Impact of Synthesis Method on the Structure and Function of High Entropy Oxides

化学 微晶 铁磁性 同质性(统计学) 微观结构 组态熵 尖晶石 分析化学(期刊) 化学物理 热力学 结晶学 磁化 磁场 物理 统计 量子力学 色谱法 数学 冶金 材料科学
作者
Mario U. González-Rivas,Solveig S. Aamlid,Megan Rutherford,Jessica Freese,Ronny Sutarto,Ning Chen,Edgar E. Villalobos-Portillo,Hiram Castillo-Michel,Minu Kim,H. Takagi,Robert J. Green,Alannah M. Hallas
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:146 (38): 26048-26059 被引量:3
标识
DOI:10.1021/jacs.4c05951
摘要

The term sample dependence describes the troublesome tendency of nominally equivalent samples to exhibit different physical properties. High entropy oxides (HEOs) are a class of materials where sample dependence has the potential to be particularly profound due to their inherent chemical complexity. In this work, we prepare a spinel HEO of identical nominal composition by five distinct methods, spanning a range of thermodynamic and kinetic conditions: solid state, high pressure, hydrothermal, molten salt, and combustion syntheses. By structurally characterizing these five samples across all length scales with a variety of X-ray methods, we find that while the average structure is unaltered, the samples vary significantly in their local structures and their microstructures. The most profound differences are observed at intermediate length scales, both in terms of crystallite morphology and cation homogeneity. As revealed by X-ray fluorescence microscopy ideal cation homogeneity is achieved only in the case of combustion synthesis. These structural differences in turn significantly alter the observed functional properties, which we demonstrate via characterization of their magnetic response. While ferrimagnetic order is retained across all five samples, the sharpness of the transition, the size of the saturated moment, and the coercivity all show marked variations with synthesis method. We conclude that the chemical flexibility inherent to HEOs is complemented by strong synthesis method dependence, providing another axis along which to optimize these materials for a wide range of applications.
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