TY - JOUR
T1 - Ultra-rapid Synthesis of High-entropy MAX Phases and Their Derivative MXenes for Battery Electrodes
AU - Zhang, Liang
AU - Li, Huicong
AU - Zhang, Xiaoyu
AU - Liu, Chunxue
AU - Sun, Yifei
AU - Zhang, Yiyuan
AU - Fang, Zhen
AU - He, Jiangang
AU - Wang, Rongming
AU - Jiang, Kai
AU - Chen, Di
N1 - Publisher Copyright:
© 2024 Wiley-VCH GmbH.
PY - 2024
Y1 - 2024
N2 - High-entropy materials hold immense promise for energy storage, owing to their varied compositions and unforeseen physicochemical properties, yet, which poses challenges in synthesis due to tendentious phase separation and extended sintering durations. Herein, an ultra-rapid strategy based on spark plasma sintering (SPS) techniques is proposed to synthesize high-entropy MAX phases within 15 minutes, including a new phase of (Ti0.2V0.2Cr0.2Nb0.2Mo0.2)4AlC3 and several phases of 413-type TiVNbMoAlC3, TiVCrMoAlC3 and (Ti0.2V0.2Cr0.2Nb0.2Ta0.2)4AlC3, achieving utmost purity level up to 99.54 %. Under high temperature, the overfeed of Al with low melt point (~660 °C) can foster a liquid environment, which remits the immiscibility among starting materials and benefits to diffusion dynamics to some extents. Theoretical calculations are employed to elucidate the thermodynamic preponderance of high-entropy MAX phases in the intricate multi-element systems. Meanwhile, the varied stacking modes among MX slabs in high-entropy MAX phases and the distinct topological transformations to their derivative MXenes can be observed directly at the atomic level. Moreover, four high-entropy MXenes as electrode materials were investigated for rechargeable batteries. Among them, TiVNbMoC3 electrode demonstrates superior lithium-ion storage capabilities with 725 mAh g−1 after 1000 cycles at 1 A g−1, triggering the edification to the application of high-entropy MXenes for energy domain.
AB - High-entropy materials hold immense promise for energy storage, owing to their varied compositions and unforeseen physicochemical properties, yet, which poses challenges in synthesis due to tendentious phase separation and extended sintering durations. Herein, an ultra-rapid strategy based on spark plasma sintering (SPS) techniques is proposed to synthesize high-entropy MAX phases within 15 minutes, including a new phase of (Ti0.2V0.2Cr0.2Nb0.2Mo0.2)4AlC3 and several phases of 413-type TiVNbMoAlC3, TiVCrMoAlC3 and (Ti0.2V0.2Cr0.2Nb0.2Ta0.2)4AlC3, achieving utmost purity level up to 99.54 %. Under high temperature, the overfeed of Al with low melt point (~660 °C) can foster a liquid environment, which remits the immiscibility among starting materials and benefits to diffusion dynamics to some extents. Theoretical calculations are employed to elucidate the thermodynamic preponderance of high-entropy MAX phases in the intricate multi-element systems. Meanwhile, the varied stacking modes among MX slabs in high-entropy MAX phases and the distinct topological transformations to their derivative MXenes can be observed directly at the atomic level. Moreover, four high-entropy MXenes as electrode materials were investigated for rechargeable batteries. Among them, TiVNbMoC3 electrode demonstrates superior lithium-ion storage capabilities with 725 mAh g−1 after 1000 cycles at 1 A g−1, triggering the edification to the application of high-entropy MXenes for energy domain.
KW - high-entropy MAX phases
KW - high-entropy MXenes
KW - lithium-ion battery
KW - sodium-ion batteries
KW - ultra-rapid synthesis
UR - http://www.scopus.com/inward/record.url?scp=85210413078&partnerID=8YFLogxK
U2 - 10.1002/anie.202418538
DO - 10.1002/anie.202418538
M3 - Article
AN - SCOPUS:85210413078
SN - 1433-7851
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
ER -