2021
DOI: 10.1002/eom2.12115
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Liquid electrolyte design for metal‐sulfur batteries: Mechanistic understanding and perspective

Abstract: Metal‐sulfur batteries have received intensive research attention owing to their potential to achieve higher energy density and lower cost than conventional Li‐ion batteries. However, metal‐sulfur batteries suffer from a fundamental challenge, the shuttle effect, the crossover of soluble reaction intermediates polysulfide leading to low efficiency and poor cycle life. Electrolyte design becomes the center of the sulfur redox chemistry since it dictates the properties of the soluble polysulfide intermediates in… Show more

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Cited by 33 publications
(22 citation statements)
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“…In the Li-S system, Li 2 S is commonly believed to be the most stabilized discharge product in spite of some controversy on the existence of Li 2 S 2 as it was reported as a metastable phase that could spontaneously decompose into Li 2 S and sulfur. 56 By contrast, the thermodynamic stability of K 2 S 3 (ΔG f 0 = 528 kJ mol À1 ) is theoretically higher than K 2 S (ΔG f 0 = 410 kJ mol À1 ), indicating a sluggish reduction kinetic from K 2 S 3 to K 2 S. 57,58 This accounts for why K 2 S 3 was frequently observed as the only end discharge product of K-S batteries. 34,59,60 Similar results were also observed in Na-S batteries where Na 2 S 2 was detected as the only discharge product rather than Na 2 S. 61 By comparison, CaS and Al 2 S 3 were observed as the only discharge product in Ca-S and Mg-S batteries, respectively.…”
Section: àmentioning
confidence: 99%
“…In the Li-S system, Li 2 S is commonly believed to be the most stabilized discharge product in spite of some controversy on the existence of Li 2 S 2 as it was reported as a metastable phase that could spontaneously decompose into Li 2 S and sulfur. 56 By contrast, the thermodynamic stability of K 2 S 3 (ΔG f 0 = 528 kJ mol À1 ) is theoretically higher than K 2 S (ΔG f 0 = 410 kJ mol À1 ), indicating a sluggish reduction kinetic from K 2 S 3 to K 2 S. 57,58 This accounts for why K 2 S 3 was frequently observed as the only end discharge product of K-S batteries. 34,59,60 Similar results were also observed in Na-S batteries where Na 2 S 2 was detected as the only discharge product rather than Na 2 S. 61 By comparison, CaS and Al 2 S 3 were observed as the only discharge product in Ca-S and Mg-S batteries, respectively.…”
Section: àmentioning
confidence: 99%
“…[3][4][5][6][7] Unfortunately, some formidable challenges need to be tackled on the way to the Li-S throne, including the two arch-villains of the shuttle behavior of soluble lithium polysulfide (LiPS) intermediates as well as the uncontrolled deposition/stripping behavior of lithium anode. [8][9][10][11][12] Furthermore, there remain other critical issues, such as the inferior utilization of sulfur materials originated from the poor ionic/electronic insulation, the huge volume variation during the repeated charge/ discharge procedure, and the intrinsic flammability of ether-based electrolytes. [13][14][15] Currently, substantial efforts to conquer the aforementioned challenges have been made, which is still unable to deliver the practical potential.…”
Section: Introductionmentioning
confidence: 99%
“…Owing to the high theoretical gravimetric energy density (2600 Wh kg −1 ) and natural abundance, lithium–sulfur (Li–S) battery is always thought to be one of the most promising alternatives for practical lithium‐ion battery (LIB) to satisfy the increasing demand of energy market 3–7 . Unfortunately, some formidable challenges need to be tackled on the way to the Li–S throne, including the two arch‐villains of the shuttle behavior of soluble lithium polysulfide (LiPS) intermediates as well as the uncontrolled deposition/stripping behavior of lithium anode 8–12 . Furthermore, there remain other critical issues, such as the inferior utilization of sulfur materials originated from the poor ionic/electronic insulation, the huge volume variation during the repeated charge/discharge procedure, and the intrinsic flammability of ether‐based electrolytes 13–15 …”
Section: Introductionmentioning
confidence: 99%
“…[9] Similarly, compared to cyclic esters, ethers are more stable towards sulfur and are not susceptible towards nucleophilic attack from polysulfides, hence are also favorable for lithium-sulfur and sodium-sulfur battery chemistries. [10,11] More recently, glymes have received renewed research interest owing to their ability to coordinate to active alkali metal ions, thus enabling a reversible solvent co-intercalation behavior with Na + in graphite [12][13][14][15][16] forming ternary graphite intercalation compounds (t-GIC). This behavior is interesting, as graphite is largely inactive for Na storage in cells with conventional carbonate-based electrolytes as binary Na-GICs are energetically unfavorable.…”
Section: Introductionmentioning
confidence: 99%
“…The wide liquid range, low volatility, and relative stability towards reduced O 2 species of certain ethers like diethylene glycol dimethyl ether (2G), tetra ethylene glycol dimethyl ether (4G) make them well suited for application in Li−O 2 and Na−O 2 batteries [9] . Similarly, compared to cyclic esters, ethers are more stable towards sulfur and are not susceptible towards nucleophilic attack from polysulfides, hence are also favorable for lithium‐sulfur and sodium‐sulfur battery chemistries [10,11] . More recently, glymes have received renewed research interest owing to their ability to coordinate to active alkali metal ions, thus enabling a reversible solvent co‐intercalation behavior with Na + in graphite [12–16] forming ternary graphite intercalation compounds ( t ‐GIC).…”
Section: Introductionmentioning
confidence: 99%