Epitaxial growth mechanism and structural characterization of spinel-type LixMn2O4 electrodes realized via pulsed laser deposition

IF 3 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materialia Pub Date : 2025-03-01 DOI:10.1016/j.mtla.2025.102382

S. Sanna , P. Orgiani , O. Krymskaya , D. Di Castro , A. Galdi , M. Tkalčević , C. Aruta , A. Tebano

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Abstract

Spinel-type lithium manganese oxide (LiMn₂O₄) is considered one of the most promising cathode materials for rechargeable batteries due to its high operating voltage, reduced toxicity, and lower cost compared to cobalt-based cathodes. However, the stability of LiMn₂O₄ is a significant challenge, as it tends to degrade over time, with manganese ion segregation leading to a reduction in battery capacity.

The crystal structure of Li_xMn₂O₄ is highly dependent on the lithium content (x), and it can exist either in a single-phase or a two-phase form. These structural variations significantly affect the material's electrochemical performance. In this work, we present the growth and structural characterization of Li_xMn₂O₄ thin films, with (x) values of 1 and 0.7, aimed at improving chemical stability and overall performance.

The epitaxial Li_xMn₂O₄ films were deposited using Pulsed Laser Deposition on different single-crystal substrates, including water-soluble Sr₃Al₂O₆-buffered SrTiO₃(100). Films grown on MgO(001) for both x = 1 and x = 0.7 exhibited excellent crystallographic quality, while films deposited on SrTiO₃(001) showed good quality for x = 1, albeit with a slightly higher mosaic spread compared to those on MgO. Notably, for x = 0.7, a two-phase region was observed on the SrTiO₃ and MgO substrates, where both phases shared the same structure but differed slightly in lattice parameters.

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通过脉冲激光沉积实现的尖晶石型 LixMn2O4 电极的外延生长机理和结构表征

尖晶石型锂锰氧化物（LiMn2O4）被认为是最有前途的充电电池正极材料之一，因为与钴基正极相比，它具有工作电压高、毒性低、成本低等优点。然而，锰酸锂的稳定性是一个重大挑战，因为它往往会随着时间的推移而降解，锰离子偏析会导致电池容量降低。锰酸锂的晶体结构与锂含量（x）有很大关系，它可以以单相或两相形式存在。这些结构变化极大地影响了材料的电化学性能。在这项工作中，我们介绍了 (x) 值为 1 和 0.7 的 LixMn2O4 薄膜的生长和结构特征，旨在提高其化学稳定性和整体性能。我们采用脉冲激光沉积法在不同的单晶基底（包括水溶性 Sr3Al2O6 缓冲 SrTiO3（100））上沉积了 LixMn2O4 外延薄膜。在氧化镁（001）上生长的薄膜在 x = 1 和 x = 0.7 时都表现出极佳的晶体学质量，而在 SrTiO3（001）上沉积的薄膜在 x = 1 时也表现出良好的质量，尽管与氧化镁上的薄膜相比，镶嵌分布略高。值得注意的是，当 x = 0.7 时，在 SrTiO3 和氧化镁基底上观察到两相区域，两相具有相同的结构，但在晶格参数上略有不同。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Materialia MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

6.40

自引率

2.90%

发文量

345

审稿时长

36 days

期刊介绍： Materialia is a multidisciplinary journal of materials science and engineering that publishes original peer-reviewed research articles. Articles in Materialia advance the understanding of the relationship between processing, structure, property, and function of materials. Materialia publishes full-length research articles, review articles, and letters (short communications). In addition to receiving direct submissions, Materialia also accepts transfers from Acta Materialia, Inc. partner journals. Materialia offers authors the choice to publish on an open access model (with author fee), or on a subscription model (with no author fee).