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Evaluation of Co, La, and Mn promoted Rh catalysts for autothermal reforming of commercial diesel: Aging and characterization
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, Södertälje, Sweden)
(Volvo Group Trucks Technology, Advanced Technology and Research, Energy Efficiency and Environment, Göteborg, Sweden)
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2015 (English)In: Applied Catalysis B: Environmental, ISSN 0926-3373, E-ISSN 1873-3883, Vol. 172, 145-153 p.Article in journal (Refereed) Published
Abstract [en]

In this study three bimetallic catalysts are evaluated for autothermal reforming (ATR) 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 H2-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 ATR of complex fuels. 

Place, publisher, year, edition, pages
Elsevier, 2015. Vol. 172, 145-153 p.
Keyword [en]
autothermal reforming, characterization, diesel, deactivation, morphology
National Category
Chemical Process Engineering
URN: urn:nbn:se:kth:diva-159470DOI: 10.1016/j.apcatb.2015.02.018ISI: 000352170400018ScopusID: 2-s2.0-84924213317OAI: diva2:785050
Mistra - The Swedish Foundation for Strategic Environmental ResearchKnut and Alice Wallenberg Foundation

QC 20150519

Available from: 2015-02-02 Created: 2015-02-02 Last updated: 2015-05-19Bibliographically 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.
TRITA-CHE-Report, ISSN 1654-1081 ; 2015:6
aging · autothermal fuel reforming · CeO2-ZrO2 · characterization · diesel · H2-assisted HC-SCR · micro reactor · monolith
National Category
Chemical Engineering
Research subject
Chemical Engineering
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)
Mistra - The Swedish Foundation for Strategic Environmental Research

QC 20150202

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

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