Ernest Ahiavi, Jihen Talbi, Trang N. T. Phan, Priscillia Soudant, Fabrice Cousin, Renaud Bouchet, Didier Devaux
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引用次数: 0
Abstract
Despite the high impact lithium–sulfur (Li–S) batteries can bring in terms of specific energy and battery lifetime, their full advantage has not yet been realized due to inherent issues associated with this technology. The intermediate polysulfide products produced in the positive electrode during discharge dissolve and diffuse in the electrolyte, leading to capacity fading and low Coulombic efficiency. A promising solution to this issue is the use of a solid polymer electrolyte that combines the advantages of an ion-conducting poly(ethylene oxide) (PEO) phase and a mechanically reinforced phase, such as polystyrene (PS), that can suppress the nonuniform electrodeposition of Li onto Li metal. In this work, the possibility of using PS–PEO–PS triblock copolymer as an electrolyte or binder in a Li–S battery was investigated by characterizing the thermodynamical, morphological, and ionic transport properties of lithium polysulfides species (Li2Sx, with x = 4 and 8). Thermodynamic results showed that the long-chain lithium polysulfide (Li2S8) is more soluble in the copolymers compared to the short-chain polysulfide (Li2S4). Meanwhile, the addition of Li2S4 and Li2S8 in the mesostructured block copolymer influences both the phase transition (lamellar or hexagonal) and the domain spacing in a fashion similar to the conventional LiTFSI salt. In terms of ionic transport, the mobility of the polysulfides (S42– and S82–) in the copolymers is reduced compared to the TFSI– anion, and the cationic transference number remains in the range of 0.5 compared to 0.15 for LiTFSI. To move toward the application, the introduction of Li2S4 into the block copolymer electrolyte is also used as an additive in the presence of LiTFSI salt, resulting in a very low interfacial resistance with the Li metal electrode. The results of these investigations would guide the design of solid polymer electrolytes for application in Li–S batteries.
期刊介绍:
The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.