Facilitating the redox reaction of polysulfides by an electrocatalytic layer-modified separator for lithium–sulfur batteries

Zuo, Pengjian; Hua, Junfu; He, Meizi; Zhang, Han; Qian, Zhengyi; Ma, Yulin; Du, Chunyu; Cheng, Xinqun; Gao, Yunzhi; Yin, Geping

doi:10.1039/c7ta02245j

Cited by 84 publications

(35 citation statements)

References 62 publications

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“…Furthermore, through fitting the Tafel curves of various symmetric cells, it can be found that the exchange current density of the C‐C‐N‐Co electrode is the highest (588.8 µA cm −2 ) (Figure S12, Supporting Information). The higher exchange current density of the C‐C‐N‐Co electrode confirms that the incorporation of the NC@SA‐Co can effectively accelerate the redox kinetics of soluble polysulfides, which is in accordance with the results of EIS and CV …”

Section: Resultssupporting

confidence: 88%

A Freestanding Flexible Single‐Atom Cobalt‐Based Multifunctional Interlayer toward Reversible and Durable Lithium‐Sulfur Batteries

Zhou

et al. 2020

Small Methods

136

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The development of Li‐S batteries is greatly hindered by the polysulfide shuttling and sluggish sulfur redox kinetics, leading to low utilization of active materials and rapid capacity decay. Herein, a freestanding multifunctional interlayer, prepared by layer‐by‐layer assembling of the single‐atom cobalt‐anchored nitrogen‐doped carbon nanosheets (NC@SA‐Co) and dual network of carbon nanotube‐cellulose nanofiber (CNT‐CNF) hybrid, is proposed to effectively enhance the polysulfide immobilization and sulfur redox kinetics. The conductive CNT network acts as the physical barrier to confine the polysulfide diffusion and to facilitate the reuse of polysulfides. The oxygen‐group‐terminated CNF network allows the hopping of Li+ ion and suppresses the polysulfide crossover due to the strong electrostatic repulsion. Moreover, it is demonstrated that the 2D NC@SA‐Co with numerous well‐defined single sites of Co–N4 can effectively serve as an electrocatalyst to boost the reversible reaction of polysulfides. As a result, the assembled Li‐S batteries with the multifunctional interlayer deliver a high reversible specific capacity of 1160 mAh g−1 at 0.1 C and an ultralow capacity decay of 0.058% per cycle over 700 cycles. Even with a high sulfur loading of 7.2 mg cm−2, a high areal capacity of 8.3 mAh cm−2 can be achieved.

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Section: Resultssupporting

confidence: 88%

A Freestanding Flexible Single‐Atom Cobalt‐Based Multifunctional Interlayer toward Reversible and Durable Lithium‐Sulfur Batteries

Zhou

et al. 2020

Small Methods

136

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“…To fully utilize the sulfur species during cycling for a high‐performance functional separator, it is important to optimize the combination of a material component for the PS‐anchoring material and conducting material. Various conductive carbon materials, including 0D carbon black, 1D CNTs and 2D graphene, are normally added to the coating layer to compensate for the insulating properties of metal oxides. Compared to the carbon only functional separators, the metal oxide layers with carbon additives showed an up to fivefold increase in resistance.…”

Section: E‐functionsmentioning

confidence: 99%

“…Based on these fundamental studies, a range of catalytic materials, including MnO 2 , organometallic redox mediators, iridium (Ir), Pt, TiN–TiO 2 , MoC@MoO x , and V 2 O 5 , were assessed as functional separators to improve the kinetics of the polysulfide species. Before starting the discussion, the above‐mentioned k‐functional materials exhibiting catalytic effects can be categorized into four groups according to their mobility and target redox species: (a) mobile k‐functional materials for Li 2 S 6 /Li 2 S 4 , (b) immobile k‐functional materials for Li 2 S 6 /Li 2 S 4 , (c) mobile k‐functional materials for Li 2 S 2 /Li 2 S, and (d) immobile k‐functional materials for Li 2 S 2 /Li 2 S. Table 4 lists the four categorized k‐functional materials regardless of the component where the functional materials were used.…”

Section: K‐functionsmentioning

confidence: 99%

“…According to theoretical studies on the mechanism of Li–S batteries, the polysulfide scissoring reactions and lithium sulfide activation are the rate determining step for Li–S batteries. Recently, catalyst‐incorporated nanomaterials, e.g., organometallic redox mediators, DTT, iridium, Pt, TiN–TiO 2 , MoC@MoO x , V 2 O 5 , and MnO 2 , have been investigated to enhance the sluggish kinetics. On the other hand, a comprehensive design for dealing with all the sluggish redox species from the high‐order polysulfide chain to the lower‐order lithium sulfide and lithium disulfide simultaneously is difficult to find in the literature.…”

Section: Perspectives For Functional Interlayers/separators Of Li–s Bmentioning

confidence: 99%

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Rational Design of Nanostructured Functional Interlayer/Separator for Advanced Li–S Batteries

Jeong

Kim

Nam

et al. 2018

Adv Funct Materials

307

197

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The lithium-sulfur (Li-S) battery is considered as a promising future energy storage device owing to its high theoretical energy density, low cost of the raw active material (sulfur), and its environmental friendliness. On the other hand, there are still challenging issues for the practical applications of Li-S batteries, including low sulfur utilization, poor cyclability, and rate capability. Although considerable efforts are made to overcome the current obstacles in Li-S batteries, one is still far from meeting the requirements for the commercialization of Li-S batteries. This review outlines the recent progress in Li-S batteries based on novel configurations, such as incorporating functional interlayers/separators beyond the approach for preparing novel cathodes, and discusses the role of the configuration in Li-S batteries. The functions of the newly introduced functional interlayer/separator are highlighted to address the problems of Li-S batteries. From classification of the functions, the perspectives and outlook are presented to rationally design a novel functional interlayer/separator for high-performance Li-S batteries.

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“…The top layer took part in reversible adsorption–desorption of polysulfides, and the polysulfide trapping layer beneath rendered the mat structure with thermal and mechanical stability. Zuo et al incorporated a composite of Ketjen Black and iridium nanoparticles (KB@Ir), instead of metal oxides, to coat a commercial Celgard 2400 membrane . Highly conductive iridium catalyzed the electrochemical redox reactions at the separator surface via a strong chemical interaction with diffusive polysulfides, and Ketjen Black served as an upper current collector to facilitate the utilization of active sulfur.…”

Section: A Summary Of Recent Literature On Li‐s Battery Separators CLmentioning

confidence: 99%

Separator Membranes for Lithium–Sulfur Batteries: Design Principles, Structure, and Performance

Gupta

Sivaram

2019

Energy Tech

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Improvement in electrical energy storage systems is one of the most recent research topics of great academic and industrial interest. Lithium‐sulfur (Li‐S) battery systems offer a theoretical energy density an order of magnitude larger than the popular Li‐ion batteries. The principle of working, inherent challenges in utilizing this system for commercial applications, and the various approaches taken to address these challenges are herein discussed in detail. The polysulfide shuttle effect is a major concern that deteriorates electrochemical performance in this system. In the recent past, electrodes have been intricately engineered to tackle this problem. However, more recently, the focus has shifted to the critical role of the separator. Modifying conventional separators or fabricating novel structures to enhance the cell performance appears to be a more feasible option. Some design principles that are critical to the functioning of a separator in Li‐S batteries, namely physisorption, chemisorption, and electrostatic repulsion, are discussed. Many recent papers proposed novel cell configurations with specifically designed functional separators. These reports are classified according to three design principles, analyzed critically, and compared with a view to assess their relative merits and efficacy. Some thoughts on the future directions in the development of an efficient separator are described.

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Facilitating the redox reaction of polysulfides by an electrocatalytic layer-modified separator for lithium–sulfur batteries

Abstract: KB@Ir-modified separator shows outstanding capability in enhancing the physical/chemical adsorption and facilitating the redox reaction of polysulfide intermediates as an electrocatalytic layer.

Cited by 84 publications

References 62 publications

A Freestanding Flexible Single‐Atom Cobalt‐Based Multifunctional Interlayer toward Reversible and Durable Lithium‐Sulfur Batteries

A Freestanding Flexible Single‐Atom Cobalt‐Based Multifunctional Interlayer toward Reversible and Durable Lithium‐Sulfur Batteries

Rational Design of Nanostructured Functional Interlayer/Separator for Advanced Li–S Batteries

Separator Membranes for Lithium–Sulfur Batteries: Design Principles, Structure, and Performance

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