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铕掺杂Gd2Zr2O7透明陶瓷的制备及闪烁性能OA北大核心CSTPCD

Preparation and Scintillation Properties of Europium-Doped Gd2Zr2O7 Transparent Ceramics

中文摘要英文摘要

与传统闪烁陶瓷相比,基于立方相Gd2Zr2O7具有高密度、高光学透过率和良好的闪烁性能等特征,本工作采用真空烧结法,成功制备出系列Eu3+掺杂Gd2Zr2O7透明陶瓷,研究了掺杂离子及掺杂量对其晶体结构、光学透过率、荧光性能及闪烁性能的影响.结果表明,所制备的透明陶瓷样品具有良好的光透过能力;光谱表征发现,20%Eu3+掺杂Gd2Zr2O7具有最佳的光致荧光和辐照发光强度,其最强发射峰位于630nm.X射线成像实验表明,Gd1.8Eu0.2Zr2O7透明陶瓷的X射线成像分辨率可达11 lp·mm-1,具备对不同材质物体的成像应用潜力.在医学成像、工业探伤、高能物理等领域具有潜在的应用价值.

Introduction This paper prepared a series of Eu3+doped Gd2Zr2O7 transparent ceramics by a vacuum sintering method,and charaterized the density and optical transmittance of cubic phase Gd2Zr2O7.The effects of doping ions and their concentration on the crystal structure,optical transmittance,fluorescence performance,and scintillation performance were investigated.The results show that the prepared transparent ceramic samples have a good optical transmittance.The spectral characterization reveals that 20%Eu3+doped Gd2Zr2O7 has optimum fluorescence and irradiated luminescence intensity,and the most intense emission peak is located at 630 nm.The X-ray imaging shows that Gd1.8Eu0.2Zr2O7 transparent ceramics have an X-ray imaging resolution of up to 11 lp·mm-1,having a potential for the imaging applications. Methods High purity gadolinium oxide,europium oxide and zirconia(purity 4N)as raw materials were mixed according to a stoichiometric ratio(Gd3+,Eu3+)∶Zr4+of 1∶1.The mixed raw materials were ground in anhydrous ethanol and polyethylene glycol(PEG)in a planetary mill with zirconia grinding chamber and ballsat a ball:material mass ratio of 27∶1 for 72 h.Afterwards,the ground mixture slurry was washed with anhydrous ethanol after drying.Gd2-xEuxZr2O7 could be obtained via sintering in a box furnace at 1 400 ℃ according to the reaction∶Gd2-xEuxZr2O7(1-x/2)Gd2O3+2ZrO2+x/2Eu2O3 → Gd2-x EuxZr2O7(x=0-0.28)The ceramic blank was formed via dry pressing and cold isostatic pressing,sintered in a vacuum tungsten furnace at 1 800 ℃ for 10h,and then annealed in a box furnace in air at 1 250 ℃ for 6h.Finally,a transparent ceramic with 1 mm thickness was obtained after double-sided polishing. Results and discussion A ceramic powder prepared by ball grinding was sintered in a vacuum tungsten wire furnace to prepare transparent ceramics with a high light transmission rate.The XRD results show that when 20%Eu3+is added to Gd2Zr2O7,the crystal structure of Gd1.8Eu0.2Zr2O7 appears some superlattice diffraction peaks(331)of pyrochlore.The crystal structure changes from defective fluorite to pyrochlore.The optical transmittance spectra indicate that the optical transmittance decreases from 76%to 65%(@1 500 nm)when the doping content of Eu3+increases from 0 to 28%.There exist 6 distinct excitation peaks between 230 nm and 500 nm.A wide excitation peak at 267 nm is attributed to the charge transfer band of O2--Eu3+.In addition,five excitation peaks at 362,382,393,414 nm and 465 nm correspond to 4f-4f energy level transitions 7F0→5D4,5GJ,5L6,5D3 and 5D2 in Eu3+,respectively.Among six excitation peaks,a wide excitation peak at 267 nm has the most intense intensity.All the excitation peak intensities increase when Eu3+concentration increases from 4%to 20%.When Eu3+doping amount is 20%,the maximum excitation peak intensity appears.The further characterization of the scintillation properties of ceramic samples indicates that the X-ray irradiation intensity is a maximum value when the doping amount is 20%.At 630nm,the radiation luminescence intensity value is 1.1×104,and the material has an X-ray absorption capacity equivalent to that of BGO crystals,and also has a good anti-radiation damage ability.Finally,X-ray imaging tests on Gd1.8Eu0.2Zr2O7 ceramic samples of different materials show that the Gd1.8Eu0.2Zr2O7 ceramic sample can clearly distinguish metal and plastic materials,and has a limit spatial resolution of 11 lp·mm 1,indicating that the modified material is a potential X-ray detection material. Conclusions A series of Eu3+doped transparent ceramics were prepared by a vacuum sintering method.The crystal structure of Gd2-xEuxZr2O7 was gradually changed from defective fluorite to pyrochlore via adjusting the doping amount of Eu3+.At 630 nm,the Gd2-xEuxZr2O7 transparent ceramic sample showed the optimum fluorescence emission and X-ray irradiation intensity,and the material had a limit spatial resolution of 11 lp·mm-1,which could clearly distinguish metal and plastic materials,confirming an application potential of the A2B2O7 series of scintillating transparent ceramics X-ray imaging.

孙志成;冯桂青;王帅华;丁雨憧;吴少凡

中国科学院福建物质结构研究所,福州,350002中国科学院福建物质结构研究所,福州,350002||闽都创新实验室,福州,350108中国电子科技集团公司第二十六研究所,重庆 400060

化学工程

烧绿石缺陷萤石透明陶瓷闪烁性能空间分辨率

pyrochloredefective fluoritetransparent ceramicsscintillation propertiesspatial resolution

《硅酸盐学报》 2024 (003)

746-754 / 9

国家自然基金面上项目(22075284);福建省自然科学基金杰出青年项目(2023J06051);中国科学院青年促进会(2019304);中国科学院仪器研制项目(YJKYYQ20210039).

10.14062/j.issn.0454-5648.20230725

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