Continuous amino-functionalized University of Oslo 66 membranes as efficacious polysulfide barriers for lithium−sulfur batteries

doi:10.1007/s11705-022-2206-7

Front. Chem. Sci. Eng.

2023, Vol. 17

Issue (2) : 194-205 https://doi.org/10.1007/s11705-022-2206-7

RESEARCH ARTICLE

Continuous amino-functionalized University of Oslo 66 membranes as efficacious polysulfide barriers for lithium−sulfur batteries

Bowen Du, Yuhong Luo, Feichao Wu(

), Guihua Liu, Jingde Li(

), Wei Xue(

)

Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China

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Abstract

The shuttle effect of soluble polysulfides is a serious problem impeding the development of lithium−sulfur batteries. Herein, continuous amino-functionalized University of Oslo 66 membranes supported on carbon nanotube films are proposed as ion-permselective interlayers that overcome these issues and show outstanding suppression of the polysulfide shuttle effect. The proposed membrane material has appropriately sized pores, and can act as ionic sieves and serve as barriers to polysulfides transport while allowing the passage of lithium ions during electrochemical cycles, thereby validly preventing the shuttling of polysulfides. Moreover, a fast catalytic conversion of polysulfides is also achieved with the as-developed interlayer. Therefore, lithium−sulfur batteries with this interlayer show a desirable initial capacity of 999.21 mAh·g^–1 at 1 C and a durable cyclic stability with a decay rate of only 0.04% per cycle over 300 cycles. Moreover, a high area capacity of 4.82 mAh·cm^–2 is also obtained even under increased sulfur loading (5.12 mg·cm^–2) and a lean-electrolyte condition (E/S = 4.8 μL·mg^–1).

Keywords lithium−sulfur batteries amino-functionalized University of Oslo 66 membrane polysulfide interlayer

Corresponding Author(s): Feichao Wu,Jingde Li,Wei Xue

About author:

Changjian Wang and Zhiying Yang contributed equally to this work.

Online First Date: 17 October 2022 Issue Date: 27 February 2023

Cite this article:

Bowen Du,Yuhong Luo,Feichao Wu, et al. Continuous amino-functionalized University of Oslo 66 membranes as efficacious polysulfide barriers for lithium−sulfur batteries[J]. Front. Chem. Sci. Eng., 2023, 17(2): 194-205.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2206-7
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I2/194

Fig.1 Schematic for the synthetic procedures of the 66-NH₂/CNT interlayer.

Fig.2 (a) Surface and (b) cross-sectional SEM images of the prepared UiO-66-NH₂ membrane; (c) surface elemental mappings of Zr, N, O and C.

Fig.3 (a) XRD pattern and (b) FTIR spectrum of UiO-66-NH₂/CNT. (c) N₂ adsorption−desorption isotherms and the pore size distribution (insert) of UiO-66-NH₂ powder. (d) Zr 3d, (e) O 1s and (f) N 1s XPS spectra of the UiO-66-NH₂/CNT. Electrolyte contact angles on (g) UiO-66-NH₂/CNT, (h) CNT film and (i) PP separator.

Fig.4 (a) CV profiles of the battery with NH₂-UiO-66/CNT at 0.1 mV·s^–1; (b) cycle performance at 0.2 C and (c) rate performance of different interlayers; (d) cycle stability of UiO-66-NH₂/CNT interlayer under high sulfur loading; (e) long-term cycling durability for different interlayers at 1 C.

Fig.5 (a) Impedance Nyquist plots; (b) potentiostatic current-time curves of the symmetric cells; (c)

D L i +

for the UiO-66-NH₂/CNT, CNT film and PP separator.

Fig.6 Optical images for the Li₂S₆ diffusion tests.

Fig.7 Scheme of action mechanism for the UiO-66-NH₂/CNT interlayer.

Fig.8 (a) Digital photographs and (b) UV–Vis spectra of Li₂S₆ solutions containing UiO-66-NH₂ and CNT powder; (c–f) theoretical simulation results.

Fig.9 (a) CV profiles of symmetric cells with UiO-66-NH₂ and CNT. (b) EIS results for different interlayers before cycles (insert: equivalent circuit plot). (c) CV curves for different interlayers at 0.2 mV·s^–1. The Tafel slopes for the cathodic and anodic processes acquired according to (c): (d) peak A, (e) peak B and (f) peak C.

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