低价锆氧化物Zr_(3)O的结构、热力学和弹性性质第一性原理研究  

First-principles investigation on structural,thermodynamic,and elastic properties of suboxide Zr_(3)O phase

作　　者：周虹伶 陈莉君 杨晓玲 刘许旸[2] 孙超[3] 栾佰峰[1,4] Hong-ling ZHOU;Li-jun CHEN;Xiao-ling YANG;Xu-yang LIU;Chao SUN;Bai-feng LUAN(International Joint Laboratory for Light Alloys(Ministry of Education),Shenyang National Laboratory for Materials Science,College of Materials Science and Engineering,Chongqing University,Chongqing 400044,China;College of Aerospace Engineering,Chongqing University,Chongqing 400044,China;Science and Technology on Reactor Fuel and Materials Laboratory,Nuclear Power Institute of China,Chengdu 610213,China;State Key Laboratory of Mechanical Transmissions,Chongqing University,Chongqing 400044,China)

机构地区：[1]重庆大学材料科学与工程学院轻合金材料国际合作联合实验室,沈阳材料科学国家研究中心,重庆400044 [2]重庆大学航空航天学院,重庆400044 [3]中国核动力研究设计院反应堆燃料及材料重点实验室,成都610213 [4]重庆大学机械传动国家重点实验室,重庆400044

出　　处：《Transactions of Nonferrous Metals Society of China》2024年第3期952-965,共14页中国有色金属学报（英文版）

基　　金：financially supported by the National Natural Science Foundation of China(Nos.U20A20232,U1867202)。

摘　　要：采用第一性原理系统地研究3种Zr_(3)O晶形(空间群分别为R3c(斜方六面体)、R32(斜方六面体)和P6322(六面体))的晶格动力学及其与温度相关的热力学和力学性质。计算得到的3种Zr_(3)O晶形的晶体结构参数与实验结果一致。此外,证明3种Zr_(3)O结构在动力学和热力学上均具有稳定性。获得了3种Zr_(3)O晶形在0~1500 K温度范围内的熵、焓、吉布斯自由能、比热容、热膨胀系数和弹性模量等性质。发现3种Zr_(3)O晶形在0K时的相对稳定性顺序为Zr_(3)O(R3c)>Zr_(3)O(R32)>Zr_(3)O(P6_(3)22);然而,在50 K时Zr_(3)O(R3c)转变成Zr_(3)O(R32),在540K时转变为Zr_(3)O(P6_(3)22)。相较于其他2种Zr_(3)O相,Zr_(3)O(R32)表现出更优越的力学性能。The lattice dynamics and finite-temperature thermodynamic and mechanical properties of three Zr_(3)O polymorphs,including rhombohedral(R3-c),rhombohedral(R32),and hexagonal(P6_(3)22)phases,were theoretically investigated using the first-principles calculations.The calculated lattice parameters agree well with experimental values.It is confirmed that the three Zr_(3)O phases exhibit both dynamic and thermodynamic stability.The entropy,enthalpy,Gibbs free energy,specific heat capacity,thermal expansion coefficient,and elastic modulus as a function of temperature from 0 to 1500 K were systematically evaluated.It is found that Zr_(3)O(R3-c)is the ground state at 0 K followed by Zr_(3)O(R32)and Zr_(3)O(P6_(3)22).Structural phase transitions occur from Zr_(3)O(R3-c)to Zr_(3)O(R32)at 50 K and then to Zr_(3)O(P6_(3)22)at 540 K.Zr_(3)O(R32)displays superior mechanical properties compared to the other two Zr_(3)O phases.

关 键 词：第一性原理 Zr_(3)O 晶格动力学 热力学性质 弹性模量 

分 类 号：TQ134.12[化学工程—无机化工]