Search Results (25)

Polyampholytes combine cationic and anionic groups in one macromolecular platform and are emerging as versatile components for energy storage and conversion. This review synthesizes how their charge balance, hydration, and architecture can be engineered to address ionic transport, interfacial stability, and safety across batteries, supercapacitors, solar cells, and fuel cells. We classify annealed, quenched, and zwitterionic systems, outline molecular design strategies that tune charge ratio, distribution, and crosslinking, and compare device roles as gel or solid electrolytes, eutectogels, ionogels, binders, separator coatings, and interlayers. Comparative tables summarize ionic conductivity, cation transference number, electrochemical window, mechanical robustness, and temperature tolerance. Across Li and Zn batteries, polyampholytes promote ion dissociation, homogenize interfacial fields, suppress dendrites, and stabilize interphases. In supercapacitors, antifreeze hydrogels and poly(ionic liquid) networks maintain conductivity and elasticity under strain and at subzero temperature. In solar cells, zwitterionic interlayers improve work function alignment and charge extraction, while ordered networks in fuel cell membranes enable selective ion transport with reduced crossover. Design rules emerge that couple charge neutrality with controlled hydration and dynamic crosslinking to balance conductivity and mechanics. Key gaps include brittleness, ion pairing with multivalent salts, and scale-up. Opportunities include soft segment copolymerization, ionic liquid and DES plasticization, side-chain engineering, and operando studies to guide translation. Full article

MXene–polymer hybrids combine the high in-plane conductivity and rich surface chemistry of MXenes with the processability and mechanical tunability of polymers for lithium-metal and lithium–sulfur batteries. Most reported systems still rely on HF-etched MXenes, introducing F-rich terminations, safety and waste issues, and poorly controlled surfaces. This review instead centers on fluoride-free synthesis routes, benchmarks them against HF methods, and translates route–termination relationships into practical rules for choosing polymer backbones. We track the evolution from early linear hosts such as PEO- and PVDF-type polymers to polar nitrile or carbonyl matrices, crosslinked and ionogel networks, and emerging biopolymers and COF-type porous frameworks that are co-designed with MXene terminations to regulate ion transport, interfacial chemistry, and mechanical robustness. These chemistry–backbone pairings are linked to five scalable fabrication modes, including solution blending and film casting, in situ polymerization, surface grafting, layer-by-layer assembly, and electrospinning, and to roles as solid or quasi-solid electrolytes, artificial interphases, separator-like coatings, and electrode-facing architectures. Finally, we highlight key evidence gaps and reporting standards needed to de-risk scale-up of green MXene–polymer batteries. Full article

The pursuit of sustainable and environmentally benign energy storage solutions has propelled significant interest in organic batteries, which utilize redox-active organic compounds as electrode materials. A pivotal component in determining their electrochemical performance, safety, and long-term stability is the electrolyte. Polymer-based electrolytes (PBEs) have emerged as promising candidates owing to their intrinsic advantages, such as enhanced thermal stability, mechanical integrity, and the mitigation of leakage and flammability risks associated with conventional liquid electrolytes. Unlike previous reviews that broadly cover solid electrolytes, this review specifically focuses on the unique developments of polymer-based electrolytes tailored for organic batteries over the past few years. This review presents a comprehensive overview of the recent progress in PBEs specifically designed for organic battery systems. It systematically examines various categories, including solid polymer electrolytes (SPEs), valued for their structural simplicity and stability; gel polymer electrolytes (GPEs), noted for their high ionic conductivity and processability; and polymer-inorganic composite electrolytes, which synergistically integrate the mechanical flexibility of polymers with the ionic conductivity of inorganic fillers. Additionally, the review delves into the latest advancements in ionogels and poly(ionic liquid) electrolytes, highlighting their potential to overcome existing limitations and enable next-generation battery performance. The article concludes with a critical discussion on prevailing challenges and prospective research directions, emphasizing the importance of advanced material design, interfacial engineering, and sustainable synthesis approaches to facilitate the practical realization of high-performance organic batteries. Full article

Ionic Liquids (ILs) are composed of ions, usually an organic cation with an organic or inorganic anion, with a melting point below 100 °C and in most cases below room temperature. These compounds exhibit important and characteristic properties such as high ionic conductivity, good thermal and electrochemical stability and low toxicity and flammability. Subsequently, ILs have been studied as promising substitutes for conventional electrolytes for electrochemical applications, both as bulk liquids or confined in polymer matrices, commonly known as ionogels, which have the advantages of not leaking and enhancing safety and manipulation during device assembly. For this work, the ionogel of the IL 1-Ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([C₂C₁Im][TFSI]) was synthesized by the polymerization of Tetramethyl orthosilicate (TMOS) and Dimethyldimethoxysilane (DMDMS). Thermal analyses of the pure ionic liquid and electrochemical response of the ionogel were studied in comparison with the corresponding bulk IL by using differential scanning calorimetry (DSC), thermogravimetry (TGA) and broad-band dielectric spectroscopy (BBDS), respectively. Full article

Since the last decade, the need for deformable electronics exponentially increased, requiring adaptive energy storage systems, especially batteries and supercapacitors. Thus, the conception and elaboration of new deformable electrolytes becomes more crucial than ever. Among diverse materials, gel polymer electrolytes (hydrogels, organogels, and ionogels) remain the most studied thanks to the ability to tune the physicochemical and mechanical properties by changing the nature of the precursors, the type of interactions, and the formulation. Nevertheless, the exploitation of this category of electrolyte as a possible commercial product is still restrained, due to different issues related to the nature of the gels (ionic conductivity, evaporation of filling solvent, toxicity, etc.). Therefore, this review aims to resume different strategies to tailor the properties of the gel polymer electrolytes as well as to provide recent advancements in the field toward the elaboration of deformable batteries and supercapacitors. Full article

Realizing rechargeable cells with practical energy and power density requires electrodes with high active material loading, a remaining challenge for solid-state batteries. Here, we present a new strategy based on ionogel-derived solid-state electrolytes (SSEs) to form composite electrodes that enable high active material loading (>10 mg/cm², ~9 mA/cm² at 1C) in a scalable approach for fabricating Li-ion cells. By tuning the precursor and active materials composition incorporated into the composite lithium titanate electrodes, we achieve near-theoretical capacity utilization at C/5 rates and cells capable of stable cycling at 5.85 mA/cm² (11.70 A/g) with over 99% average Coulombic efficiency at room temperature. Finally, we demonstrate a complete polymeric solid-state cell with a composite anode and a composite lithium iron phosphate cathode with ionogel SSEs, which is capable of stable cycling at a 1C rate. Full article

In this study, tetraethyl orthosilicate (TEOS) and methyltriethoxysilane (MTES) were used as precursors for silica, combined with the ionic liquid [BMIM-ClO₄]. Lithium perchlorate was added as the lithium-ion source, and formic acid was employed as a catalyst to synthesize silica ionogel electrolytes via the sol–gel method. FT-IR and NMR identified the self-prepared ionic liquid [BMIM-ClO₄], and its electrochemical window was determined using linear sweep voltammetry (LSV). The properties of the prepared silica ionogel electrolytes were further investigated through FT-IR, DSC, and ²⁹Si MAS NMR measurements, followed by electrochemical property measurements, including conductivity, electrochemical impedance spectroscopy (EIS), LSV, and charge–discharge tests. The experimental results showed that adding methyltriethoxysilane (MTES) enhanced the mechanical strength of the silica ionogel electrolyte, simplifying its preparation process. The prepared silica ionogel electrolyte exhibited a high ionic conductivity of 1.65 × 10⁻³ S/cm. In the LSV test, the silica ionogel electrolyte demonstrated high electrochemical stability, withstanding over 5 V without oxidative decomposition. Finally, during the discharge–charge test, the second-cycle capacity reached 108.7 mAh/g at a discharge–charge rate of 0.2 C and a temperature of 55 °C. Full article

Ionogels are hybrid materials comprising an ionic liquid confined within a polymer matrix. They have garnered significant interest due to their unique properties, such as high ionic conductivity, mechanical stability, and wide electrochemical stability. These properties make ionogels suitable for various applications, including energy storage devices, sensors, and solar cells. However, optimizing the electrochemical performance of ionogels remains a challenge, as the relationship between specific capacitance, ionic conductivity, and electrolyte solution concentration is yet to be fully understood. In this study, we investigate the impact of electrolyte solution concentration on the electrochemical properties of ionogels to identify the correlation for enhanced performance. Our findings demonstrate a clear relationship between the specific capacitance and ionic conductivity of ionogels, which depends on the availability of mobile ions. The reduced number of ions at low electrolyte solution concentrations leads to decreased ionic conductivity and specific capacitance due to the scarcity of a double layer, constraining charge storage capacity. However, at a 31 vol% electrolyte solution concentration, an ample quantity of ions becomes accessible, resulting in increased ionic conductivity and specific capacitance, reaching maximum values of 58 ± 1.48 μS/cm and 45.74 F/g, respectively. Furthermore, the synthesized ionogel demonstrates a wide electrochemical stability of 3.5 V, enabling diverse practical applications. This study provides valuable insights into determining the optimal electrolyte solution concentration for enhancing ionogel electrochemical performance for energy applications. It highlights the impact of ion pairs and aggregates on ion mobility within ionogels, subsequently affecting their resultant electrochemical properties. Full article

Nuclear Magnetic Resonance (NMR) spin relaxation times have been an instrumental tool in deciphering the local environment of ionic species, the various interactions they engender and the effect of these interactions on their dynamics in conducting media. Of particular importance has been their application in studying the wide range of electrolytes for energy storage, on which this review is based. Here we highlight some of the research carried out on electrolytes in recent years using NMR relaxometry techniques. Specifically, we highlight studies on liquid electrolytes, such as ionic liquids and organic solvents; on semi-solid-state electrolytes, such as ionogels and polymer gels; and on solid electrolytes such as glasses, glass ceramics and polymers. Although this review focuses on a small selection of materials, we believe they demonstrate the breadth of application and the invaluable nature of NMR relaxometry. Full article

In this study, an ionogel electrolyte (PAIM-X) consisting of 1-vinyl-3-methylimidazole bis (trifluoromethyl sulfonyl) imide ([VMIM][TFSI]), Polyacrylamide (PAAm), and MXene were prepared. The conductivity of PAIM-X and integral area of the voltammetric curve of the supercapacitor (PAIMSC) were improved by adding MXene. The addition of [VMIM][TFSI] enhanced the conductivity and applicable temperature of the ionogel electrolyte. At 90 °C, the conductivity of PAIM-4 can reach 36.4 mS/cm. In addition, spherical polyaniline with good electrochemical properties was synthesized and coated on graphite paper as an active substance. An all-solid-state supercapacitor was composed of PAIM-4, polyaniline electrode with 1.2 V potential window, pseudo-capacitors and high quality capacitors. The solvent 1-ethyl-3-methylimidazolium bis (trifluoromethyl sulfonyl imide) ([EMIM][TFSI]) and methanesulfonic acid (MSA) were introduced into the ionogel to promote the redox reaction of polyaniline (PANI). The mass specific capacitance of PAIMSC was 204.6 F/g and its energy density could reach 40.92 Wh/kg, which shows great potential for practical application at high temperature. The device had good rate performance and cycle performance, and its capacitance retention rate was still 91.56% after 10,000 cycles. In addition, the supercapacitor can work within the temperature range of −20 °C to 90 °C. These excellent electrochemical properties indicate that PAAm/IL/Mxene-X has broad application space and prospect. Full article

The purpose of this work is to check the viability of mixtures of ionic liquids and lithium salt as electrolytes in Li- batteries. Firstly, the determination of the thermo-electrical properties of liquid mixtures of the ionic liquid N-butyl-N-methyl-pyrrolidinium bis(trifluoromethanesulfonyl)imide [BMPyrr][TFSI] with [Li][TFSI] salt at different concentrations was performed. Additionally, these results were compared with the corresponding ionogels of these mixtures designed by two different gelation methods, one of them using Poly (vinylidene fluoride) (PVDF) as a supporting matrix and the other one using a silica matrix. Full article

Composite structural supercapacitors (SSC) are an attractive technology for aerospace vehicles; however, maintaining strength whilst adding energy storage to composite structures has been difficult. Here, SSCs were manufactured using aerospace-grade composite materials and CNT mat electrodes. A new design methodology was explored where the supercapacitor electrolyte was localised within the composite structure, achieving good electrochemical performance within the active region, whilst maintaining excellent mechanical performance elsewhere. The morphologies of these localised SSC designs were characterised with synchrotron X-ray fluorescence microscopy and synchrotron X-ray micro-computed tomography and could be directly correlated with both electrochemical and mechanical performance. One configuration used an ionogel with an ionic liquid (IL) electrolyte, which assisted localisation and achieved 2640 mW h kg⁻¹ at 8.37 W kg⁻¹ with a corresponding short beam shear (SBS) strength of 71.5 MPa in the active area. A separate configuration with only IL electrolyte achieved 758 mW h kg⁻¹ at 7.87 W kg⁻¹ with SBS strength of 106 MPa in the active area. Both configurations provide a combined energy and strength superior to results previously reported in the literature for composite SSCs. Full article

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 (T_g 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. Full article

This study is focused on the structural influence of 1,2,4-triazolium ionic liquid (IL), that is, the effect of the length of the substituent and the type of substitution (1-methyl-4-alkyl or 1-alkyl-4-methyl) used in the mixture with propylene carbonate (PC) on the properties of thiol–ene polymer ionogels and on the preparation of an ionogel with satisfactory mechanical and conductive properties. PC allows for higher conductivity but also causes electrolyte leakage from the gel. When using triazolium IL (instead of the imidazolium one), because of the stronger interactions between components of the system, the ionogels do not leak. In this study, 1,4-dialkyl-1,2,4-triazolium ILs were successfully synthesized by the alkylation of 1,2,4-triazole. Subsequently, gel polymer electrolytes were obtained by one-pot thiol–ene photopolymerization reactions of tetrafunctional thiols with different chemical structures: pentaerythritol tetra(3-mercaptopropionate) (PETMP) or pentaerythritol tetra(3-mercaptobutyrate) (PETMB) and trifunctional ene (TATT) in the presence of a mixture of 1,4-dialkyl-1,2,4-triazolium IL with PC. Measurements made by electrochemical impedance spectroscopy showed that all ionogels with TATT+PETMB as a polymer matrix presented smaller relative ionic conductivity compared to ionogels containing TATT+PETMP. The puncture resistance and elongation at puncture, measured by the puncture resistance method, were higher for ionogels with poly(TATT+PETMB) than for those with poly(TATT+PETMP). Moreover, ILs containing a methyl group in position N1 of the 1,2,4-triazole ring presented lower puncture resistance than ionogels with ILs containing a methyl group in position N4, especially for shorter alkyl chains. Additionally, the photo-differential scanning calorimetry method was employed to characterize the course of photopolymerization. The compositions and their constituents were characterized by UV and IR spectroscopy. Full article

Owing to the potential of sodium as an alternative to lithium as charge carrier, increasing attention has been focused on the development of high-performance electrolytes for Na batteries in recent years. In this regard, gel-type electrolytes, which combine the outstanding ionic conductivity of liquid electrolytes and the safety of solid electrolytes, demonstrate immense application prospects. However, most gel electrolytes not only need a number of specific techniques for molding, but also typically suffer from breakage, leading to a short service life and severe safety issues. In this study, a supramolecular thixotropic ionogel electrolyte is proposed to address these problems. This thixotropic electrolyte is formed by the supramolecular self-assembly of D-gluconic acetal-based gelator (B8) in an ionic liquid solution of a Na salt, which exhibits moldability, a high ionic conductivity, and a rapid self-healing property. The ionogel electrolyte is chemically stable to Na and exhibits a good Na⁺ transference number. In addition, the self-assembly mechanism of B8 and thixotropic mechanism of ionogel are investigated. The safe, low-cost and multifunctional ionogel electrolyte developed herein supports the development of future high-performance Na batteries. Full article