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Direct Catalytic Conversion of Ethanol to C5+ Ketones: Role of Pd-Zn Alloy on Catalytic Activity and Stability

Journal Article · · Angewandte Chemie International Edition

Ethanol can be used as a platform molecule for synthesizing valuable chemicals and fuel precursors. Direct synthesis of C5+ ketones, building block for lubricants and hydrocarbon fuels, from ethanol was achieved over a stable Pd-promoted ZnO-ZrO2 catalyst. The sequence of reaction steps involved in the C5+ ketone formation from ethanol and the key reaction step was found to be the in situ generation of the acetone intermediate and the cross aldol condensation between the reaction intermediates acetaldehyde and acetone. The formation of Pd-Zn alloy in situ at the reaction condition was identified to be the key factor in maintaining high yield to the C5+ ketones and the stability to the catalyst. The yield of >70% to C5+ ketones was achieved over a 0.1%Pd-ZnO-ZrO2 mixed oxide catalyst, and the catalyst was demonstrated to be stable beyond 2500 hours on stream without any catalyst deactivation.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1647347
Report Number(s):
PNNL-SA-148910
Journal Information:
Angewandte Chemie International Edition, Journal Name: Angewandte Chemie International Edition Journal Issue: 34 Vol. 59
Country of Publication:
United States
Language:
English

References (29)

Particle Size Effect of Hydride Formation and Surface Hydrogen Adsorption of Nanosized Palladium Catalysts: L 3 Edge vs K Edge X-ray Absorption Spectroscopy journal July 2009
Selective production of phase-separable product from a mixture of biomass-derived aqueous oxygenates journal December 2018
New Insights into the Nature of Co-components and Their Impact on Pd Structure: X-ray Absorption Studies on Toluene Acetoxylation Catalysts journal September 2015
In situ intermediate-energy X-ray catalysis research at the advanced photon source beamline 9-BM journal April 2013
Hybrid Biological–Chemical Approach Offers Flexibility and Reduces the Carbon Footprint of Biobased Plastics, Rubbers, and Fuels journal October 2018
Ethanol reforming processes over ZnO-supported palladium catalysts: Effect of alloy formation journal May 2006
Ethanol from biomass: A comparative overview journal December 2017
A study of ZnxZryOz mixed oxides for direct conversion of ethanol to isobutene journal October 2013
Comparative techno‐economic analysis and process design for indirect liquefaction pathways to distillate‐range fuels via biomass‐derived oxygenated intermediates upgrading journal September 2016
Polymerization and decarbonylation reactions of aldehydes on the Pd(111) surface journal March 1989
Conversion of syngas-derived C2+ mixed oxygenates to C3–C5 olefins over ZnxZryOz mixed oxide catalysts journal January 2016
Selective Catalytic Hydrogenolysis of Carbon–Carbon σ Bonds in Primary Aliphatic Alcohols over Supported Metals journal November 2015
Novel pathways for fuels and lubricants from biomass optimized using life-cycle greenhouse gas assessment journal June 2015
Aldol Condensation of Acetaldehyde over Titania, Hydroxyapatite, and Magnesia journal April 2016
Structural identification of ZnxZryOz catalysts for Cascade aldolization and self-deoxygenation reactions journal October 2018
PdZn Intermetallic Nanostructure with Pd–Zn–Pd Ensembles for Highly Active and Chemoselective Semi-Hydrogenation of Acetylene journal January 2016
Ethanol as a Renewable Building Block for Fuels and Chemicals journal February 2020
PdZnAl catalysts for the reactions of water-gas-shift, methanol steam reforming, and reverse-water-gas-shift journal June 2008
Integration of chemical catalysis with extractive fermentation to produce fuels journal November 2012
PdZn nanoparticle catalyst formation for ethanol dehydrogenation: Active metal impregnation vs incorporation journal April 2018
Distinct water activation on polar/non-polar facets of ZnO nanoparticles journal November 2015
Direct Conversion of Bio-ethanol to Isobutene on Nanosized Zn x Zr y O z Mixed Oxides with Balanced Acid–Base Sites journal July 2011
X-ray tomography measurements identify structure-reactivity correlations in catalysts for oxygenates coupling reactions journal October 2019
Poisoning and deactivation of palladium catalysts journal September 2001
Synergistic Effects in Bimetallic Palladium–Copper Catalysts Improve Selectivity in Oxygenate Coupling Reactions journal May 2016
Key Roles of Lewis Acid–Base Pairs on Zn x Zr y O z in Direct Ethanol/Acetone to Isobutene Conversion journal December 2015
Promotion of Pd nanoparticles by Fe and formation of a Pd3Fe intermetallic alloy for propane dehydrogenation journal February 2019
Kinetic and Mechanistic Assessment of Alkanol/Alkanal Decarbonylation and Deoxygenation Pathways on Metal Catalysts journal September 2015
Selectivity tuning over monometallic and bimetallic dehydrogenation catalysts: effects of support and particle size journal January 2018

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