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Title: Development of Highly Selective Support for CO Hydrogenation to Light Olefins with Partially Passivated Iron Catalysts

Journal Article · · ChemCatChem

To rule out disturbances from water=soluble efficient promoters (e. g., K2O or combination of S/Na), a simplified iron/support catalyst system was employed to investigate novel supports for the catalytic conversion of syngas (CO+H2) to light olefins (FTO). A series of supports with nominal compositions of ZnAl2O4xAl2O3 (x=1, 2, 3) were prepared by coprecipitation and subsequent high temperature calcination at 1200 °C for 24 h to generate partially passivated ZnAl2O4 and Al2O3 phases, through which each formed component of a catalyst may minimize interactions among them and exhibit unique activity. Iron catalysts were prepared by incipient wetness of iron salts over these supports. At a total pressure of ca. 20 bar and a CO conversion of 35 %, a catalyst with a nominal composition of 15 %Fe/85 %(ZnAl2O4 ∙ 3Al2O3) exhibits a surprising C2=-C4= hydrocarbon distribution of 58 %, which reaches a huge increase by almost 100 % in comparison with iron catalysts over regular supports (e. g., carbon, gamma-Al2O3, etc.). This catalyst demonstrates the 1200 °C passivated ZnAl2O4 ∙ 3Al2O3 as probably the most selective support material for iron-based FTO catalysts. At CO conversion of 35 %, the contents of ethylene in C2, propylene in C3, and butylene in C4 products achieve extraordinary values of 82%, 92%, and 91%, respectively.

Research Organization:
Univ. of Connecticut, Storrs, CT (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Natural Science Foundation of China (NSFC)
Grant/Contract Number:
FG02-86ER13622; 21571161
OSTI ID:
1598234
Journal Information:
ChemCatChem, Vol. 11, Issue 14; ISSN 1867-3880
Publisher:
ChemPubSoc EuropeCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 9 works
Citation information provided by
Web of Science

References (45)

Effects of sodium and sulfur on catalytic performance of supported iron catalysts for the Fischer–Tropsch synthesis of lower olefins journal July 2013
Selective conversion of syngas to light olefins journal March 2016
Stability and Reactivity of ϵ−χ−θ Iron Carbide Catalyst Phases in Fischer−Tropsch Synthesis: Controlling μ C journal October 2010
Effect of preparation and operation conditions on the catalytic performance of cobalt-based catalysts for light olefins production journal January 2012
CO activation pathways and the mechanism of Fischer–Tropsch synthesis journal June 2010
Variation Trends of CO Hydrogenation Performance of (Al)–O–(Zn) Supported Cobalt Nanocomposites: Effects of Gradual Doping with Zn–O Lewis Base journal January 2016
Highly Tunable Selectivity for Syngas-Derived Alkenes over Zinc and Sodium-Modulated Fe 5 C 2 Catalyst journal July 2016
Effects of Water Addition on CO Hydrogenation Over Zinc-Containing Spinel-Supported Cobalt Catalyst journal September 2015
N-doped graphene as an electron donor of iron catalysts for CO hydrogenation to light olefins journal January 2015
Status and prospects in higher alcohols synthesis from syngas journal January 2017
Inorganic Synthesis for the Stabilization of Nanoparticles:  Application to Cu/Al 2 O 3 Nanocomposite Materials journal September 2007
Active phase, catalytic activity, and induction period of Fe/zeolite material in nonoxidative aromatization of methane journal June 2016
Fischer–Tropsch synthesis: A review of water effects on the performances of unsupported and supported Co catalysts journal September 2008
Co-based hydrotalcites as new catalysts for the Fischer–Tropsch synthesis process journal March 2014
Characterization of surface species on iron synthesis catalysts by X-ray photoelectron spectroscopy journal June 1988
Direct and Highly Selective Conversion of Synthesis Gas into Lower Olefins: Design of a Bifunctional Catalyst Combining Methanol Synthesis and Carbon-Carbon Coupling journal March 2016
On carbonaceous deposit formation in carbon monoxide hydrogenation on a natural iron catalyst journal February 1999
Effect of Mn on Co/HMS-Mn and Co/SiO2-Mn catalysts for the Fischer-Tropsch reaction journal May 2019
Influences of Al2O3 on the structure and reactive performance of Co/ZnO catalyst journal July 2012
Supported Iron Nanoparticles as Catalysts for Sustainable Production of Lower Olefins journal February 2012
Effect of component interaction on the activity of Co/CuZnO for CO hydrogenation journal January 2012
Effect of reduction and carburization pretreatment on iron catalyst for synthesis of light olefins from CO hydrogenation journal July 2017
Eco-friendly prepared iron-ore-based catalysts for Fischer-Tropsch synthesis journal May 2019
Improved cytotoxicity of paclitaxel loaded in nanosized lipid carriers by intracellular delivery journal January 2015
Coprecipitated Fe/K/spinel nanocomposites for Fischer-Tropsch to lower olefins journal July 2018
The role of electrophilic species in the Fischer–Tropsch reaction journal January 2009
Cobalt nanoparticles confined in carbon matrix for probing the size dependence in Fischer-Tropsch synthesis journal January 2019
Co-Support Compound Formation in Alumina-Supported Cobalt Catalysts journal November 2001
Novel cobalt zinc oxide Fischer–Tropsch catalysts synthesised using supercritical anti-solvent precipitation journal January 2014
Mechanistic pathway for C2+ hydrocarbons over an Fe/K catalyst journal April 2014
Role of Carbon Monoxide in Catalyst Reconstruction for CO Hydrogenation: First-Principles Study of the Composition, Structure, and Stability of Cu/Co(101̅2) as a Function of CO Pressure journal January 2017
Fischer–Tropsch synthesis on Co/ZnO – Two step activation procedure for improved performance journal June 2014
Cobalt carbide nanoprisms for direct production of lower olefins from syngas journal October 2016
Heterogeneous Catalytic Conversion of Dry Syngas to Ethanol and Higher Alcohols on Cu-Based Catalysts journal May 2011
Spatially confined cobalt nanoparticles on zirconium phosphate-modified KIT-6 for an enhanced stability of CO hydrogenation to hydrocarbons journal March 2019
Catalysts for Production of Lower Olefins from Synthesis Gas: A Review journal August 2013
Effect of in-situ sulfur poisoning on zinc-containing spinel-supported cobalt CO hydrogenation catalyst journal March 2016
The effect of cobalt and zinc precursors on Co (10%)/Zn (x%)/TiO2 (x=0, 5) Fischer–Tropsch catalysts journal January 2005
Crystal chemistry of hexaaluminates: β-alumina and magnetoplumbite structures journal November 1989
Modified alumina as catalyst support for cobalt in the Fischer–Tropsch synthesis journal November 2011
Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity (Recommendations 1984) journal January 1985
Heats of chemisorption on promoted iron surfaces and the role of alkali in Fischer-Tropsch synthesis journal October 1969
Fischer–Tropsch synthesis: Group II alkali-earth metal promoted catalysts journal June 2003
Direct and Highly Selective Conversion of Synthesis Gas into Lower Olefins: Design of a Bifunctional Catalyst Combining Methanol Synthesis and Carbon-Carbon Coupling journal March 2016
Highly Tunable Selectivity for Syngas-Derived Alkenes over Zinc and Sodium-Modulated Fe 5 C 2 Catalyst journal July 2016