Surface-enhanced redox chemistry of polysulphides on a metallic and polar host for lithium-sulphur batteries

Pang, Quan; Kundu, Dipan; Cuisinier, Marine; Nazar, Linda F.

doi:10.1038/ncomms5759

Cited by 1,170 publications

(910 citation statements)

References 43 publications

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“…Such changes are more visually obvious in the corresponding voltage profiles obtained in galvanostatic mode (Fig. 1B), where a single, well-defined plateau at ∼2.5 V represents the discharge/charge of S-KB in the WiBS electrolyte, significantly differing from the two plateaus found at ∼2.3 and 2.1 V in nonaqueous electrolyte (20). Apparently, the electrochemical reaction of sulfur in this superconcentrated aqueous electrolyte proceeds via a new reaction mechanism that is hitherto unknown.…”

Section: Resultsmentioning

confidence: 86%

Unique aqueous Li-ion/sulfur chemistry with high energy density and reversibility

Yang

Suo

Borodin

et al. 2017

Proc. Natl. Acad. Sci. U.S.A.

165

182

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Leveraging the most recent success in expanding the electrochemical stability window of aqueous electrolytes, in this work we create a unique Li-ion/sulfur chemistry of both high energy density and safety. We show that in the superconcentrated aqueous electrolyte, lithiation of sulfur experiences phase change from a highorder polysulfide to low-order polysulfides through solid-liquid two-phase reaction pathway, where the liquid polysulfide phase in the sulfide electrode is thermodynamically phase-separated from the superconcentrated aqueous electrolyte. The sulfur with solid-liquid two-phase exhibits a reversible capacity of 1,327 mAh/(g of S), along with fast reaction kinetics and negligible polysulfide dissolution. By coupling a sulfur anode with different Li-ion cathode materials, the aqueous Li-ion/sulfur full cell delivers record-high energy densities up to 200 Wh/(kg of total electrode mass) for >1,000 cycles at ∼100% coulombic efficiency. These performances already approach that of commercial lithium-ion batteries (LIBs) using a nonaqueous electrolyte, along with intrinsic safety not possessed by the latter. The excellent performance of this aqueous battery chemistry significantly promotes the practical possibility of aqueous LIBs in large-format applications.water-in-salt | rechargeable aqueous battery | aqueous sulfur battery | gel polymer electrolyte | phase separation I n the past two decades, rechargeable lithium-ion batteries (LIBs) have revolutionized consumer electronics with their high energy density and excellent cycling stability, and are the state-of-the-art candidates for applications ranging from kilowatt hours for electric vehicles up to megawatt hours for grids (1, 2). The latter applications in large-format present much more stringent requirements for safety, cost, and environmental friendliness, besides energy density and cycle life. The shortcomings of LIB are mostly due to the flammable and toxic nonaqueous electrolytes and moderate energy densities (<400 Wh·kg −1 ) provided by the electrochemical couples currently used (3). Among the various "beyond Li-ion" high-energy chemistries (>500 Wh·kg −1 ) explored currently, the nonaqueous lithium/sulfur (Li/S) battery based on sulfur as a cathode (theoretical capacity of 1,675 mAh·g −1 ) and metallic lithium as an anode seems to be the most practical, as evidenced by the mushrooming literature and significant advances in this system in the past 5 y (4-7). However, commercialization of this system still faces challenges because of severe safety concerns associated with the dendrite growth of metallic Li anode in highly inflammable ether-based electrolytes (8), and the high self-discharge associated with parasitic shuttling of the intermediate polysulfide species. Moreover, the moisture-sensitive nature of the nonaqueous electrolyte would contribute significantly to the cost of the Li/S battery pack due to the stringent moisture-exclusion infrastructure required during the manufacturing, processing, and packaging of the cells. The indispensabl...

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Section: Resultsmentioning

confidence: 86%

Unique aqueous Li-ion/sulfur chemistry with high energy density and reversibility

Yang

Suo

Borodin

et al. 2017

Proc. Natl. Acad. Sci. U.S.A.

165

182

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“…However, the severe shuttle effect and dendrite growth, and the inferior Coulombic efficiency that characterize these Li‐S batteries have greatly limited their lifespan 4, 8, 9, 10. Although much effort has been expended in the development of novel sulfur‐host electrodes,11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36 separators,37, 38, 39, 40 and electrolytes41, 42, 43, 44, 45 to resolve these issues, some of which are rather dangerous, the results have been at best minimal in improving current Li‐S battery technology. As a result, the cycling life and Coulombic efficiency of Li‐S batteries, especially in the high‐rate regime, are still far behind the state of the art in lithium‐ion battery technology.…”

Section: Introductionmentioning

confidence: 99%

Simultaneous Suppression of the Dendrite Formation and Shuttle Effect in a Lithium–Sulfur Battery by Bilateral Solid Electrolyte Interface

et al. 2018

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Although the reversible and inexpensive energy storage characteristics of the lithium–sulfur (Li‐S) battery have made it a promising candidate for electrical energy storage, the dendrite growth (anode) and shuttle effect (cathode) hinder its practical application. Here, it is shown that new electrolytes for Li‐S batteries promote the simultaneous formation of bilateral solid electrolyte interfaces on the sulfur‐host cathode and lithium anode, thus effectively suppressing the shuttle effect and dendrite growth. These high‐capacity Li‐S batteries with new electrolytes exhibit a long‐term cycling stability, ultrafast‐charge/slow‐discharge rates, super‐low self‐discharge performance, and a capacity retention of 94.9% even after a 130 d long storage. Importantly, the long cycle stability of these industrial grade high‐capacity Li‐S pouch cells with new electrolytes will provide the basis for creating robust energy dense Li‐S batteries with an extensive life cycle.

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“…The battery delivers a reversible discharge capacity of 1250 mAh g −1 at current rate of 0.1 C that slowly reduced to 1130 mAh g −1 at 0.2 C , 930 mAh g −1 at 0.5 C , 753 mAh g −1 at 1 C , and 685 mAh g −1 at 2 C . Even at high rate of 4 C (6680 mA g −1 ), the leaf‐like GO/S cathode still can deliver a capacity of 468 mAh g −1 , which is almost the best rate performance of C/S composite cathode 8, 10, 11, 12, 14, 15, 16, 17, 18, 19, 20, 21, 22, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 45, 46, 48, 51, 52, 53…”

Section: Resultsmentioning

confidence: 92%

“…According to their report, strong chemical interaction between S and the functional groups on GO happens and S can partially reduce the GO. Especially, according to very recent investigations,41, 46 the hydrophilic surface groups of GO should be quite important for immobilizing the hydrophilic lithium polysulfide intermediates. Furthermore, GO network can also accommodates the volume change of the electrode during the Li–S electrochemical reaction.…”

Section: Introductionmentioning

confidence: 99%

“…Then, more and more researches have focused on GO/S composites and modified GO/S composites, and further improvements in cyclability of Li–S battery have been achieved by smartly designing GO/S composites in recent years 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35. However, one of the most salient problems of GO also arises from the functional groups on the surface that lead to poor electronic conductivity 46. Therefore, the achieved rate performances in most previous reports about GO/S composites are generally below the rate of 2 C (1 C = 1675 mA g −1 ) 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35.…”

Section: Introductionmentioning

confidence: 99%

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Leaf‐Like Graphene‐Oxide‐Wrapped Sulfur for High‐Performance Lithium–Sulfur Battery

et al. 2015

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Carbon/sulfur composites are attracting extensive attention because of their improved performances for Li–S batteries. However, the achievements are generally based on the low S‐content in the composites and the low S‐loading on the electrode. Herein, a leaf‐like graphene oxide (GO), which includes an inherent carbon nanotube midrib in the GO plane, is synthesized for preparing GO/S composites. Owing to the inherent high conductivity of carbon nanotube midribs and the abundant surface groups of GO for S‐immobilization, the composite with an S‐content of 60 wt% exhibits ultralong cycling stability over 1000 times with a low capacity decay of 0.033% per cycle and a high rate up to 4C. When the S‐content is increased to 75 wt%, the composite still shows a perfect cycling performance over 1000 cycles. Even with the high S‐loading of 2.7 mg cm−2 on the electrode and the high S‐content of 85 wt%, it still shows a promising cycling performance over 600 cycles.

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Surface-enhanced redox chemistry of polysulphides on a metallic and polar host for lithium-sulphur batteries

Cited by 1,170 publications

References 43 publications

Unique aqueous Li-ion/sulfur chemistry with high energy density and reversibility

Unique aqueous Li-ion/sulfur chemistry with high energy density and reversibility

Simultaneous Suppression of the Dendrite Formation and Shuttle Effect in a Lithium–Sulfur Battery by Bilateral Solid Electrolyte Interface

Leaf‐Like Graphene‐Oxide‐Wrapped Sulfur for High‐Performance Lithium–Sulfur Battery

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