Development of low-cost sodium-aqueous polysulfide hybrid batteries

Gross, Martha; Manthiram, Arumugam

doi:10.1016/j.ensm.2019.03.026

Cited by 31 publications

(30 citation statements)

References 45 publications

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“…Besides, in light of these results, the nanopore technology stands as being a powerful sensing tool to probe at the molecular level the sulfur speciation in aqueous Na-ion/polysulfide medias [39][40][41] and to test the hypothesis of manufacturing such membrane proposed in Fig. 6.…”

Section: Discussionmentioning

confidence: 99%

“…Herein we report a protein channel, α-hemolysin (α-HL) nanopore, with a β-cyclodextrin adapter as a simplified model to understand the encapsulation of polysulfides by cyclodextrins to be extended to smart membrane design for Li-S batteries. As a proof of concept of both cyclodextrins affinity towards (S n ) 2− and nanopore sensitivity, we have used Na-based polysulfide species Na 2 S n (n = 3, 4, 5) in aqueous media that can be found as catholyte in aqueous Na-ion/polysulfide batteries [39][40][41] . In this contribution, the reversible equilibrium complexation between sodium polysulfides and cyclodextrins is demonstrated and their interaction characterized by complementary NMR spectroscopy, nanopore experiments and molecular docking calculations.…”

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confidence: 99%

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Single-sulfur atom discrimination of polysulfides with a protein nanopore for improved batteries

et al. 2020

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Research on batteries mostly focuses on electrodes and electrolytes while few activities regard separator membranes. However, they could be used as a toolbox for injecting chemical functionalities to capture unwanted species and enhance battery lifetime. Here, we report the use of biological membranes hosting a nanopore sensor for electrical single molecule detection and use aqueous sodium polysulfides encountered in sulfur-based batteries for proof of concept. By investigating the host-guest interaction between polysulfides of different chain-lengths and cyclodextrins, via combined chemical approaches and molecular docking simulations, and using a selective nanopore sensor inserted into a lipid membrane, we demonstrate that supramolecular polysulfide/cyclodextrin complexes only differing by one sulfur can be discriminated at the single molecule level. Our findings offer innovative perspectives to use nanopores as electrolyte sensors and chemically design membranes capable of selective speciation of parasitic molecules for battery applications and therefore pave the way towards smarter electrochemical storage systems.

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Section: Discussionmentioning

confidence: 99%

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confidence: 99%

Single-sulfur atom discrimination of polysulfides with a protein nanopore for improved batteries

et al. 2020

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“…To facilitate the electrochemical study of the conversion reaction between Na 2 S 2 and Na 2 S 4 , we control the counterelectrode as a pure Na + provider by utilizing the sodium metal with stable 1 m NaClO 4 /PC organic electrolyte. [ 16 ] In this experiment, we use 1 m Na 2 S 4 /2 m NaOH as the catholyte in the initial discharge process for the hybrid cell. Based on the whole reactions from S 8 to

{normalS}_{2}^{2 -}

, the state of charge (SOC) for Na 2 S 4 and Na 2 S 2 solution corresponds to 75% and 50%, respectively.…”

Section: Resultsmentioning

confidence: 99%

“…In agreement with previous reports, there is a uniform voltage plateau located around 2.1 V for the discharge process and 2.3 V for the charging process. [ 16 ] Despite only discharging one quarter of the capacity of sulfur, the sulfur‐specific capacity of the aqueous cell still reaches up to ≈418 mA h g −1 . The corresponding sulfur‐based energy density was estimated to be 910 Wh kg −1 , which is much higher than that of other aqueous redox species and shows great promise.…”

Section: Resultsmentioning

confidence: 99%

“…The corresponding sulfur‐based energy density was estimated to be 910 Wh kg −1 , which is much higher than that of other aqueous redox species and shows great promise. [ 16 ] Moreover, the APS reactions delivered good reversibility with a stable cycling performance over 80 cycles. However, the voltage profile on the 83th discharge shows a second plateau.…”

Section: Resultsmentioning

confidence: 99%

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Electrochemical Reactions and Failure Mechanism Study of Sodium‐Aqueous Polysulfide Conversion Reactions in Redox Flow Batteries

2020

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Low‐cost aqueous polysulfide (APS) chemistry has recently attracted intensive research as it is a promising candidate for redox flow batteries. However, the intrinsic properties, electrochemical stability, and compatibility with sodium super ionic conductor (NASICON) membrane have been rarely demonstrated to clarify the challenges on the road to practical application. Herein, a detailed study on the electrochemical reactions and failure mechanism of aqueous polysulfides is presented. Starting from investigating the intrinsic stability, the optimized concentration of NaOH is determined. Through constructing a hybrid Na‐APS cell to avoid the effect from the counterelectrode, the cycling behavior is found to be stable under the capacity cut‐off condition, while severe decay occurs after ≈80 cycles. Comprehensive analysis of the decay mechanism shows the decomposition and loss of active materials during the long‐term cycles. Meanwhile, the NASICON separator surface is found to be corrosive after electrochemical exposure with APS solution under a high‐pH environment. It is anticipated that the systematic study of the APSs’ electrochemical reactions and decay mechanism could be beneficial for their further application in redox flow batteries.

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Initiating a Reversible Aqueous Zn/Sulfur Battery through a “Liquid Film”

et al. 2020

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Sulfur cathodes have been under intensive study in various systems, such as Li/S, Na/S, Mg/S, and Al/S batteries. However, to date, Zn/S chemistry has never been reported. The first reliable aqueous Zn/polysulfide system activated by a “liquid film” comprising 4‐(3‐butyl‐1‐imidazolio)‐1‐butanesulfoni ionic liquid (IL) encapsulated within PEDOT:PSS. CF3SO3− anions in the IL operating as Zn2+‐transfer channels is reported. Moreover, the PEDOT:PSS network retains the IL, which renders Zn2+‐transfer channels and a polysulfide cathode with enhanced structural stability. The Zn/polysulfide system delivers extraordinary capacity of 1148 mAh g−1 and overwhelming energy density of 724.7 Wh kg−1cathode at 0.3 Ag−1. During the discharging phase, S62− is dominantly reduced by Zn to S2− (S6 → S2−). During the charging phase, these short chains are oxidized to form long‐chain ZnxLiyS3‐6. A further optimized high‐concentrated salt electrolyte is used to improve the reversibility of the battery, demonstrating an extended lifetime over 1600 cycles at 1 Ag−1 with a capacity retention of 204 mAh g−1. This facile approach and the superior performance of the developed aqueous Zn/S chemistry provide a new platform for sulfur‐based battery and potentially solve the problems of other metal/sulfur batteries.

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Development of low-cost sodium-aqueous polysulfide hybrid batteries

Cited by 31 publications

References 45 publications

Single-sulfur atom discrimination of polysulfides with a protein nanopore for improved batteries

Single-sulfur atom discrimination of polysulfides with a protein nanopore for improved batteries

Electrochemical Reactions and Failure Mechanism Study of Sodium‐Aqueous Polysulfide Conversion Reactions in Redox Flow Batteries

Initiating a Reversible Aqueous Zn/Sulfur Battery through a “Liquid Film”

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