Xiaoyu Ji , Penghui Lei , Jiahao Chen , Jie Qiu , Qing Peng , Di Yun
{"title":"放电等离子烧结固结（Gd0.2Sm0.2Dy0.2Er0.2Yb0.2）2Ti2O7高熵焦绿石废弃物的合成及辐照行为","authors":"Xiaoyu Ji , Penghui Lei , Jiahao Chen , Jie Qiu , Qing Peng , Di Yun","doi":"10.1016/j.vacuum.2024.113893","DOIUrl":null,"url":null,"abstract":"<div><div>The development of spent fuel reprocessing, which generates large amounts of high-level waste, necessitates effective management of waste containing radioactive elements. Pyrochlore (A<sub>2</sub>B<sub>2</sub>O<sub>7</sub>) is considered one of the most promising immobilized matrixes for high-level waste due to its excellent physicochemical stability and irradiation resistance. A novel kind of high-entropy pyrochlore ceramic (Gd<sub>0.2</sub>Sm<sub>0.2</sub>Dy<sub>0.2</sub>Er<sub>0.2</sub>Yb<sub>0.2</sub>)<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub>, as an improved waste form matrix, was successfully synthesized using spark plasma sintering in this work. The mechanical properties, physical density, and microstructure of the densified pellets have been investigated in relation to different sintering temperatures (ranging from 1000 °C to 1400 °C). A single-component pyrochlore phase high-entropy ceramic was densified at 1300 °C, achieving a maximum hardness of 12.68 GPa and a density of 97.64 %. The irradiation tolerance of high-entropy pyrochlore was assessed by ion irradiation of 400 keV He<sup>+</sup> with 10 × 10<sup>17</sup> ions/cm<sup>2</sup> at room temperature (RT). Ion irradiation can induce the transformation of the pyrochlore superlattice of (Gd<sub>0.2</sub>Sm<sub>0.2</sub>Dy<sub>0.2</sub>Er<sub>0.2</sub>Yb<sub>0.2</sub>)<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub> into a fluorite sublattice. Compared to Gd<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub>, (Gd<sub>0.2</sub>Sm<sub>0.2</sub>Dy<sub>0.2</sub>Er<sub>0.2</sub>Yb<sub>0.2</sub>)<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub> exhibits significantly reduced irradiation damage with suppressed generation and coalescence of helium bubbles due to chemical disorder and lattice distortion. High-entropy pyrochlore (Gd<sub>0.2</sub>Sm<sub>0.2</sub>Dy<sub>0.2</sub>Er<sub>0.2</sub>Yb<sub>0.2</sub>)<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub> exhibits superior mechanical properties and irradiation resistance, suggesting its application as a promising immobilization matrix for nuclear waste.</div></div>","PeriodicalId":23559,"journal":{"name":"Vacuum","volume":"232 ","pages":"Article 113893"},"PeriodicalIF":3.8000,"publicationDate":"2024-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synthesis and irradiation behavior of (Gd0.2Sm0.2Dy0.2Er0.2Yb0.2)2Ti2O7 high-entropy pyrochlore waste forms consolidated by spark plasma sintering\",\"authors\":\"Xiaoyu Ji , Penghui Lei , Jiahao Chen , Jie Qiu , Qing Peng , Di Yun\",\"doi\":\"10.1016/j.vacuum.2024.113893\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The development of spent fuel reprocessing, which generates large amounts of high-level waste, necessitates effective management of waste containing radioactive elements. Pyrochlore (A<sub>2</sub>B<sub>2</sub>O<sub>7</sub>) is considered one of the most promising immobilized matrixes for high-level waste due to its excellent physicochemical stability and irradiation resistance. A novel kind of high-entropy pyrochlore ceramic (Gd<sub>0.2</sub>Sm<sub>0.2</sub>Dy<sub>0.2</sub>Er<sub>0.2</sub>Yb<sub>0.2</sub>)<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub>, as an improved waste form matrix, was successfully synthesized using spark plasma sintering in this work. The mechanical properties, physical density, and microstructure of the densified pellets have been investigated in relation to different sintering temperatures (ranging from 1000 °C to 1400 °C). A single-component pyrochlore phase high-entropy ceramic was densified at 1300 °C, achieving a maximum hardness of 12.68 GPa and a density of 97.64 %. The irradiation tolerance of high-entropy pyrochlore was assessed by ion irradiation of 400 keV He<sup>+</sup> with 10 × 10<sup>17</sup> ions/cm<sup>2</sup> at room temperature (RT). Ion irradiation can induce the transformation of the pyrochlore superlattice of (Gd<sub>0.2</sub>Sm<sub>0.2</sub>Dy<sub>0.2</sub>Er<sub>0.2</sub>Yb<sub>0.2</sub>)<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub> into a fluorite sublattice. Compared to Gd<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub>, (Gd<sub>0.2</sub>Sm<sub>0.2</sub>Dy<sub>0.2</sub>Er<sub>0.2</sub>Yb<sub>0.2</sub>)<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub> exhibits significantly reduced irradiation damage with suppressed generation and coalescence of helium bubbles due to chemical disorder and lattice distortion. High-entropy pyrochlore (Gd<sub>0.2</sub>Sm<sub>0.2</sub>Dy<sub>0.2</sub>Er<sub>0.2</sub>Yb<sub>0.2</sub>)<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub> exhibits superior mechanical properties and irradiation resistance, suggesting its application as a promising immobilization matrix for nuclear waste.</div></div>\",\"PeriodicalId\":23559,\"journal\":{\"name\":\"Vacuum\",\"volume\":\"232 \",\"pages\":\"Article 113893\"},\"PeriodicalIF\":3.8000,\"publicationDate\":\"2024-11-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Vacuum\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0042207X24009394\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Vacuum","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0042207X24009394","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
Synthesis and irradiation behavior of (Gd0.2Sm0.2Dy0.2Er0.2Yb0.2)2Ti2O7 high-entropy pyrochlore waste forms consolidated by spark plasma sintering
The development of spent fuel reprocessing, which generates large amounts of high-level waste, necessitates effective management of waste containing radioactive elements. Pyrochlore (A2B2O7) is considered one of the most promising immobilized matrixes for high-level waste due to its excellent physicochemical stability and irradiation resistance. A novel kind of high-entropy pyrochlore ceramic (Gd0.2Sm0.2Dy0.2Er0.2Yb0.2)2Ti2O7, as an improved waste form matrix, was successfully synthesized using spark plasma sintering in this work. The mechanical properties, physical density, and microstructure of the densified pellets have been investigated in relation to different sintering temperatures (ranging from 1000 °C to 1400 °C). A single-component pyrochlore phase high-entropy ceramic was densified at 1300 °C, achieving a maximum hardness of 12.68 GPa and a density of 97.64 %. The irradiation tolerance of high-entropy pyrochlore was assessed by ion irradiation of 400 keV He+ with 10 × 1017 ions/cm2 at room temperature (RT). Ion irradiation can induce the transformation of the pyrochlore superlattice of (Gd0.2Sm0.2Dy0.2Er0.2Yb0.2)2Ti2O7 into a fluorite sublattice. Compared to Gd2Ti2O7, (Gd0.2Sm0.2Dy0.2Er0.2Yb0.2)2Ti2O7 exhibits significantly reduced irradiation damage with suppressed generation and coalescence of helium bubbles due to chemical disorder and lattice distortion. High-entropy pyrochlore (Gd0.2Sm0.2Dy0.2Er0.2Yb0.2)2Ti2O7 exhibits superior mechanical properties and irradiation resistance, suggesting its application as a promising immobilization matrix for nuclear waste.
期刊介绍：
Vacuum is an international rapid publications journal with a focus on short communication. All papers are peer-reviewed, with the review process for short communication geared towards very fast turnaround times. The journal also published full research papers, thematic issues and selected papers from leading conferences.
A report in Vacuum should represent a major advance in an area that involves a controlled environment at pressures of one atmosphere or below.
The scope of the journal includes:
1. Vacuum; original developments in vacuum pumping and instrumentation, vacuum measurement, vacuum gas dynamics, gas-surface interactions, surface treatment for UHV applications and low outgassing, vacuum melting, sintering, and vacuum metrology. Technology and solutions for large-scale facilities (e.g., particle accelerators and fusion devices). New instrumentation ( e.g., detectors and electron microscopes).
2. Plasma science; advances in PVD, CVD, plasma-assisted CVD, ion sources, deposition processes and analysis.
3. Surface science; surface engineering, surface chemistry, surface analysis, crystal growth, ion-surface interactions and etching, nanometer-scale processing, surface modification.
4. Materials science; novel functional or structural materials. Metals, ceramics, and polymers. Experiments, simulations, and modelling for understanding structure-property relationships. Thin films and coatings. Nanostructures and ion implantation.
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