Polymer electrolytes containing Li-ion conducting fillers are among the extensively investigated materials for the development of solid-state Li metal batteries. The practical realization of these electrolytes is, however, impeded by their low Li-ion conductivity, which is related to the filler and the interplay between the filler and the polymer. Therefore, we performed an in-depth analysis on the influence of the filler content (0, 10, and 20 wt%) and filler morphology (particles and nanowires) on the electrical and electrochemical properties of the PEO-based composite electrolyte using a wide spectrum of characterization techniques, such as 3D micro-X-ray computed tomography, cross-sectional scanning electron microscopy, X-ray diffraction, and differential scanning calorimetry, impedance spectroscopy, and galvanostatic cycling. The studies reveal that the filler materials are well distributed within the membranes, without any indications for the formation of agglomerates. For 10 wt% filler, a decrease in the crystallinity compared to PEO was observed, in contrast to 20 wt% filler showing an increase in crystallinity. Impedance spectroscopic studies on the Li-ion conductivity of the membranes have shown that the change in the Li-ion conductivity is solely related to the change in the crystallinity, rather than to the participation of LLZO as an active transport mediator. The PEO membranes containing 10 wt% LLZO have been tested in terms of their rate capability in symmetrical Li cells by galvanostatic cycling. A critical current density of up to 1 mA cm−2 at 60°C was observed.
Using water as monomer in polymerization reactions presents a unique and exquisite strategy towards more sustainable chemistry. Herein, the feasibility thereof is demonstrated by the introduction of the oxa-Michael polyaddition...
One way to obtain recyclable polymeric materials is to include reversible bonds in polymers. Herein, we study the reversibility of the oxa-Michael reaction, explore its scope and limitations in simple...
Poly(ether)s represent an important class of polymers and are typically formed by ring-opening polymerization, Williamson ether synthesis, or self-condensation of alcohols. The oxa-Michael reaction presents another method to form poly(ether)s with additional functional groups in the polymer backbone starting from di- or triols and electron deficient olefins such as acrylates, sulfones, or acrylamides. However, research on oxa-Michael polymerization is still limited. Herein, we outline the principles of the oxa-Michael polymerization and focus on the synthesis and preparation of poly(ether-sulfone)s, poly(ether-ester)s, poly(ether)s, and poly(ether-amide)s. Further, challenges as well as future perspectives of the oxa-Michael polymerization are discussed.
Graphical abstract
Using water as monomer in polymerization reactions presents a unique and exquisite strategy towards more sustainable chemistry. Herein, the feasibility thereof is demonstrated by the introduction of the oxa-Michael polyaddition of water and divinyl sulfone. Upon nucleophilic or base catalysis, the corresponding aliphatic polyethersulfone is obtained in an interfacial polymerization at room temperature in high yield (> 97%) within an hour. The polyethersulfone is characterized by relatively high molar mass averages and a dispersity around 2.5. The polymer was tested as a solid polymer electrolyte with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) as salt. Free standing amorphous membranes were prepared by a melt process in a solvent free manner. The polymer electrolyte containing 15 wt.% LiTFSI featured an oxidation stability of up to 5.5 V vs. Li/Li+ at 45 °C and a conductivity of 1.45 × 10-8 S/cm at room temperature.
Poly(ether)s represent an important class of polymers and are typically formed by ring-opening polymerization, Williamson ether synthesis or self-condensation of alcohols. The oxa-Michael reaction presents another method to form poly(ether)s with additional functional groups in the polymer backbone starting from di- or triols and electron deficient olefins such as acrylates, sulfones or acrylamides. However, research on oxa-Michael polymerization is still limited. Herein, we outline the principles of the oxa-Michael polymerization and focus on the synthesis and preparation of poly(ether-sulfone)s, poly(ether-ester)s, poly(ether)s and poly(ether-amide)s. Further, challenges as well as future perspectives of the oxa-Michael polymerization are discussed.
Herein we propose an auto-tandem catalytic approach towards the preparation of poly(ester-ether)s from simple alkyl acrylates and diols. By combining oxa-Michael addition with transesterification the preparation of hydroxy functionalised acrylate monomers can be avoided.<br>
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