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Influence of the dual charge compensator on solid solution of the air-sintered Ca1-xCexZrTi2-2xFexCrxO7 zirconolite
Affiliation:1. School of Electromechanical Engineering, Guangdong University of Technology, Guangzhou, 510006, China;2. School of Material Science and Energy Engineering, Foshan University, Foshan, 528000, China;3. The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, China;4. Immobilisation Science Laboratory, Department of Materials Science and Engineering, University of Sheffield, Sheffield, S1 3JD, UK;5. Department of Radiochemistry, China Institute of Atomic Energy, Beijing, 102413, China;1. MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, PR China;2. Laboratory of Single Crystal Growth, South Ural State University, 76, Lenin av., Chelyabinsk, 454080, Russia;3. Laboratory of Semiconductor Oxide Materials, Moscow Institute of Physics and Technology (National Research University), Dolgoprudny, 141701, Moscow, Russia;4. Chelyabinsk State University, 129, Bratiev Kashirinykh st., Chelyabinsk, 454001, Russia;5. Laboratory of Terahertz Spectroscopy, Center for Photonics and 2D Materials, Moscow Institute of Physics and Technology (National Research University), Dolgoprudny, 141701, Moscow, Russia;6. Smart Sensors Laboratory, Department of Electronic Materials Technology, National University of Science and Technology MISiS, 4, Leninskiy av., Moscow, 119049, Russia;7. SSPA “Scientific and Practical Materials Research Centre of NAS of Belarus”, 19, P. Brovki str., Minsk, 220072, Belarus;8. L.N. Gumilyov Eurasian National University, Astana, 010000, Kazakhstan;1. Technische Universität Bergakademie Freiberg, Institute for Nonferrous Metallurgy and Purest Materials, Leipziger Straße 34, 09599, Freiberg, Germany;2. Technische Universität Bergakademie Freiberg, Institute of Ceramics, Refractories and Composite Materials, Agricolastr 17, 09599, Freiberg, Germany;1. Department of Physics, University of Lucknow, Lucknow, 226007, Uttar Pradesh, India;2. Department of Prosthodontics, King George Medical University, Shah Mina Road, Chowk, Lucknow, 226003, Uttar Pradesh, India;3. Department of Mechanical Engineering, Indian Institute of Technology, Banaras Hindu University, Varanasi, 221005, UP, India;1. Science and Technology on Advanced High Temperature Structural Materials Laboratory, Beijing Institute of Aeronautical Materials, Beijing, 100095, China;2. Leicester International Institute, Dalian University of Technology, Dalian, 124000, China;3. School of Materials Science & Engineering, Chang''an University, Xi''an, 710061, China;1. State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China;2. Engineering Research Center of Ceramic Materials for Additive Manufacturing, Ministry of Education, Wuhan, 430074, China
Abstract:In this study, a dual charge-compensator formulation was developed for zirconolite with the nominal composition Ca1-xCexZrTi2-2xFexCrxO7 (x = 0–0.30). The design strategy here was such that trivalent Fe and Cr were both targeted to substitute across the Ti site(s) to charge balance an inventory of CeO2 included as a structural analogue for Pu. The targeted solid solution was prepared by sintering constituent oxides at 1400 °C for 10 h under an air atmosphere. By means of powder XRD refinement and selected area electron diffraction analysis, the dominant zirconolite polytype was confirmed to be 2M across the solid solution. The obtained product density was significantly increased when compared to the previously discussed Ca1-xCexZrTi2-2xCr2xO7 system, suggesting that the partial inclusion of Fe in a 1:1 molar ratio with Cr may improve sintering behaviour. The limit of solid solution was reached at approximately x = 0.30, for which the segregation of CeO2 and Cr2O3 phases was clearly evidenced. An evaluation of obtained chemical compositions and bulk oxidation states was performed to inform the solid solution mechanism of Ce, Cr and Fe within zirconolite.
Keywords:Zirconolite  Plutonium  Solid solution  Wasteform
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