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Zone-coated Rh-based monolithic catalyst for autothermal reforming of diesel
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology.
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2011 (English)In: Applied Catalysis B: Environmental, ISSN 0926-3373, E-ISSN 1873-3883, Vol. 101, no 3-4, 226-238 p.Article in journal (Refereed) Published
Abstract [en]

In this work we present results of hydrogen generation from diesel via autothermal reforming (AIR) obtained with monolithic catalysts consisting of either one or two layers of monometallic Rh and bimetallic RhPt washcoats. The Rh metal loading of the monometallic washcoats was varied between 0.5, 1.0 and 3.0 wt%, while the weight ratio of Rh:Pt in the bimetallic washcoats was kept constant at 1:1. Furthermore, non-doped and CeLa-doped catalysts were also tested to detect differences in catalyst activity. The catalysts consisting of two layers of washcoats were termed zoned catalysts and each layer was applied to some given length in the axial direction of the monolith. All catalysts were prepared by impregnation using the incipient wetness technique with delta-Al2O3 B as support and deposited onto 400 cpsi cordierite monoliths. A total of eight catalysts, including both single layered and zone-coated, were tested in a bench-scale reactor using low-sulfur diesel as fuel at operating conditions H2O/C=2.5, O-2/C=0.49 (lambda = 0.33), GHSV 17,000 h(-1) and P = 1 atm. The results showed that the zoned catalyst, covered with the two washcoats Rh1.0Pt1.0-Ce10La5.0/delta-Al2O3 and Rh-3.0-Ce10La10/delta-Al2O3, respectively, was most active in terms of fuel conversion and hydrogen production. The zoned catalyst's long-term performance and stability was also evaluated in a full-scale reactor using low-sulfur and Fischer-Tropsch diesels at operating conditions H2O/C = 2.5, O-2/C = 0.49 (lambda =0.33), GHSV= 10,800 h(-1), P = 1 atm, and at H2O/C = 2.4, 02/C = 0.39 (lambda=0.26), GHSV- 10,200 h(-1), P = 1 atm. respectively. The results showed that high fuel conversion and hydrogen production were obtained from both fuels. In addition, partial oxidation and steam reforming reactions were identified by closely studying the distribution of the analyzed product gas composition and the temperature measurements. Fresh and aged samples of the catalysts were characterized by N-2-BET, H-2 chemisorption, XRD, H-2-TPR, O-2-TPO and XPS analyses.

Place, publisher, year, edition, pages
2011. Vol. 101, no 3-4, 226-238 p.
Keyword [en]
Autothermal reforming, Diesel, Rhodium, Zone-coated monolithic catalyst
URN: urn:nbn:se:kth:diva-31649DOI: 10.1016/j.apcatb.2010.09.027ISI: 000287068400009ScopusID: 2-s2.0-78650307598OAI: diva2:405107
QC 20110321Available from: 2011-03-21 Created: 2011-03-21 Last updated: 2011-04-18Bibliographically approved
In thesis
1. Rhodium diesel-reforming catalysts for fuel cell applications
Open this publication in new window or tab >>Rhodium diesel-reforming catalysts for fuel cell applications
2011 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Heavy-duty diesel truck engines are routinely idled at standstill to provide cab heating or air conditioning, and in addition to supply electricity to comfort units such as radio and TV. Idling is an inefficient and unfavorable process resulting in increased fuel consumption, increased emissions, shortened engine life, impaired driver rest and health, and elevated noise. Hydrogen-fueled, polymer-electrolyte fuel-cell auxiliary power unit (PEFC-APU) as a silent external power supply, working independently of the main engine, is proposed as viable solution for better fuel economy and abatement of idling emissions. In a diesel PEFC-APU, the hydrogen storage problem is circumvented as hydrogen can be generated onboard from diesel by using a catalytic reformer. In order to make catalytic diesel PEFC-APU systems viable for commercialization research is still needed. Two key areas are the development of reforming catalyst and reformer design, which both are the scope of this thesis. For diesel-reforming catalysts, low loadings of Rh and RhPt alloys have proven to exhibit excellent reforming and hydrogen selectivity properties. For the development of a stable reforming catalyst, more studies have to be conducted in order to find suitable promoters and support materials to optimize and sustain the long-term performance of the Rh catalyst. The next step will be full-scale tests carried out at realistic operating conditions in order to fully comprehend the overall reforming process and to validate promising Rh catalysts. This thesis can be divided into two parts; the first part addresses the development of catalysts in the form of washcoated cordierite monoliths for autothermal reforming (ATR) of diesel. A variety of catalyst compositions were developed containing Rh or RhPt as active metals, CeO2, La2O3, MgO, Y2O3 as promoters and Al2O3, CeO2-ZrO2, SiO2 and TiO2 as support materials. The catalysts were tested in a bench-scale reactor and characterized by using N2-BET, XRD, H2 chemisorption, H2-TPR, O2-TPO, XPS and TEM analyses. The second part addresses the development and testing of full-scale reformers at various realistic operating conditions using promising Rh catalysts.

The thesis shows that a variety of Rh on alumina catalysts was successfully tested for ATR of diesel (Papers I-IV). Also, zone-coating, meaning adding two washcoats on specific parts of the monolith, was found to have beneficial effects on the ATR catalyst performance (Paper II). In addition, RhPt supported on CeO2-ZrO2 was found to be one of the most active and promising catalyst candidates for ATR of diesel. The superior performance may be attributed to higher reducibility of RhiOx species and greater dispersion of Rh and Pt on the support (Paper IV). Finally, two full-scale diesel reformers were successfully developed and proven capable of providing high fuel conversion and hydrogen production from commercial diesel over selected Rh catalysts (Papers II-III, V-VI).

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2011. x, 81 p.
Trita-CHE-Report, ISSN 1654-1081 ; 2011:28
Autothermal reforming, auxiliary power unit, BET, chemisorption, diesel, fuel cell, hydrogen, monolith, reforming catalyst, reformer design, Rh, RhPt alloy, TEM, TPO, TPR, XRD, XPS, zone coating
National Category
Chemical Engineering
urn:nbn:se:kth:diva-32647 (URN)978-91-7415-945-5 (ISBN)
Public defence
2011-04-29, KTH - Sal F3, Lindstedtsvägen 26, Stockholm, 10:00 (English)
QC 20110418Available from: 2011-04-18 Created: 2011-04-18 Last updated: 2011-04-18Bibliographically approved

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