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Intrinsic Defects in LiMn2O4: First-Principles Calculations
ACS Omega ( IF 3.7 ) Pub Date : 2021-08-12 , DOI: 10.1021/acsomega.1c01162 Xu Li 1 , Jianchuan Wang 1 , Shiwei Zhang 1 , Lixian Sun 2 , Weibin Zhang 3 , Feng Dang 3 , Hans J Seifert 4 , Yong Du 1
ACS Omega ( IF 3.7 ) Pub Date : 2021-08-12 , DOI: 10.1021/acsomega.1c01162 Xu Li 1 , Jianchuan Wang 1 , Shiwei Zhang 1 , Lixian Sun 2 , Weibin Zhang 3 , Feng Dang 3 , Hans J Seifert 4 , Yong Du 1
Affiliation
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Spinel LiMn2O4 has attracted wide attention due to its advantages of a high-voltage plateau, good capacity, environmental friendliness, and low cost. Due to different experimental synthesis methods and conditions, there are many intrinsic point defects in LiMn2O4. By means of first-principles calculations based on a reasonable magnetic configuration, we studied the formation energies, local structures, and charge compensation mechanism of intrinsic point defects in LiMn2O4. The formation energies of defects under the assumed O-rich equilibrium conditions were examined. It was found that O, Li, and Mn vacancies, Mn and Li antisites, and Li interstitial could appear in the lattice at some equilibrium conditions, but Mn interstitial is hard to form. The charge was compensated mainly by adjusting the oxidation state of Mn around the defect, except for the defects at the 8a Wyckoff site. The binding energies between point defects were calculated to shed light on the clustering of point defects. Furthermore, the diffusion of Li ions around the defects was discussed. Cation antisites led to a decrease of the Li diffusion barrier but O vacancy caused an increase of the barrier. This study provides theoretical support for understanding point defects in spinel LiMn2O4.
中文翻译：
LiMn2O4 的固有缺陷：第一性原理计算
尖晶石LiMn 2 O 4因其电压平台高、容量好、环境友好、成本低等优点而受到广泛关注。由于实验合成方法和条件不同，LiMn 2 O 4 中存在许多本征点缺陷。通过基于合理磁构型的第一性原理计算，我们研究了LiMn 2 O 4中本征点缺陷的形成能、局域结构和电荷补偿机制。. 检查了假设的富氧平衡条件下的缺陷形成能。发现在某些平衡条件下，晶格中可能出现 O、Li 和 Mn 空位、Mn 和 Li 反位点以及 Li 间隙，但 Mn 间隙很难形成。除了 8 a Wyckoff 位点的缺陷外，电荷主要通过调整缺陷周围 Mn 的氧化态来补偿。计算点缺陷之间的结合能以阐明点缺陷的聚类。此外，还讨论了锂离子在缺陷周围的扩散。阳离子反位导致Li扩散势垒降低，但O空位导致势垒增加。该研究为理解尖晶石LiMn 2 中的点缺陷提供了理论支持○ 4。
更新日期：2021-08-24
中文翻译：
LiMn2O4 的固有缺陷：第一性原理计算
尖晶石LiMn 2 O 4因其电压平台高、容量好、环境友好、成本低等优点而受到广泛关注。由于实验合成方法和条件不同，LiMn 2 O 4 中存在许多本征点缺陷。通过基于合理磁构型的第一性原理计算，我们研究了LiMn 2 O 4中本征点缺陷的形成能、局域结构和电荷补偿机制。. 检查了假设的富氧平衡条件下的缺陷形成能。发现在某些平衡条件下，晶格中可能出现 O、Li 和 Mn 空位、Mn 和 Li 反位点以及 Li 间隙，但 Mn 间隙很难形成。除了 8 a Wyckoff 位点的缺陷外，电荷主要通过调整缺陷周围 Mn 的氧化态来补偿。计算点缺陷之间的结合能以阐明点缺陷的聚类。此外，还讨论了锂离子在缺陷周围的扩散。阳离子反位导致Li扩散势垒降低，但O空位导致势垒增加。该研究为理解尖晶石LiMn 2 中的点缺陷提供了理论支持○ 4。
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