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Research Papers

Cathode Loading Effect on Sulfur Utilization in Lithium–Sulfur Battery

[+] Author and Article Information
Ke Sun

Energy Sciences Directorate,
Brookhaven National Laboratory,
Upton, NY 11973

Helen Liu

Department of Material Science and
Chemical Engineering,
Stony Brook University,
Stony Brook, NY 11790

Hong Gan

Energy Sciences Directorate,
Brookhaven National Laboratory,
Upton, NY 11973
e-mail: hgan@bnl.gov

1Corresponding author.

Manuscript received July 15, 2016; final manuscript received September 6, 2016; published online October 4, 2016. Assoc. Editor: Partha Mukherjee.

J. Electrochem. En. Conv. Stor. 13(2), 021002 (Oct 04, 2016) (9 pages) Paper No: JEECS-16-1095; doi: 10.1115/1.4034738 History: Received July 15, 2016; Revised September 06, 2016

The lithium–sulfur (Li–S) battery is under intensive research in recent years due to its potential to provide higher energy density and lower cost than the current state-of-the-art lithium-ion battery technology. To meet cost target for transportation application, high-sulfur loading up to 8 mAh cm−2 is predicted by modeling. In this work, we have investigated the sulfur loading effect on the galvanostatic charge/discharge cycling performance of Li–S cells with theoretical sulfur loading ranging from 0.5 to 7.5 mAh cm−2. We found that the low sulfur utilization of electrodes with sulfur loading of > 3.0 mAh cm−2 is due to their inability to deliver capacities at the voltage plateau of 2.1 V, which corresponds to the conversion of soluble Li2S4 to insoluble Li2S2/Li2S. This electrochemical conversion process recovers to deliver the expected sulfur utilization after several activation cycles for electrodes with sulfur loading up to 4.5 mAh cm−2. For electrodes with 7.0 mAh cm−2 loading, no sulfur utilization recovery was observed for 100 cycles. The root cause of this phenomenon is elucidated by SEM/EDS and EIS investigation. Carbon-interlayer cell design and low-rate discharge activation are demonstrated to be effective mitigation methods.

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Copyright © 2016 by ASME
Topics: Electrodes , Sulfur , Cycles
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Figures

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Fig. 1

(a) Electrode thickness and sulfur loading, (b) TGA curve of an electrode with 4.50 mg cm−2 loading, (c) loading capacity as a function of coating gap, (d)–(f) SEM images of electrodes with sulfur loading of 0.80, 1.83, and 2.71 mg cm−2, and (g) overlap of EDS spectrum of these electrodes

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Fig. 2

(a) Cycling performance of sulfur electrodes with different loading, (b) first cycle areal discharge capacity as a function of sulfur loading, (c) 30th cycle areal discharge capacity as a function of sulfur loading, and (d) Coulombic efficiency as a function of sulfur loading for selected cycles

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Fig. 3

(a) First discharge voltage profile of sulfur electrodes with different loading, (b)–(d) discharge voltage profile of selected cycles of sulfur electrodes with 1.28, 2.23, and 4.18 mg cm−2 loading, (e) SEM micrographs of sulfur electrodes with loading ∼2.36 mg cm−2 at different stages of cycling, and (f) EDS spectrum of samples in (e), inset is the S/C peak maximum ratio plotted with cycle number

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Fig. 4

(a) and (b) Nyquist plots of sulfur electrode with loading 0.77 and 2.62 mg cm−2, respectively, during the first cycle, (c) equivalent circuit used for fitting and comparison between fitted results and original data for a specific curve, and (d)–(g) capacity, contact resistance R2, charge transfer resistance R1, and electrolyte resistance R3 as a function of cycle number for the two cells in (a) and (b). 1.8 V, 2.1 V, and 2.6 V in the legend correspond to the voltage cut-off chosen for the impedance spectrum to be taken, as it was introduced in the experimental details

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Fig. 5

(a) Capacity evolution for electrodes with higher sulfur loading with low-rate first discharge activation, (b) capacity evolution for electrodes with higher sulfur loading with a carbon-interlayer cell design, (c) first discharge curves of electrodes of similar loading with and without carbon-coated interlayers, (d) initial areal discharge as a function of sulfur loading, and (e) 30th cycle areal discharge capacity as a function of sulfur loading

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