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density functional theory (DFT) and ab initio molecular dynamics has sought to understand processes by which the cathode and SSE interface with S8 or Li2S (Figure 4) [87]. The authors specifically explored β-Li3PS4, Li6PS5Cl, and Li7P2S8I, as these materials have demonstrated superionic conductivity of Li+. The simulations provide some insight into adhesion and interfacial energy for these materials, allowing for some speculation on the mechanisms of interfacial reactions. These simulations should be followed up with experiments and imaging techniques in an effort to validate Electrochem 2020, 1 234 them and, if the simulations prove predictive, further simulations will guide additional work in the field. Figure 4. Interfacial interactions between solid-state electrolytes (SSEs) and either S8 or Li2S provide Figure 4. Interfacial interactions between solid-state electrolytes (SSEs) and either S8 or Li2S provide insight into electron transport in their composite Li-S batteries. Reprinted with permission from insight into electron transport in their composite Li-S batteries. Reprinted with permission from reference [87]. Copyright 2020 American Chemical Society. reference [87]. Copyright 2020 American Chemical Society. A potential issue holding back the development of solid state electrolytes is that they generally have poor kinetics compared to solution systems. An interesting approach to improving the kinetics A potential issue holding back the development of solid state electrolytes is that they generally is to add a eutectic accelerator. In one case, tellurium was employed in this role [43]. The solid have poor kinetics compared to solution systems. An interesting approach to improving the kinetics is electrolyte interface was set up on a mesoporous carbon (CMK-3)/sulfur cathode. Tellurium doping to add a eutectic accelerator. In one case, tellurium was employed in this role [43]. The solid electrolyte (1 wt%) was observed to improve diffusion kinetics and produces a solid electrolyte interface with interface whaigshsleithuiupmoinonacmonedsuocptivoirtyouansdcalorwboimnp(CedManKce-.3A)/fsteurlf2u00r cyactlheso,dthee. cTelllhuardiuamhigdhorpeivnegrsi(b1lewt %) was specific capacities of 1150 mA h g−1 and 727 mA h g−1 at 0.1 C and 0.2 C, respectively. This study observed to improve diffusion kinetics and produces a solid electrolyte interface with high lithium ion illustrates an effective strategy for improving kinetics in solid state electrolyte cells that have conductivity and low impedance. After 200 cycles, the cell had a high reversible specific capacities inherently low shuttle effects. of 1150 mAh g−1 and 727 mAh g−1 at 0.1 C and 0.2 C, respectively. This study illustrates an effective 3.2. Polymer and Gel Electrolytes and Electrolyte Carriers strategy for improving kinetics in solid state electrolyte cells that have inherently low shuttle effects. One source of shuttle problems is the solubility of polysulfides and related species in the organic 3.2. Polymer and Gel Electrolytes and Electrolyte Carriers electrolytes of traditional Li-S batteries. One potential solution to this issue is to use a polymerized or polymer gel electrolyte [12]. For example, a Li-S battery comprising a sulfur cathode and a gel One source of shuttle problems is the solubility of polysulfides and related species in the organic polymer electrolyte of poly(ethyleneoxide)-modified poly(vinylidene fluoride-co- electrolytehsexoafflturoardopitriopnyalelnLe)i-(SPEbOa-tPteVrDieF)s.wOasnefapbroictaetnedtiainl swohluicthioanltaoyetrhoisf ipsesnutaeerisytthorituolseteatrapkoislymerized (divinyladipate) was further added to suppress polysulfide permeability (Figure 5) [88]. These or polymer gel electrolyte [12]. For example, a Li-S battery comprising a sulfur cathode and a gel polymers were selected because they are known to exhibit high thermal stability and low thermal polymer electrolyte of poly(ethyleneoxide)-modified poly(vinylidene fluoride-co-hexafluoropropylene) expansion, as well as their permeability and ion conductivity potential. The battery so composed (PEO-PVDF) was fabricated in which a layer of pentaerythritol tetrakis (divinyladipate) was further featured a porous membrane that could take up 280% by mass of electrolyte, resulting in an ionic addedtosucopnpdurectsisviptyoolyfs9u.6lfi×d10e−4pSercm−e1abndiliatylit(hFiuigmurcaeti5o)n[L8i8+]t.raTnhsfesrenpceolnyumbeerrsowfe0.r7e1saetl2e5ct°eCd.Tbhecausethey coulombic efficiency remains near quantitative over 300 cycles with retention over 85% capacity even are known to exhibit high thermal stability and low thermal expansion, as well as their permeability after 300 cycles at 2 C. Electrochem 2020, 2, FOR PEER REVIEW 10 and ion conductivity potential. The battery so composed featured a porous membrane that could take up 280% by mass of electrolyte, resulting in an ionic conductivity of 9.6 × 10−4 S cm−1 and a lithium cation Li+ transference number of 0.71 at 25 ◦C. The coulombic efficiency remains near quantitative over 300 cycles with retention over 85% capacity even after 300 cycles at 2 C. Figure 5. A highly crosslinked network provides a scaffold that resists dimensional changes in Figure 5. A highly crosslinked network provides a scaffold that resists dimensional changes in response to temperature. Reprinted with permission from reference [88]. Copyright 2020 American response to temperature. Reprinted with permission from reference [88]. Copyright 2020 American Chemical Society. Chemical Society. Organic polymers can also be incorporated into batteries in the form of crosslinked micelles that can also carry electrolyte. In one such illustration [44], a copolymer of polyethylene oxide and polypropylene oxide comprising carboxylate and sulfonate groups was used to form the micelles (Figure 6) wherein lithium polysulfides (LiPS) are envisioned to interact along the polar polymer chains. These highly polar and ionic polymer segments, as expected, have a very high affinity for LiPS. Cells having this polymer micelle binder exhibited a reversible capacity of 571 mAh g−1 and, over 100 cycles at 0.5 C, showed a capacity loss of only 0.032%/cycle. These new polymer micelle- containing cells outperform older technologies such as Li-S batteries comprising fluoropolymerPDF Image | Lithium-Sulfur Batteries: Advances and Trends
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