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Title: Strong electrostatic adsorption of Pt onto SiO2 partially overcoated Al2O3—Towards single atom catalysts

Abstract

It is frequently desired to synthesize supported metal catalysts that consist of very small clusters or single atoms. In this work, we combine strong electrostatic adsorption (SEA) of H2PtCl6 and engineered oxide supports to ultimately produce very small Pt clusters, including a large fraction of single Pt atoms. The supports are synthesized by depositing controlled amounts of SiO2 onto Al2O3 (SiO2@Al2O3) that has been previously grafted with bulky organic templates. After the templates are removed, the oxide supports are largely negatively charged, like SiO2, but have small patches of positively charged Al2O3, derived from the regions previously covered by the template. The overall point of zero charge of these materials decreases from pH 6.4 for 1 cycle of SiO2 deposition to a SiO2-like <2 for materials with more than 5 cycles of SiO2 deposition. SEA at pH 4 on templated SiO2@Al2O3 deposits from 1 wt. % to 0.05 wt. % Pt as the amount of SiO2 increases. Pt loadings drop to near zero in the absence of a template. The resulting Pt nanoparticles are generally <1 nm and have dispersion near 100% by CO chemisorption. Finally, CO DRIFTS shows that the CO nanoparticles become increasingly well defined and have amore » higher percentage of Pt single atoms as the amount of SiO2 increases on the SiO2@Al2O3 particles. Overall, this method of synthesizing patches of charge on a carrier particle appears to be a viable route to creating extremely highly dispersed supported metal catalysts.« less

Authors:
 [1];  [1];  [1]; ORCiD logo [1];  [2]; ORCiD logo [1]
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  1. Northwestern Univ., Evanston, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1870987
Alternate Identifier(s):
OSTI ID: 1577020
Grant/Contract Number:  
FG02-03ER15457
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 21; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Bo, Zhenyu, McCullough, Lauren R., Dull, Samuel, Ardagh, M. Alexander, Wang, Jie, and Notestein, Justin. Strong electrostatic adsorption of Pt onto SiO2 partially overcoated Al2O3—Towards single atom catalysts. United States: N. p., 2019. Web. doi:10.1063/1.5128934.
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Bo, Zhenyu, McCullough, Lauren R., Dull, Samuel, Ardagh, M. Alexander, Wang, Jie, & Notestein, Justin. Strong electrostatic adsorption of Pt onto SiO2 partially overcoated Al2O3—Towards single atom catalysts. United States. https://doi.org/10.1063/1.5128934
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Bo, Zhenyu, McCullough, Lauren R., Dull, Samuel, Ardagh, M. Alexander, Wang, Jie, and Notestein, Justin. Sat . "Strong electrostatic adsorption of Pt onto SiO2 partially overcoated Al2O3—Towards single atom catalysts". United States. https://doi.org/10.1063/1.5128934. https://www.osti.gov/servlets/purl/1870987.
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@article{osti_1870987,
title = {Strong electrostatic adsorption of Pt onto SiO2 partially overcoated Al2O3—Towards single atom catalysts},
author = {Bo, Zhenyu and McCullough, Lauren R. and Dull, Samuel and Ardagh, M. Alexander and Wang, Jie and Notestein, Justin},
abstractNote = {It is frequently desired to synthesize supported metal catalysts that consist of very small clusters or single atoms. In this work, we combine strong electrostatic adsorption (SEA) of H2PtCl6 and engineered oxide supports to ultimately produce very small Pt clusters, including a large fraction of single Pt atoms. The supports are synthesized by depositing controlled amounts of SiO2 onto Al2O3 (SiO2@Al2O3) that has been previously grafted with bulky organic templates. After the templates are removed, the oxide supports are largely negatively charged, like SiO2, but have small patches of positively charged Al2O3, derived from the regions previously covered by the template. The overall point of zero charge of these materials decreases from pH 6.4 for 1 cycle of SiO2 deposition to a SiO2-like <2 for materials with more than 5 cycles of SiO2 deposition. SEA at pH 4 on templated SiO2@Al2O3 deposits from 1 wt. % to 0.05 wt. % Pt as the amount of SiO2 increases. Pt loadings drop to near zero in the absence of a template. The resulting Pt nanoparticles are generally <1 nm and have dispersion near 100% by CO chemisorption. Finally, CO DRIFTS shows that the CO nanoparticles become increasingly well defined and have a higher percentage of Pt single atoms as the amount of SiO2 increases on the SiO2@Al2O3 particles. Overall, this method of synthesizing patches of charge on a carrier particle appears to be a viable route to creating extremely highly dispersed supported metal catalysts.},
doi = {10.1063/1.5128934},
journal = {Journal of Chemical Physics},
number = 21,
volume = 151,
place = {United States},
year = {Sat Dec 07 00:00:00 EST 2019},
month = {Sat Dec 07 00:00:00 EST 2019}
}
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https://doi.org/10.1063/1.5128934
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