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Understanding the Configurational Entropy Evolution in Metal‐Phosphorus Solid Solution for Highly Reversible Li‐Ion Batteries

The high‐entropy materials (HEM) have attracted increasing attention in catalysis and energy storage due to their large configurational entropy and multiunique properties. However, it is failed in alloying‐type anode due to their Li‐inactive transition‐metal compositions. Herein, inspired by high‐en...

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Autores principales: Wei, Yaqing, Yao, Runzhe, Liu, Xuhao, Chen, Wen, Qian, Jiayao, Yin, Yiyi, Li, De, Chen, Yong
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10037993/
https://www.ncbi.nlm.nih.gov/pubmed/36793114
http://dx.doi.org/10.1002/advs.202300271
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author Wei, Yaqing
Yao, Runzhe
Liu, Xuhao
Chen, Wen
Qian, Jiayao
Yin, Yiyi
Li, De
Chen, Yong
author_facet Wei, Yaqing
Yao, Runzhe
Liu, Xuhao
Chen, Wen
Qian, Jiayao
Yin, Yiyi
Li, De
Chen, Yong
author_sort Wei, Yaqing
collection PubMed
description The high‐entropy materials (HEM) have attracted increasing attention in catalysis and energy storage due to their large configurational entropy and multiunique properties. However, it is failed in alloying‐type anode due to their Li‐inactive transition‐metal compositions. Herein, inspired by high‐entropy concept, the Li‐active elements instead of transition‐metal ones are introduced for metal‐phosphorus synthesis. Interestingly, a new Zn(x)Ge(y)Cu(z)Si(w)P(2) solid solution is successfully synthesized as proof of concept, which is first verified to cubic system in F‐43m. More specially, such Zn(x)Ge(y)Cu(z)Si(w)P(2) possesses wide‐range tunable region from 9911 to 4466, in which the Zn(0.5)Ge(0.5)Cu(0.5)Si(0.5)P(2) accounts for the highest configurational entropy. When served as anode, Zn(x)Ge(y)Cu(z)Si(w)P(2) delivers large capacity (>1500 mAh g(−1)) and suitable plateau (≈0.5 V) for energy storage, breaking the conventional view that HEM is helpless for alloying anode due to its transition‐metal compositions. Among them, the Zn(0.5)Ge(0.5)Cu(0.5)Si(0.5)P(2) exhibits the highest initial coulombic efficiency (ICE) (93%), Li‐diffusivity (1.11 × 10(−10)), lowest volume‐expansion (34.5%), and best rate performances (551 mAh g(−1) at 6400 mA g(−1)) owing to its largest configurational entropy. Possible mechanism reveals the high entropy stabilization enables good accommodation of volume change and fast electronic transportation, thus supporting superior cyclability and rate performances. This large configurational entropy strategy in metal‐phosphorus solid solution may open new avenues to develop other high‐entropy materials for advanced energy storage.
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spelling pubmed-100379932023-03-25 Understanding the Configurational Entropy Evolution in Metal‐Phosphorus Solid Solution for Highly Reversible Li‐Ion Batteries Wei, Yaqing Yao, Runzhe Liu, Xuhao Chen, Wen Qian, Jiayao Yin, Yiyi Li, De Chen, Yong Adv Sci (Weinh) Research Articles The high‐entropy materials (HEM) have attracted increasing attention in catalysis and energy storage due to their large configurational entropy and multiunique properties. However, it is failed in alloying‐type anode due to their Li‐inactive transition‐metal compositions. Herein, inspired by high‐entropy concept, the Li‐active elements instead of transition‐metal ones are introduced for metal‐phosphorus synthesis. Interestingly, a new Zn(x)Ge(y)Cu(z)Si(w)P(2) solid solution is successfully synthesized as proof of concept, which is first verified to cubic system in F‐43m. More specially, such Zn(x)Ge(y)Cu(z)Si(w)P(2) possesses wide‐range tunable region from 9911 to 4466, in which the Zn(0.5)Ge(0.5)Cu(0.5)Si(0.5)P(2) accounts for the highest configurational entropy. When served as anode, Zn(x)Ge(y)Cu(z)Si(w)P(2) delivers large capacity (>1500 mAh g(−1)) and suitable plateau (≈0.5 V) for energy storage, breaking the conventional view that HEM is helpless for alloying anode due to its transition‐metal compositions. Among them, the Zn(0.5)Ge(0.5)Cu(0.5)Si(0.5)P(2) exhibits the highest initial coulombic efficiency (ICE) (93%), Li‐diffusivity (1.11 × 10(−10)), lowest volume‐expansion (34.5%), and best rate performances (551 mAh g(−1) at 6400 mA g(−1)) owing to its largest configurational entropy. Possible mechanism reveals the high entropy stabilization enables good accommodation of volume change and fast electronic transportation, thus supporting superior cyclability and rate performances. This large configurational entropy strategy in metal‐phosphorus solid solution may open new avenues to develop other high‐entropy materials for advanced energy storage. John Wiley and Sons Inc. 2023-02-15 /pmc/articles/PMC10037993/ /pubmed/36793114 http://dx.doi.org/10.1002/advs.202300271 Text en © 2023 The Authors. Advanced Science published by Wiley‐VCH GmbH https://creativecommons.org/licenses/by/4.0/This is an open access article under the terms of the http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
spellingShingle Research Articles
Wei, Yaqing
Yao, Runzhe
Liu, Xuhao
Chen, Wen
Qian, Jiayao
Yin, Yiyi
Li, De
Chen, Yong
Understanding the Configurational Entropy Evolution in Metal‐Phosphorus Solid Solution for Highly Reversible Li‐Ion Batteries
title Understanding the Configurational Entropy Evolution in Metal‐Phosphorus Solid Solution for Highly Reversible Li‐Ion Batteries
title_full Understanding the Configurational Entropy Evolution in Metal‐Phosphorus Solid Solution for Highly Reversible Li‐Ion Batteries
title_fullStr Understanding the Configurational Entropy Evolution in Metal‐Phosphorus Solid Solution for Highly Reversible Li‐Ion Batteries
title_full_unstemmed Understanding the Configurational Entropy Evolution in Metal‐Phosphorus Solid Solution for Highly Reversible Li‐Ion Batteries
title_short Understanding the Configurational Entropy Evolution in Metal‐Phosphorus Solid Solution for Highly Reversible Li‐Ion Batteries
title_sort understanding the configurational entropy evolution in metal‐phosphorus solid solution for highly reversible li‐ion batteries
topic Research Articles
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10037993/
https://www.ncbi.nlm.nih.gov/pubmed/36793114
http://dx.doi.org/10.1002/advs.202300271
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