铈（x）钍（1-x）氧化物固溶体中氧空位的形成与迁移。

Oxygen vacancy formation and migration in Ce(x)Th(1-x)O2 solid solution.

机构信息

Department of Materials Science & Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States.

出版信息

J Phys Chem B. 2011 May 26;115(20):6524-33. doi: 10.1021/jp202016s. Epub 2011 May 5.

DOI:10.1021/jp202016s

Abstract

A local-density approximation with the Hubbard U correction (LDA+U) method has been employed to investigate oxygen vacancy formation and migration in Ce(x)Th(1-x)O(2). The addition of CeO(2) into ThO(2) significantly decreases the oxygen vacancy formation and migration energies. ThO(2) containing 50% CeO(2) exhibits the lowest calculated formation energy, 3.7 eV, and the lowest calculated migration energy, 0.2 eV, occurs for a CeO(2) content of 75%, suggesting that introducing CeO(2) into ThO(2) promotes the formation of mobile oxygen vacancies. If the ceria content is less than about 35%, the reduced Ce(x)Th(1-x)O(2) becomes antiferromagnetic (AFM), whereas the ferromagnetic (FM) state dominates for x values above about 35%, which may allow the tailoring of magnetic properties by varying the CeO(2) content.

摘要

采用带有 Hubbard U 修正的局域密度近似（LDA+U）方法研究了 Ce(x)Th(1-x)O(2)中氧空位的形成和迁移。在 ThO(2)中添加 CeO(2)显著降低了氧空位的形成和迁移能。CeO(2)含量为 50%的 ThO(2)具有最低的计算形成能，为 3.7 eV，而 CeO(2)含量为 75%时计算得到的最低迁移能为 0.2 eV，表明在 ThO(2)中引入 CeO(2)促进了可移动氧空位的形成。如果氧化铈的含量小于约 35%，则还原的 Ce(x)Th(1-x)O(2)会呈现反铁磁（AFM）态，而当 x 值大于约 35%时，亚铁磁（FM）态占主导地位，这可能允许通过改变 CeO(2)的含量来调整磁性。