Liang Jingjing, Liu Junlin, Wang Huiliu, Li Zeyuan, Cao Guanghui, Zeng Ziyue, Liu Sheng, Guo Yuzheng, Zeng Mengqi, Fu Lei
The Institute for Advanced Studies, Wuhan University, Wuhan 430072, China.
College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, China.
J Am Chem Soc. 2024 Mar 20;146(11):7118-7123. doi: 10.1021/jacs.3c10868. Epub 2024 Mar 4.
High-entropy oxides (HEOs) with an ultrathin geometric structure are especially expected to exhibit extraordinary performance in different fields. The phase structure is deemed as a key factor in determining the properties of HEOs, rendering their phase control synthesis tempting. However, the disparity in intrinsic phase structures and physicochemical properties of multiple components makes it challenging to form single-phase HEOs with the target phase. Herein, we proposed a self-lattice framework-guided strategy to realize the synthesis of ultrathin HEOs with desired phase structures, including rock-salt, spinel, perovskite, and fluorite phases. The participation of the Ga assistor was conducive to the formation of the high-entropy mixing state by decreasing the formation energy. The as-prepared ultrathin spinel HEOs were demonstrated to be an excellent catalyst with high activity and stability for the oxygen evolution reaction in water electrolysis. Our work injects new vitality into the synthesis of HEOs for advanced applications and undoubtedly expedites their phase engineering.
具有超薄几何结构的高熵氧化物(HEOs)尤其有望在不同领域展现出非凡性能。相结构被视为决定HEOs性质的关键因素,这使得它们的相控合成颇具吸引力。然而,多种组分在固有相结构和物理化学性质上的差异使得形成具有目标相的单相HEOs具有挑战性。在此,我们提出了一种自晶格框架引导策略,以实现具有所需相结构的超薄HEOs的合成,包括岩盐相、尖晶石相、钙钛矿相和萤石相。Ga助剂的参与通过降低形成能有利于形成高熵混合态。所制备的超薄尖晶石HEOs被证明是一种用于水电解析氧反应的具有高活性和稳定性的优异催化剂。我们的工作为用于先进应用的HEOs合成注入了新的活力,无疑加快了它们的相工程进程。