首页|Activation mechanism of conventional electrolytes with amine solvents:Species evolution and hydride-containing interphase formation

Activation mechanism of conventional electrolytes with amine solvents:Species evolution and hydride-containing interphase formation

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Rechargeable magnesium(Mg)-metal batteries have brought great expect to overcome the safety and energy density concerns of typical lithium-ion batteries.However,interfacial passivation of the Mg-metal anode impairs the reversible Mg plating/stripping chemistries,resulting in low Coulombic effi-ciency and large overpotential.In this work,a facile isobutylamine(IBA)-assisted activation strategy has been proposed and the fundamental mechanism has been unveiled in a specific way of evolving active species and forming MgH2-based solid-electrolyte interphase.After introducing IBA into a typical electrolyte of magnesium bis(trifluoromethanesulfonyl)imide(Mg(TFSI)2)in diglyme(G2)solvents,elec-trolyte species of[Mg2+(IBA)5]2+and protonated amine-based cations of[(IBA)H]+have been detected by nuclear magnetic resonance and mass spectra.This not only indicates direct solvation of IBA toward Mg2+but also suggests its ionization,which is central to mitigating the decomposition of G2 and TFSI anions by forming neutrally charged[(IBAH+)(TFSI-)]0 and other complex ions.A series of experiments,including cryogenic-electron microscopy,D2O titration-mass spectra,and time of flight secondary ion mass spec-trometry results,reveal a thin,non-passivated,and MgH2-containing interphase on the Mg-metal anode.Besides,uniform and dendrite-free Mg electrodeposits have been revealed in composite electrolytes.Benefiting from the activation effects of IBA,the composite electrolyte displays superior electrochemical performance(overpotential is approximately 0.16 V versus 2.00 V for conventional electrolyte;Coulombic efficiency is above 90％versus＜10％for conventional electrolyte).This work offers a fresh direction to advanced electrolyte design for next-generation rechargeable batteries.

Rechargeable magnesium batteriesAmine solventsIonizationMgH2-based solid-electrolyte interphase

Jinlei Zhang、Ning Yuan、Jing Liu、Xiaosong Guo、Xi Chen、Zhenfang Zhou、Zhonghua Zhang、Guicun Li

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College of Materials Science and Engineering,Qingdao University of Science and Technology,Qingdao 266042,Shandong,China

School of Materials Science and Engineering,Tongji University,Shanghai 201804,China

Department of Pharmacy,Jining Medical University,Rizhao 276826,Shandong,China

Department of Physics,Xi'an Jiaotong-Liverpool University,Suzhou 215123,Jiangsu,China

Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University,Tianjin 300071,China

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2024

10.1016/j.jechem.2024.07.015

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.98(11)