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

Abstract

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, Al 2O 3, and CeO 2. 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 Al 2O 3 and CeO 2, 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.

Authors:
 [1];  [2];  [1]
  1. Indiana Univ., Bloomington, IN (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1472130
Alternate Identifier(s):
OSTI ID: 1495267
Grant/Contract Number:  
AC02-06CH11357; SC0016367
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 365; Journal Issue: C; Journal ID: ISSN 0021-9517
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Pt catalyst; hydrosilylation catalysis; metal-ligand self-assembly; oxide support; single-site catalyst; x-ray absorption spectroscopy

Citation Formats

Chen, Linxiao, Sterbinsky, George E., and Tait, Steven L. Synthesis of platinum single-site centers through metal-ligand self-assembly on powdered metal oxide supports. United States: N. p., 2018. Web. doi:10.1016/j.jcat.2018.07.004.
Chen, Linxiao, Sterbinsky, George E., & Tait, Steven L. Synthesis of platinum single-site centers through metal-ligand self-assembly on powdered metal oxide supports. United States. doi:10.1016/j.jcat.2018.07.004.
Chen, Linxiao, Sterbinsky, George E., and Tait, Steven L. Sat . "Synthesis of platinum single-site centers through metal-ligand self-assembly on powdered metal oxide supports". United States. doi:10.1016/j.jcat.2018.07.004. https://www.osti.gov/servlets/purl/1472130.
@article{osti_1472130,
title = {Synthesis of platinum single-site centers through metal-ligand self-assembly on powdered metal oxide supports},
author = {Chen, Linxiao and Sterbinsky, George E. and Tait, Steven L.},
abstractNote = {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.},
doi = {10.1016/j.jcat.2018.07.004},
journal = {Journal of Catalysis},
issn = {0021-9517},
number = C,
volume = 365,
place = {United States},
year = {2018},
month = {7}
}

Journal Article:
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