Different mechanisms of A-site and B-site high entropy effect on radiation tolerance of pyrochlores  

作　　者：Yuxin Li Yiming Lei Hao Xiao Shuang Zhao Yugang Wang Zini Cao Jie Zhang Jingyang Wang Guowei Lu Liuxuan Cao Chenxu Wang 

机构地区：[1]State Key Laboratory of Nuclear Physics and Technology,Center for Applied Physics and Technology,Peking University,Beijing 100871,China [2]Shenyang National Laboratory for Materials Science,Institute of Metal Research,Chinese Academy of Sciences,Shenyang 110016,China [3]State Key Laboratory for Mesoscopic Physics,Frontiers Science Center for Nano-Optoelectronics&Collaborative Innovation Center of Quantum Matter,School of Physics,Peking University,Beijing 100871,China [4]College of Energy,Xiamen University,Xiamen 361102,China

出　　处：《Journal of Materials Science & Technology》2024年第24期250-258,共9页材料科学技术(英文版)

基　　金：supported by the National Natural Science Foundation of China(Grant Nos.12275009,12192280,and 11935004);the National Magnetic Confinement Fusion Energy Research Project(No.2021YFE031100).

摘　　要：The properties of high entropy pyrochlore have been studied extensively,but there is no consistent conclusion on its radiation tolerance.Besides,the mechanism of the high entropy effect on the radiation tolerance of pyrochlore is still unclear.In this work,combined with experiments and calculations of pyrochlores with similar cationic radius ratios,the A-site and B-site high entropy effects on structural evolution under irradiation are analyzed.In situ irradiation experiments were carried out on A-site high entropy pyrochlores such as(La_(0.2)Nd_(0.2)Sm_(0.2)Gd_(0.2)Er_(0.2))_(2)Zr_(2)O_(7),B-site Gd_(2)(Ti_(1/3)Sn_(1/3)Zr_(1/3))_(2)O_(7),and ternary pyrochlore Sm_(2)Zr_(2)O_(7) and Gd_(2)Sn_(2)O_(7) for comparison.The A-site high entropy pyrochlore can maintain a stable structure under high fluence irradiation like corresponding ternary pyrochlore,demonstrated by high angle annular dark field scanning transmission electron microscopy(HAADF-STEM),energy dispersive spectroscopy(EDS)mapping and Raman spectrum.The additional irradiation experiments on A-site high entropy pyrochlores(La_(1/3)Nd_(1/3)Gd_(1/3))_(2)Zr_(2)O_(7) and(Nd_(1/3)Sm_(1/3)Gd_(1/3))_(2)Zr_(2)O_(7) also confirm the similarity under irradiation between A-site high entropy and ternary pyrochlores.However,the B-site high entropy pyrochlore Gd_(2)(Ti_(1/3)Sn_(1/3)Zr_(1/3))_(2)O_(7) becomes amorphous at exceptionally low irradiation fluences,indicating a significantly distinct radiation tolerance compared with the A-site high entropy.The difference between the A-site and B-site high entropy effect is analyzed from cationic lattice distortion,bond strength,and inner electron binding energy by first-principles calculations.The results reveal the role and mechanism of the high entropy effect in pyrochlores and lay a foundation for material design and future applications.

关 键 词：High entropy pyrochlores In situ irradiation Crystal overlap Hamilton population Electron binding energy 

分 类 号：TG139[一般工业技术—材料科学与工程]