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Iontogel 3

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1. Energy density

Ionogels are 3D polymer networks that contain ionic liquids that possess excellent thermal, electrochemical and chemical stability. They have low flammability, no vapor pressure, and a broad potential window, making them ideal for supercapacitors. Moreover, the presence of Ionic liquids in their structure provides them with mechanical integrity. Ionogels can be utilized without encapsulation, and are compatible with harsh conditions like high temperatures.

They are therefore promising candidates for wearable and portable electronics. They are not compatible with electrodes due to of their large ion sizes as well as their high viscosity. This results in slow ionic diffusion, and a gradual decrease in capacitance. To overcome this problem researchers integrated ionogels in solid-state capacitors (SC) to attain high energy density and long durability. The resulting SCs based on iontogel outperformed previously reported ILs and gel-based ILSCs.

To make the iontogel-based SCs, 0.6 g of the copolymer P(VDF-HFP) was mixed with 1.8 g of the hydrophobic EMIMBF4 ionic liquid (IL). The solution was cast onto a Ni-based film, and sandwiched between MCNN/CNT/CNT film and CCNN/CNT/CNT/CNT film, which were used as positive and negative electrodes. The electrolyte of ionogel was evaporated in an Ar-filled glovebox to create a symmetric FISC, with a the potential of 3.0 V.

The iontogel-based FISCs showed excellent endurance, with a capacitance retention of as high as 88 percent after 1000 cycles in straight and bending conditions. Additionally, they showed excellent stability, sustaining an even potential window when bending. These results indicate that iontogels are an efficient and long-lasting alternative to conventional electrolytes based on ionic liquids, and they may pave the way for the future development of solid-state flexible lithium-ion supercapacitors. Furthermore, these FISCs made of iontogel can be easily customized to suit various applications. They can be shaped in accordance to the dimensions of the device and are capable of charging and discharging at different angles. This makes them a good choice for applications where the size of the device and bent angles are not fixed.

2. Conductivity of Ionics

The structure of the polymer networks may have a significant effect on the conductivity of ions. A polymer with high crystallinity and Tg has higher ionic conductivity than one with low crystallinity or Tg. Therefore, iontogels with high ionic conductivity are required for applications that require electrochemical performance. Recently we have developed an ionogel that self-healable with superior mechanical properties and high Ionic conductivity. This new ionogel is prepared by locking ionic liquids, 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMIM TFSI), into poly(aminopropyl-methylsiloxane) grafted with [2-(methacryloyloxy)ethyl] trimethylammonium chloride (METAC), in the presence of tannic acid (TA). The result is an unidirectional crosslinked system that is fully physical and consists of ionic clusters forming between METAC, the TA and PAPMS and hydrophobic networks between TA, PAPMS and iontogel 3

The ionogel is a chemically crosslinked material with excellent mechanical properties such as high elastic strain-to break and high strain recovery. It also has excellent thermal stability and ionic conductivity up to 1.19 mS cm-1 at 25 degrees Celsius. In addition, the ionogel is able to completely heal after 12 hours at room temperature with a recovery of up to 83%. This is due to the formation of a totally physical dual crosslinked networks between METAC and TA as well as hydrogen bonding between iontogel3 and the TA.

We have also been able alter the mechanical properties of the material by with different ratios of trithiols and dithiols. By increasing the concentrations of dithiols, we are able to reduce the amount of crosslinking networks in Ionogels. We also discovered that altering the thiol acrylate ratio has a significant impact on the ionogels polymerization kinetics and mechanical properties.

The ionogels also possess a very high dynamic viscoelasticity, with a storage modulus up to 105 Pa. The Arrhenius plots for the Ionic Fluid BMIMBF4 as well as Ionogels with varying amounts hyperbranched polymer exhibit typical rubber-like behaviour. Over the temperature range studied, the storage modulus is independent of frequency. The ionic conductivity in Ionogels is also unaffected by frequency which is a crucial feature for applications as electrolytes that are solid-state.

3. Flexibility

Ionogels made up of polymer and ionic liquid have excellent stability and superior electrical properties. They are a promising material for iontronic devices such as triboelectric nanogenerators, ionic thermoelectric materials and strain sensors. Their flexibility is a major issue. To tackle this issue, we designed a flexible ionogel with ionic conductivity and self-healing capability by using the reversibility of weak and strong interactions. This ionogel is extremely resistant to both stretching and shear forces and is able to stretch up to 10 times its original size without losing the ionic conducting properties.

The ionogel is made up of the monomer acrylamide that has the carboxyl group attached to a polyvinylpyrrolidone (PVDF) chain. It is soluble in water, ethanol and acetone. It has a high modulus of 1.6MPa and break length of 9.1 percent. Solution casting is a straightforward method to apply the ionogel on non-conductive surfaces. It is also a candidate for ionogel supercapacitor as it possesses a specific capacity of 62 F g-1, a current density of 1 A g-1, as well as excellent stability in cyclic conditions.

In addition it is able to generate electromechanical signals at significant frequency and power as shown by the paper fan as an example of a flexible strain sensor Iontogel (Fig. 5C). The ionogel coated paper can produce consistent and reproducible electromechanical responses when it is repeatedly folded and shut like an accordion.

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4. Healability

The unique properties of Iontogel 3 make it a promising choice for a myriad of applications, such as information security, Iontogel soft/wearable electronics, and energy harvesters (e.g. convert mechanical energy into electrical energy). Ionogels are transparent and self-healing when crosslinking's reversible reaction is managed in a controlled manner.

To prepare ionogels, a block copolymer of poly(styrene)-b-poly(N,N-dimethylacrylamide-r-acrylic acid) (P(St)-b-P(DMAAm-r-AAc)) is cast into an ionic liquid (IL) and crosslinked using the thermoresponsive Diels-Alder reaction. The resulting ionogels have high Ionic conductivity, tensile strength, and resilience while also having a large thermal stability window.

For a more advanced application, the ionogels were doped with carbon quantum dots through dynamic covalent cross-linking of chitosan with glutaraldehyde and chemical cross-linking of acrylamide in 1-ethyl-3-methylimidazolium chloride (EMIMCl). Additionally, ionogels can be fabricated to form a stretchable and flexible membrane by incorporating the ionic dipole interactions between DMAAm-r-AAc block. The ionogels were also found to exhibit excellent transparency and self-healing properties when subjected to cyclic stretching.

A different approach to endow materials with self-healing capabilities is to utilize photo-responsive chromophores that create dimers when exposed to light through [2-2] and [4-4] cycloaddition reactions as illustrated in Figure 8b. This method allows the creation of Ion block copolymer gels reversible that self-heal by heating the dimers back to their initial state.

Another benefit of these reversible bonds is that it eliminates the need for expensive crosslinking agents and permits easy modification of the material's properties. Ionogels are versatile and can be utilized for industrial and consumer applications because they are able to control the irreversible reaction. These ionogels are also engineered to perform differently at different temperatures. This is done by varying the concentrations of the ionic fluid and synthesis conditions. In addition to the mentioned applications self-healing ionogels are ideal for use in outer space since they can maintain their shape and ionic conductivity even at very low pressures of vapor. Further research is needed to create self-healing Ionogels that are stronger and more robust. For example Ionogels might need to be reinforced with more rigid materials, like carbon fibers or cellulose, to ensure adequate protection against environmental stressors.