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Hollow/Mesoporous Spherical La(Cr0.2 Fe0.2Co0.2Ni0.2Mn0.2)O3 High-entropy Oxide Anode toward Ultrafast and Stable Lithium Storage

Journal 2025 · IF 4.7 · 发表于 2025 年 4 月 25 日
作者: Mengfan Bao,Shijie Chen,Hongxiang Xie,Cuihong Zheng,Juan Chen,Aiqin Mao,Saisai Li
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摘要

Transition-metal-based high-entropy oxides (HEOs) have gained significant attention as advanced anode materials for lithium-ion batteries (LIBs) owing to their compositional flexibility and entropy-driven structural stabilization. However, the low intrinsic conductivity and unsatisfactory rate capability remain largely unresolved. Herein, a unique hollow/mesoporous La(Cr 0.2 Fe 0.2 Co 0.2 Ni 0.2 Mn 0.2 )O 3 HEO is developed through an innovative sacrificial template-assisted solution combustion synthesis. As expected, the as-synthesized HEO exhibits a hollow/mesoporous spherical structure with a 49.0 m 2 g -1 surface area and 60.2% surface oxygen vacancy concentration, synergistically facilitating the electronic/ionic transport kinetics and structural stability, and demonstrating an interfacial charge storage mechanism. Benefiting from these combined properties, the engineered hollow/mesoporous HEO anode demonstrates superior rate capability (281 mAh g -1 at 3000 mA g -1 , ∼59% retention of its initial 475 mAh g -1 at 100 mA g -1 ), while maintaining unprecedented cycling stability with 1288 mAh g -1 after 250 cycles at 200 mA g -1 and 1246 mAh g -1 even after 900 cycles at 1000 mA g -1 with continuous capacity enhancement during prolonged cycling. This study establishes a paradigm for enhancing high-rate capabilities in HEO-based anodes through rational morphological design, providing new insights into structure-performance relationships for next-generation LIB applications.