| 1. |
- Lindström, B., et al.
(författare)
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Diesel fuel reformer for automotive fuel cell applications
- 2009
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Ingår i: International journal of hydrogen energy. - : Elsevier BV. - 0360-3199 .- 1879-3487. ; 34:8, s. 3367-3381
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Tidskriftsartikel (refereegranskat)abstract
- Fuel economy and emission abatement are issues, which are highly prioritized areas in the automotive industry of today. The debate about climate change has in recent years even more emphasized the importance of these issues and has increased the search for finding sustainable technical solutions. This paper describes an effort to develop an innovative and environmentally-benign hydrogen generation system operating on commercial diesel fuel to avoid running the engine to supply electricity at stand-still. The use of a fuel cell-based auxiliary power unit (APU) has the potential of delivering electricity at high efficiencies independent of the heavy-duty truck engine. During the reformer development phase, spray formation and mixing of reactants proved to be crucial to obtain high reforming efficiencies and low diesel slip. The diesel is being injected through a nozzle creating a spray of fine droplets of a size which can establish rapid evaporation. Air and steam are being pre-heated and injected into the mixture chamber and subsequently mixed with the evaporated diesel fuel. Depending on the operating parameters, a part of the fuel is being oxidized and produces heat. Autothermal reforming was chosen to circumvent the heat transfer problem in catalytic steam reforming. By supplying heat directly to the catalyst surface by an oxidation reaction the heat demand of the strongly endothermic steam reforming reaction can be fulfilled. We employed CFD calculations, which revealed the importance of avoiding large recirculation zones leading to a prolonged residence time of the hydrocarbon molecules and causing auto-ignition and excessive temperatures in the catalyst. Five different reformer generations are being described and discussed in detail in this publication. The first one was based on a fixed bed reactor, while the other four all relied on catalytic monoliths enabling low pressure drops. The early reactor designs all suffered from auto-ignition and instability problems. The latter generations exhibited a considerably more stable temperature profile in the reformer. The conversion of diesel and the reformer efficiencies are significantly higher than the early generation diesel reformers.
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| 2. |
- DAWODY, JAZAER, 1959, et al.
(författare)
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E4-Mistra, a research program for the development of an energy efficient low emission exhaust aftertreatment system for heavy duty vehicles
- 2012
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Ingår i: World Renewable Energy Forum, WREF 2012, Including World Renewable Energy Congress XII and Colorado Renewable Energy Society (CRES) Annual Conference. - : American Solar Energy Society. - 9781622760923 ; , s. 4530-4536
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Konferensbidrag (refereegranskat)abstract
- This paper presents a unique system approach applied in a joint academic - industrial research program, E4 Mistra, to reach the goals of energy efficiency and low emissions exhaust aftertreatment system for heavy duty vehicles. The high energy efficiency is achieved by heat recuperation, on-board hydrogen production for use in both an auxiliary power unit and for NOx reduction and by finding new solutions for making the after-treatment system active at low exhaust temperatures. To reach low particulate emissions a mechanical filter using a sintered metal filter is developed. Low NOx emissions are achieved by an efficient NOx reduction catalyst. The system is based on four technological advances: Thermoelectric material s for heat recuperation, catalytic reduction of NOx over innovative catalyst substrates using hydrocarbons from the fuel and H2 from a high efficiency fuel reformer, and particulate filtration over a porous metal filter.
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| 3. |
- Creaser, Derek, 1966, et al.
(författare)
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Kinetic modeling of autothermal reforming of dimethyl ether
- 2010
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Ingår i: Industrial & Engineering Chemistry Research. - : American Chemical Society (ACS). - 1520-5045 .- 0888-5885. ; 49:20, s. 9712-9719
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Tidskriftsartikel (refereegranskat)abstract
- A global kinetic model was developed for the autothermal reforming of dimethyl ether (DME) over a Pd-Zn/Al2O3 catalyst on a cordierite monolith. A kinetic model consisting of five key overall reactions was found to capture the main features of experimental data. The modeling also accounted for heat transport effects in the reactor that are of importance when coupling the exothermic oxidation reactions with endothermic steam reforming reactions. The modeling confirmed that oxidation reactions dominate near the inlet of the reactor, generating a local hot spot. The heat from oxidation reactions accelerates the reforming reactions. Water adsorption was found to have a weak detrimental influence on the activity. Based on the model, the influence of the reactor scale and oxygen supply by air feed on the performance of the reactor was examined.
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| 4. |
- Creaser, Derek, 1966, et al.
(författare)
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Modeling study of 5 kWe-scale autothermal diesel fuel reformer
- 2011
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Ingår i: Applied Catalysis A: General. - : Elsevier BV. - 1873-3875 .- 0926-860X. ; 404, s. 129-140
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Tidskriftsartikel (refereegranskat)abstract
- A model was developed that successfully describes key operating features of a 5 kWe-scale autothermal diesel fuel reformer with an engineered monolith-supported Rh based catalyst. The model consisted of a kinetic model comprised of four overall reactions including total oxidation, fuel steam reforming, methane formation via fuel decomposition and the water–gas shift reaction. The model also accounted for heat and mass transport effects that were of importance when coupling the exothermic oxidation reactions with endothermic steam reforming reactions in a full-scale reformer. According to the model, the total oxidation and steam reforming reactions occurred simultaneously, however the heat effects of the oxidation reaction dominated near the reactor inlet resulting in a local hot spot. Transport resistances were found to hinder the rates of the main reactions, especially at higher temperature operating conditions. The model was primarily based on experimental data for a commercial low-sulphur diesel fuel (MK1), however it was found to also reasonably well describe the operation of the reactor with a diesel surrogate (n-tetradecane).
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| 5. |
- Granlund, Moa Z., 1983-, et al.
(författare)
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Evaluation of Co, La, and Mn promoted Rh catalysts for autothermal reforming of commercial diesel
- 2014
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Ingår i: Applied Catalysis B. - : Elsevier BV. - 0926-3373 .- 1873-3883. ; 154, s. 386-394
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Tidskriftsartikel (refereegranskat)abstract
- The objective of this paper was to study the influence three promoters (Co, La, Mn) had on the catalytic activity of Rh-based catalysts for autothermal reforming of diesel. The catalysts were supported on CeO2ZrO2 and the loading was 1 wt.% Rh and 6 wt.% promoter. The catalytic activity was evaluated in a monolith bench scale reactor with Swedish Environmental diesel, MK1. The process parameters employed at the ATR experiments were; O-2/C similar to 0.45, H2O/C similar to 2.5 and GHSV similar to 50,000h(-1), meanwhile the reactor temperature was ramped from 700 degrees C to 950 degrees C. The catalysts were compared based on their fuel conversion, H-2 yield and the selectivity of different short-chain hydrocarbons. The results showed that all three catalysts had both high fuel conversion and H-2 yield in the optimal ATR operation temperatures. The H-2 yield and fuel conversion were increasing in the order Rh/Mn, Rh/La, Rh/Co. To get further insight in the difference between the materials the fresh and aged catalytic materials were characterized. The characterization methods used were H-2-temperature programmed reduction (H-2-TPR), powder X-ray diffraction (XRD), and BET surface measurements. The BET surface measurements showed that promotion with La gave improved thermal stability of the material. The XRD showed a high dispersion of all metals except Co, which was present as crystals in the size range of the particles of the support.
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| 6. |
- Granlund, Moa Z., et al.
(författare)
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Evaluation of Co, La, and Mn promoted Rh catalysts for autothermal reforming of commercial diesel : Aging and characterization
- 2015
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Ingår i: Applied Catalysis B. - : Elsevier BV. - 0926-3373 .- 1873-3883. ; 172, s. 145-153
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Tidskriftsartikel (refereegranskat)abstract
- In this study, three bimetallic catalysts are evaluated for autothermal reforming (AIR) of fuels (1 wt.% Rh and 6 wt.% X (X= Co, La or Mn) supported on high-surface area CeO2-ZrO2). The catalysts are aged for approximately 35 h and carefully characterized both as fresh and aged materials. The objective is to illuminate the changes in material properties after time on stream as well as the differences among the materials. The changes in material properties are evaluated by H-2-TPR, BET surface area analysis, TEM, SEM, and STEM. The material's tendency to coke is investigated by TPO analysis. The three materials exhibit promising initial activity. However, the Co-promoted sample decreases sharply in activity after 25 h of operation. Meanwhile, the other two materials display a more stable activity throughout the evaluated time. The deactivation of the Co-promoted material could be linked to the high amount of coke deposited during operation. Based on the results from the activity evaluation and characterization, the material promoted with lanthanum displays the most promising results. The addition of lanthanum resulted in a catalyst that was both stable and had high activity, even though a low rhodium loading is used. The material also shows superior thermal resistance compared to the other two materials. In addition, the tendency to coke is significantly lower compered to the other materials, which is especially beneficial when dealing with AIR of complex fuels.
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| 7. |
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| 8. |
- Gunnarsson, Fredrik, 1983, et al.
(författare)
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Combining HC-SCR over Ag/Al2O3 and hydrogen generation over Rh/CeO2-ZrO2 using biofuels : An integrated system approach for real applications
- 2015
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Ingår i: Applied Catalysis B. - : Elsevier BV. - 0926-3373 .- 1873-3883. ; 162, s. 583-592
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Tidskriftsartikel (refereegranskat)abstract
- Abstract We report on a high NOx reduction activity over Ag/Al2O3 catalysts, using hydrogen produced in a fuel reformer. The focus of the study is to evaluate the performance of a hydrocarbon selective catalytic reduction (HC-SCR) catalyst in real conditions. Initially, the catalytic materials for the fuel reformer (Rh/CeO2-ZrO2) and the HC-SCR (Ag/Al2O3) were evaluated in separate bench-scale reactor setups. These two setups were subsequently joined into an integrated bench-scale reactor setup with the aim to evaluate the influence of the reformate on the HC-SCR activity in a controlled environment. In the final phase of the study a 4 wt.% Ag/Al2O3 catalyst doped with 100 ppm(w) Pt was scaled up and tested in a pilot-scale reactor setup. The pilot-scale reactor setup enabled evaluation of the HC-SCR activity in real exhaust gases generated by a single cylinder engine (genset) together with a hydrogen-rich gas supplied from a fuel reformer. Commercial biodiesel (NExBTL) was used as reducing agent for the HC-SCR as well as fuel in the fuel reformer for both the bench-scale and pilot-scale experiments. This study gives an excellent link between evaluations of the catalytic materials, controlled bench-scale experiments and applied engine experiments, proving a viable concept for lean NOx reduction together with onboard hydrogen production. A NOx conversion of above 70% was reached at temperatures below 250 °C, in bench-scale experiments when hydrogen produced in the fuel reformer is added.
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| 9. |
- Karatzas, Xanthias, et al.
(författare)
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Characterization and optimization of an autothermal diesel and jet fuel reformer for 5 kW(e) mobile fuel cell applications
- 2010
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Ingår i: Chemical Engineering Journal. - : Elsevier BV. - 1385-8947 .- 1873-3212. ; 156:2, s. 366-379
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Tidskriftsartikel (refereegranskat)abstract
- The present paper describes the characterization of an autothermal reformer designed to generate hydrogen by autothermal reforming (ATR) from commercial diesel fuel (similar to 10 ppm S) and jet fuel (similar to 200 ppm S) for a 5 kW(e) polymer electrolyte fuel cell (PEFC). Commercial noble metal-based catalysts supported on 900 cpsi cordierite monoliths substrates were used for ATR with reproducible results. Parameters investigated in this study were the variation of the fuel inlet temperature, fuel flow and the H2O/C and O-2/C ratios. Temperature profiles were studied both in the axial and radial directions of the reformer. Product gas composition was analyzed using gas chromatography. It was concluded from the experiments that an elevated fuel inlet temperature (>= 60 degrees C) and a higher degree of fuel dispersion, generated via a single-fluid pressurized-swirl nozzle at high fuel flow, significantly improved the performance of the reformer. Complete fuel conversion, a reforming efficiency of 81% and an H-2 selectivity of 96% were established for ATR of diesel at P=5kW(e), H2O/C = 2.5, O-2/C = 0.49 and a fuel inlet temperature of 60 degrees C. No hot-spot formation and negligible coke formation were observed in the reactor at these operating conditions. The reforming of jet fuel resulted in a reforming efficiency of only 42%. A plausible cause is the coke deposition, originating from the aromatics present in the fuel, and the adsorption of S-compounds on the active sites of the reforming catalyst. Our results indicate possibilities for the developed catalytic reformer to be used in mobile fuel cell applications for energy-efficient hydrogen production from diesel fuel.
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| 10. |
- Karatzas, Xanthias, et al.
(författare)
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Microemulsion and incipient wetness prepared Rh-based catalyst for diesel reforming
- 2011
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Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 175:1, s. 515-523
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Tidskriftsartikel (refereegranskat)abstract
- The role of the catalyst preparation technique was investigated for diesel reforming. Reverse microemulsion (ME) and incipient wetness (IW) techniques were used for the preparation of Rh-based monolithic catalysts that were employed for hydrogen generation of low-sulfur diesel via autothermal reforming (ATR). The washcoat of the tested catalysts consisted of 0.5 wt% Rh, 1 wt% Rh, and 1: 1 wt% Rh: Pt supported on gamma-alumina. All washcoats were deposited on 400 cpsi cordierite monoliths. The reaction condition was T(feed) = 650 degrees C, H(2)O/C similar to 2.5, O(2)/C similar to 0.49, TOS = 3 h, GHSV similar to 13 000 h(-1) and P = 1 atm. Fresh and aged powder samples of the catalyst were characterized by N(2)-BET, H(2) chemisorption, XRD, H(2)-TPR, O(2)-TPO and TEM. The activity results established that Rh and RhPt formulations, prepared by ME and IW, are highly active for ATR of diesel where fuel conversions above 92% were obtained. FTIR and NDIR analysis also showed that the highest formation of ethylene was found in the product gas stream from the bimetallic samples indicating that RhPt/Al(2)O(3) is less resistant towards carbon deposition. The latter observation was confirmed by O(2)-TPO analysis of the aged samples where high loads of coke were found both on the active metals and on the support. Interestingly, these effects were less significant on the ME samples. The characterization results clearly showed differences in morphology between the ME and the IW samples. N(2)-BET analysis showed that higher surface area, similar to 268-285 m(2)/g, was obtained with the ME samples. Also, H(2) chemisorption analysis showed that the rhodium dispersion was similar to 10% higher for the ME samples (H/Rh similar to 60-66%). XRD analysis showed that crystalline phases of gamma-alumina were present on all samples. The diffractograms also showed small traces of metallic Pt (similar to 16-30 nm) in the bimetallic samples. H(2)-TPR analysis, showed peaks ascribed to bulk rhodium oxides and rhodium aluminates. It was also noted that the addition of Pt on the support lowered the reducibility of the different rhodium species. TEM analysis performed on the fresh and aged ME and IW bimetallic samples showed mainly Rh(x)Pt(1-x) alloys with an average particle size of similar to 20-50 nm were present on the alumina support. Also, for the aged samples, no sintering effects were noted. Furthermore, rhodium was found to switch oxidation state from e. g. Rh(3+) to Rh(0) while Pt remained in the metallic state.
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