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Title: Phosphate modified ceria as a Brønsted acidic/redox multifunctional catalyst

Abstract

Deposition of trimethylphosphate onto ceria followed by thermal treatment resulted in the formation of surface phosphates with retention of the ceria fluorite structure. The structural and chemical properties of the phosphate-functionalized ceria were studied using 31P solid-state NMR, XPS, zeta titration, ammonia thermal desorption, pyridine adsorption, and model reactions. The introduction of phosphates generated Brønsted acid sites and decreased the number of Lewis acid sites on the surface. The relative amount of Lewis and Brønsted acids can be controlled by the amount of trimethylphosphate used in the synthesis. Upon deposition of Pd, the multifunctional material showed enhanced activity for the hydrogenolysis of eugenol and guaiacol compared to Pd on the unmodified ceria support. As a result, this was attributed to the cooperativity between the Lewis acid sites, which activate the substrate for dearomatization, and the redox/Brønsted acid properties, which catalyze hydrogenolysis.

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Ames Lab. and Iowa State Univ., Ames, IA (United States)
Publication Date:
Research Org.:
Ames Lab., Ames, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1347404
Report Number(s):
IS-J-9220
Journal ID: ISSN 2050-7488; JMCAET
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 5; Journal Issue: 9; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Nelson, Nicholas C., Wang, Zhuoran, Naik, Pranjali, Manzano, J. Sebastian, Pruski, Marek, and Slowing, Igor I.. Phosphate modified ceria as a Brønsted acidic/redox multifunctional catalyst. United States: N. p., 2017. Web. doi:10.1039/C6TA08703E.
Nelson, Nicholas C., Wang, Zhuoran, Naik, Pranjali, Manzano, J. Sebastian, Pruski, Marek, & Slowing, Igor I.. Phosphate modified ceria as a Brønsted acidic/redox multifunctional catalyst. United States. https://doi.org/10.1039/C6TA08703E
Nelson, Nicholas C., Wang, Zhuoran, Naik, Pranjali, Manzano, J. Sebastian, Pruski, Marek, and Slowing, Igor I.. Fri . "Phosphate modified ceria as a Brønsted acidic/redox multifunctional catalyst". United States. https://doi.org/10.1039/C6TA08703E. https://www.osti.gov/servlets/purl/1347404.
@article{osti_1347404,
title = {Phosphate modified ceria as a Brønsted acidic/redox multifunctional catalyst},
author = {Nelson, Nicholas C. and Wang, Zhuoran and Naik, Pranjali and Manzano, J. Sebastian and Pruski, Marek and Slowing, Igor I.},
abstractNote = {Deposition of trimethylphosphate onto ceria followed by thermal treatment resulted in the formation of surface phosphates with retention of the ceria fluorite structure. The structural and chemical properties of the phosphate-functionalized ceria were studied using 31P solid-state NMR, XPS, zeta titration, ammonia thermal desorption, pyridine adsorption, and model reactions. The introduction of phosphates generated Brønsted acid sites and decreased the number of Lewis acid sites on the surface. The relative amount of Lewis and Brønsted acids can be controlled by the amount of trimethylphosphate used in the synthesis. Upon deposition of Pd, the multifunctional material showed enhanced activity for the hydrogenolysis of eugenol and guaiacol compared to Pd on the unmodified ceria support. As a result, this was attributed to the cooperativity between the Lewis acid sites, which activate the substrate for dearomatization, and the redox/Brønsted acid properties, which catalyze hydrogenolysis.},
doi = {10.1039/C6TA08703E},
journal = {Journal of Materials Chemistry. A},
number = 9,
volume = 5,
place = {United States},
year = {Fri Jan 06 00:00:00 EST 2017},
month = {Fri Jan 06 00:00:00 EST 2017}
}

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