Rare earth-first-row transition metal perovskites as catalysts for the autothermal reforming of hydrocarbon fuels to generate hydrogen |
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| Authors: | Jennifer R Mawdsley Theodore R Krause |
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| Affiliation: | 1. School of Physics and NANOTEC-SUT Center of Excellence on Advanced Functional Nanomaterials, Suranaree University of Technology, Nakhon Ratchasima 30000, Thailand;2. Synchrotron Light Research Institute, Nakhon Ratchasima 30000, Thailand;3. Thailand Center of Excellence in Physics (ThEP Center), Commission on Higher Education, Bangkok 10400, Thailand;4. Department of Physics, Faculty of Science, Kasetsart University, Bangkok 10900, Thailand;1. Instituto Nacional de Tecnologia, Av. Venezuela 82, 20081-312, Rio de Janeiro, Brazil;2. Universidade Federal Fluminense, Rua Passo da Pátria 156, 24210-240, Niterói, Brazil;3. Department of Physical Chemistry and Materials Science, University of Szeged, Aradi Vértanúk tere 1, H-6720 Szeged, Hungary;1. Centre of Polymer and Carbon Materials Polish Academy of Sciences, Marii Curie Skłodowskiej 34, 41-819 Zabrze, Poland;2. Silesian University of Technology, Faculty of Chemistry, M. Strzody 9, 44-100 Gliwice, Poland;3. Saigon University, Faculty of Education of Natural Sciences, 273 An Duong Vuong Dis.5, HCMC, Vietnam;4. Laboratoire Réactivité de Surface, University Pierre et Marie Curie, Paris 6, UMR 7197-CNRS, 3 rue Galilée, 94200 Ivry, France;5. IAMS, Vietnam Academy of Science and Technology (VAST), 1 Mac Dinh Chi Dis.1, HCMC, Vietnam;6. On leave from University Pierre and Marie Curie, Paris, France;1. Department of Chemical and Materials Engineering, University of Alberta, Edmonton, AB T6G 1H9, Canada;2. Department of Civil and Environmental Engineering, University of Alberta, Edmonton, AB T6G 1H9, Canada;3. Department of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China;4. CanmetMATERIALS, Natural Resources Canada, Hamilton, ON L8P 0A5, Canada;1. Clean Energy Research Center, Korea Institute of Science and Technology, 5, Hwarang-ro 14-gil, Seongbuk-gu, Seoul, South Korea;2. Clean Energy & Chemical Engineering, University of Science and Technology, 217, Gajeong-ro, Yuseong-gu, Daejeon, South Korea;3. Department of Chemical & Biological engineering, Korea University, 145, Anam-ro, Seongbuk-gu, Seoul, South Korea |
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| Abstract: | Perovskite oxides (ABO3) containing rare earth elements on the A-site and first-row transition metal elements on the B-site were studied as catalysts for autothermal reforming of liquid hydrocarbon fuels to produce hydrogen for fuel cell systems. Experiments were conducted in a fixed bed microreactor at temperatures of 600–800 °C and gas-hourly space velocities (GHSV) ranging from 4600 to 28,000 h−1 using 2,2,4-trimethylpentane (isooctane) as a surrogate fuel. We have found that the two binary oxides, LaNiO3 and LaCoO3, produced high yields of H2, but were not structurally stable. These perovskites decomposed to La2O3 and Ni/NiO or Co/CoO under the reducing conditions present in the reformer. Three other binary oxides, LaCrO3, LaFeO3, and LaMnO3, were structurally stable but significantly less active than LaNiO3 and LaCoO3. The partial substitution of chromium, iron, aluminum, gallium, or manganese on the B-site of LaNiO3 to yield LaBxNi1−xO3 was shown to improve the structural stability without a significant decrease in the H2 yield. The effects of substituting rare earth elements for La and the substitution of alkaline earth elements on the A-site (La1−yAyBxNi1−xO3) on catalyst performance and stability were also investigated. Finally, La0.8Sr0.2M0.9Ni0.1O3 catalysts (where M = Cr, Mn, or Fe) were tested with a “benchmark fuel” mixture containing from 0 to 50 ppmw sulfur. These tests showed that using chromium as a stabilizing element in LaNiO3 imparts the most sulfur tolerance. |
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