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The present article introduces a strategy for controlling oxidation and reduction reactions within polymer electrolyte membrane (PEM) networks as a means of enhancing storage capacity through the complexation of dissociated lithium cations with multifunctional groups of the polymer network. Specifically, co-polymer networks based on polysulfide (PS) and polyoxide (PO) precursors, photo-cured in the presence of succinonitrile (SCN) and lithium bis(trifluoro methane sulfonyl imide) (LiTFSI) salt, exhibited ionic conductivity on the order of mid 10−4 S/cm at ambient temperature in the 30/35/35 (weight %) composition. Lithium titanate (LTO, Li4Ti5O12) electrode was chosen as an anode (i.e., a potential source of Li ions) against lithium iron phosphate (LFP, LiFePO4) cathode in conjunction with polysulfide-co-polyoxide dual polyelectrolyte networks to control viscosity for 3D printability on conformal surfaces of drone and aeronautic vehicles. It was found that the PS-co-PO dual network-based polymer electrolyte containing SCN plasticizer and LiTFSI salt exhibited extra storage capacity (i.e., specific capacity of 44 mAh/g) with the overall specific capacity of 170 mAh/g (i.e., for the combined LTO electrode and PEM) initially that stabilized at 153 mAh/g after 50th cycles with a reasonable capacity retention of over 90% and Coulombic efficiency of over 99%. Of particular interest is the observation of the improved electrochemical performance of the polysulfide-co-polyoxide electrolyte dual-network relative to that of the polyoxide electrolyte single-network. 

Vinyl-benzaldehyde (VB) monomers containing four functional groups were newly synthesized using the Williamson ether synthesis method. The two aldehyde groups of the synthesized monomers were able to react with amine-terminated macromonomers to form flexible networks. In addition, the two vinyl groups were found to be capable of inverse vulcanization with sulfur by conducting qualitative chemical analysis. The lithium−sulfur battery prepared using the VB-based cathode binder achieved high specific capacity with excellent capacity retention compared to conventional sulfur batteries, demonstrating the potential of the new binder. 

The year 1975 can be claimed to be the year of inception for the research and development of solid polymer electrolytes (SPEs) for Lithium-Ion Batteries (LIB), when the ionic conductivity of polyethylene oxide–alkaline metal ion complex was found by Peter Wright from the University of Sheffield. However, SPE research has undergone a leapfrog development, with conductivity values improving from 1 × 10–7 S·cm−1 to 1 × 10– 1 S·cm−1. The seed of development of SPEs spurs from the need for introducing design freedom to battery structures as well as the need for leak-proof electrolytes, greater operational safety, higher energy density, and other considerations. While the benefits of SPEs are evident, poor interfacial contact is a major factor limiting their application. This review presents the history of SPEs and shows how the additive manufacturing (AM) could prove beneficial for the improvement of performance and the functional implementation of SPEs. While the article articulates a technical review of additively manufactured SPEs, it also provides a lab-to-market perspective that could aid in shaping the future of green technology in energy storage. It also aims to provide an overall picture about the evolution and diversity of research advances in the development of greener SPEs through AM technology. 

The first study of the flexo-ionic effect, i.e., mechanical deformation-induced electric signal, of the recently discovered ionic liquid crystal elastomers (iLCEs) is reported. The measured flexo-ionic coefficients were found to strongly depend on the director alignment of the iLCE films and can be over 200 µC/m. This value is orders of magnitude higher than the flexo-electric coefficient found in insulating liquid crystals and is comparable to the well-developed ionic polymers (iEAPs). The shortest response times, i.e., the largest bandwidth of the flexo-ionic responses, is achieved in planar alignment, when the director is uniformly parallel to the substrates. These results render high potential for iLCE-based devices for applications in sensors and wearable micropower generators. 

Abstract The present article entails the emergence of diverse crystal polymorphs following thermal quenching into various coexistence regions of binary azobenzene chromophore (ACh)/diacrylate (DA) solution and of azobenzene/nematic liquid crystal (E7) mixture. Development of various crystal topologies encompassing rhomboidal and hexagonal shapes can be witnessed in a manner dependent on thermal quenched depths into the crystal + liquid coexistence region of ACh/DA system. Upon spraying with compressed carbon dioxide (CO₂) fluid, the local temperature gradient is generated resulting in spherulitic morphology showing discrete lamellae undergoing twisting locally in some regions and branched dendrites or seaweeds in another. When ACh/E7 blend is sprayed using compressed CO₂fluid, hierarchical organization of various discrete faceted single crystals including needle, rectangular, rhombus, and truncated hexagonal crystals radiating from the spherulite core can be discerned in a brighter region (off cross‐polarization) polarized optical microscopy (POM) and nematic disclination in a darker cross‐polarized region. Of particular interest is that the observed faceted single‐crystal polymorphs in ACh/E7 may be contrasted to the lamellar twisting and branching observed in the ACh/DA system and plausible mechanisms of polymer spherulitic growth are discussed. 

Abstract Preparation and low voltage induced bending (converse flexoelectricity) of crosslinked poly(ethylene glycol) diacrylate (PEGDA), modified with thiosiloxane (TS) and ionic liquid (1‐hexyl‐3‐methylimidazolium hexafluorophosphate) (IL) are reported. In between 2µm PEDOT:PSS electrodes at 1 V, it provides durable (95% retention under 5000 cycles) and relatively fast (2 s switching time) actuation with the second largest strain observed so far in ionic electro‐active polymers (iEAPs). In between 40 nm gold electrodes under 8 V DC voltage, the film can be completely curled up (270° bending angle) with 6% strain that, to the best of the knowledge, is unpreceded among iEAPs. These results render great potential for the TS/PEGDA/IL based electro‐active actuators for soft robotic applications. 

Abstract This paper describes the preparation, physical properties, and electric bending actuation of a new class of active materials—ionic liquid crystal elastomers (iLCEs). It is demonstrated that iLCEs can be actuated by low‐frequency AC or DC voltages of less than 1 V. The bending strains of the unoptimized first iLCEs are already comparable to the well‐developed ionic electroactive polymers. Additionally, iLCEs exhibit several novel and superior features, such as the alignment that increases the performance of actuation, the possibility of preprogrammed actuation patterns at the level of the cross‐linking process, and dual (thermal and electric) actuations in hybrid samples. Since liquid crystal elastomers are also sensitive to magnetic fields and can also be light sensitive, iLCEs have far‐reaching potentials toward multiresponsive actuations that may have so far unmatched properties in soft robotics, sensing, and biomedical applications.