Electron Paramagnetic Resonance investigation of the nature of active species involved in carbon black oxidation on ZrO2 and Cu/ZrO2 catalysts |
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| Affiliation: | 1. Université Lille Nord de France, F-59000 Lille, France;2. Unité de Chimie Environnementale et Interactions sur le Vivant, EA 4492, Université du Littoral Côte d''Opale, 145, avenue Maurice Schumann, F-59140 Dunkerque, France;3. Laboratory of Physical Chemistry of Materials, Faculty of sciences II, Lebanese University, Fanar, BP 90656 Jdeidet El-Metn, Lebanon;1. Institute of Electrochemistry and Energy Systems, BAS, Acad. G. Bonchev bl. 10, 1113 Sofia, Bulgaria;2. Georgi Nadjakov Institute of Solid State Physics, BAS, Tzarigradsko Chaussee Blvd. 72, 1784 Sofia, Bulgaria;3. Institute of General and Inorganic Chemistry, BAS, Acad. G. Bonchev St, bl. 11, 1113 Sofia, Bulgaria;4. Rostislaw Kaischew Institute of Physical Chemistry, BAS, Acad. G. Bonchev St, bl. 11, 1113 Sofia, Bulgaria;1. Univ Bourgogne Franche Comte, CNRS, Lab ICB, UMR 6303, Site UTBM, F-90010 Belfort, France;2. School of Materials Science and Engineering, Anhui University of Technology, Ma’anshan 243002, PR China;3. Key Lab of Safety Science of Pressurized System, Ministry of Education, School of Mechanical and Power Engineering, East China University of Science and Technology, Shanghai 200237, PR China;1. School of Materials Science and Engineering, Dalian Jiaotong University, Dalian 116028, Liaoning Province, China;2. School of Physics and Materials Engineering, Dalian Minzu University, Dalian 116600, PR China;3. Academy of Fundamental and Interdisciplinary Sciences, Harbin Institute of Technology, Harbin 150080, PR China |
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| Abstract: | To identify the nature of active paramagnetic species involved in the carbon black (CB) oxidation, an Electron Paramagnetic Resonance (EPR) study of (CB–ZrO2) and (CB–Cu/ZrO2) loose contact mixtures treated under argon flow has been undertaken. In the presence of pure zirconia catalysts, it was found that ZrO2 interacts with CB and can be reduced into Zr3+ formed in tetragonal phase of this oxide support. In parallel, several EPR signals assigned to carbonaceous radicals were detected: i) carbonaceous radicals on CB surface, ii) radicals located at the CB–ZrO2 interface and iii) oxygen deficit carbonaceous radicals observed at high treatment temperature. The carbonaceous signals disappeared completely after CB oxidation in agreement with a regeneration of the catalyst treated under air.For copper supported on zirconia catalysts, oxygen surrounding isolated Cu(II) species and oxygen from tetragonal ZrO2 lattice are involved in carbon black oxidation. The phenomenon is reversible and this catalyst is also regenerated by air. Carbonaceous radical signals were also observed for (CB–Cu/ZrO2) mixture and their intensity decrease versus temperature appeared in good agreement with the better activity of Cu/ZrO2 compared to pure ZrO2. |
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