A density functional theory(DFT)study was employed to investigate the mechanical property,thermal conductivity,Debye temperature,electronic structure and defect chemistry of(Gd_(1-x)Sm_(x))_(2)Zr_(2)O_(7).All the(Gd_(...A density functional theory(DFT)study was employed to investigate the mechanical property,thermal conductivity,Debye temperature,electronic structure and defect chemistry of(Gd_(1-x)Sm_(x))_(2)Zr_(2)O_(7).All the(Gd_(1-x)Sm_(x))_(2)Zr_(2)O_(7) compounds exhibit an excellent structural and mechanical stability(Gd_(0.25)Sm_(0.75))_(2)Zr_(2)O_(7) has the lowest Young’s modulus of 213.7 GPa,the largest Possion’s ratio of 0.292,the lowest Debye temperature of 491.8 K and the lowest thermal conductivity.The calculated thermal conductivities of(Gd_(1-x)Sm_(x))_(2)Zr_(2)O_(7) are 1.17-1.21 W/(m·K)by the Clark’s model and 1.32-1.36 W/(m·K)by the Cahall’s model,respectively.The formation energies of O vacancies at 48f site are negative,which increase with the Sm content,however,the formation energies of O vacancies at 8b site are almost invariable.In addition,Sm partly occupying the Gd-site reduces distinctly the formation energies of defects such as A-site vacancies,cation antisite defects,anion Frenkel pairs of oxygen at 8b site and cation interstitials,which suggests that Sm-doped Gd_(2)Zr_(2)O_(7),especially equimolar GdSmZr_(2)O_(7),has a better irradiation tolerance.After the 16 MeVTa-ion irradiation at a fluence of 1×10^(14) or 2×10^(14) ions/cm^(2),the crystal structure of GdSmZr_(2)O_(7) transforms from pyrochlore to a defect fluorite without obvious amorphous phase.展开更多
基金Project supported by the National Natural Science Foundation of China(51621091,51321061,51021002)the National Science and Technology Major Project(2017-Ⅵ-0020-0093)。
文摘A density functional theory(DFT)study was employed to investigate the mechanical property,thermal conductivity,Debye temperature,electronic structure and defect chemistry of(Gd_(1-x)Sm_(x))_(2)Zr_(2)O_(7).All the(Gd_(1-x)Sm_(x))_(2)Zr_(2)O_(7) compounds exhibit an excellent structural and mechanical stability(Gd_(0.25)Sm_(0.75))_(2)Zr_(2)O_(7) has the lowest Young’s modulus of 213.7 GPa,the largest Possion’s ratio of 0.292,the lowest Debye temperature of 491.8 K and the lowest thermal conductivity.The calculated thermal conductivities of(Gd_(1-x)Sm_(x))_(2)Zr_(2)O_(7) are 1.17-1.21 W/(m·K)by the Clark’s model and 1.32-1.36 W/(m·K)by the Cahall’s model,respectively.The formation energies of O vacancies at 48f site are negative,which increase with the Sm content,however,the formation energies of O vacancies at 8b site are almost invariable.In addition,Sm partly occupying the Gd-site reduces distinctly the formation energies of defects such as A-site vacancies,cation antisite defects,anion Frenkel pairs of oxygen at 8b site and cation interstitials,which suggests that Sm-doped Gd_(2)Zr_(2)O_(7),especially equimolar GdSmZr_(2)O_(7),has a better irradiation tolerance.After the 16 MeVTa-ion irradiation at a fluence of 1×10^(14) or 2×10^(14) ions/cm^(2),the crystal structure of GdSmZr_(2)O_(7) transforms from pyrochlore to a defect fluorite without obvious amorphous phase.
