Wang Wenze, Zhang Qian, Yang Liting, Liang Guisheng, Xiong Xuhui, Cheng Yifeng, Wu Limin, Lin Chunfu, Che Renchao
College of Physics, Donghua University, Shanghai, 201620, China.
Laboratory of Advanced Materials, Shanghai Key Lab of Molecular Catalysis and Innovative Materials, Academy for Engineering & Technology, Advanced Coatings Research Center of Ministry of Education of China, Fudan University, Shanghai, 200438, China.
Adv Sci (Weinh). 2025 Jan;12(1):e2411291. doi: 10.1002/advs.202411291. Epub 2024 Nov 4.
High-entropy materials (HEMs) are extremely popular for electrochemical energy storage nowadays. However, the detailed effects of four core factors of high entropy on the electrochemical properties of HEMs are still unclear. Here, a high-entropy LaCePrNdNbO (HE-LaNbO) oxide is prepared through multiple rare-metal-ion substitution in LaNbO, and uses HE-LaNbO as a model material to systematically study the effects of the four core factors of high entropy on electrochemical energy-storage materials. The high-entropy effect lowers the calcination temperature for obtaining pure HE-LaNbO. The lattice distortion in HE-LaNbO leads to its decreased unit-cell-volume variations, which benefits its cyclability. Based on the restrained diffusion arising from the lattice distortion, the Li diffusivity of HE-LaNbO at room temperature (25 °C) is limited, which causes its lowered rate capability. However, the Li diffusivity of HE-LaNbO at high temperature (60 °C) becomes faster than that of LaNbO, which is attributed to the alleviated lattice distortion at the high-temperature, resulting in higher rate capability. The cocktail effects in HE-LaNbO enable its larger electronic conductivity, better electrochemical activity, more intensive Nb ↔ Nb redox reaction, and larger reversible capacity. The insight gained here can provide a guide for the rational design of new HEMs with good energy-storage properties.
如今,高熵材料(HEMs)在电化学储能领域极其受欢迎。然而,高熵的四个核心因素对高熵材料电化学性能的具体影响仍不明确。在此,通过在LaNbO中进行多种稀土金属离子取代制备了一种高熵LaCePrNdNbO(HE-LaNbO)氧化物,并以HE-LaNbO作为模型材料,系统研究高熵的四个核心因素对电化学储能材料的影响。高熵效应降低了获得纯HE-LaNbO的煅烧温度。HE-LaNbO中的晶格畸变导致其单位晶胞体积变化减小,这有利于其循环稳定性。基于晶格畸变引起的扩散受限,HE-LaNbO在室温(25℃)下的Li扩散率受到限制,这导致其倍率性能降低。然而,HE-LaNbO在高温(60℃)下的Li扩散率比LaNbO更快,这归因于高温下晶格畸变的缓解,从而具有更高的倍率性能。HE-LaNbO中的协同效应使其具有更大的电子电导率、更好的电化学活性、更强烈的Nb↔Nb氧化还原反应以及更大的可逆容量。此处获得的见解可为合理设计具有良好储能性能的新型高熵材料提供指导。