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Phase-Transitional Ionogel-Based Supercapacitors for a Selective Operation.

ABSTRACT: As the demand for energy storage devices increases, the importance of electrolytes for supercapacitors (SCs) is further emphasized. However, since ions in electrolytes are always in an active state, it is difficult to store energy for a long time due to ion diffusion. Here, we have synthesized a phase-transitional ionogel and fabricated an SC based on the ionogel. The 1-ethyl-3-methylimidazolium nitrate ([EMIM]⁺[NO₃]^-) ionogel changes its phase from crystal to amorphous when the temperature was elevated above its phase transition temperature (∼44 °C). When the temperature is elevated from 25 to 45 °C, the resistivity of the gel is decreased from 2318.4 kΩ·cm to 43.2 Ω·cm. At the same time, the capacitance is boosted from 0.02 to 37.35 F g^-1, and this change was repeatable. Furthermore, the SC exhibits an energy density of 7.77 Wh kg^-1 with a power density of 4000 W kg^-1 at 45 °C and shows a stable capacitance retention of 87.5% after 3000 cycles of test. The phase transition can switch the SCs from "operating mode" to "storage mode" when the temperature drops. A degree of self-discharge is greatly suppressed in the storage mode, storing 89.51% of charges after 24 h in self-discharge tests.

SUBMITTER: Park J

PROVIDER: S-EPMC9136841 | biostudies-literature | 2022 May

REPOSITORIES: biostudies-literature

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Phase-Transitional Ionogel-Based Supercapacitors for a Selective Operation.

Park Jinwoo J Sun Jeong-Yun JY

ACS applied materials & interfaces 20220512

As the demand for energy storage devices increases, the importance of electrolytes for supercapacitors (SCs) is further emphasized. However, since ions in electrolytes are always in an active state, it is difficult to store energy for a long time due to ion diffusion. Here, we have synthesized a phase-transitional ionogel and fabricated an SC based on the ionogel. The 1-ethyl-3-methylimidazolium nitrate ([EMIM]+[NO3]-) ionogel changes its phase from crystal to am ...[more]

PMID: 35549004

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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.

Project description:We present an approach for the rational development of stimuli-responsive ionogels which can be formulated for precise control of multiple unique ionogel features and fill niche pharmaceutical applications. Ionogels are captivating materials, exhibiting self-healing characteristics, tunable mechanical and structural properties, high thermal stability, and electroconductivity. However, the majority of ionogels developed require complex chemistry, exhibit high viscosity, poor biocompatibility, and low biodegradability. In our work, we overcome these limitations. We employ a facile production process and strategically integrate silk fibroin, the biocompatible ionic liquids (ILs) choline acetate ([Cho][OAc]), choline dihydrogen phosphate ([Cho][DHP]), and choline chloride ([Cho][Cl]), traditional pharmaceutical excipients, and the model antiepileptic drug phenobarbital. In the absence of ILs, we failed to observe gel formation; yet in the presence of ILs, thermoresponsive ionogels formed. Systems were assessed via visual tests, transmission electron microscopy, confocal reflection microscopy, dynamic light scattering, zeta potential and rheology measurements. We formed diverse ionogels of strengths ranging between 18 and 642 Pa. Under 25 °C storage, formulations containing polyvinylpyrrolidone (PVP) showed an ionogel formation period ranging over 14 days, increasing in the order of [Cho][DHP], [Cho][OAc], and [Cho][Cl]. Formulations lacking PVP showed an ionogel formation period ranging over 32 days, increasing in the order of [Cho][OAc], [Cho][DHP] and [Cho][Cl]. By heating from 25 to 60 °C, immediately following preparation, thermoresponsive ionogels formed below 41 °C in the absence of PVP. Based on our experimental results and density functional theory calculations, we attribute ionogel formation to macromolecular crowding and confinement effects, further enhanced upon PVP inclusion. Holistically, applying our rational development strategy enables the production of ionogels of tunable physicochemical and rheological properties, enhanced drug solubility, and structural and energetic stability. We believe our rational development approach will advance the design of biomaterials and smart platforms for diverse drug delivery applications.

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Phase-Transitional Ionogel-Based Supercapacitors for a Selective Operation.

Publications

Phase-Transitional Ionogel-Based Supercapacitors for a Selective Operation.

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