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Title: Reduction of Propanoic Acid over Pd-Promoted Supported WO x Catalysts

Abstract

Here, silica-, titania-, and zirconia-supported tungsten oxide catalysts were synthesized by wetness impregnation techniques. When promoted with Pd, these materials catalyzed the reduction of propanoic acid to 1-propanol at 433 K with a selectivity of up to 92% (13.5% conversion) in atmospheric pressure of H 2. Over Pd-promoted WO x/TiO 2, the observed orders of reaction were 0.2 in H 2 and 0.7 in propanoic acid, and the apparent activation energy was 54 kJ mol –1. In situ X-ray absorption spectroscopy of Pd-promoted WO x/SiO 2 revealed a slight reduction of the W from +6 to an average oxidation state of about +5 during H 2 treatment above 473 K. In situ infrared spectroscopy indicated the catalyst surface was covered mostly by propanoate species during reaction. For comparison, supported phosphotungstic acid was also evaluated as a catalyst under identical conditions, yet the resulting high acidity of the catalyst was deleterious to alcohol selectivity.

Authors:
 [1];  [1];  [1];  [2];  [1]
+ Show Author Affiliations
  1. Univ. of Virginia, Charlottesville, VA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)
OSTI Identifier:
1579487
Report Number(s):
BNL-212379-2019-JAAM
Journal ID: ISSN 1867-3880
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
ChemCatChem
Additional Journal Information:
Journal Volume: 11; Journal ID: ISSN 1867-3880
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Carboxylic acids; infrared spectroscopy; reduction; tungsten; X-ray absorption spectroscopy

Citation Formats

Kammert, James D., Brezicki, Gordon, Miyake, Naomi, Stavitski, Eli, and Davis, Robert J. Reduction of Propanoic Acid over Pd-Promoted Supported WOx Catalysts. United States: N. p., 2019. Web. doi:10.1002/cctc.201901302.
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Kammert, James D., Brezicki, Gordon, Miyake, Naomi, Stavitski, Eli, & Davis, Robert J. Reduction of Propanoic Acid over Pd-Promoted Supported WOx Catalysts. United States. doi:10.1002/cctc.201901302.
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Kammert, James D., Brezicki, Gordon, Miyake, Naomi, Stavitski, Eli, and Davis, Robert J. Mon . "Reduction of Propanoic Acid over Pd-Promoted Supported WOx Catalysts". United States. doi:10.1002/cctc.201901302.
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@article{osti_1579487,
title = {Reduction of Propanoic Acid over Pd-Promoted Supported WOx Catalysts},
author = {Kammert, James D. and Brezicki, Gordon and Miyake, Naomi and Stavitski, Eli and Davis, Robert J.},
abstractNote = {Here, silica-, titania-, and zirconia-supported tungsten oxide catalysts were synthesized by wetness impregnation techniques. When promoted with Pd, these materials catalyzed the reduction of propanoic acid to 1-propanol at 433 K with a selectivity of up to 92% (13.5% conversion) in atmospheric pressure of H2. Over Pd-promoted WOx/TiO2, the observed orders of reaction were 0.2 in H2 and 0.7 in propanoic acid, and the apparent activation energy was 54 kJ mol–1. In situ X-ray absorption spectroscopy of Pd-promoted WOx/SiO2 revealed a slight reduction of the W from +6 to an average oxidation state of about +5 during H2 treatment above 473 K. In situ infrared spectroscopy indicated the catalyst surface was covered mostly by propanoate species during reaction. For comparison, supported phosphotungstic acid was also evaluated as a catalyst under identical conditions, yet the resulting high acidity of the catalyst was deleterious to alcohol selectivity.},
doi = {10.1002/cctc.201901302},
journal = {ChemCatChem},
number = ,
volume = 11,
place = {United States},
year = {2019},
month = {9}
}
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DOI:  10.1002/cctc.201901302
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