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Evaluation of Co, La, and Mn promoted Rh catalysts for autothermal reforming of commercial diesel
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology.ORCID iD: 0000-0001-9601-1959
Stockholm University, Arrhenius Laboratory, Department of Materials and Environmental Chemistry.
Scania CV AB, Materials Technology, Engine Performance and Emissions.
Volvo Group Trucks Technology, Advanced Technology & Research, Energy Efficiency & Environmen.
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2014 (English)In: Applied Catalysis B: Environmental, ISSN 0926-3373, E-ISSN 1873-3883, Vol. 154, 386-394 p.Article in journal (Refereed) Published
Abstract [en]

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.

Place, publisher, year, edition, pages
2014. Vol. 154, 386-394 p.
Keyword [en]
Autothermal reforming, Rhodium, Bimetallic, Diesel, Monolith
National Category
Chemical Process Engineering
Research subject
Chemical Engineering
Identifiers
URN: urn:nbn:se:kth:diva-145711DOI: 10.1016/j.apcatb.2014.02.043ISI: 000335098800045Scopus ID: 2-s2.0-84896119618OAI: oai:DiVA.org:kth-145711DiVA: diva2:719893
Funder
Mistra - The Swedish Foundation for Strategic Environmental Research
Note

QC 20150623

Available from: 2014-05-27 Created: 2014-05-27 Last updated: 2017-12-05Bibliographically approved
In thesis
1. Fuel Reforming for Hydrogen Production in Heavy-Duty Vehicle Applications
Open this publication in new window or tab >>Fuel Reforming for Hydrogen Production in Heavy-Duty Vehicle Applications
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The depletion of fossil fuels together with growing environmental concerns have created incitement for developing a more energy-efficient and environmentally-friendly vehicle fleet. The development towards cleaner heavy-duty vehicles started already in the 80’s with the introduction of emission legislations. Initially, engine optimization was enough for reaching the legislated levels of emissions. However, at present engine optimization is not enough but exhaust aftertreatment has become an essential part of heavy-duty vehicles, in order to meet the emission standards. Today, the total emissions are targeted which means that there is an interest in decreasing the idling emissions as well as the emissions during operation. To reduce the overall emissions several states in the USA have introduced idling legislations. Due to the limitations in idling time alternative solutions for power generation during rests are requested. A possible alternative is a fuel cell auxiliary power unit, combining a fuel cell with a fuel reformer (FC-APU). 

The focus of this thesis is the development of the fuel reformer for an FC-APU, in which the hydrogen to the fuel cell is generated from diesel in a high-temperature catalytic process. The produced hydrogen can also be used in other heavy-duty vehicle applications i.e. selective catalytic reduction of NOx (HC-SCR), where addition of hydrogen is essential for reaching high conversion at low temperatures. The effect of using hydrogen from a fuel reformer in HC-SCR is included in this work. The catalytic material development is focused on developing promoted materials with lower rhodium content but with catalytic activity comparable to that of materials with higher rhodium content. This includes evaluation and extensive characterization of both fresh and aged promoted materials. The work also includes reactor design where a micro reactor with multiple air inlets is evaluated.

This work has contributed to increased knowledge of catalytic materials suitable for reforming of diesel. By changing the support material from the traditionally used alumina to ceria-zirconia, increased H2 yield was achieved. In addition, the ceria-zirconia supported material was less prone to coke. By promoting the material with cobalt or lanthanum it was possible to decrease the rhodium content by 2/3 with enhanced catalytic performance. It was also discovered that promotion with lanthanum decreased the tendency for coking even further. Additionally, the lanthanum-promoted material had higher thermal stability as well as a stable highly dispersed rhodium phase.

Furthermore, the work has contributed to an increased knowledge concerning the fuel reformer’s effect on HC-SCR. The work displays clear evidence of benefits with using hydrogen-rich gas from a fuel reformer instead of pure hydrogen. The benefits are derived from the content of low molecular weight hydrocarbons present in the hydrogen-rich gas, which are strong reducing agents increasing the NOx reduction. This finding proves that fuel reforming in combination with HC-SCR is a viable option for NOx abatement.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2015. xi, 66 p.
Series
TRITA-CHE-Report, ISSN 1654-1081 ; 2015:6
Keyword
aging · autothermal fuel reforming · CeO2-ZrO2 · characterization · diesel · H2-assisted HC-SCR · micro reactor · monolith
National Category
Chemical Engineering
Research subject
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-159423 (URN)978-91-7595-412-7 (ISBN)
Public defence
2015-02-27, Kollegiesalen, Brinellvägen 8, KTH, Stockholm, 10:00 (English)
Opponent
Supervisors
Funder
Mistra - The Swedish Foundation for Strategic Environmental Research
Note

QC 20150202

Available from: 2015-02-02 Created: 2015-01-29 Last updated: 2015-02-02Bibliographically approved

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Granlund, Moa Z.

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