Reduction of Propanoic Acid over Pd-Promoted Supported WOx 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 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.
- Authors:
-
- Univ. of Virginia, Charlottesville, VA (United States)
- 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). Chemical Sciences, Geosciences, and 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.
Kammert, James D., Brezicki, Gordon, Miyake, Naomi, Stavitski, Eli, & Davis, Robert J. Reduction of Propanoic Acid over Pd-Promoted Supported WOx Catalysts. United States. https://doi.org/10.1002/cctc.201901302
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. https://doi.org/10.1002/cctc.201901302. https://www.osti.gov/servlets/purl/1579487.
@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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Works referenced in this record:
Beyond Petrochemicals: The Renewable Chemicals Industry
journal, October 2011
- Vennestrøm, P. N. R.; Osmundsen, C. M.; Christensen, C. H.
- Angewandte Chemie International Edition, Vol. 50, Issue 45
Nach der Petrochemie: eine chemische Industrie auf der Basis erneuerbarer Ressourcen
journal, October 2011
- Vennestrøm, P. N. R.; Osmundsen, C. M.; Christensen, C. H.
- Angewandte Chemie, Vol. 123, Issue 45
Technology development for the production of biobased products from biorefinery carbohydrates—the US Department of Energy’s “Top 10” revisited
journal, January 2010
- Bozell, Joseph J.; Petersen, Gene R.
- Green Chemistry, Vol. 12, Issue 4, p. 539-554
The Catalytic Hydrogenation of Organic Compounds over Copper Chromite
journal, March 1931
- Adkins, Homer.; Connor, Ralph.
- Journal of the American Chemical Society, Vol. 53, Issue 3
Hydrogenolysis of Esters, Particularly Perfluorinated Esters
journal, June 1965
- Yan, T. Y.; Albright, L. F.; Case, L. C.
- Industrial & Engineering Chemistry Product Research and Development, Vol. 4, Issue 2
Structural and reactivity effects in the copper-catalyzed hydrogenolysis of aliphatic esters
journal, July 1984
- Evans, J.
- Journal of Catalysis, Vol. 88, Issue 1
Catalytic Reduction of Acetic Acid, Methyl Acetate, and Ethyl Acetate over Silica-Supported Copper
journal, July 2000
- Santiago, M. A. Natal; Sánchez-Castillo, M. A.; Cortright, R. D.
- Journal of Catalysis, Vol. 193, Issue 1
Rhenium and its Compounds as Hydrogenation Catalysts
journal, October 1967
- Broadbent, H. Smith
- Annals of the New York Academy of Sciences, Vol. 145, Issue 1 Catalytic Hyd
Hydrogenation of Carboxylic Acids and Synergistic Catalysts
journal, January 1981
- Trivedi, Bhupendra C.; Grote, Dace; Mason, Thomas O.
- Journal of the American Oil Chemists' Society, Vol. 58, Issue 1
Liquid phase hydrogenation of carboxylic acid catalyzed by supported bimetallic RuSnalumina catalyst: effects of tin compounds in impregnation method
journal, July 1996
- Tahara, Katsuhiko; Nagahara, Eiji; Itoi, Yasushi
- Journal of Molecular Catalysis A: Chemical, Vol. 110, Issue 1
Aqueous-phase hydrodeoxygenation of propanoic acid over the Ru/ZrO2 and Ru–Mo/ZrO2 catalysts
journal, January 2012
- Chen, Lungang; Zhu, Yulei; Zheng, Hongyan
- Applied Catalysis A: General, Vol. 411-412
Heterogeneous and homogeneous catalysis for the hydrogenation of carboxylic acid derivatives: history, advances and future directions
journal, January 2015
- Pritchard, James; Filonenko, Georgy A.; van Putten, Robbert
- Chemical Society Reviews, Vol. 44, Issue 11
Isomerization and disproportionation of olefins over tungsten oxides supported on various oxides
journal, October 1980
- Yamaguchi, T.
- Journal of Catalysis, Vol. 65, Issue 2
Synthesis of Solid Superacid of Molybdenum Oxide Supported on Zirconia and Its Catalytic Action
journal, June 1989
- Hino, Makoto; Arata, Kazushi
- Chemistry Letters, Vol. 18, Issue 6
Isotopic and Chemical Titration of Acid Sites in Tungsten Oxide Domains Supported on Zirconia
journal, February 2001
- Baertsch, Chelsey D.; Soled, Stuart L.; Iglesia, Enrique
- The Journal of Physical Chemistry B, Vol. 105, Issue 7
Relating n -Pentane Isomerization Activity to the Tungsten Surface Density of WO x /ZrO 2
journal, September 2010
- Soultanidis, Nikolaos; Zhou, Wu; Psarras, Antonis C.
- Journal of the American Chemical Society, Vol. 132, Issue 38
Synthesis, characterization, and catalytic function of novel highly dispersed tungsten oxide catalysts on mesoporous silica
journal, April 2006
- Herrera, J.; Kwak, J.; Hu, J.
- Journal of Catalysis, Vol. 239, Issue 1
Structure and Electronic Properties of Solid Acids Based on Tungsten Oxide Nanostructures
journal, January 1999
- Barton, David G.; Shtein, Max; Wilson, Ryan D.
- The Journal of Physical Chemistry B, Vol. 103, Issue 4
Genesis of Brønsted Acid Sites during Dehydration of 2-Butanol on Tungsten Oxide Catalysts
journal, January 2002
- Baertsch, Chelsey D.; Komala, Kenny T.; Chua, Yong-Hwee
- Journal of Catalysis, Vol. 205, Issue 1
New insights into the nature of the acidic catalytic active sites present in ZrO2-supported tungsten oxide catalysts
journal, May 2008
- Rossmedgaarden, E.; Knowles, W.; Kim, T.
- Journal of Catalysis, Vol. 256, Issue 1
Heteropoly Acids and Related Compounds as Catalysts for Fine Chemical Synthesis
journal, May 1995
- Kozhevnikov, Ivan V.
- Catalysis Reviews, Vol. 37, Issue 2
Heterogeneous Catalysis by Heteropoly Compounds of Molybdenum and Tungsten
journal, June 1987
- Misono, Makoto
- Catalysis Reviews, Vol. 29, Issue 2-3
Heteropoly acids as efficient acid catalysts in the one-step conversion of cellulose to sugar alcohols
journal, January 2011
- Palkovits, Regina; Tajvidi, Kameh; Ruppert, Agnieszka M.
- Chem. Commun., Vol. 47, Issue 1
Esterification by solid acid catalysts—a comparison
journal, December 2004
- Shanmugam, S.; Viswanathan, B.; Varadarajan, T. K.
- Journal of Molecular Catalysis A: Chemical, Vol. 223, Issue 1-2
Effect of water on silica-supported phosphotungstic acid catalysts for 1-butene double bond shift and alkane skeletal isomerization
journal, August 2000
- Bardin, Billy B.; Davis, Robert J.
- Applied Catalysis A: General, Vol. 200, Issue 1-2
Carboxylic acid reductase: a new tungsten enzyme catalyses the reduction of non-activated carboxylic acids to aldehydes
journal, September 1989
- White, Hiltrud; Strobl, Gerd; Feicht, Richard
- European Journal of Biochemistry, Vol. 184, Issue 1
Reactions of Carboxylic Acids on Oxides
journal, June 1997
- Pestman, R.; Koster, R. M.; Pieterse, J. A. Z.
- Journal of Catalysis, Vol. 168, Issue 2
Tungsten-Based Catalysts for Selective Deoxygenation
journal, April 2013
- Gosselink, Robert W.; Stellwagen, Daniel R.; Bitter, Johannes H.
- Angewandte Chemie International Edition, Vol. 52, Issue 19
Comparison of Tungsten and Molybdenum Carbide Catalysts for the Hydrodeoxygenation of Oleic Acid
journal, November 2013
- Hollak, Stefan A. W.; Gosselink, Robert W.; van Es, Daan S.
- ACS Catalysis, Vol. 3, Issue 12
Hydrogenation of succinic acid to tetrahydrofuran (THF) over ruthenium–carbon composite (Ru–C) catalyst
journal, January 2014
- Hong, Ung Gi; Kim, Jeong Kwon; Lee, Joongwon
- Applied Catalysis A: General, Vol. 469
Promoting effect of WOx on selective hydrogenolysis of glycerol to 1,3-propanediol over bifunctional Pt–WOx/Al2O3 catalysts
journal, March 2015
- Zhu, Shanhui; Gao, Xiaoqing; Zhu, Yulei
- Journal of Molecular Catalysis A: Chemical, Vol. 398
SiO2 promoted Pt/WOx/ZrO2 catalysts for the selective hydrogenolysis of glycerol to 1,3-propanediol
journal, October 2014
- Zhu, Shanhui; Gao, Xiaoqing; Zhu, Yulei
- Applied Catalysis B: Environmental, Vol. 158-159
Metabolic engineering of Escherichia coli for efficient free fatty acid production from glycerol
journal, September 2014
- Wu, Hui; Karanjikar, Mukund; San, Ka-Yiu
- Metabolic Engineering, Vol. 25
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005
- Ravel, B.; Newville, M.
- Journal of Synchrotron Radiation, Vol. 12, Issue 4
Kubelka-Munk Theory and the Prediction of Reflectance
journal, June 1985
- Nobbs, James H.
- Review of Progress in Coloration and Related Topics, Vol. 15, Issue 1
Cesium exchanged heteropoly tungstate supported on zirconia as an efficient and selective catalyst for the preparation of unsymmetrical ethers
journal, May 2009
- Venkateswara Rao, K. T.; Rao, P. S. N.; Sai Prasad, P. S.
- Catalysis Communications, Vol. 10, Issue 10
Selective hydrogenation of fatty acids to alcohols over highly dispersed ReO /TiO2 catalyst
journal, August 2015
- Rozmysłowicz, Bartosz; Kirilin, Alexey; Aho, Atte
- Journal of Catalysis, Vol. 328
Strong metal-support interactions. Group 8 noble metals supported on titanium dioxide
journal, January 1978
- Tauster, S. J.; Fung, S. C.; Garten, R. L.
- Journal of the American Chemical Society, Vol. 100, Issue 1
Chemisorption and disproportionation of carbon monoxide on palladium/silica catalysts of differing percentage metal exposed
journal, January 1987
- Joyal, Cheryl L. M.; Butt, John B.
- Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 83, Issue 9
XAFS Study of Tungsten L 1 - and L 3 -Edges: Structural Analysis of WO 3 Species Loaded on TiO 2 as a Catalyst for Photo-oxidation of NH 3
journal, May 2008
- Yamazoe, Seiji; Hitomi, Yutaka; Shishido, Tetsuya
- The Journal of Physical Chemistry C, Vol. 112, Issue 17
X-ray absorption spectroscopy study of the titania- and alumina-supported tungsten oxide system
journal, September 1991
- Hilbrig, Frank; Goebel, Herbert E.; Knoezinger, Helmut
- The Journal of Physical Chemistry, Vol. 95, Issue 18
Structure of surface tungsten oxide species in the tungsten trioxide/alumina supported oxide system from x-ray absorption near-edge spectroscopy and Raman spectroscopy
journal, July 1987
- Horsley, J. A.; Wachs, I. E.; Brown, J. M.
- The Journal of Physical Chemistry, Vol. 91, Issue 15
Estimation of mean size and shape of small metal particles by EXAFS
journal, January 1999
- Jentys, Andreas
- Physical Chemistry Chemical Physics, Vol. 1, Issue 17
Anomalous isotope effect in the H bonds of acetic acid dimers
journal, November 1973
- Bournay, Jacques; Marechal, Yves
- The Journal of Chemical Physics, Vol. 59, Issue 9
Infrared spectroscopic studies of adsorption and catalysis. Part 3. Carboxylic acids and their derivatives adsorbed on silica
journal, June 1969
- Young, R. P.
- Canadian Journal of Chemistry, Vol. 47, Issue 12
Heterogeneous chemistry of monocarboxylic acids on α-Al 2 O 3 at different relative humidities
journal, January 2010
- Tong, S. R.; Wu, L. Y.; Ge, M. F.
- Atmospheric Chemistry and Physics, Vol. 10, Issue 16
Reactions of Acetaldehyde on CeO2 and CeO2-Supported Catalysts
journal, September 1995
- Idriss, H.; Diagne, C.; Hindermann, J. P.
- Journal of Catalysis, Vol. 155, Issue 2
FT-IR and TPD studies on support-metal and promoter-metal interaction. Pt and Pd catalysts
journal, January 1991
- Boujana, S.; Demri, D.; Cressely, J.
- Catalysis Letters, Vol. 7, Issue 5-6
Acetic Acid Reduction by H2 over Supported Pt Catalysts: A DRIFTS and TPD/TPR Study
journal, April 2002
- Rachmady, Willy; Vannice, M. Albert
- Journal of Catalysis, Vol. 207, Issue 2
Reduction of Propionic Acid over a Pd-Promoted ReO x /SiO 2 Catalyst Probed by X-ray Absorption Spectroscopy and Transient Kinetic Analysis
journal, July 2018
- Kammert, James D.; Xie, Jiahan; Godfrey, Ian J.
- ACS Sustainable Chemistry & Engineering, Vol. 6, Issue 9
Acetic acid hydrogenation over supported platinum catalysts
journal, June 2000
- Rachmady, W.; Vannice, M.
- Journal of Catalysis, Vol. 192, Issue 2
Selective hydrogenation of higher saturated carboxylic acids to alcohols using a ReOx–Pd/SiO2 catalyst
journal, January 2012
- Takeda, Yasuyuki; Nakagawa, Yoshinao; Tomishige, Keiichi
- Catalysis Science & Technology, Vol. 2, Issue 11
Characterization of Re–Pd/SiO 2 Catalysts for Hydrogenation of Stearic Acid
journal, October 2015
- Takeda, Yasuyuki; Tamura, Masazumi; Nakagawa, Yoshinao
- ACS Catalysis, Vol. 5, Issue 11
Aqueous-Phase Hydrogenation of Biomass-Based Succinic Acid to 1,4-Butanediol Over Supported Bimetallic Catalysts
journal, May 2010
- Minh, Doan Pham; Besson, Michèle; Pinel, Catherine
- Topics in Catalysis, Vol. 53, Issue 15-18
Evaluation of Pt and Re oxidation state in a pressurized reactor: difference in reduction between gas and liquid phase
journal, January 2011
- Sá, Jacinto; Kartusch, Christiane; Makosch, Martin
- Chemical Communications, Vol. 47, Issue 23
Effect of Addition Mode of Re in Bimetallic Pd–Re/TiO2 Catalysts Upon the Selective Aqueous-Phase Hydrogenation of Succinic Acid to 1,4-Butanediol
journal, June 2012
- Ly, Bao Khanh; Minh, Doan Pham; Pinel, Catherine
- Topics in Catalysis, Vol. 55, Issue 7-10
Platinum-Like Behavior of Tungsten Carbide in Surface Catalysis
journal, August 1973
- Levy, R. B.; Boudart, M.
- Science, Vol. 181, Issue 4099
Thermochemistry of hydrogen tungsten bronze phases HxWO3
journal, June 1973
- Dickens, P. G.; Moore, J. H.; Neild, D. J.
- Journal of Solid State Chemistry, Vol. 7, Issue 2
Experimental and theoretical assessment of the mechanism and site requirements for ketonization of carboxylic acids on oxides
journal, January 2017
- Wang, Shuai; Iglesia, Enrique
- Journal of Catalysis, Vol. 345
Reaction Paths in the Hydrogenolysis of Acetic Acid to Ethanol over Pd(111), Re(0001), and PdRe Alloys
journal, July 2002
- Pallassana, Venkataraman; Neurock, Matthew
- Journal of Catalysis, Vol. 209, Issue 2
On the reduction of tungsten trioxide accelerated by platinum and water
journal, April 1966
- Benson, J.; Kohn, H.; Boudart, M.
- Journal of Catalysis, Vol. 5, Issue 2