Tetrathiafulvalene as a multifunctional electrolyte additive for simultaneous interface amelioration, electron conduction, and polysulfide redox regulation in lithium-sulfur batteries

Wu, Tong; Ye, Jin-Ting; Li, Tunan; Liu, Yuong; Liu, Jia; Sun, Liqun; Liu, Jinghai; Xie, Haiming

doi:10.1016/j.jpowsour.2022.231482

Cited by 16 publications

(5 citation statements)

References 46 publications

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“…Different from the cathode side, the S–O and thiosulfate doublet peaks observed in the anode side are more likely to be due to the oxidation of LiPSs by LiNO 3 , resulting in the formation of Li 2 SO 3 and Li 2 SO 4 on the Li anode while LiNO 3 is reduced to LiNO 2 (Figure S18). − It is widely reported that the LiNO 3 -induced passivation layer is capable of suppressing Li corrosion caused by LiPSs and alleviating the shuttle effect; however, it is insufficient to restrain the irreversible capacity decay, especially upon the depletion of LiNO 3 . This results in rich short-chain Li 2 S 2 /Li 2 S deposits on the Li surface upon prolonged cycling, producing a high interface impedance.…”

Section: Results and Discussionmentioning

confidence: 99%

Catalytic Effect of Ammonium Thiosulfate as a Bifunctional Electrolyte Additive for Regulating Redox Kinetics in Lithium–Sulfur Batteries by Altering the Reaction Pathway

Lu,

Liu,

Zhang

et al. 2024

ACS Appl. Mater. Interfaces

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Sluggish sulfur redox kinetics and incessant shuttling of lithium polysulfides (LiPSs) greatly influence the electrochemical properties of lithium−sulfur (Li−S) batteries and their practical applications. For this reason, ammonium thiosulfate (AMTS) with effective redox regulation capability has been proposed as a functional electrolyte additive to promote the bidirectional conversion of sulfur species and inhibit the shuttle effect of soluble LiPSs. During discharging, the S 2 O 3 2− in AMTS can trigger the rapid reduction of LiPSs from long chains to short chains by a spontaneous chemical reaction with sulfur species, thereby decreasing the accumulation of LiPSs in the electrolyte. During charging, the NH 4 + in the AMTS enhances the dissociation/dissolution of Li 2 S 2 /Li 2 S by hydrogen-binding interactions, which alleviates the electrode surface passivation and facilitates the reversible oxidation of short-chain sulfides back to long chains. The enhanced bidirectional redox kinetics brought about by AMTS endows Li−S cells with high reversible capacity, excellent cycle stability, and rate capability even under lean electrolyte conditions. This work not only illustrates an effective redox regulation strategy by an electrolyte additive but also investigates its catalytic reaction mechanism and Li corrosion behavior. The crucial criteria for screening additives that enable bidirectional redox mediation analogous to AMTS are summarized, and its application perspectives/challenges are further discussed.

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Section: Results and Discussionmentioning

confidence: 99%

Catalytic Effect of Ammonium Thiosulfate as a Bifunctional Electrolyte Additive for Regulating Redox Kinetics in Lithium–Sulfur Batteries by Altering the Reaction Pathway

Lu,

Liu,

Zhang

et al. 2024

ACS Appl. Mater. Interfaces

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“…Up to now, various strategies have been adopted to address the abovementioned issues for Li-S batteries [10][11][12][13].…”

Section: Introductionmentioning

confidence: 99%

Porous FeNi Prussian blue cubes derived carbon-based phosphides as superior sulfur hosts for high-performance lithium–sulfur batteries

Zhang,

Wei,

Liu

et al. 2024

Nanotechnology

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In contrast to lithium-ion batteries, lithium–sulfur batteries have higher theoretical energy density and lower cost, so they would become competitive in the practical application. However, the shuttle effect of polysulfides and slow oxidation–reduction kinetics can degrade their electrochemical performance and cycle life. In this work, we have first developed the porous FeNi Prussian blue cubes as precursors. The calcination in different atmospheres was employed to make precursors convert into common pyrolysis products or novel carbon-based phosphides, and sulfides, labeled as FeNiP/A-C, FeNiP/A-P, and FeNiP/A-S. When these products serve as host materials in the sulfur cathode, the electrochemical performance of lithium–sulfur batteries is in the order of S@FeNiP/A-P > S@FeNiP/A-S > S@FeNiP/A-C. Specifically, the initial discharge capacity of S@FeNiP/A-P can reach 679.1 mAh g−1 at 1 C, and the capacity would maintain 594.6 mAh g−1 after 300 cycles. That is because the combination of carbon-based porous structure and numerous well-dispersed Ni2P/Fe2P active sites contribute FeNiP/A-P to obtain larger lithium-ion diffusion, lower resistance, stronger chemisorption, and more excellent catalytic effect than other samples. This work may deliver that metal–organic framework-derived carbon-based phosphides are more suitable to serve as sulfur hosts than carbon-based sulfides or common pyrolysis products for enhancing Li–S batteries’ performance.

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“…[8,9] In the past few decades, researchers have gained a profound understanding of the lithium ion battery system through extensive exploration of the failure mechanism and made significant improvements in sulfur cathodes, [10,11] lithium anodes, [12,13] and electrolytes. [14] It is important to note that electrolytes or electrolyte additives play a key role in LSB, [15,16] so the development of electrolytes and electrolyte additives that can both protect the battery and maintain or improve the efficiency of the battery remains an important area of battery research. Hou et al [17] significantly improved the high-rate cycle performance of Li-S batteries by introducing fluoroalkyl ether 2,2,2-trifluor-oethyl-1,1,2,3,3,3-hexafluoropropyl ether (THE) directly into commercial ether electrolytes.…”

Section: Introductionmentioning

confidence: 99%

“…In terms of electrolyte additives, multifunctional electrolyte additives are being widely studied, [18,19] most of which are designed to form a protective film on the electrode surface to prevent parasitic solvent reduction or oxidation. By optimizing electrolytic liquefaction, Wu et al [15] used tetrathiafulvalene (TTF) as a multifunctional catalyst for high-performance LSB. The addition of TTF additives to the electrolyte, which acts as a π-electron donor molecule, improves the electron transport of Li 2 S x through van der Waals interaction, and promotes the formation of a highly conductive passivating layer from LiNO 3 to Li 3 N on the lithium anode (lithium anode), which protects the lithium anode.…”

Section: Introductionmentioning

confidence: 99%

First‐Principles Investigations to Evaluate NiCl₂/NiF₂ as Cycle‐Catalyzed Electrolyte Additives to Improve Li–S Batteries’ Performance

Wang

Zhang

et al. 2023

Energy Tech

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The potential application of two electrolyte additives, NiCl2‐DME and NiF2‐DME, in lithium–sulfur batteries is investigated by density functional theory calculations. The results show that both electrolyte additives can effectively adsorb soluble lithium polysulfide (LiPSs) in the electrolyte. With the progress of the charging–discharge reaction, NiCl2 and NiF2 separate from Li2Sn when it is converted to S8 and recombine with 1,2‐dimethoxy‐ethane (DME) to achieve the purpose of cyclic adsorption of polysulfide in the electrolyte. At the same time, NiF2 and NiCl2 also have a catalytic effect in the cycling process. When adsorbed with Li2Sn, the bond length of the Li–S bond in Li2Sn is elongated, which causes the reduction of the Li2Sn activation energy, making it easier to be oxidized, and accelerating the conversion speed of Li2Sn and reducing Li2S, Li2S2 deposition on the surface of the electrode. Therefore, NiCl2‐DME and NiF2‐DME are ideal dual‐function electrolyte additives.

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Tetrathiafulvalene as a multifunctional electrolyte additive for simultaneous interface amelioration, electron conduction, and polysulfide redox regulation in lithium-sulfur batteries

Cited by 16 publications

References 46 publications

Catalytic Effect of Ammonium Thiosulfate as a Bifunctional Electrolyte Additive for Regulating Redox Kinetics in Lithium–Sulfur Batteries by Altering the Reaction Pathway

Catalytic Effect of Ammonium Thiosulfate as a Bifunctional Electrolyte Additive for Regulating Redox Kinetics in Lithium–Sulfur Batteries by Altering the Reaction Pathway

Porous FeNi Prussian blue cubes derived carbon-based phosphides as superior sulfur hosts for high-performance lithium–sulfur batteries

First‐Principles Investigations to Evaluate NiCl₂/NiF₂ as Cycle‐Catalyzed Electrolyte Additives to Improve Li–S Batteries’ Performance

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Tetrathiafulvalene as a multifunctional electrolyte additive for simultaneous interface amelioration, electron conduction, and polysulfide redox regulation in lithium-sulfur batteries

Cited by 16 publications

References 46 publications

Catalytic Effect of Ammonium Thiosulfate as a Bifunctional Electrolyte Additive for Regulating Redox Kinetics in Lithium–Sulfur Batteries by Altering the Reaction Pathway

Catalytic Effect of Ammonium Thiosulfate as a Bifunctional Electrolyte Additive for Regulating Redox Kinetics in Lithium–Sulfur Batteries by Altering the Reaction Pathway

Porous FeNi Prussian blue cubes derived carbon-based phosphides as superior sulfur hosts for high-performance lithium–sulfur batteries

First‐Principles Investigations to Evaluate NiCl2/NiF2 as Cycle‐Catalyzed Electrolyte Additives to Improve Li–S Batteries’ Performance

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First‐Principles Investigations to Evaluate NiCl₂/NiF₂ as Cycle‐Catalyzed Electrolyte Additives to Improve Li–S Batteries’ Performance