通过钠离子电池的高熵揭示高电压下 NASICON 的快速 Na 扩散动力学,Advanced Energy Materials

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通过钠离子电池的高熵揭示高电压下 NASICON 的快速 Na 扩散动力学
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-12-06 , DOI: 10.1002/aenm.202302733
Muhammad Tayyab Ahsan ₁ , Daping Qiu ₁ , Zeeshan Ali ₁ , Zhi Fang ₁ , Wanting Zhao ₁ , Tong Shen ₁ , Yanglong Hou _{1,

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Affiliation

钒基钠超离子导体（NASICON）由于其高结构稳定性和优异的Na ⁺离子扩散性而引起了前所未有的关注。然而，由于低电子电导率和V ⁴⁺ /V ^{5+的不可逆相变，Na}₄ VM(PO ₄ ) ₃在高电压(≈4.0 V)下存在低倍率性能和容量衰减。本文设计了一种高熵Na ₄ VFe _0.6 Mn _0.2 Cr _0.1 (CoMgAl) _0.1 (PO ₄ ) ₃ (NVFP-HE) NASICON材料，利用多金属的本征效应实现了优异的高电压倍率性能。，良好的离子和电子导电性。该NVFP-HE正极不仅在1C下具有141.98mAh g ^-1的高放电容量，而且在高达50C电流倍率下也具有85.77mAh g ^{-1的优异容量。}此外，NVFP-HE在50C下经过10000次充放电循环后还可以保留66.7%的初始容量。需要强调的是，高熵减轻了 4 V 下不可逆相变引起的性能衰减。有趣的是，NVFP-HE//HC 全电池在 0.2C 时提供 81 mAh g ^-1。这种高熵效应及其概念证明可以帮助寻找独特的组合和合理设计的先进阴极材料以实现广泛的应用。

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Unraveling the Fast Na Diffusion Kinetics of NASICON at High Voltage via High Entropy for Sodium-Ion Battery

Vanadium based sodium superionic conductors (NASICON) have attracted unpreceded attention owing to their high structural stability and excellent Na⁺ ion diffusion. However, Na₄VM(PO₄)₃ suffer from low-rate capability and capacity decay at high voltage (≈4.0 V) due to low electronic conductivity and irreversible phase transition of V⁴⁺/V⁵⁺. Herein, a high entropy Na₄VFe_0.6Mn_0.2Cr_0.1(CoMgAl)_0.1(PO₄)₃ (NVFP-HE) NASICON material is designed, which allows the intrinsic effect of multi-metal to achieve the excellent rate capability at high voltage, good ionic as well as electronic conductivity. This NVFP-HE cathode not only delivers a high discharge capacity of 141.98 mAh g⁻¹ at 1C, but also presents an exceptional capacity of 85.77 mAh g⁻¹ at as high as 50C current rate. Additionally, NVFP-HE can also retain 66.7% of initial capacity after 10 000 charge–discharge cycles at 50C. It is important to highlight that the high entropy mitigates the performance decay that arises from the irreversible phase change at 4 V. Interestingly, NVFP-HE//HC full cell delivers 81 mAh g⁻¹ at 0.2C. This high entropy effect and its proof of concept can allow to look for unique combinations and rationally designed advanced cathode materials for wide applications.

更新日期：2023-12-06

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