Highly stable garnet solid electrolyte based Li-S battery with modified anodic and cathodic interfaces

Lu, Yang; Huang, Xiao; Song, Zhen; Rui, Kun; Wang, Qingsong; Gu, Shuang‐Xi; Yang, Jianhua; Xiu, Tongping; Badding, Michael E.; Zhang, Wen

doi:10.1016/j.ensm.2018.05.018

Cited by 135 publications

(92 citation statements)

References 40 publications

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“…Nevertheless, "allsolid-state" Li-S batteries are in the initial stage of research with difficulties regarding low ion conductivity, poor interfacial contacts, and inferior cycling stability. [42] Growing attentions and more efforts are being devoted in this field.…”

Section: Principles and Challenges Of Lean-electrolyte Li-s Batteriesmentioning

confidence: 99%

Lithium–Sulfur Batteries under Lean Electrolyte Conditions: Challenges and Opportunities

et al. 2020

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The development of energy‐storage devices has received increasing attention as a transformative technology to realize a low‐carbon economy and sustainable energy supply. Lithium–sulfur (Li–S) batteries are considered to be one of the most promising next‐generation energy‐storage devices due to their ultrahigh energy density. Despite the extraordinary progress in the last few years, the actual energy density of Li–S batteries is still far from satisfactory to meet the demand for practical applications. Considering the sulfur electrochemistry is highly dependent on solid‐liquid‐solid multi‐phase conversion, the electrolyte amount plays a primary role in the practical performances of Li–S cells. Therefore, a lean electrolyte volume with low electrolyte/sulfur ratio is essential for practical Li–S batteries, yet under these conditions it is highly challenging to achieve acceptable electrochemical performances regarding sulfur kinetics, discharge capacity, Coulombic efficiency, and cycling stability especially for high‐sulfur‐loading cathodes. In this Review, the impact of the electrolyte/sulfur ratio on the actual energy density and the economic cost of Li–S batteries is addressed. Challenges and recent progress are presented in terms of the sulfur electrochemical processes: the dissolution–precipitation conversion and the solid–solid multi‐phasic transition. Finally, prospects of future lean‐electrolyte Li–S battery design and engineering are discussed.

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Section: Principles and Challenges Of Lean-electrolyte Li-s Batteriesmentioning

confidence: 99%

Lithium–Sulfur Batteries under Lean Electrolyte Conditions: Challenges and Opportunities

et al. 2020

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“…However, the lithium/garnet interface appeared to have a remarkably large impedance due to the poor interfacial contact . This motivates a variety of studies to turn garnet from lithiophobic to lithiophilic by coating garnet with metal, metal oxides, semi‐conductors, polymer interlayers, and graphite . Although these approaches have shown great progress, they mainly addressed the interface issue from garnet side.…”

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confidence: 99%

Lithium–Graphite Paste: An Interface Compatible Anode for Solid‐State Batteries

et al. 2019

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cathodes, [10][11][12] silicon-based anodes, [13][14][15][16] and optimizing organic liquid electrolytes. [17,18] However, the safety challenges related to the electrolyte are serious because operation of LIBs is exothermic and organic liquid electrolytes mostly with ester carbonates are highly flammable, generating massive heat. [19,20] Dendritic lithium in LIB represents a further challenge considering internal short circuit would occur if the dendrite punctures the separator. [21,22] Therefore, solutions for safety of LIBs are urgently required.Inorganic ceramic solid-state electrolyte (SSE) provides an ideal alternative to liquid flammable electrolytes for the design of safe ASSBs, since ceramic SSE is nonflammable and it has adequate fracture toughness to prevent internal short circuit from lithium dendrite. [23][24][25] Furthermore, lithium metal anode, the ultimate anode with the highest specific capacity and lowest electrochemical potential has been demonstrated in ASSBs, which exhibited intrinsic safety under rigorous conditions. [26][27][28][29][30] In the search for SSEs, while most of the superionic conductors with conductivity >1 mS cm −1 are based on sulfides, such as Li 10 GeP 2 S 12 , [31,32] Li 9.54 Si 1.74 P 1.44 S 11.7 Cl 0.3 , [33] and Li 9.6 P 3 S 12 , [34] it has shown that garnet-type oxides are the most stable SSEs with lithium metal anode. [35][36][37][38][39] However, the lithium/garnet interface appeared to have a remarkably large impedance due to the poor interfacial contact. [40] This motivates a variety of studies to turn garnet from lithiophobic to lithiophilic by coating garnet with metal, [41][42][43][44] metal oxides, [45,46] semi-conductors, [47,48] polymer interlayers, [49,50] and graphite. [51] Although these approaches have shown great progress, they mainly addressed the interface issue from garnet side. As a result, ample opportunities remain on lithium metal side.Here we introduce a new strategy to synthesize a ceramic compatible lithium anode by using graphite additives. Our scheme to implement a lithium/garnet interface experiment is sketched in Figure 1. We find that pure lithium is not compatible with garnet, which is consistent with that expected for lithiophobic garnet surface and previous reports (Figure 1a). [52] On the other side, lithium-graphite (Li-C) composite presents lower fluidity and higher viscosity compared to pure Li. So the Li-C composite, like a paste, can be casted onto garnet and exhibits an intimate contact (Figure 1b). As expected, All-solid-state batteries (ASSBs) with ceramic-based solid-state electrolytes (SSEs) enable high safety that is inaccessible with conventional lithium-ion batteries. Lithium metal, the ultimate anode with the highest specific capacity, also becomes available with nonflammable SSEs in ASSBs, which offers promising energy density. The rapid development of ASSBs, however, is significantly hampered by the large interfacial resistance as a matched lithium/ ceramic interface that is not easy to pursue. Here, a lithium-graphite...

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“…[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. Additionally, the common shuttle effect of intermediate polysulfide also leads to an obvious capacity loss during charging and discharging.…”

mentioning

confidence: 99%

“…[10][11][12][13][14][15] Thus, new strategies are urgent in addressing the problems of high-capacity sulfur cathodes for Li-S batteries. Additionally, the common shuttle effect of intermediate polysulfide also leads to an obvious capacity loss during charging and discharging.…”

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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Highly stable garnet solid electrolyte based Li-S battery with modified anodic and cathodic interfaces

Cited by 135 publications

References 40 publications

Lithium–Sulfur Batteries under Lean Electrolyte Conditions: Challenges and Opportunities

Lithium–Sulfur Batteries under Lean Electrolyte Conditions: Challenges and Opportunities

Lithium–Graphite Paste: An Interface Compatible Anode for Solid‐State Batteries

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

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