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

被引：42

作者：

Wei, Yaqing ^{[1
]}

Yao, Runzhe ^{[1
]}

Liu, Xuhao ^{[1
]}

Chen, Wen ^{[1
]}

Qian, Jiayao ^{[1
]}

Yin, Yiyi ^{[1
]}

Li, De ^{[1
]}

Chen, Yong ^{[2
]}

机构：

[1] Hainan Univ, Sch Mat Sci & Engn, State Key Lab Marine Resource Utilizat South China, Hainan Prov Key Lab Res Utilizat Si Zr Ti Resource, 58 Renmin Rd, Haikou 570228, Hainan, Peoples R China

[2] Foshan Univ, Sch Mat Sci & Hydrogen Energy, Guangdong Key Lab Hydrogen Energy Technol, Foshan 528000, Peoples R China

来源：

ADVANCED SCIENCE | 2023年 / 10卷 / 09期

基金：

中国国家自然科学基金; 海南省自然科学基金;

关键词：

anode material; high entropy alloy; initial coulombic efficiency; lithium-ion batteries; volume expansion; HIGH-PERFORMANCE ANODES; LITHIUM-ION; ALLOY;

D O I：

10.1002/advs.202300271

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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 ZnxGeyCuzSiwP2 solid solution is successfully synthesized as proof of concept, which is first verified to cubic system in F-43m. More specially, such ZnxGeyCuzSiwP2 possesses wide-range tunable region from 9911 to 4466, in which the Zn0.5Ge0.5Cu0.5Si0.5P2 accounts for the highest configurational entropy. When served as anode, ZnxGeyCuzSiwP2 delivers large capacity (>1500 mAh g(-1)) and suitable plateau (approximate to 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 Zn0.5Ge0.5Cu0.5Si0.5P2 exhibits the highest initial coulombic efficiency (ICE) (93%), Li-diffusivity (1.11 x 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.

引用

页数：10

共 52 条

[1] Building better batteries [J].