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Transformation of cyclohexene on palladium catalysts: activity and deactivation
Affiliation:1. National Research Council of Italy, Institute for Photonics and Nanotechnologies – Padova, Via Trasea 7, 35131, Padova, Italy;2. University of Padova, Department of Industrial Engineering, Via Marzolo 9, 35131, Padova, Italy;3. University of Padova, Department of Physics and Astronomy, Via Marzolo8, 35131, Padova, Italy;4. Italian Institute of Technology, Via Morego 30, 16163, Genova, Italy;5. University of Padova, Department of Information Engineering, Via Gradenigo 6/B, 35131, Padova, Italy;1. Department of BIN Convergence Technology, Chonbuk National University, Jeonju 561-756, South Korea;2. Department of Organic Materials and Fiber Engineering, Chonbuk National University, Jeonju 561-756, South Korea;1. Department of Chemistry, Biology and Biotechnology and Centro di Eccellenza sui Materiali Innovativi Nanostrutturati (CEMIN) University of Perugia, via Elce di Sotto 8, 06123 Perugia, Italy;2. Department of Organic Chemistry, Faculty of Chemical Engineering and Technology, University of Zagreb, Marulićev trg 19, 10000 Zagreb, Croatia;3. NMR Center, Rudjer Bošković Institute, Bijenička cesta 54, 10000 Zagreb, Croatia;1. Fachbereich Physik und Zentrum für Materialwissenschaften, Philipps-Universität, D-35032 Marburg, Germany;2. Institut für Angewandte Physik, Justus-Liebig-Universität Giessen, D-35392 Giessen, Germany;1. Key Laboratory of Luminescence and Real-Time Analytical Chemistry (Southwest University), Ministry of Education, College of Pharmaceutical Sciences, Southwest University, Chongqing, 400715, People’s Republic of China;2. Institute for Drug and Instrument Control of Health Dept GLD of PLA, Beijing, 100071, People’s Republic of China
Abstract:The transformation of cyclohexene on palladium catalysts can take place via two competitive processes: disproportionation and dehydrogenation. A study conducted over a broad temperature range revealed that disproportionation prevails at low temperatures and dehydrogenation at high temperatures. When the reaction develops under continuous-flow conditions (viz. in a tubular reactor connected online to a mass spectrometer), a transition temperature exists for each catalyst above which hydrogen is formed in detectable amounts. Metal catalysts are strongly deactivated during the transformation of cyclohexene. This led us to examine the process by performing thermal programmed experiments, desorptions and thermal oxidations, which showed catalyst deactivation in this process to be the result of surface adsorption of benzene and carbon deposition. Finally, desorption and subsequent oxidation were found to effectively regenerate the catalysts, which thus regained their initial activity.
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