Designing nanostructure exsolution-self-assembly in a complex concentrated oxide
Designing nanostructure exsolution-self-assembly in a complex concentrated oxide
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DOI：
10.1016/j.matt.2023.12.012
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发表时间：
2024-03-06
期刊：
影响因子：
18.9
通讯作者：
Bowman，William J.
中科院分区：
文献类型：
--
作者：
Guo，Huiming;Mead，Christopher;Bowman，William J.
复杂浓缩氧化物 (CCO) 是一类新兴材料，包括高熵和熵稳定氧化物，其特性源于无序诱导的电子结构和由超过 5 个阳离子的稳定固溶体引起的化学反应。将 CCO 集成到复合材料中将扩展材料设计，超越单相范式。我们通过一种简单的方法展示了可调节的 CCO 衍生纳米结构：外溶自组装 (ESA)，这是一种指导纳米复合材料中纳米粒子和纳米棒演化的一步方法。我们使用原子级探针对 CCO 的驱动力和形成机制有了基本的了解，这表明 ESA 可以使用 CCO 钙钛矿 LaFe0.7Ni0.1Co0.1Pd0.05Ru0.05O3-δ 模型中的 Ellingham 阳离子还原性模型来指导。这种方法能够实现多元素纳米棒和纳米颗粒复合结构的定制生长，其形成与室温下超过 0.1 S/cm 的电子电导率相关。鉴于 CCO 的巨大组合空间，ESA 有望通过集成各种成分和晶体结构而具有高度可扩展性。
Complex concentrated oxides (CCOs) are an emerging material class that includes high-entropy and entropy-stabilized oxides whose properties stem from disorder-induced electronic structure and chemistry caused by stabilizing solid solutions of >5 cations. Integrating CCOs into composites will expand material design beyond the single-phase paradigm. We demonstrate tunable CCO-derived nanostructures by a simple method: exsolution-self-assembly (ESA), a one-step approach to direct the evolution of nanoparticles and nanorods in nanocomposites. We have developed a fundamental understanding of driving forces and formation mechanisms in CCOs using atomic-scale probes, which reveal that ESA can be directed using Ellingham's model of cation reducibility in a model CCO perovskite LaFe0.7Ni0.1Co0.1Pd0.05Ru0.05O3-δ. This approach enables tailored growth of multielement nanorod and nanoparticle composite structures whose formation is correlated with electronic conductivity that exceeds 0.1 S/cm at room temperature. Given the vast combinatorial space of CCOs, ESA is expected to be highly extensible via the integration of various compositions and crystal structures.