Heterogeneous/Homogeneous Mediators for High‐Energy‐Density Lithium–Sulfur Batteries: Progress and Prospects

Zhang, Zewen; Peng, Hong‐Jie; Zhao, Meng; Huang, Jia‐Qi

doi:10.1002/adfm.201707536

Cited by 292 publications

(187 citation statements)

References 205 publications

(143 reference statements)

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“…Li–S batteries have to overcome a pronounced initial energy barrier for the charge process due to limited conductive surface availability and low LiPS concentration that acts as a self‐mediator to promote Li 2 S 1/2 dissolution . Driven conversion from solid Li 2 S 1/2 to liquid LiPSs can also be boosted by Co‐N‐C electrocatalysts, evidenced by occurrence of current hump in the potentiostatic charge process at 2.30 V (Figure D).…”

Section: Introductionmentioning

confidence: 61%

“…Li-S batteries have to overcome a pronounced initial energy barrier for the charge process due to limited conductive surface availability and low LiPS concentration that acts as a self-mediator to promote Li 2 S 1/2 dissolution. 36,[65][66][67] Driven conversion from solid Li 2 S 1/2 to liquid LiPSs can also be boosted by Co-N-C electrocatalysts, evidenced by occurrence of current hump in the potentiostatic charge process at 2.30 V ( Figure 2D). The capability of Li 2 S 1/2 conversion enabled by atomic Co-N-C electrocatalysts is quantified by integral of current density against time at 2.30 V, exhibiting that the calculated capacity of the Co-N-C based cell is almost three times higher that of the C based cell (161 mAh g −1 for Co-N-C vs 58 mAh g −1 for C ( Figure 2E).…”

Section: Introductionmentioning

confidence: 99%

“…[71][72][73][74] The energy chemistry of Li-S batteries involves multielectron and multistep electrochemical reactions, which are complicated by the shuttle of liquid LiPSs and insulating nature of S/Li 2 S 1/2 . 66,[75][76][77] Powering the rapid LiPS conversion is critically important to realize high-capacity, fast-charge, and long-term Li-S batteries. Based on these considerations, various electrocatalysts are applied in a working Li-S battery.…”

Section: Introductionmentioning

confidence: 99%

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Expediting redox kinetics of sulfur species by atomic‐scale electrocatalysts in lithium–sulfur batteries

Kong

Chang-xin

et al. 2019

InfoMat

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285

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Lithium–sulfur (Li–S) batteries have extremely high theoretical energy density that make them as promising systems toward vast practical applications. Expediting redox kinetics of sulfur species is a decisive task to break the kinetic limitation of insulating lithium sulfide/disulfide precipitation/dissolution. Herein, we proposed a porphyrin‐derived atomic electrocatalyst to exert atomic‐efficient electrocatalytic effects on polysulfide intermediates. Quantifying electrocatalytic efficiency of liquid/solid conversion through a potentiostatic intermittent titration technique measurement presents a kinetic understanding of specific phase evolutions imparted by the atomic electrocatalyst. Benefiting from atomically dispersed “lithiophilic” and “sulfiphilic” sites on conductive substrates, the finely designed atomic electrocatalyst endows Li–S cells with remarkable cycling stablity (cyclic decay rate of 0.10% in 300 cycles), excellent rate capability (1035 mAh g−1 at 2 C), and impressive areal capacity (10.9 mAh cm−2 at a sulfur loading of 11.3 mg cm−2). The present work expands atomic electrocatalysts to the Li–S chemistry, deepens kinetic understanding of sulfur species evolution, and encourages application of emerging electrocatalysis in other multielectron/multiphase reaction energy systems.

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Section: Introductionmentioning

confidence: 61%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Expediting redox kinetics of sulfur species by atomic‐scale electrocatalysts in lithium–sulfur batteries

Kong

Chang-xin

et al. 2019

InfoMat

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“…In general, both physical confinement and chemical adsorption have been used to resolve the shuttle effect by capturing LiPSs within the cathode region . Recently, a unique conception of electrocatalysis has been introduced, in which some metals (Pt, Ni, Co) and metal sulfides or oxides (CoS 2 , WS 2 , MoS 2 , Nb 2 O 5 ) can expedite kinetic conversion and thus assist the shuttling of LiPSs . In general, during the discharge/charge process, the soluble long‐chain LiPSs can move between the cathode and anode; therefore, a fast conversion of sulfur species may be conducive to preventing the dissolution of polysulfides and restraining the polysulfide shuttle effect, to some extent .…”

Section: Introductionmentioning

confidence: 99%

Rational Fabrication of Nitrogen and Sulfur Codoped Carbon Nanotubes/MoS₂ for High‐Performance Lithium–Sulfur Batteries

Xiang

Wen

et al. 2019

ChemSusChem

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“…[33,34] The N 1s spectrum exhibits three obviously peaks at a binding energy of 398.8 eV (Pyridinic-N), 401.3 eV (Pyrrolic-N), and 401.3 eV (Graphitic-N), respectively ( Figure S4b, Supporting Information). [35][36][37] Adv. According to previous literature reports, CoNC structure plays an effective role in the catalytic conversion of polysulfides.…”

mentioning

confidence: 99%

Polysulfide Confinement and Highly Efficient Conversion on Hierarchical Mesoporous Carbon Nanosheets for Li–S Batteries

Chen

et al. 2019

Advanced Energy Materials

109

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performance of Li-S batteries is still restricted by poor conductivity of sulfur itself and discharge products (Li 2 S/Li 2 S 2 ), which makes hard conversion of sulfur. Additionally, the common shuttle effect of intermediate polysulfide also leads to an obvious capacity loss during charging and discharging. [10][11][12][13][14][15] Thus, new strategies are urgent in addressing the problems of high-capacity sulfur cathodes for Li-S batteries.To design high-performance cathode, dispersing nanostructured sulfur particles on carbon materials have attracted particular interests, which not only stabilize sulfur and intermediates but also promotes electron transfer during charging/ discharging. [16][17][18][19][20][21] Although carbon materials have been the first choice to disperse sulfur particles, the nonpolar carbon suffers a weak binding force to the intermediate product, which results in serious shuttle effect and making it difficult to reuse the polysulfide (Scheme 1a). To address these issues, plenty of work has begun to focus on the modification of nonpolar carbon by introducing heteroatoms (B, N, O, or S). [22][23][24][25] This is because the lone pair of electrons on the heteroatoms forms an electrostatic attraction (Li bond) with the polysulfide, which can effectively prevent shuttle of polysulfides. [26,27] However, the high loading and the easy aggregation of sulfur are hard to be balanced, since sulfur are getting easier to migrate and aggregate at surface of carbon supports, which lead to the low concentration loading or limited sulfur utilization. Therefore, sulfur confinement and simultaneous highly efficient conversion remains a challenge for the next-generation Li-S batteries.Herein, we develop honeycomb-like mesoporous carbon nanosheets (MC-NS) with abundant defects and Co-N-C catalytic site as efficient host for simultaneously confinement and efficient conversion of polysulfides, which shows significantly enhanced performance for Li-S batteries cathode (Scheme 1b). The as-prepared MC-NS exhibits an excellent 2D conductive network with a high specific surface area of 335.4 m 2 g −1 and abundant mesopores that provide high storage space and expansion space for sulfur. Moreover, the density functional theory (DFT) calculation and experiments manifest that the presence of abundant defects on the carbon skeleton MC-Ns Lithium-sulfur (Li-S) batteries have attracted increasing attention due to their extremely high theoretical specific capacity and a promising power density. However, practical applications of Li-S batteries are still limited by the relatively low performance, owing to poor conductivity of sulfur itself and discharge products (Li 2 S/Li 2 S 2 ) as well as the shuttle effect of the intermediate polysulfide. Herein, honeycomb-like mesoporous Co, N-doped carbon nanosheets (MC-NS) with a high specific surface area and abundant defects are developed which, simultaneously enable polysulfide confinement and highly efficient conversion. Moreover, density functional theory calculations and experime...

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Heterogeneous/Homogeneous Mediators for High‐Energy‐Density Lithium–Sulfur Batteries: Progress and Prospects

Cited by 292 publications

References 205 publications

Expediting redox kinetics of sulfur species by atomic‐scale electrocatalysts in lithium–sulfur batteries

Expediting redox kinetics of sulfur species by atomic‐scale electrocatalysts in lithium–sulfur batteries

Rational Fabrication of Nitrogen and Sulfur Codoped Carbon Nanotubes/MoS₂ for High‐Performance Lithium–Sulfur Batteries

Polysulfide Confinement and Highly Efficient Conversion on Hierarchical Mesoporous Carbon Nanosheets for Li–S Batteries

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Heterogeneous/Homogeneous Mediators for High‐Energy‐Density Lithium–Sulfur Batteries: Progress and Prospects

Cited by 292 publications

References 205 publications

Expediting redox kinetics of sulfur species by atomic‐scale electrocatalysts in lithium–sulfur batteries

Expediting redox kinetics of sulfur species by atomic‐scale electrocatalysts in lithium–sulfur batteries

Rational Fabrication of Nitrogen and Sulfur Codoped Carbon Nanotubes/MoS2 for High‐Performance Lithium–Sulfur Batteries

Polysulfide Confinement and Highly Efficient Conversion on Hierarchical Mesoporous Carbon Nanosheets for Li–S Batteries

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Rational Fabrication of Nitrogen and Sulfur Codoped Carbon Nanotubes/MoS₂ for High‐Performance Lithium–Sulfur Batteries