In this study, Ce-doped zirconolite was synthesized through high-temperature solid-state reaction at 1250 ℃ in air for 96 h. The crystal phase, microstructure and valence transition were studied by X-ray diffraction ...In this study, Ce-doped zirconolite was synthesized through high-temperature solid-state reaction at 1250 ℃ in air for 96 h. The crystal phase, microstructure and valence transition were studied by X-ray diffraction （XRD）, scanning electron microscopy （SEM）, and X-ray photoelectron spectroscopy （XPS）. Phase relations of CaZrl xCexTi207 systems were determined by XRD analyses and Rietveld refinements. Four different phases are identified, namely zirconolite, perovskite, pyrochlore, and cerianite. The phase transformation （2M-zirconolite → 4M-zirconolite →Ce-pyrochlore） is caused by cations rearrangement as cerium content increases. The solubility limit of cerium ions in CaZrl .xCexTi207 system is estimated to be approximately 0.80. Under sintering air atmosphere, partial reduction of Ce^4＋ in Ce^3＋ is detected in Ce 3d XPS soectra, and the ratio of Ce^3＋ and Ce^4＋ significantly decreases as cerium content increases.展开更多
基金Project supported by Foundation of Laboratory of National Defense Key Discipline for Nuclear Waste and Environmental Safety,Southwest University of Science and Technology(15yyhk16,17LZX606)National Natural Science Foundation of China(41302027)+3 种基金973 project(2014CB8460003)One-Thousand-Talents Scheme in Sichuan ProvinceHebei Outstanding Young ScholarsScience and Technology Program of Hebei Province(D2016403064,160446012 and 15211121)
文摘In this study, Ce-doped zirconolite was synthesized through high-temperature solid-state reaction at 1250 ℃ in air for 96 h. The crystal phase, microstructure and valence transition were studied by X-ray diffraction （XRD）, scanning electron microscopy （SEM）, and X-ray photoelectron spectroscopy （XPS）. Phase relations of CaZrl xCexTi207 systems were determined by XRD analyses and Rietveld refinements. Four different phases are identified, namely zirconolite, perovskite, pyrochlore, and cerianite. The phase transformation （2M-zirconolite → 4M-zirconolite →Ce-pyrochlore） is caused by cations rearrangement as cerium content increases. The solubility limit of cerium ions in CaZrl .xCexTi207 system is estimated to be approximately 0.80. Under sintering air atmosphere, partial reduction of Ce^4＋ in Ce^3＋ is detected in Ce 3d XPS soectra, and the ratio of Ce^3＋ and Ce^4＋ significantly decreases as cerium content increases.
