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Development of operando XRD coin cells for lithium-sulfur batteries

Yu-Chuan Chien, Ashok S. Menon, William R. Brant, Daniel Brandell, Matthew J. Lacey

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

yuchuan.chien@kemi.uu.se

Motivation

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]. Several works [2–7] on operando X-ray diffraction (XRD) of the Li-S system have been published; however, their cell setups were not optimal considering the excessive electrolyte [8], non-uniform stack pressure and electronic contact [9]. This work aims for a cell design that satisfies these criteria in order to obtain operando XRD data from a Li-S cell optimized towards practical requirements.

Experimental design

Li S/C on Al

Proof of concept Preliminary result

Future work

References

[1] S. Urbonaite, et al., Adv. Energy Mater. 5 (2015) [2] J. Nelson, et al., J. Am. Chem. Soc. 134 (2012) [3] N.A. Cañas, et al., J. Power Sources 226 (2013) [4] S. Waluś, et al., Chem. Commun. 49 (2013)

[5] M. a. Lowe, et al., RSC Adv. 4 (2014)

[6] J. Kulisch, et al., Phys. Chem. Chem. Phys. 16 (2014)

 Find a substitute for the Kapton window so that the background can be reduced with the removal of the pouch

 Complement structural information with electrochemical properties through ‘online’ electrochemical characterization techniques, e.g. Intermittent Current Interruption (ICI) method [11]

 Refine the diffraction data to extract phase fraction and crystallite size

Acknowledgement

Be Be

Dectris Mythen 1K strip detector X-ray source

(Cu K

α

) Kapton® tape

Stainless steel coin cell casing with 5-mm drilled holes

At the moment, the coin cell is then sealed in a modified pouch bag due to the imperfect sealing

of the coin cell.

Lithium-sulfur system

Li S embedded in C

Li+

e-

+ -

Overall reaction:

S + 2Li → Li2S

Typical potential profile of Li-S cells 1

2

Proposed reaction route[10]

S

8

→ Li

2

S

8

Li

2

S ← (Li

2

S

2

) ← Li

2

S

4

↓ Li

2

S

6

1st plateau 2nd plateau

Solid state

Dissolved in electrolyte

Research questions:

 How are the dissolution and precipitation processes

affected by operational parameters?

 How is the reaction

influenced by the structure of the C-matrix and other cell components?

 The cell showed typical potential

profile of Li-S cells with 10 µL mgS-1 electrolyte at cycling rate C/50

 The large overpotential of the 1st discharge resulted from the high S-loading (4.9 mg cm-2)

 β-S was detected after the 1st charge (75th hour) in agreement with [4]

 Li2S only showed up as diffuse peaks

 The pouch contributed significantly to the background

discharge

Diffractometer:

STOE STADI P in transmission setup

charge

The authors thank Swedish Energy Agency for financial support through Sulfur Technology Advanced Research Concept (Y.C.) and Swedish Foundation for Strategic Research for funding

(A.M.).

 Broad peaks around 21° and 23 ° were contributed from the modified pouch

[7] J. Conder, et al., Nat. Energy 2 (2017) [8] M.J. Lacey, ChemElectroChem (2017)

[9] O.J. Borkiewicz, et al., J. Phys. Chem. Lett. 6 (2015) [10] M. Wild, et al., Energy Environ. Sci. 8 (2015)

[11] M.J. Lacey, ChemElectroChem 4 (2017)

References

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