Healable Ionoelastomer Designed from Polymeric Ionic Liquid and Vitrimer Chemistry
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PROVIDER: S-EPMC9844214 | biostudies-literature | 2022 Dec
REPOSITORIES: biostudies-literature
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Project description:Ionogels are solid polymer gel networks loaded with ionic liquid (IL) percolating throughout each other, giving rise to ionically conducting solid electrolytes. They combine the mechanical properties of polymer networks with the ionic conductivity, non-volatility, and non-flammability of ILs. In the frame of their applications in electrochemical-based flexible electronics, ionogels are usually subjected to repeated deformation, making them susceptible to damage. It appears critical to devise a simple and effective strategy to improve their durability and lifespan by imparting them with healing ability through vitrimer chemistry. In this work, we report the original in situ synthesis of polythioether (PTE)-based vitrimer ionogels using fast photopolymerization through thiol-acrylate Michael addition. PTE-based vitrimer was prepared with a constant amount of the trithiol crosslinker and varied proportions of static dithiol spacers and dynamic chain extender BDB containing dynamic exchangeable boronic ester groups. The dynamic ionogels were prepared using 50 wt% of either 1-Ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl) imide or 1-Ethyl-3-methylimidazolium trifluoromethanesulfonate, both of which were selected for their high ionic conductivity. They are completely amorphous (Tg below -30 °C), suggesting they can be used at low temperatures. They are stretchable with an elongation at break around 60%, soft with Young's modulus between 0.4 and 0.6 MPa, and they have high ionic conductivities for solid state electrolytes in the order of 10-4 S·cm-1 at room temperature. They display dynamic properties typical of the vitrimer network, such as stress relaxation and healing, retained despite the large quantity of IL. The design concept illustrated in this work further enlarges the library of vitrimer ionogels and could potentially open a new path for the development of more sustainable, flexible electrochemical-based electronics with extended service life through repair or reprocessing.
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Project description:The alignment is a key factor to fully exploit the potential of graphene in reinforcement of polymer composites. However, it is still a challenge to orientate graphene in thermosets because of the insoluble and infusible features of the later. In this paper, we report a facile and scalable hot press method to fabricate aligned graphene nanoplate (GnP)/epoxy composites by utilizing the dynamic character of epoxy vitrimer. The bond exchange and topological rearrangement associated viscous flow of epoxy vitrimer during hot press allows the spontaneous orientation of GnP in matrix because the 2D structure and volume exclusion effect. SEM images demonstrate the orientation of GnP, while tensile test reveals the significantly increased reinforcement effect of GnP on matrix after hot press. Moreover, the dynamic reaction of epoxy vitrimer confers good healability and recyclability to the aligned composites as confirmed by the nearly fully recovered mechanical properties of the healed sample after cutting, and the recycled sample after grinding. This work is expected to provide new opportunity for fabrication of aligned thermosetting composites.
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Project description:Developing degradable and self-healable elastomers composed of reusable resources is of great value but is rarely reported because of the undegradable molecular chains. Herein, we report a class of degradable and self-healable vitrimers based on non-isocyanate polyurethane elastomer. Such vitrimers are fabricated by copolymerizing bis(6-membered cyclic carbonate) and amino-terminated liquid nitrile rubber. The networks topologies can rearrange by transcarbonation exchange reactions between hydroxyl and carbonate groups at elevated temperatures; as such, vitrimers after reprocessing can recover 82.9-95.6% of initial tensile strength and 59-131% of initial storage modulus. Interestingly, the networks can be hydrolyzed and decarbonated in the strong acid solution to recover 75% of the pure di(trimethylolpropane) monomer. Additionally, the elastomer exhibits excellent self-healing efficiency (~88%) and fracture strain (~1,200%) by tuning the monomer feeding ratio. Therefore, this work provides a novel strategy to fabricate the sustainable elastomers with minimum environmental impact.
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Project description:Vitrimer-based liquid-crystalline elastomers (LCEs) exhibit great advantages over the traditional LCEs due to their inherent processability to realize monodomain alignment and construction of LCE actuators with complex 3D structures in a robust way. Though exciting progress has been made, how to achieve a proper balance between processability and actuation durability/stability remains a big challenge. Here, we report a strategy to mitigate the conflict between processability and actuation stability by reducing the catalyst content in an epoxy/acid LCE vitrimer system. With a relatively low catalyst content (0.25 mol% to carboxyl group), monodomain LCEs with large actuation strain (∼95%) and excellent actuation stability (the actuation strain is completely maintained after 100 heating-cooling cycles and more than 90% of the initial strain is retained even after 500 cycles) could be easily prepared. Moreover, the monodomain LCEs can still be readily realigned or directly reconfigured into complex reversible 3D actuators.
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Project description:In this contribution, we report the facile preparation of cross-linked polymerizable ionic liquid (PIL)-based nanoparticles via thiol-ene photopolymerization in a miniemulsion. The synthesized PIL nanoparticles with a diameter of about 200 nm were fully characterized with regard to their chemical structures, morphologies, and properties using different techniques, such as Fourier transform infrared spectroscopy, thermogravimetric analysis, scanning electron microscopy, and transmission electron microscopy. To gain an in-depth understanding of the physical and morphological structures of the PIL nanoparticles in an emulsion, small-angle neutron scattering and ultra-small-angle neutron scattering were used. Neutron scattering studies revealed valuable information regarding the formation of cylindrical ionic micelles in the spherical nanoparticles, which is a unique property of this system. Furthermore, the PIL nanoparticle emulsion was utilized as an inhibitor in a self-assembled nanophase particle (SNAP) coating. The corrosion protection ability of the resultant coating was examined using potentiodynamic polarization and electrochemical impedance spectroscopy. The results show that the PIL nanoparticle emulsion in the SNAP coating acts as an inhibitor of corrosion and is promising for fabricating advanced coatings with improved barrier function and corrosion protection.
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Project description:Simultaneous capture of carbon dioxide (CO2) and its utilization with subsequent work-up would significantly enhance the competitiveness of CO2-based sustainable chemistry over petroleum-based chemistry. Here we report an interfacial catalytic reaction platform for an integrated autonomous process of simultaneously capturing/fixing CO2 in gas-liquid laminar flow with subsequently providing a work-up step. The continuous-flow microreactor has built-in silicon nanowires (SiNWs) with immobilized ionic liquid catalysts on tips of cone-shaped nanowire bundles. Because of the superamphiphobic SiNWs, a stable gas-liquid interface maintains between liquid flow of organoamines in upper part and gas flow of CO2 in bottom part of channel. The intimate and direct contact of the binary reagents leads to enhanced mass transfer and facilitating reactions. The autonomous integrated platform produces and isolates 2-oxazolidinones and quinazolines-2,4(1H,3H)-diones with 81-97% yields under mild conditions. The platform would enable direct CO2 utilization to produce high-valued specialty chemicals from flue gases without pre-separation and work-up steps.
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Project description:In this study, varying concentrations of linear pNIPAAM have been incorporated for the first time into a thermo-responsive polymeric ionic liquid (PIL) hydrogel, namely tributyl-hexyl phosphonium 3-sulfopropylacrylate (P-SPA), to produce semi-interpenetrating polymer networks. The thermal properties of the resulting hydrogels have been investigated along with their thermo-induced shrinking and reswelling capabilities. The semi-interpenetrating networks (IPN) hydrogels were found to have improved shrinking and reswelling properties compared with their PIL counterpart. At elevated temperatures (50-80 °C), it was found that the semi-IPN with the highest concentration of hydrophobic pNIPAAM exhibited the highest shrinking percentage of ~40% compared to the conventional P-SPA, (27%). This trend was also found to occur for the reswelling measurements, with semi-IPN hydrogels producing the highest reswelling percentage of ~67%, with respect to its contracted state. This was attributed to an increase in water affinity due to the presence of hydrophilic pNIPAAM. Moreover, the presence of linear pNIPAAM in the polymer matrix leads to improved shrinking and reswelling response compared to the equivalent PIL.
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Project description:In this study, we develop a stretchable/self-healable polymer, PEDOT:PAAMPSA:PA, with remarkably high ionic thermoelectric (iTE) properties: an ionic figure-of-merit of 12.3 at 70% relative humidity (RH). The iTE properties of PEDOT:PAAMPSA:PA are optimized by controlling the ion carrier concentration, ion diffusion coefficient, and Eastman entropy, and high stretchability and self-healing ability are achieved based on the dynamic interactions between the components. Moreover, the iTE properties are retained under repeated mechanical stress (30 cycles of self-healing and 50 cycles of stretching). An ionic thermoelectric capacitor (ITEC) device using PEDOT:PAAMPSA:PA achieves a maximum power output and energy density of 4.59 μW‧m-2 and 1.95 mJ‧m-2, respectively, at a load resistance of 10 KΩ, and a 9-pair ITEC module produces a voltage output of 0.37 V‧K-1 with a maximum power output of 0.21 μW‧m-2 and energy density of 0.35 mJ‧m-2 at 80% RH, demonstrating the potential for a self-powering source.
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Project description:The self-healing properties and ionic sensing capabilities of the human skin offer inspiring groundwork for the designs of stretchable iontronic skins. However, from electronic to ionic mechanosensitive skins, simultaneously achieving autonomously superior self-healing properties, superior elasticity, and effective control of ion dynamics in a homogeneous system is rarely feasible. Here, we report a Cl-functionalized iontronic pressure sensitive material (CLiPS), designed via the introduction of Cl-functionalized groups into a polyurethane matrix, which realizes an ultrafast, autonomous self-healing speed (4.3 µm/min), high self-healing efficiency (91% within 60 min), and mechanosensitive piezo-ionic dynamics. This strategy promotes both an excellent elastic recovery (100%) and effective control of ion dynamics because the Cl groups trap the ions in the system via ion-dipole interactions, resulting in excellent pressure sensitivity (7.36 kPa-1) for tactile sensors. The skin-like sensor responds to pressure variations, demonstrating its potential for touch modulation in future wearable electronics and human-machine interfaces.
| S-EPMC9744819 | biostudies-literature
Project description:Laccase immobilization is a promising method that can be used for the recyclable treatment of refractory phenolic pollutants (e.g., chlorophenols) under mild conditions, but the method is still hindered by the trade-off limits of supports in terms of their high specific surface area and rich functional groups. Herein, confined polymerization was applied to create abundant amino-functionalized polymeric ionic liquids (PILs) featuring a highly specific surface area and mesoporous structure for chemically immobilizing laccase. Benefiting from this strategy, the specific surface area of the as-synthesized PILs was significantly increased by 60-fold, from 5 to 302 m2/g. Further, a maximum activity recovery of 82% towards laccase was recorded. The tolerance and circulation of the immobilized laccase under harsh operating conditions were significantly improved, and the immobilized laccase retained more than 84% of its initial activity after 15 days. After 10 cycles, the immobilized laccase was still able to maintain 80% of its activity. Compared with the free laccase, the immobilized laccase exhibited enhanced stability in the biodegradation of 2,4-dichlorophenol (2,4-DCP), recording around 80% (seven cycles) efficiency. It is proposed that the synergistic effect between PILs and laccase plays an important role in the enhancement of stability and activity in phenolic pollutant degradation. This work provides a strategy for the development of synthetic methods for PILs and the improvement of immobilized laccase stability.
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