锂离子电池Li$_{3}$OCl固态电解质中替代缺陷的$Ab$ $initio$研究
$Ab$ $initio$ Study of Substitutional Defects in Li$_{3}$OCl Solid Electrolyte for Li-ion Batteries
浏览论文内容
中文总结 AI 辅助
本研究通过密度泛函理论计算，探讨了中子辐照产生的B、He、H替代缺陷对反钙钛矿固态电解质Li$_3$OCl缺陷化学的调控作用，为全固态电池材料设计提供了新策略。
中文摘要 AI 辅助
改善固态电解质和正极涂层中的离子传输仍然是全固态锂离子电池的关键挑战，因为其室温离子电导率仍远低于液态电解质。在我们之前的实验与理论联合研究中，我们表明热中子辐照能够通过$^6$Li和$^{10}$B的嬗变在LiBO$_2$中实现缺陷工程，产生晶格空位，从而增强离子电导率。在此，我们考察这种方法能否推广到Li$_3$OCl——一种代表性的反钙钛矿固态电解质。利用密度泛函理论，我们研究了与B掺杂及中子俘获反应$^{6}\mathrm{Li}+n\rightarrow\\,^{3}\mathrm{H}+\alpha$和$^{10}\mathrm{B}+n\rightarrow\\,^{7}\mathrm{Li}+\alpha+\gamma$相关的Li位点上的B、He和H替代缺陷。我们评估了缺陷形成能、由此产生的结构畸变，并将这些替代缺陷与Li位点上的其他单阳离子、双阳离子和三阳离子替代进行了比较。我们的结果表明，与中子辐照相关的替代缺陷为调控反钙钛矿固态电解质的缺陷化学提供了一条可行途径，并支持将中子驱动的缺陷工程作为开发高性能全固态锂离子电池先进材料的策略。
英文摘要
Improving ion transport in solid electrolytes and cathode coatings remains a key challenge for all-solid-state Li-ion batteries because their room-temperature ionic conductivity is still substantially lower than that of liquid electrolytes. In our previous combined experimental and theoretical study, we showed that thermal neutron irradiation enables defect engineering in LiBO$_2$ through the transmutation of $^6$Li and $^{10}$B, generating lattice vacancies that enhance ionic conductivity. Here, we examine whether this approach can be extended to Li$_3$OCl, a representative antiperovskite solid electrolyte. Using density functional theory, we investigate substitutional defects at Li sites involving B, He, and H, associated with B doping and the neutron-capture reactions $^{6}\mathrm{Li}+n\rightarrow\,^{3}\mathrm{H}+α$ and $^{10}\mathrm{B}+n\rightarrow\,^{7}\mathrm{Li}+α+γ$. We evaluate defect formation energetics, the resulting structural distortions, and compare these substitutional defects with other mono-, di-, and trication substitutions at Li sites. Our results show that substitutional defects associated with neutron irradiation provide a feasible route to tune the defect chemistry of antiperovskite solid electrolytes and support neutron-driven defect engineering as a strategy for developing advanced materials for high-performance all-solid-state Li-ion batteries.
发表机构
- University of Missouri Research Reactor, University of Missouri（密苏里大学研究反应堆，密苏里大学）
- Department of Physics and Astronomy, University of Missouri（密苏里大学物理与天文学系）
- Materials Science and Engineering Institute, University of Missouri（密苏里大学材料科学与工程研究所）
- Department of Chemical and Biomedical Engineering, University of Missouri（密苏里大学化学与生物医学工程系）
机构由 AI 辅助整理，请以论文原文为准。
