Capacity Fade Analysis of Sulfur Cathodes in Lithium–Sulfur Batteries

Yan, Jianhua; Liu, Xingbo; Li, Bingyun

doi:10.1002/advs.201600101

Cited by 250 publications

(174 citation statements)

References 50 publications

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“…[10] In the current model, the shuttle and any associated degradation are considered to take place only during charge. While self discharge mechanisms do take place during rest, and have been associated with the polysulfide shuttle, 22,23 the relation between the shuttle during cycling and the self discharge during rest is not established.…”

Section: Modelmentioning

confidence: 99%

“…the accumulation of a non-conductive film of insoluble Li 2 S 2 /Li 2 S, was shown to be correlated to the largest capacity fade, from amongst three possible causes. 10 Discharging below 1.8 V was shown to greatly accelerate degradation in coin cells with catholyte and shuttle suppressant, effect interpreted to be the result of producing poorly reversible Li 2 S from Li 2 S 2 . 11 Most of these studies, however, are performed on coin cells with excess electrolyte and low electrode loading, which were shown to have markedly different capacity fade rate and mechanism 12,13 compared to a commercially viable cell.…”

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confidence: 99%

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Irreversible vs Reversible Capacity Fade of Lithium-Sulfur Batteries during Cycling: The Effects of Precipitation and Shuttle

Marinescu

O’Neill

Zhang

et al. 2017

J. Electrochem. Soc.

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Lithium-sulfur batteries could deliver significantly higher gravimetric energy density and lower cost than Li-ion batteries. Their mass adoption, however, depends on many factors, not least on attaining a predictive understanding of the mechanisms that determine their performance under realistic operational conditions, such as partial charge/discharge cycles. This work addresses a lack of such understanding by studying experimentally and theoretically the response to partial cycling. A lithium-sulfur model is used to analyze the mechanisms dictating the experimentally observed response to partial cycling. The zero-dimensional electrochemical model tracks the time evolution of sulfur species, accounting for two electrochemical reactions, one precipitation/dissolution reaction with nucleation, and shuttle, allowing direct access to the true cell state of charge. The experimentally observed voltage drift is predicted by the model as a result of the interplay between shuttle and the dissolution bottleneck. Other features are shown to be caused by capacity fade. We propose a model of irreversible sulfur loss associated with shuttle, such as caused by reactions on the anode. We find a reversible and an irreversible contribution to the observed capacity fade, and verify experimentally that the reversible component, caused by the dissolution bottleneck, can be recovered through slow charging. This model can be the basis for cycling parameters optimization, or for identifying degradation mechanisms relevant in applications. Lithium sulfur (LiS) batteries have the potential to provide a step change in performance, compared to Li-ion batteries, with an expected practical energy density of 700 Wh kg −1 compared to that of the intercalation Li-ion batteries, of 210 Wh kg −1 . 1,2 Added benefits, such as a potential low cost due to the abundance of the active materials, low toxicity and relative safety, 3 make them an attractive energy storage solution for a wide variety of applications, such as space exploration 4 and low temperature energy delivery. 5 However, the relatively low power capabilities, significant self discharge and low cycle life have so far hindered mainstream adoption of LiS cells. Degradation mechanisms such as lithium anode corrosion, self discharge and low coulombic efficiency have all been related to the polysulfide shuttle. As a result, most effort in the research community is currently directed toward decreasing the amount of shuttle through material design, and assessing the properties of the proposed materials through coin cell characterization.We argue that equally important for accelerating the adoption of this battery chemistry is the understanding of how real cells behave under real operating conditions, which often include incomplete charge/discharge cycles, noisy current loads and rest periods at various states of charge (SoC). Understanding and detecting the mechanisms leading to degradation, such as capacity fade, are intermediate steps crucial to predicting cycle life. Such understanding can...

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Section: Modelmentioning

confidence: 99%

mentioning

confidence: 99%

Irreversible vs Reversible Capacity Fade of Lithium-Sulfur Batteries during Cycling: The Effects of Precipitation and Shuttle

Marinescu

O’Neill

Zhang

et al. 2017

J. Electrochem. Soc.

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“…According to monitored galvanostatic discharge-charge behaviors of prepared cathodes at 0.2 C (Figure 2a), the deposited Se Adv. [17] Lower polarization (lower voltage difference) represents a more kinetically efficient reaction process with a smaller barrier. 2020, 10,1903477 electrode at −1.2 V also showed a high specific capacity and low voltage difference between charge and discharge plateau.…”

mentioning

confidence: 99%

High‐Performance Li–Se Battery Enabled via a One‐Piece Cathode Design

Kim

Cho

Lee

2019

Advanced Energy Materials

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conductivity, and high volumetric energy density. [8][9][10] Moreover, Se is a reasonably priced element, being around $ 32 per kg when purchased in industrial quantities. [4] Comparable to the S cathode, a Se cathode also has major concerns regarding volume expansion of Se (>97%) and shuttle effects by polyselenide intermediates. [11,12] To address these concerns, most studies have focused on the incorporation of functional materials such as porous carbons, conductive polymers, and metal oxides. [5][6][7] In general, the Se cathode is prepared by complicated multistep processes, which are consisted of encapsulating of Se into porous carbon (Se/C composite), slurry preparation using high energy ball-mixing of Se/C composites and other additives, deposition of the slurry on a current collector, and finally pressing the cathode. [11][12][13] In the Se cathode, there exist complex interfaces due to multicomponents system. Furthermore, all the additives do not contribute to electrochemical redox reaction lowering energy density and polymer binder even can increase interfacial resistance. Thus, it would be highly desirable to provide a simple fabrication process and stable cycling to Li-Se battery. [14][15][16] Herein, we introduced a new design of Se cathode, which was simply prepared by electrochemical deposition of Se on Nifoam and subsequent coating of a thin layer of solid polymer electrolyte (SPE). The electrodeposition of Se on Ni-foam is an easy process, and direct contacts of Se on current collector provide facile charge transport. The SPE was easily prepared via crosslinking reaction of poly(ethylene glycol) diglycidyl ether (DE-PEG) and diamino-poly(propylene oxide) (DA-PPG) with subsequent immersion in a LiPF 6 based carbonate electrolyte. The elastic SPE layer is able to protect the delamination problem of Se from the Ni-foam controlling the volume expansion of Se, to provide facile ionic pathway, and to suppress Li-dendrite growth. The designed "One-piece" Se cathode was produced by facile manufacturing process and exhibited an ultrastable cycling performance of 0.001% capacity degradation per cycle for 3000 cycles at 1 C rate.A schematic preparation of the one-piece Se cathode is shown in Figure 1. In the preparation of the one-piece Se cathode, Se was electrodeposited on the Ni-foam and a prepolymer solution of SPE was poured on the Se/Ni-foam to fill the pore. The prepolymer was thermally cross-linked and liquid electrolyte was impregnated. At the bottom of Ni-foam, a thin layer (≈20 µm) of SPE was formed which was directly contacted with Li metal foil. Moreover, the thickness of SPE in A high-performance Li-Se battery is demonstrated by adopting a novel Se cathode design. The Se cathode is a one-piece body combined with a Se deposited current collector and a solid polymer electrolyte (SPE). In the preparation of the Se cathode, Se is electrodeposited on Ni-foam, and the pores are filled with SPE layers. Through this electrodeposition, the cathode is easily fabricated, and charge transports are facile...

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“…Cycle life is further limited by other degradation mechanisms inside the cell e.g., deposition of poorly soluble/insoluble products (Li 2 S 2 , Li 2 S) at the cathode, mechanical decomposition of the cathode carbon skeleton and polysulfide reaction with the electrolyte [31]. Nevertheless, these limitations seem to be less of an issue compared to the problems arising from metallic lithium anode.…”

Section: Limitations Of Lithium-sulfurmentioning

confidence: 99%

“…Much of today's research into Li-S batteries concerns the development and understanding of materials, construction and the fundamental scientific understanding of cell behavior [22][23][24][25][26][27][28][29][30][31].…”

Section: Introductionmentioning

confidence: 99%

Lithium-Sulfur Battery Technology Readiness and Applications—A Review

et al. 2017

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Lithium Sulfur (Li-S) battery is generally considered as a promising technology where high energy density is required at different applications. Over the past decade, there has been an ever increasing volume of Li-S academic research spanning materials development, fundamental understanding and modelling, and application-based control algorithm development. In this study, the Li-S battery technology, its advantages and limitations from the fundamental perspective are firstly discussed. In the second part of this study, state-of-the-art Li-S cell modelling and state estimation techniques are reviewed with a focus on practical applications. The existing studies on Li-S cell equivalent-circuit-network modelling and state estimation techniques are then discussed. A number of challenges in control of Li-S battery are also explained such as the flat open-circuit-voltage curve and high sensitivity of Li-S cell's behavior to temperature variation. In the last part of this study, current and future applications of Li-S battery are mentioned.

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Capacity Fade Analysis of Sulfur Cathodes in Lithium–Sulfur Batteries

Cited by 250 publications

References 50 publications

Irreversible vs Reversible Capacity Fade of Lithium-Sulfur Batteries during Cycling: The Effects of Precipitation and Shuttle

Irreversible vs Reversible Capacity Fade of Lithium-Sulfur Batteries during Cycling: The Effects of Precipitation and Shuttle

High‐Performance Li–Se Battery Enabled via a One‐Piece Cathode Design

Lithium-Sulfur Battery Technology Readiness and Applications—A Review

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