Effects of Pt precursors on Pt/CeO2 to water-gas shift (WGS) reaction activity with Langmuir-Hinshelwood model-based kinetics |
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Affiliation: | 1. School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu-ro, Jangan-gu, Suwon, Gyeonggi-do, 16419, Republic of Korea;2. Department of Chemical Engineering, Ajou University, Suwon, Gyeonggi-do, 16499, Republic of Korea;1. Department of Environmental Engineering, Yonsei University, 1 Yonseidae-gil, Wonju, Gangwon-do, 26493, Republic of Korea;2. Department of Environmental and Energy Engineering, Kyungnam University, 7 Kyungnamdaehak-ro, Changwon, Gyeongnam, 51767, Republic of Korea;3. School of Chemical Engineering, Sungkyunkwan University, 2066 Seobu-ro, Suwon, Gyeonggi-do, 16419, Republic of Korea;4. Green Energy Process Laboratory, Korea Institute of Energy Research, 152 Gajeong-ro, Yuseong-gu, Daejeon, 34129, Republic of Korea;5. Department of Earth Resources and Environmental Engineering, Hanyang University, 222 Wangsimni-ro, Seongdong-gu, Seoul, 04763, Republic of Korea;1. Department of Industrial Engineering, University of Salerno, Via Giovanni Paolo II 132, 84084, Fisciano (SA), Italy;2. Electron Microscopy Facility, Istituto Italiano di Tecnologia, Via Morego 30, 16163, Genoa, Italy |
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Abstract: | The crystallite size effects of Pt nanoparticles on the CeO2 (Pt/CeO2) prepared with four different Pt precursors were investigated in terms of their thermal stability and catalytic activity for a water-gas shift (WGS) reaction using the compositions of reformates after a typical steam reforming of propane. The Pt/CeO2 prepared with a diamine dinitroplatinum (Pt(NO2)2(NH3)3) precursor, which forms the cationic Pt(NH3)22+ species on the negatively-charged CeO2 surfaces, revealed a superior catalytic activity and thermal stability by forming the partially oxidized smaller Pt nanoparticles decorated with metallic Pt surfaces as well as by forming the strongly interacted PtOx-CeO2 interfaces. The stable preservation of the pristine smaller Pt nanoparticles with small aggregations even under the hysteresis test from 250 to 400 °C was mainly attributed to the strong metal-support interactions. The optimized Pt/CeO2 was further studied to obtain kinetic equations derived by Langmuir-Hinshelwood (LH) model, and the optimal operating conditions of WGS reaction were found to be ~280 °C and H2O/CO molar ratio of 9 with the activation energy of ~78.4 kJ/mol. |
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Keywords: | Water-gas shift (WGS) reaction Syngas Pt precursors Kinetics |
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