Chaoxian ^[1]; Guo, Zhiyong ^[1]; Zeng, Xiao Cheng ^[2]; Huang, Wenyu ^[1]

Iowa State Univ., Ames, IA (United States); Ames Lab., Ames, IA (United States)
Univ. of Nebraska, Lincoln, NE (United States)

Control of heterogeneous catalytic sites through their surrounding chemical environment at an atomic level is crucial to catalyst design. Here we synthesize Pd nanoclusters (NCs) in an atomically tunable chemical environment using isoreticular metal–organic framework (MOF) supports (Pd@UiO-66-X, X = H, NH₂, OMe). In an aerobic reaction between benzaldehyde and ethylene glycol, these catalysts show product distributions that are completely altered from the acetal to the ester when we change the functional groups on the MOF linkers from –NH₂ to –H/–OMe. Diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) studies, along with density functional theory (DFT) calculations, show that the coordination of the –NH₂ groups to the Pd NCs could weaken their oxidation capability to a greater extent in comparison to that of the –OMe group. Moreover, the limited number of –NH₂ groups per cavity in the MOF change the electronic properties of the Pd NCs while still leaving open sites for catalysis.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; AC02-07CH11358

OSTI ID:: 1255289

Alternate ID(s):: OSTI ID: 1321918

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 6 Vol. 6; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Catalysts
Metal organic frameworks
Organic compounds
Oxidation
Palladium

Controlling Catalytic Properties of Pd Nanoclusters through Their Chemical Environment at the Atomic Level Using Isoreticular Metal–Organic Frameworks

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