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Electrochemical Analysis of Modified Separators for Li-S Batteries

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Electrochemical Analysis of

Modified Separators for Li-S Batteries

Yu-Chuan Chien, Ruijun Pan, Leif Nyholm, Daniel Brandell, Matthew J. Lacey

Department of Chemistry – Ångström Laboratory, Uppsala University Box 538, SE-751 21 Uppsala, SWEDEN

[email protected]

Motivation

Capacity & C.E.

The lithium-sulfur system is considered a promising energy storage technology due to the high theoretical energy density (2500 Wh kg-1) and abundance of sulfur [1]. However, the problem of the redox shuttle of polysulfides (PS) needs to be solved in order to enhance the cycling

stability for further commercialization [1]. Various concepts for modification of separators have been proposed to address this issue, such as metal oxide coatings [2] or conductive interlayers [3]. Performance improvements have been ascribed to a suppression of polysulfide

transport across the separator, even though this has not always been correlated with the difference in electrochemistry.

Experimental setup

Li S/C Li S/C Li S/C Li S/C

Celgard

®

2400 Al

2

O

3

-coated

PE (ACPE) Nanocellulose CNT-coated

nanocellulose (CCC)

Voltage & resistance

[4]

profiles

Rate-capability Self-discharge

cycle number

discharge

charge

Li morphology after the 2

nd

charge

Conclusion

References

[1] S. Urbonaite, et al., Adv. Energy Mater. 5 (2015) [2] Z. Zhang, et al., Electrochim. Acta 129 (2014) [3] H. Yao, et al., Energy Environ. Sci. 7 (2014)

V = 5 kV

WD = 6.7 mm Mag. = 1 kX SE2 detector

100 µm

Celgard ACPE

Cellulose CCC

S-loading: 2~2.5 mg cm-2 | S/C electrode: 65% S, 28% C, 7% PEO:PVP | Electrolyte: 1M LiTFSI 0.25M LiNO3 DME:DOL | Velec. = 6 µL mgS-1

Separator chemistry has considerable influence on S utilization, rate capability and redox shuttle behavior. S utilization is not strongly

correlated with the degree of the redox shuttle. Results indicate restriction of PS mobility in cells with LiNO3 can be counter-productive, as Li passivation may be negatively affected.

 Al2O3-coating increases the resistance at the end of the 1st discharge plateau

CNT-interlayer decreases the resistance significantly but increases PS-shuttle

 CNT-layer helps at high C-rates  CNT-layer does not stop PS- transport at a large time scale

 Cellulose-based separators improve Li morphology [5], but the pitting at fully-charged state indicates inferior passivation of Li

 Cellulose separators give lower CE

 CNT-layer increases capacity but

endless redox shuttle despite LiNO3

*The PS diffusion tests were done in DME:DOL without salts. Pictures were taken after 15 min.

[4] M.J. Lacey, et al., Chem. Commun. 2 (2015)

[5] Z. Wang, et al., ACS Appl. Energy Mater. (2018)

Celgard

ACPE

Cellulose

CCC

Celgard

ACPE

Cellulose

CCC

Celgard

ACPE

Cellulose

CCC

Celgard

ACPE

Cellulose

CCC

References

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