Ctlti Rf i fL iti dAlt ti F l Catalytic Reforming of ...Catalyst carrier: Monolithic honeycomb or...
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C t l ti Rf i fL i ti d Alt ti F l Helmholtz Research School Energy-Related Catalysis Institute for Chemical Technology and Polymer Chemistry Claudia Diehm [email protected] Catalytic Reforming of Logistic and Alternative Fuels Research Fundamentals Personal Details Name: Claudia Diehm Department: Department of Chemistry and Biosciences Supervisor: Prof. Dr. Olaf Deutschmann Cosupervisor: Prof. Dr.-Ing. Roland Dittmeyer Higher Education: 10/2005 - 08/2010 Karlsruhe Institute of Technology (KIT), Germany Subject: Chemistry Final result: Diplom, outstanding (1.2) Focus: Chemical Technology Efficient power generation for mobile applications by using APUs (Auxiliary Power Unit): Reduction of greenhouse gas emissions and Fuel reformer • CPOX • Steam reforming H 2 + CO Fuel cell • SOFC • PEMFC after gas cleaning Commercial fuel Electricity Diploma thesis Honours and Awards: 10/2009 - 07/2010 Scholarship by “Karlsruher Universitätsgesellschaft e.V.” Catalytic Partial Oxidation of Ethanol blended Fuels on Rh coated Catalyst binary mixtures of ethanol and i-octane as model surrogates Features of catalytic partial oxidation (CPOX) reformers [1] : Reaction equation Catalyst [2] : Catalyst carrier: Monolithic honeycomb or foam structures Washcoat: -Al 2 O 3 Catalytically active metal: Rhodium Reduction of greenhouse gas emissions and lower consumption of limited fossil fuels CO x H 2 y O 2 z - x O H C 2 2 z y x over 80 % hydrogen selectivity for all blends in millisecond contact times maximum hydrogen selectivity shifts to leaner conditions for increasing ethanol concentration avoidance of side-products such as methane, ethylene, and acetaldehyde i i fd t f l ll Catalytically active metal: Rhodium Short residence time High fuel throughput and syngas yields Nearly adiabatically operating compact reactors Suitable for: logistic fuels, e.g. gasoline, and diesel alternative fuels, e.g. bioethanol [3] mixtures of both e g ethanol blended fuels operating catalyst poisoning of downstream fuel cell selectivity to side-products rises with increasing ethanol percentage exception to this trend for 10 vol% ethanol observed properties of ethanol iso-octane blends not solely explicable by the properties of the pure substances interactions between the components during the simultaneous conversion on the catalytic surface mixtures of both, e.g. ethanol blended fuels CPOX reformers are most suitable for on-board hydrogen supply [4] Features of fuel cells [5] : SOFC: Hydrogen and carbon monoxide can be reformed PEMFC: Poisoned by carbon monoxide Both show incompatibility to hydrocarbons [6] PhD thesis Catalyst Development Experimental Setup Properties [1] Well-defined boundary conditions Homogeneous, pulse-free reactant flow uniform temperature profile Analysis of product stream by: FT IR Improvement and optimization of CPOX reformers by: Understanding the complex reaction system in the reformer for different fuels Commercial gasoline Commercial diesel Biofuels Developing alternative catalysts to replace expensive rhodium catalysts References Development Alteration of catalytically active metal along length of monolithic channel Noble metal doped catalysts e.g. perovskite or pyrochlore structures Non-precious metal catalysts e.g. group 6 transition metal carbides Reactor FT-IR MS GC/MS Time-resolved monitoring Approach for every fuel: from model surrogate to commercial fuel One component model surrogate Complex mixtures of hydrocarbons Commercial fuel Catalyst after test-cycle Improvement of the marketability and efficiency of APUs KIT – University of the State of Baden-Wuerttemberg and National Research Center of the Helmholtz Association Contact: Claudia Diehm, Institute of Chemical Technology and Polymer Chemistry, Engesserstr. 18, Geb. 11.23, R: 109 References [1] M. Hartmann, L. Maier, H. D. Minh, O. Deutschmann, Combustion and Flame 2010,157, 1771. [2] M. Hartmann, L. Maier, O. Deutschmann, Applied Catalysis A: General, doi:10.1016/j.apcata.2010.08.051. [3] N. Hebben, C. Diehm, O. Deutschmann, Applied Catalysis A: General 2010, 388, 225. [4] M. Hartmann, S. Lichtenberg, N. Hebben, D. Zhang, O. Deutschmann, Chemie Ingenieur Technik 2009, 81, 909. [5] J. Larminie, A. Dicks, Fuel cell systems explained, 2. edition, John Wiley & Sons, Chichester, 2003, 207+ [6] A. J. McEvoy, Materialwissenschaft und Werkstofftechnik 2002, 33, 331. Presented at Opening Workshop of Helmholtz Research School, Karlsruhe/Germany, November 17, 2010 Designed for accurate and rapid mixing of up to 8 gaseous reactants below auto-ignition temperature [4]
Transcript of Ctlti Rf i fL iti dAlt ti F l Catalytic Reforming of ...Catalyst carrier: Monolithic honeycomb or...
C t l ti R f i f L i ti d Alt ti F l
Helmholtz Research School Energy-Related Catalysis
Institute for Chemical Technology and Polymer Chemistry
Claudia Diehm
Catalytic Reforming of Logistic and Alternative Fuels
Research FundamentalsPersonal DetailsName: Claudia Diehm
Department: Department of Chemistry and Biosciences
Supervisor: Prof. Dr. Olaf Deutschmann
Cosupervisor: Prof. Dr.-Ing. Roland Dittmeyer
Higher Education:
10/2005 - 08/2010 Karlsruhe Institute of Technology (KIT), Germany
Subject: Chemistry
Final result: Diplom, outstanding (1.2)
Focus: Chemical Technology
Efficient power generation for mobile applications by using APUs (Auxiliary Power Unit):
Reduction of greenhouse gas emissions and
Fuel reformer
• CPOX• Steam
reforming
H2 + CO
Fuel cell
• SOFC• PEMFC
after gas cleaning
Commercial fuel
Electricity
Diploma thesis
Honours and Awards:
10/2009 - 07/2010 Scholarship by “Karlsruher Universitätsgesellschaft e.V.”
Catalytic Partial Oxidation of Ethanol blended Fuels on Rh coated Catalyst
binary mixtures of ethanol and i-octane as model surrogates
Features of catalytic partial oxidation (CPOX) reformers[1] :Reaction equation
Catalyst[2]:Catalyst carrier: Monolithic honeycomb or foam structuresWashcoat: -Al2O3
Catalytically active metal: Rhodium
Reduction of greenhouse gas emissions and lower consumption of limited fossil fuels
CO x H 2
y O
2
z-x OHC 22zyx
over 80 % hydrogen selectivity for all blends in millisecond contact times
maximum hydrogen selectivity shifts to leaner conditions for increasing ethanol concentration
avoidance of side-products such as methane, ethylene, and acetaldehyde
i i f d t f l ll
Catalytically active metal: Rhodium
Short residence time
High fuel throughput and syngas yields
Nearly adiabatically operating compact reactors
Suitable for:logistic fuels, e.g. gasoline, and dieselalternative fuels, e.g. bioethanol[3]
mixtures of both e g ethanol blended fuels
operating catalyst
poisoning of downstream fuel cell
selectivity to side-products rises with increasing ethanol percentage
exception to this trend for 10 vol% ethanol
observed properties of ethanol iso-octane blends not solely explicable by the properties of the pure substances
interactions between the components during the simultaneous conversion on the catalytic surface
mixtures of both, e.g. ethanol blended fuels
CPOX reformers are most suitable for on-board hydrogen supply[4]
Features of fuel cells[5]:SOFC: Hydrogen and carbon monoxide can be reformed
PEMFC: Poisoned by carbon monoxide
Both show incompatibility to hydrocarbons[6]
PhD thesis
Catalyst Development
Experimental Setup
Properties[1]
Well-defined boundary conditionsHomogeneous, pulse-free
reactant flowuniform temperature profile
Analysis of product stream by:FT IR
Improvement and optimization of CPOX reformers by:Understanding the complex reaction system in the
reformer for different fuelsCommercial gasolineCommercial dieselBiofuels
Developing alternative catalysts to replace expensive rhodium catalysts
References
Development
Alteration of catalytically active metal along length
of monolithic channel
Noble metal doped catalysts
e.g. perovskite or pyrochlorestructures
Non-precious metal catalysts
e.g. group 6 transition metal
carbides
Reactor
FT-IRMSGC/MSTime-resolved monitoring
Approach for every fuel:from model surrogate to commercial fuel
One component
model surrogate
Complex mixtures of
hydrocarbons
Commercial fuel
Catalyst after test-cycle
Improvement of the marketability and efficiency of APUs
KIT – University of the State of Baden-Wuerttemberg andNational Research Center of the Helmholtz Association
Contact: Claudia Diehm, Institute of Chemical Technology and Polymer Chemistry, Engesserstr. 18, Geb. 11.23, R: 109
References[1] M. Hartmann, L. Maier, H. D. Minh, O. Deutschmann, Combustion and Flame 2010,157, 1771.[2] M. Hartmann, L. Maier, O. Deutschmann, Applied Catalysis A: General, doi:10.1016/j.apcata.2010.08.051.[3] N. Hebben, C. Diehm, O. Deutschmann, Applied Catalysis A: General 2010, 388, 225.[4] M. Hartmann, S. Lichtenberg, N. Hebben, D. Zhang, O. Deutschmann, Chemie Ingenieur Technik 2009, 81, 909.[5] J. Larminie, A. Dicks, Fuel cell systems explained, 2. edition, John Wiley & Sons, Chichester, 2003, 207+[6] A. J. McEvoy, Materialwissenschaft und Werkstofftechnik 2002, 33, 331.
Presented at Opening Workshop of Helmholtz Research School, Karlsruhe/Germany, November 17, 2010
Designed for accurate and rapid mixing of up to 8 gaseous reactants below auto-ignition temperature[4]
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