How Do the Four Core Factors of High Entropy Affect the Electrochemical Properties of Energy‐Storage Materials?

Abstract 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 La1/4Ce1/4Pr1/4Nd1/4Nb3O9 (HE‐LaNb3O9) oxide...

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Main Authors: Wenze Wang, Qian Zhang, Liting Yang, Guisheng Liang, Xuhui Xiong, Yifeng Cheng, Limin Wu, Chunfu Lin, Renchao Che
Format: Article
Language:English
Published: Wiley 2025-01-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202411291
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author Wenze Wang
Qian Zhang
Liting Yang
Guisheng Liang
Xuhui Xiong
Yifeng Cheng
Limin Wu
Chunfu Lin
Renchao Che
author_facet Wenze Wang
Qian Zhang
Liting Yang
Guisheng Liang
Xuhui Xiong
Yifeng Cheng
Limin Wu
Chunfu Lin
Renchao Che
author_sort Wenze Wang
collection DOAJ
description Abstract 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 La1/4Ce1/4Pr1/4Nd1/4Nb3O9 (HE‐LaNb3O9) oxide is prepared through multiple rare‐metal‐ion substitution in LaNb3O9, and uses HE‐LaNb3O9 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‐LaNb3O9. The lattice distortion in HE‐LaNb3O9 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‐LaNb3O9 at room temperature (25 °C) is limited, which causes its lowered rate capability. However, the Li+ diffusivity of HE‐LaNb3O9 at high temperature (60 °C) becomes faster than that of LaNb3O9, which is attributed to the alleviated lattice distortion at the high‐temperature, resulting in higher rate capability. The cocktail effects in HE‐LaNb3O9 enable its larger electronic conductivity, better electrochemical activity, more intensive Nb5+ ↔ Nb3+ 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.
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spelling doaj-art-e852481e18274e05bf77977a92e81f412025-08-20T02:47:33ZengWileyAdvanced Science2198-38442025-01-01121n/an/a10.1002/advs.202411291How Do the Four Core Factors of High Entropy Affect the Electrochemical Properties of Energy‐Storage Materials?Wenze Wang0Qian Zhang1Liting Yang2Guisheng Liang3Xuhui Xiong4Yifeng Cheng5Limin Wu6Chunfu Lin7Renchao Che8College of Physics Donghua University Shanghai 201620 ChinaInstitute of Materials for Energy and Environment School of Materials Science and Engineering Qingdao University Qingdao 266071 ChinaLaboratory 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 ChinaLaboratory 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 ChinaLaboratory 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 ChinaZhejiang Laboratory Hangzhou 311100 ChinaInner Mongolia University Hohhot 010021 ChinaCollege of Physics Donghua University Shanghai 201620 ChinaCollege of Physics Donghua University Shanghai 201620 ChinaAbstract 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 La1/4Ce1/4Pr1/4Nd1/4Nb3O9 (HE‐LaNb3O9) oxide is prepared through multiple rare‐metal‐ion substitution in LaNb3O9, and uses HE‐LaNb3O9 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‐LaNb3O9. The lattice distortion in HE‐LaNb3O9 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‐LaNb3O9 at room temperature (25 °C) is limited, which causes its lowered rate capability. However, the Li+ diffusivity of HE‐LaNb3O9 at high temperature (60 °C) becomes faster than that of LaNb3O9, which is attributed to the alleviated lattice distortion at the high‐temperature, resulting in higher rate capability. The cocktail effects in HE‐LaNb3O9 enable its larger electronic conductivity, better electrochemical activity, more intensive Nb5+ ↔ Nb3+ 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.https://doi.org/10.1002/advs.202411291electrochemical propertyfour core factors of high entropyhigh‐entropy materialhigh‐temperature operationin situ characterization
spellingShingle Wenze Wang
Qian Zhang
Liting Yang
Guisheng Liang
Xuhui Xiong
Yifeng Cheng
Limin Wu
Chunfu Lin
Renchao Che
How Do the Four Core Factors of High Entropy Affect the Electrochemical Properties of Energy‐Storage Materials?
Advanced Science
electrochemical property
four core factors of high entropy
high‐entropy material
high‐temperature operation
in situ characterization
title How Do the Four Core Factors of High Entropy Affect the Electrochemical Properties of Energy‐Storage Materials?
title_full How Do the Four Core Factors of High Entropy Affect the Electrochemical Properties of Energy‐Storage Materials?
title_fullStr How Do the Four Core Factors of High Entropy Affect the Electrochemical Properties of Energy‐Storage Materials?
title_full_unstemmed How Do the Four Core Factors of High Entropy Affect the Electrochemical Properties of Energy‐Storage Materials?
title_short How Do the Four Core Factors of High Entropy Affect the Electrochemical Properties of Energy‐Storage Materials?
title_sort how do the four core factors of high entropy affect the electrochemical properties of energy storage materials
topic electrochemical property
four core factors of high entropy
high‐entropy material
high‐temperature operation
in situ characterization
url https://doi.org/10.1002/advs.202411291
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