Physically and chemically mixed TiO2-supported Pd and Au catalysts: unexpected synergistic effects on selective hydrogenation of citral in supercritical CO2 |
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| Authors: | Ruixia Liu Yancun Yu Kazuki Yoshida Guiming Li Haoxi Jiang Minhua Zhang Fengyu Zhao Shin-ichiro Fujita Masahiko Arai |
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| Affiliation: | 1. State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, PR China;2. Division of Chemical Process Engineering, Graduate School of Engineering, Hokkaido University, Sapporo 060-8628, Japan;3. Key Laboratory for Green Chemical Technology of Ministry of Education, Research and Development Center for Petrochemical Technology, Tianjin University, Tianjin 300072, PR China;1. Centro de Pesquisas Leopoldo Miguez de Melo, CENPES/Petrobras S.A., Rio de Janeiro, Brazil;2. Instituto Alberto Luiz Coimbra de Pós-Graduação e Pesquisa em Engenharia (COPPE), Programa de Engenharia Química, Universidade Federal do Rio de Janeiro, Rio de Janeiro, Brazil;3. Programa de Pós-Graduação em Engenharia Química, Instituto de Química, Universidade do Estado do Rio de Janeiro, Rio de Janeiro, Brazil;1. Centro de Pesquisas Leopoldo Miguez de Melo – CENPES/Petrobras, Rio de Janeiro, Brazil;2. Instituto Alberto Luiz Coimbra de Pós-Graduação e Pesquisa em Engenharia (COPPE), Rio de Janeiro, Brazil;3. Programa de Pós-Graduação em Engenharia Química, Instituto de Química, UERJ, Rio de Janeiro, Brazil;1. State Key Laboratory of Electroanalytical Chemistry, Laboratory of Green Chemistry and Process, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, PR China;2. Division of Chemical Process Engineering, Faculty of Engineering, Hokkaido University, Sapporo 060-8628, Japan;1. CNRS, LCC (Laboratoire de chimie de coordination), composante ENSIACET, 4, allée Émile-Monso, BP 44099, 31030 Toulouse cedex 4, France;2. Université de Toulouse, UPS, INPT, 31077 Toulouse cedex 4, France;3. Université de Toulouse, INSA, UPS, CNRS, LPCNO (IRSAMC), 135, avenue de Rangueil, 31077 Toulouse, France;1. Department of Chemistry, Jahangirnagar University, Savar, Dhaka 1342, Bangladesh;2. Department of Chemistry, University College London, 20 Gordon Street, London WC1H OAJ, UK;3. Department of Chemistry, University of North Texas, Denton, TX 76203, USA;4. Georg-August University, Institute of Inorganic Chemistry, Tammannstr. 4, D-37077 Göttingen, Germany |
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| Abstract: | The selective hydrogenation of citral was studied with various TiO2-supported monometallic and bimetallic Pd and Au catalysts and their physical mixtures in supercritical CO2 (scCO2). Significant synergistic effects appeared when active Pd species was chemically or physically mixed with less active Au species. The total rate of conversion was greatly enhanced and the selectivity to citronellal (CAL) was improved. The physical properties of those catalysts were characterized by TEM, HRTEM-EDS, XPS, and UV/Vis and their features of H2 desorption were examined by TPD. The physical and chemical characterization results were used to discuss the reasons for the unexpected synergistic effects observed. The same selective hydrogenation was also conducted in a conventional non-polar organic solvent of n-hexane to examine the roles of scCO2. The use of scCO2 was effective for accelerating the hydrogenation of citral and improving the selectivity to CAL. |
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