Synthesis of platinum single-site centers through metal-ligand self-assembly on powdered metal oxide supports

Chen, Linxiao; Sterbinsky, George E.; Tait, Steven L.

doi:10.1016/j.jcat.2018.07.004

Title: Synthesis of platinum single-site centers through metal-ligand self-assembly on powdered metal oxide supports

Journal Article · Sat Jul 21 00:00:00 EDT 2018 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2018.07.004· OSTI ID:1472130

Chen, Linxiao ^[1]; Sterbinsky, George E. ^[2]; Tait, Steven L. ^[1]

Indiana Univ., Bloomington, IN (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Developing single-site metal catalysts has been regarded as a promising strategy to improve activity and selectivity in heterogeneous catalysis. Here, we report a metal-ligand self-assembly method to create Pt single-site centers on powdered oxide supports. Impregnating Pt and a ligand 3,6-di-2-pyridyl-1,2,4,5- tetrazine (DPTZ) simultaneously (one-step) creates Pt-DPTZ single-sites on powdered MgO, Al₂O₃, and CeO₂. MgO has the most uniform single-sites due to a strong, non-competitive support-ligand interaction, and a support-metal interaction of appropriate strength. Pt(II) centers are stabilized between the N binding pockets of DPTZ, with minimal metallic nanoparticle formation. This system was characterized by XAS, XPS, TEM, XRD, and CO adsorption. Sequential impregnation of Pt and DPTZ (two-step) was also tested on Al₂O₃ and CeO₂, but is not as effective as the one-step method due to limited Pt accessibility and mobility. These oxide-supported Pt-DPTZ single-sites were found to be effective catalysts in hydrosilylation reactions. In conclusion, this work demonstrates a metal-ligand self-assembly strategy to create metal singlesite centers on high surface area catalyst supports.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: AC02-06CH11357; SC0016367

OSTI ID:: 1472130

Alternate ID(s):: OSTI ID: 1495267

Journal Information:: Journal of Catalysis, Vol. 365, Issue C; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 21 works

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Title: Synthesis of platinum single-site centers through metal-ligand self-assembly on powdered metal oxide supports

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