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Understanding the Configurational Entropy Evolution in Metal-Phosphorus Solid Solution for Highly Reversible Li-Ion
Yaqing Wei1, Runzhe Yao1, Xuhao Liu1
1State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan Provincial Key Laboratory of Research on Utilization of Si-Zr-Ti Resources, School of Materials Science and Engineering, Hainan University, 58 Renmin Road, Haikou, Hainan, 570228, P. R. China.
Advanced Science (Weinheim, Baden-Wurttemberg, Germany)
|February 16, 2023
Summary
High-entropy materials, typically inactive in anodes, are now viable for energy storage. A novel ZnGeCuSiP2 solid solution demonstrates high capacity and stability, overcoming previous limitations.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- High-entropy materials (HEM) show promise in catalysis and energy storage due to unique properties.
- Traditional HEM are unsuitable for alloying anodes because of inactive transition-metal compositions.
- A new strategy is needed to utilize HEM's potential in advanced energy storage applications.
Purpose of the Study:
- To introduce Li-active elements into metal-phosphorus compounds to create novel high-entropy anode materials.
- To synthesize and characterize a new ZnₓGe<0xE1><0xB5><0xA7>Cu<0xE2><0x82><0x91>Si<0xE1><0xB5><0xA3>P₂ solid solution for energy storage.
- To demonstrate the feasibility of high-entropy concept in developing effective alloying anodes.
Main Methods:
- Synthesis of a new ZnₓGe<0xE1><0xB5><0xA7>Cu<0xE2><0x82><0x91>Si<0xE1><0xB5><0xA3>P₂ solid solution with tunable composition.
- Crystallographic analysis to verify the cubic system (F-43m) and determine configurational entropy.
- Electrochemical testing as an anode material in energy storage devices.
Main Results:
- Successful synthesis of ZnₓGe<0xE1><0xB5><0xA7>Cu<0xE2><0x82><0x91>Si<0xE1><0xB5><0xA3>P₂ solid solution with a wide tunable composition range.
- The Zn₀.₅Ge₀.₅Cu₀.₅Si₀.₅P₂ composition exhibited the highest configurational entropy.
- This material delivered high capacity (>1500 mAh g⁻¹), a suitable plateau (≈0.5 V), high initial coulombic efficiency (93%), excellent Li-diffusivity, low volume expansion (34.5%), and superior rate performance (551 mAh g⁻¹ at 6400 mA g⁻¹).
Conclusions:
- The developed ZnₓGe<0xE1><0xB5><0xA7>Cu<0xE2><0x82><0x91>Si<0xE1><0xB5><0xA3>P₂ solid solution effectively functions as an alloying anode, challenging previous assumptions about HEM.
- High configurational entropy stabilizes the structure, accommodating volume changes and facilitating fast ion transport for enhanced performance.
- This strategy opens new pathways for designing high-entropy materials for advanced energy storage.
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