An integrally-designed, flexible polysulfide host for high-performance lithium-sulfur batteries with stabilized lithium-metal anode

Xu, Henghui; Qie, Long; Manthiram, Arumugam

doi:10.1016/j.nanoen.2016.05.028

Cited by 97 publications

(40 citation statements)

References 50 publications

(43 reference statements)

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“…It has been recognized that fabricating thick sulfur cathodes via-traditional slurry coating with a large fraction of carbon (>40%) is problematic due to cracking and peeling off problems. 102 Manthiram et al adopted alternate approaches with carbon nanotubes, i.e., i) a dual-layer design with carbon nanofibers as host in which lithium polysulfide solution was active material 103 and ii) a flexible and robust paper electrode consisting of carbon nanotubes (CNT) and activated carbon nanofibers (ACNF) loaded with MnO 2 nanosheets to serve as an efficient sulfur host 104 for Li/dissolved polysulfide batteries. Even though high loadings are possible in some of the approaches, these methods yield low volumetric/gravimetric energy densities and are not readily relevant to conventional large scale cell manufacturing.…”

Section: Resultsmentioning

confidence: 99%

Metal Sulfide-Blended Sulfur Cathodes in High Energy Lithium-Sulfur Cells

Bugga

Jones

Pasalic

et al. 2016

J. Electrochem. Soc.

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Lithium-sulfur cells exhibit poor cycle life, due to the well-known 'polysulfide shuttle' enabled by the dissolution of the sulfur reduction products in organic electrolyte. Different strategies have been implemented to reduce the shuttle effects, with limited success, especially through use of low sulfur loadings (1-2 mg/cm 2 ). Dense electrodes with high sulfur loadings are essential for high energy cells, however, such electrodes experience more serious polysulfide effects. In this paper, we describe the benefits of blending sulfur with a transition metal sulfide (here, TiS 2 and MoS 2 ) to form dense composite cathodes with enhanced conductivity. There is an improvement in both the initial capacity from sulfur utilization (∼800 mAh/g based on sulfur content), the coulombic efficiency (>96%) and also in cycle life upon blending with the metal sulfide. High sulfur loadings (>12 mg/cm 2 or ∼6 mAh/cm 2 per side) were demonstrated to display high sulfur utilization in Li-S cells containing the metal sulfide blends either with or without coatings over the sulfur cathode. XRD studies were carried out to understand the redox behavior of the metal sulfide additive during charge/discharge cycling of the sulfur cathodes. DC polarization and Potentiometric Intermittent Titration Technique (PITT) measurements were made on sulfur cathodes with and without metal sulfide blends to determine the charge transfer and diffusional kinetics. Since their inception in 1991, Li-ion batteries 1 have progressed at a rapid pace, with a three-fold enhancement in their performance achieved through many advances in both electrode materials and electrolytes.2-9 Current Li-ion cells from commercial vendors (e.g., Panasonic, LG and Samsung) provide an impressive specific energy of >250 Wh/kg and energy density of >600 Wh/l which are benefiting a wide range of applications including portable electronic devices, electric vehicles and aerospace needs. Yet, many of the emerging markets such as electric vehicles and renewable energy technologies place even higher demands on the battery technologies, both in terms of performance and cost. It is believed that the performance of lithium-ion technologies has reached a plateau, and any future improvements will only be marginal. Replacement of graphite anodes with Si, and conventional 4 V cathodes with the high voltage Li-rich layered-layered composite cathodes, 10,11 has not yet successfully been applied to commercial batteries. Accordingly, any gains in specific energy and energy density have been modest so far after a decade of development. 12,13 There is, thus, a pursuit for more energetic battery technologies beyond Li-ion batteries. This has led to a renewed interest in the lithiumsulfur system, which has the highest theoretical specific energy of all the known rechargeable systems (due to the high capacity of sulfur, 1672 mAh/g, ∼ 6-10x of Li-ion cathodes), with the notable exception of Li-O 2 which itself has several serious fundamental hurdles that are not close to being overcome.14-16 The spe...

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Section: Resultsmentioning

confidence: 99%

Metal Sulfide-Blended Sulfur Cathodes in High Energy Lithium-Sulfur Cells

Bugga

Jones

Pasalic

et al. 2016

J. Electrochem. Soc.

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“…Thes olid electrolyte can efficiently block the polysulfide shuttle,w hich is as evere problem in Li-S batteries. [15] Thet otal resistance of the cells with LLZT and LLZT-2LiF in Figure 4a were 1000 and 2620 W cm À2 ,r espectively.T he cells with LLZT and LLZT-LiF display welldefined discharge/charge plateaus and low overpotentials, suggesting full electrolyte wetting. Thec ell with LLZT-2LiF exhibited am uch lower voltage gap (0.34 V) than that with LLZT (0.59 V) at the current density of 200 mAcm À2 .T he much reduced interfacial resistance allows the cells to be cycled at high current densities.A ss hown in Figure 4c, discharge capacities of 1137, 1074, and 1042 mAh g À1 can be obtained at the rates of 100, 200 and 300 mAcm À2 ,r espectively.Notably,since the polysulfide shuttle can be completely blocked by the solid electrolyte,t he hybrid cells assembled also exhibit astable cyclability at 200 mAcm À2 .The reversible capacity stabilized at 988 mAh g À1 after 100 cycles with the retention of 93 %ofthe stabilized capacity in the second cycle (Figure 4d).…”

Section: Angewandte Chemiementioning

confidence: 96%

Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium‐Ion Batteries

Li¹,

Xu³

et al. 2016

Angewandte Chemie

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112

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Li 7 La 3 Zr 2 O 12 -based Li-rich garnets react with water and carbon dioxide in air to form a Li-ion insulating Li 2 CO 3 layer on the surface of the garnet particles, which results in a large interfacial resistance for Li-ion transfer. Here, we introduce LiF to garnet Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZT) to increase the stability of the garnet electrolyte against moist air; the garnet LLZT-2 wt % LiF (LLZT-2LiF) has less Li 2 CO 3 on the surface and shows a small interfacial resistance with Li metal, a solid polymer electrolyte, and organic-liquid electrolytes. An all-solid-state Li/polymer/LLZT-2LiF/ LiFePO 4 battery has a high Coulombic efficiency and long cycle life; a Li-S cell with the LLZT-2LiF electrolyte as a separator, which blocks the polysulfide transport towards the Li-metal, also has high Coulombic efficiency and kept 93 % of its capacity after 100 cycles.

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Section: à2mentioning

confidence: 96%

Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium‐Ion Batteries

et al. 2016

Angew Chem Int Ed

Self Cite

485

311

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Li La Zr O -based Li-rich garnets react with water and carbon dioxide in air to form a Li-ion insulating Li CO layer on the surface of the garnet particles, which results in a large interfacial resistance for Li-ion transfer. Here, we introduce LiF to garnet Li La Zr Ta O (LLZT) to increase the stability of the garnet electrolyte against moist air; the garnet LLZT-2 wt % LiF (LLZT-2LiF) has less Li CO on the surface and shows a small interfacial resistance with Li metal, a solid polymer electrolyte, and organic-liquid electrolytes. An all-solid-state Li/polymer/LLZT-2LiF/LiFePO battery has a high Coulombic efficiency and long cycle life; a Li-S cell with the LLZT-2LiF electrolyte as a separator, which blocks the polysulfide transport towards the Li-metal, also has high Coulombic efficiency and kept 93 % of its capacity after 100 cycles.

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An integrally-designed, flexible polysulfide host for high-performance lithium-sulfur batteries with stabilized lithium-metal anode

Cited by 97 publications

References 50 publications

Metal Sulfide-Blended Sulfur Cathodes in High Energy Lithium-Sulfur Cells

Metal Sulfide-Blended Sulfur Cathodes in High Energy Lithium-Sulfur Cells

Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium‐Ion Batteries

Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium‐Ion Batteries

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