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Research Article

Lamellar quasi-solid electrolyte with nanoconfined deep eutectic solvent for high-performance lithium battery

Shiwei Liu, Jing Wang, Keqi Wu, Zhirong Yang( ), Yan Dai, Junmei Zhang, Wenjia Wu( ), Jingtao Wang
School of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, China
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Graphical Abstract

Lamellar quasi-solid electrolyte was fabricated by confining deep eutectic solvent into the regular channel of vermiculite lamellar framework, where the nanoconfinement effect and interaction of channel walls jointly open the solvation shell to release more free lithium-ions, achieving high ionic conductivity and lithium-ion transference number.

Abstract

Electrolytes with high-efficiency lithium-ion transfer and reliable safety are of great importance for lithium battery. Although having superior ionic conductivity (10−3–10−2 S·cm−1), traditional liquid-state electrolytes always suffer from low lithium-ion transference number ( tLi+, < 0.4) and thus undesirable battery performances. Herein, the deep eutectic solvent (DES) is vacuum-filtered into the ~ 1 nm interlayer channel of vermiculite (Vr) lamellar framework to fabricate a quasi-solid electrolyte (Vr-DES QSE). We demonstrate that the nanoconfinement effect of interlayer channel could facilitate the opening of solvation shell around lithium-ion. Meanwhile, the interaction from channel wall could inhibit the movement of anion. These enable high-efficiency lithium-ion transfer: 2.61 × 10−4 S·cm−1 at 25 °C. Importantly, the tLi+ value reaches 0.63, which is 4.5 times of that of bulk DES, and much higher than most present liquid/quasi-solid electrolytes. In addition, Vr-DES QSE shows significantly improved interfacial stability with Li anode as compared with DES. The assembled Li symmetric cell can operate stably for 1000 h at 0.1 mA·cm−2. The lithium iron phosphate (LFP)|Vr-DES QSE|Li cell exhibits high capacity of 142.1 mAh·g−1 after 200 cycles at 25 °C and 0.5 C, with a capacity retention of 94.5%. The strategy of open solvation shell through nanoconfinement effect of lamellar framework may shed light on the development of advanced electrolytes.

Keywords

quasi-solid electrolytedeep eutectic solventlamellar structurelithium-ion transference numbersolvation shell

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Nano Research
Volume 17 Issue 7,
July 2024
Pages 6176-6183
DOI: 10.1007/s12274-024-6620-7
Cite this article:
Liu S, Wang J, Wu K, et al. Lamellar quasi-solid electrolyte with nanoconfined deep eutectic solvent for high-performance lithium battery. Nano Research, 2024, 17(7): 6176-6183. https://doi.org/10.1007/s12274-024-6620-7
Topics:
Lithium batteries

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Received: 24 January 2024
Revised: 29 February 2024
Accepted: 11 March 2024
Published: 15 April 2024
© Tsinghua University Press 2024
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