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Oxidation of Fuels in the Cool Flame Regime for Combustion and Reforming for Fuel Cells

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Oxidation of Fuels in the Cool Flame Regime for Combustion and Reforming for Fuel Cells BNL-69349 Informal Report Oxidation of Fuels in the Cool Flame Regime for Combustion and Reforming for Fuel Cells Manuscript submitted to: Progress in Energy and Combustion Science A. Naidja, C.R. Krishna, T. Butcher and D. Mahajan August 2002 Energy Sciences and Technology Department Energy Resources Division Brookhaven National Laboratory Brookhaven Science Associates Upton, New York 11973-5000 Under Contract No. DE-AC02-98CH10886 with the United States Department of Energy DISCLAlMER This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereox nor any employees, nor any of their contractors, subcontractors or their employees, makes any warranty, express or implied, or assumes any legal liability or responsibilityfor the accuracy, completeness, or any third party's use or the results of such use of any information, apparatus, product, or process disclosed, or represents tliat its use would not infringeprivately owned rights. Reference. herein to any speciJic commercial product, process, or service by trade name, trademark, manufacturer, or.otherwise, does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof or its contractors or subcontractors. The views and opinions of authors expressed herein do not necessarily state or reflect ~ those of the United States Government or any agency thereoJ: Available electronically at- http://www.doe.gov/bridge Available to US. Department of Energy and its contractors in paper from- US.Department of Energy Office of Scientific and Technical Information P.O.Box 62 Oak Ridge, TN 3783 1 (423) 576-8401 Available to' the public from- US. Department of Commerce National Technical Information Service 5285 Port Royal Road Springfield, VA 22 131 (703) 487-4650 @ Printed on recycled paper 1 1 Manuscript submitted to: Progress in Energy and Combustion Science 2 3 Oxidation of Fuels in the Cool Flame Regime for Combustion 4 and Reforming for Fuel Cells 5 6 7 A. Naidja, C.R. Krishna, T. Butcher and D. Mahajan" 8 9 10 Energy Sciences and Technology Department, Brookhaven National Laboratory, 11 Upton, NY 1 I973 USA 12 13 14 *Corresponding author: Dr. Devinder Mahajan 15 Brookhaven National Laboratory 16 Energy Sciences and Technology Deparfment 17 Blg. 815, Upon, NY11973 USA 18 Tel: (631) 344-4985 19 Fax: (631) 344-7905 20 E-mail: [email protected] 21 2 1 Abstract 2 The pmpose of this review was to integrate the most recent and relevcant investigations on 3 the auto-oxidation of fuel oils and their reforming into hydrogen-rich gas that conld serve 4 as a feed for fiiel cells and combustion systems. We consider the incorporation of partial 5 oxidation under cool flame conditions to be a significant step in the reforming process for 6 generation of hydrogen-rich gas. Therefore, we have paid particnlm attention to the I partial oxidation of fiiels at low temperatnre in the cool flame region. This is still not a 8 well-understood featnre in the oxidation of fiiels and can potentially serve as a precursor 9 to low NO, emissions and low soot formation. Pretreatment, including atomization, 10 vaporization and burner technology are also briefly reviewed. The oxidation of reference I1 fuels (n-heptane C7H16, iso-octane CaHls and to a lesser extent cetane Cl~H34)in the 12 intermediate and high temperahire ranges have been stndied extensively and it is 13 examined here to show the significant progress made in modeling the kinetics and 14 mechanisms, and in the evaluation of ignition delay times. However, due to the complex 15 nature of real fuels such as petroleum distillates (diesel and jet fuel) <and biofnek, much 16 less is known on the kinetics and mechanisms of their oxidation, as well as on the 17 resulting reaction prodncts formed during partial oxidation. The rich literature on the 18 oxidation of fiiels is, hence, limited to the cited main reference fiiels. We have illso 19 covered recent developments in the catalytic reforming of hiels. In the presence of 20 catalysts, the fiiels can be reformed throngh partial oxidation, steam reforming and 21 autothermal reforming to generate hydrogen. Bnt optimnm routes to produce cost 22 effective hydrogen hiel from conventional or derivative fuels are'still debatable. It is 23 suggested that the use of prodncts emanating from partial oxidation of fiiels under cool ' ti. 3 1 flame conditions could be attractive in such refoiming processes, but this is as yet 2 untested. The exploitation of developments in oxidation, combustion and reforming 3 processes is always impacted by the resulting emission of pollutants, including NO,, SO,, 4 CO and soot, which have an impact on the health of the fragile ecosystem. Attention is 5 paid to the progress made in innovative techniques developed to reduce the level of 6 pollutants resulting from oxidation and reforming processes. In the last part, we I summarize the present status of the topics covered and present prospects for fiihire 8 research. This information forms the basis for recommended themes that are vital in 9 developing the next generation energy-efficient combustion and fiiel-cell technologies. 10 11 [Keywords: Cool flame, Oxidation, Combustion, Fuel oils, Kinetics, Riel cell, Fuel 12 reforming] 4 1 Contents 2 Abstract 3 1. Introduction 4 2. Preparation of the fiiels for oxidation: atomization and vaporization, burner and 5 reactor concepts 6 3. Oxidation and combustion of liqnid fuels I 3.1. Oxidation of fiiels at low lemperahire and cool flame regime 8 3.2. Role of oxidation reactions in the ignition of fiiels 9 3.3. Kinetics and mechanisms of the oxidation and combustion of reference fiiels 10 3.4. Oxidation of commercial fiiels and biofuels 11 4. Reforming of fuels for fiiel cell technology 12 4.1, Reforming of methane, nahiral gas and methanol 13 4.1 .I. Reforming of methane 14 4.1.2. Reforming of nahird gas 15 4.1.3. Reforming of methanol 16 4.2. Reforming of gasoline, diesels and biodiesels 17 5. Impact of NO, emissions and soot formation on the oxidation anL :eforming of fii~ 18 and the evolution of bnrner technology 19 5.1. Impact of NO, emissions on bniner technology 20 5.2. Impact of soot formation on burner technology 21 6. Conclnsions and prospects for hihire research 22 Acknowledgements 23 Appendix 24 References 25 26 5 1 1) Intrciduction 2 As a sonrce .of energy, fossil fuels have a tremendous impact on the planet in different 3 ways, including human welfare and the environment. In order to deal with the problem of 4 petroleum derived fiiels as a source of energy, and also, as a source of pollution, scientists 5 are investigating the means to improve the yield of energy conversion with a minimnm 6 level of toxic efflnents. This is possible by making engines and burners more efficient, 7 removing impurities such as sulfur and nitrogen from fiiels, lowering soot and coking, 8 which are precursors to carcinogenic polyaromatic hydrocarbons (PAH). SO,, NO,, COz 9 and paticnlate emissions all contribute variously to acid rain, photochemical smog, green 10 house effects and desti-tiction of ozone in the stratosphere [l-31 and may lead to global 11 warming and severe damages to the ecosystem health. 12 In the dawn of this twenty-first century, fossil fuels remain the main source of energy 13 for the planet and by far exceed geothermal, wind and solar energy. Nuclear energy was 14 considered very promising in the 1970s until mid 1980s till incidents snch as that at 15 Chernobyl disaster made this path questionable. Hydrogen is an environmentally friendly 16 and “clean” fuel. Despite its abundance in the hydrosphere, generating hydrogen by 17 electrolysis from water is still not economical. However, the oxidation of conventional 18 gaseous and liquid ftiels, including nahiral gas, petroleum distillates (gasoline, diesel and 19 Jet-fiiels) and biodiesels to light hydrocarbons and oxygen-contai~ng.substances, may 20 form a major step in the preparation of the fuel for reforming and production of hydrogen 21 for use in fuel cells. The hiel cell, an attractive but challenging technology, transforms 22 chemical energy directly to electrical energy, with less pollution when compared to 23 buining fossil fuels [4]. It is well lcnown that hydrogen is the best-suited hiel for fuel cell 6 1 systems; unfortunately hydrogen intrastnictnre costs are currently unacceptably high 2 compared to the existing natnral gas or petroleum distillate facilities [5]. Although 3 methanol can yield an appreciable proportion of hydrogen throngh its transformation into 4 synthesis gas (Hz + CO) [61, still it is a secondary derivative €tiel and reqnires new 5 infrastrncture. Therefore, on station or onboard processing of nahiral gas and petrolenm 6 distillates remains a viable alternative for the generation of hydrogen and will be 7 discnssed in detail in the third part of this paper. Bnt prior to that and to shed more light 8 on the partial oxidation of complex hiels like diesel and jet propulsion (JP) oils, we focus 9 on the oxidation of reference fiiels and their mixtures, especially at low temperatures in 10 the cool flame region. This phenomenon is still not well understood and may play a 11 significant role in the formation of the reaction prodncts prior to reforming, as well as in 12 snbseqnent low NO, emission systems [7-8]. 13 14 During the last decade, progress has been made in the experimental and theoretical 15 modeling of thc kinetics and l’ormation of reaction products during the oxidation 16 reactions of reference fiiels [9-131. Indeed, numerous shidics have been carried ont on the 17 oxidation and conversion of major (single component) reference fuels, such as n-heptane 18 [10,14], iso-octane [lo] and n-hexadecane (cetane) [151.
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