Solution Casting Research Articles

In-situ halloysite functionalization of anionic hybrid gels possessing easily implemented site-specific (alkyl)amide and carboxyl groups

Design of functional materials with tunable properties based on anionically-modified copolymer network of poly (N-isopropyl acrylamide-co-methacrylic acid) P(NIPA-co-MA) containing linear polyacrylamide and various amounts of Halloysite nanotubes (Hal) was presented using a facile route of solution casting. The organic/inorganic nanostructures based on thermo-responsive PNIPA were constructed to create hybrid materials via in situ polymerization with different Hal-loading and then used for the removal of cationic methylene blue (MB) dye from aqueous solutions. To achieve the desired mechanical property, the optimum composition of hybrids was determined following a simple and cost-effective synthesis procedure. In situ one-pot polymerization was promoted by semi-IPN formation, following a much simpler route than traditional preparation approaches for stable cross-linked hybrid formation. The swelling of hybrids decreased by 2.9-fold with loading of 5.40 % Hal, confirming the hydrogen bonding interactions between Hal and PAAm/P(NIPA-co-MA) network. The mechanical properties of Hal-doped hybrid gels showed an increase–decrease tendency with increase of Hal-content from 0.80 to 5.40 % (w/v) due to the high aspect ratio of Hal and strong secondary interactions between Hal and PAAm/P(NIPA-co-MA) chains. The effective cross-link density for Hal-doped hybrids was expressed by a cubic polynomial as a function of Hal concentration. Temperature-sensitive swelling results showed that the advantage of sustained release property of Hal can be combined with excellent controllability of PNIPA-based network. Adsorption results of MB onto Hal-doped hybrids bearing methacrylic acid moieties demonstrated their potential as efficient adsorbents for the removal of cationic dyes. A new route offered by the proposed procedure for design of hybrids containing “green” one-dimensional nanofillers creates an innovative perspective on robust hybrid structures for practical applications.

Impact of citric acid on guar gum carboxymethylcellulose crosslinked blend films

AbstractThis research intends to create biodegradable packaging films using solution casting method. The films are composed of guar gum, carboxymethylcellulose, and blends of these materials with citric acid as a crosslinking agent. The concentration of citric acid ranges from 10 to 30% (w w−1). This study performs a curing treatment at 140°C for 30 min on the dried films containing the crosslinking additive to promote the esterification between the polymeric matrix and the crosslinking agent. The thin films have a smooth, homogeneous, and transparent aspect. Although the crosslinking reaction – evidenced by FTIR spectra – does not affect the thickness of the material, it causes a slight color variation making the samples assume a yellowish shade. Moreover, the crosslinking process enhances the water resistance, decreases the crystallinity index, and improves the water vapor barrier and thermal resistance of the films. The SEM images reveal the excess of unreacted crosslinking agent accumulated on the samples; these particles work as a plasticizer, affecting the morphology of the films as well as their water resistance, crystallinity, and thermal resistance.

Hydroxyapatite-Based Natural Biopolymer Composite for Tissue Regeneration.

Hydroxyapatite (HAp) polymer composites have gained significant attention due to their applications in bone regeneration and tooth implants. This review examines the synthesis, properties, and applications of Hap, highlighting various manufacturing methods, including wet, dry, hydrothermal, and sol-gel processes. The properties of HAp are influenced by precursor materials and are commonly obtained from natural calcium-rich sources like eggshells, seashells, and fish scales. Composite materials, such as cellulose-hydroxyapatite and gelatin-hydroxyapatite, exhibit promising strength and biocompatibility for bone and tissue replacement. Metallic implants and scaffolds enhance stability, including well-known titanium-based and stainless steel-based implants and ceramic body implants. Biopolymers, like chitosan and alginate, combined with Hap, offer chemical stability and strength for tissue engineering. Collagen, fibrin, and gelatin play crucial roles in mimicking natural bone composition. Various synthesis methods like sol-gel, hydrothermal, and solution casting produce HAp crystals, with potential applications in bone repair and regeneration. Additionally, the use of biowaste materials, like eggshells and snails or seashells, not only supports sustainable HAp production but also reduces environmental impact. This review emphasizes the significance of understanding the properties of calcium-phosphate (Ca-P) compounds and processing methods for scaffold generation, highlighting novel characteristics and mechanisms of biomaterials in bone healing. Comparative studies of these methods in specific applications underscore the versatility and potential of HAp composites in biomedical engineering. Overall, HAp composites offer promising solutions for improving patient outcomes in bone replacement and tissue engineering and advancing medical practices.

Enhancing the radiation shielding performance of polyepoxide composites based on cement bypass dust

In this study, radiation shielding composite materials were created by combining epoxy with cement bypass dust (CBPD) at different weight percentages (0%, 10%, 20%, and 30%). The solution casting technique was employed to construct these materials. The FTIR spectra confirmed the formation of the composites and the production of complexes. The morphology and elemental content of the produced composite samples were illustrated using SEM pictures and EDX spectra. In addition, the research findings demonstrated that the composites exhibited improved resistance to changes in temperature as the loading of CBPD increased. The gamma-ray attenuation coefficients of composites consisting of Epoxy + x% CBPD exhibited an increase, along with an increase in the neutron removal cross-section. However, there was a gradual increase in both the mean free path (MFP) as well as the half value layer (HVL) with increasing energy. Additionally, the experimental and theoretical data for attenuation parameters were compared using the Phy-X/PSD software. The relationship between the effective atomic and electron numbers of the Epoxy + x% CBPD composites has been studied. The values of fast and thermal neutron attenuation were analyzed using the NGCal software. In general, these composites are appropriate for use in radiation shielding applications.

Incorporation of zeolitic imidazolate framework-8 (ZIF-8) in the polyamide and polysulfone layers of forward osmosis membranes for enhancing aquaculture wastewater recovery and PPCPs removal

Wastewater recovery is essential to alleviate water resource shortages, and this can be achieved through a high-energy-efficient forward osmosis (FO) process combined with an emerging material, zeolitic imidazolate framework-8 (ZIF-8). Here, we create thin-film composite FO membranes (TF-CFOMs) by incorporating ZIF-8 into the active polyamide (PA) and/or support polysulfone (PSf) layers to address the challenges of low water flux and loss of draw solutes during operation. Experimental factors included the dosage of ZIF-8 nanoparticles in PA preparation solutions and the dosages of 2-methylimidazole (2-Hmim) and zinc nitrate hexahydrate (ZNH) in n-methyl-2-pyrrolidone (NMP) to fabricate the PSf casting solutions with in-situ formed ZIF-8 nanoparticles. Successful ZIF-8 incorporation on the TF-CFOM surface was confirmed, and the ZIF-8 TF-CFOMs exhibited increased surface hydrophilicity and separation performance. Only modifying the PA layer by adding 0.025 wt% ZIF-8 nanoparticles in trimesoyl chloride (TMC) resulted in the membrane (PA0.025T-PSf0) with water flux 2.3 times higher than the pristine TF-CFOM (4.9 LMH). The pristine and modified TF-CFOMs were further applied for aquaculture wastewater (AWW) recovery and removal of pharmaceuticals and personal care products (PPCPs). Results of water recovery demonstrated that the recovery rate reached 89.1% in 3.5 days when using the dual-layer modified TF-CFOM. Results of PPCP removal indicated that both pristine and modified TF-CFOMs can achieve high PPCP rejection efficiency (>90%), with the modified TF-CFOM (PA0.025T-PSf2.0) performing the best. Overall, the PA0.025T-PSf2.0 TF-CFOM achieved high and stable separation efficiency in long-duration AWW recovery, making it well-suited for practical field applications.

Polyvinyl alcohol/carboxymethyl cellulose blended polymers doped with PPy/milled MWCNTs filler for Flexible optoelectronic and Energy Storage Applications

Using the solution casting procedure, poly (vinyl alcohol)/carboxymethyl cellulose/polypyrene/milled multiwall carbon nanotubes, PVA/CMC/PPy/x wt% milled MWCNTs blended polymers were formed. X-ray diffraction and scanning electron microscopy were employed to inspect the structure and morphology of the resulted blends. The lowest direct and indirect optical band gaps are (5, 4.3) eV and (4.37, 3.38) eV, respectively, achieved when the MWCNTs content in the doped blend was 0.25 wt %. By incorporating varying quantities of milled MWCNTs into the PVA/CMC/PPy blended polymer, consistent enhancements were observed in the optical dielectric constant and optical conductivity values. The blend with 0.25 wt% MWCNTs exhibited the maximum values of refractive index. The maximum electric dielectric constant and energy density values were attained as x = 0.15. The temperature impacted the dielectric constants and energy storage values. All blends fit with the CBH model. The impact of MWCNTs doping level and the temperature on the impedance spectroscopy and electric modulus of the host blend was explored. The sample with x = 0.15 has the smallest relaxation time. The impact of MWCNTs doping level on the dc conductivity, activation energy and conductivity mechanism of the host blend was explored. The doped blends with x = 0.15 is viable materials for energy storage purposes.

Synthesis and improved optical, electrical, and dielectric properties of PEO/PVA/CuCo2O4 nanocomposites

This study investigates the development of novel nanocomposite films based on a blend of polyethylene oxide (PEO) and polyvinyl alcohol (PVA) loaded with varying weight percentages of copper cobaltite nanoparticles (CuCo2O4 NPs). The primary objective was to fabricate these nanocomposites using a solution casting technique and explore the influence of CuCo2O4 content on their structural, optical, electrical, and dielectric properties. Spinel-type CuCo2O4 NPs were synthesized via the hydrothermal method and incorporated into the PEO/PVA blend. X-ray diffraction (XRD) analysis revealed the transformation of the polymer matrix towards an amorphous state with increasing CuCo2O4 content. UV–Vis spectroscopy studies demonstrated a decrease in both the direct and indirect band gaps of the nanocomposites, suggesting potential applications in optoelectronic devices. Impedance spectroscopy measurements revealed a significant enhancement in ionic conductivity (three orders of magnitude higher than the pristine blend) for the nanocomposite film containing 1.8 wt% CuCo2O4. The real permittivity (ε′) and imaginary permittivity (ε″) of the polymer nanocomposites exhibited a decrease with increasing frequency due to the interplay of various polarization mechanisms. Notably, incorporating 1.8 wt% CuCo2O4 nanoparticles led to a remarkable improvement in energy density compared to the pristine blend. Additionally, a significant decrease in the potential barrier was observed. These findings demonstrate the successful fabrication of PEO/PVA-CuCo2O4 nanocomposite films with enhanced optical, electrical, and dielectric properties. The observed improvements suggest promising applications for these materials in energy storage devices and potentially in optoelectronic devices like light-emitting diodes.

Quasi-Gel Polymer Electrolyte Interfaced with Electrodes through Solvent-Swollen Poly(ethylene oxide) for High-Performance Lithium/Lithium-Ion Batteries.

Solid polymer electrolytes (SPEs) are regarded as a superior alternative to traditional liquid electrolytes of lithium-ion batteries (LIBs) due to their improved safety features. The practical implementation of SPEs faces challenges, such as low ionic conductivity at room temperature (RT) and inadequate interfacial contact, leading to high interfacial resistance across the electrode and electrolyte interfaces. In this study, we addressed these issues by designing a quasi-gel polymer electrolyte (QGPE), a blend of poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), poly(ethylene oxide) (PEO), and succinonitrile (SN), with the desired mechanical strength, ionic conductivity, and interfacial stability through a simple solution casting technique. The QGPE features a thin solvated PEO layer on its surface, which wets the electrode, reducing the interfacial resistance and ensuring a homogeneous Li-ion flux across the interface. The optimized QGPE exhibits a good lithium-ion conductivity of 1.14 × 10-3 S cm-1 with a superior lithium-ion transference number of 0.7 at 25 °C. The Li/QGPE/Li symmetric cell exhibits a highly reversible lithium plating/stripping process for over 1300 h with minimal voltage polarization of ∼20 mV. The Li/QGPE/LiFePO4 full cell demonstrates good rate capability and excellent long-term cycling performance at a 0.1 C rate at 25 °C, maintaining a specific discharge capacity of 148 mAh g-1 over 200 cycles. The effectiveness of QGPE for LIBs is proven using a graphite/QGPE/LiFePO4 4 × 4 cm pouch cell, showcasing outstanding flexibility and tolerance against intentional abuse.

Multi-walled carbon nanotube-enhanced polyurethane composite materials and the application in high-performance 3D printed flexible strain sensors

Flexile strain sensors hold vast potential for applications in monitoring human motion, enabling human-machine interaction, and facilitating information transfer, etc. However, the available materials and manufacturing techniques for fabricating flexible strain sensors with high sensitivity and extended sensing range still face significant challenges. By utilizing solution casting and twin-screw extrusion techniques, this study prepared high-performance thermoplastic polyurethane/multi-walled carbon nanotube (TPU/MWCNT) nanocomposite 3D printable filaments, and employed material extrusion 3D printing technology to facilely fabricate flexible strain sensors. The 1-pyrene carboxylic acid (PCA)-modified TPU/MWCNT(3 wt%) nanocomposite exhibited outstanding mechanical properties, with a tensile strength of 24.3 ± 0.5 MPa and a fracture elongation of 625.8 ± 12.3 %. The 3D printed TPU/MWCNT(3 wt%)/PCA flexible strain sensors demonstrated amazing sensitivity (GFmax = 10279.95) within a wide strain range (0–300 % strain). The addition of PCA brings the benefits of improved dispersion of MWCNTs in the TPU composite, as well as enhanced thermal stability, and upgraded mechanical and electrical properties under different tensile strains. Meanwhile, the 3D printed samples displayed remarkable durability and reproducibility. Finally, the flexible strain sensors fabricated from this nanocomposite material could accurately perceive human motion, providing great prospects for wearable device applications.

Biobased rubber toughened poly(lactic acid) blend for sustainable packaging films: The role of optical purity of poly(lactic acid)

AbstractThis study investigates the novel effect of poly(lactic acid) (PLA) optical purity on PLA/liquid natural rubber (LNR) blend films fabricated by solution casting. An investigation was conducted to examine how different levels of PLA optical purity affect the mechanical, structural, morphological, thermal, and barrier properties of PLA/LNR films. Infrared spectroscopy analysis revealed that the D‐isomer content of PLA significantly affected the chemical interactions between the LNR and PLA. The favorable chemical interaction between the LNR and PLA with a high D‐isomer content also increased the elongation at break by 300%. Morphological investigations proved that the chemical interaction also improved the dispersion and reduced the size of the LNR droplets formed in the PLA matrix. Notably, while low D‐isomer PLA blends showed decreased crystallinity (Xc) upon LNR addition, high D‐isomer PLA blends exhibited increased Xc by 460%, leading to a 42% increase in oxygen transmission rate. Additionally, hydrolytic degradation of high D‐isomer PLA increased by 259% with increasing LNR content. Overall, optical purity of PLA plays an important role in determining the properties of PLA blends.

Exploration of the structural and electrical characteristics and solar cell applications of an electrolyte membrane derived from acacia gum

The natural and eco-friendly solid-state electrolytes were prepared using varying concentrations (wt%) of ZnSO4.7H2O salt and pure acacia gum through the solution cast method. Multiple analytical methods were employed to characterize the resulting acacia gum electrolyte samples. XRD analysis confirmed the increased presence of the amorphous phase with the introduction of salt. FTIR analysis explored the formation of interlinking bands and their complex nature upon salt incorporation. The ionic conductivity was found from room temperature (RT) to 100 °C range. The optimized high ionic conductivity value was found to be 1.11 × 10−4 S/cm at 100 °C for the electrolyte composed of 70 wt% acacia gum and 30 wt% ZnSO4.7H2O, while at RT it was 1.06 × 10−5 S/cm for the same composition. Activation energy values fell within the 0.6–0.92 eV range for all samples. Complex dielectric (real and imaginary) and complex electric modulus analyses were conducted. Dielectric permittivity and electrical modulus analyses revealed a significant interaction between the segmental movements of acacia gum and salt ions. Ionic relaxation processes were explored in terms of conductivity relaxation time using the electrical modulus. The presence of a long tail in the complex dielectric modulus study indicated that the acacia-based solid electrolyte displayed favorable capacitance properties. Further, the Solar Cell (dye-sensitized solar cell) device was fabricated with (Acacia gum + ZnSO4.7H2O) electrolyte. The current density-voltage (J-V) characteristics of the prepared device were investigated. The outstanding results were optimized in the present work, Voc = 0.81 V, Jsc = 9.56 mA/cm2, Fill Factor of 0.67, and optimum power conversion efficiency ƞ = 5.17 % for the electrolyte composed of 70 wt% acacia gum and 30 wt% ZnSO4.7H2O device.

Fabrication of rare earth-doped ZnO-PVDF flexible nanocomposite films for ferroelectric response and their application in piezo-responsive bending sensors.

The present study covers the fabrication of flexible piezoelectric nanogenerators and their application towards sustainable power generation. The rod-like structure of erbium-doped ZnO (EZ) nanoparticles prepared by the hydrothermal synthesis route was successfully incorporated inside the polyvinylidene fluoride (PVDF) matrix using the solution casting method. Solution casting is an easy and cost-effective method for fabricating laminated, thin, flexible and lightweight EZ-PVDF nanocomposite films. The formation of the desired crystallographic phase of EZ-PVDF nanocomposite films and the presence of rod-like EZ nanoparticles inside the PVDF matrix were confirmed using X-ray diffraction and FESEM. The enhancement of the β-phase fraction of the EZ-PVDF nanocomposite films as compared to bare PVDF was estimated using FTIR spectroscopy. The presence of a ferroelectric phase in the EZ-PVDF nanocomposite films was found due to the formation of a large area of interfaces between the EZ nanoparticles and the PVDF matrix. The maximum polarizations of 0.00696 μC cm-2 and 0.00683 μC cm-2 for two samples (EZP1 and EZP2, respectively) were observed at an electric field of 1.25 kV cm-1. The piezoelectric voltages were observed at relatively low frequencies for both nanocomposite films. The maximum piezoelectric voltages of 18.9 V and 15.5 V were observed at a 1 Hz frequency for EZP1 and EZP2, respectively. The output piezoelectric current of 16.88 mA and the maximum power density of 7773.68 W m-3 for EZP1 ensure its potential as an efficient piezoelectric nanogenerator with greater efficiency than those reported previously in published articles. The change in the piezoelectric voltage response of the nanocomposite films as a function of mechanical movement of human external body parts renders them the most suitable candidate for human-machine interfacing (HMI) applications, such as bending sensors and human motion sensors.

One-pot in situ synthesis of ZIF particles to prepare thin-film nanocomposite membranes for CO2 separation

Mixed matrix membranes (MMMs) are more likely to break the Robeson upper bound because they combine the pros of both organic and inorganic membranes. However, in the conventional MMM preparation processes, multi-steps are normally needed and, in many cases, the particle agglomeration and consequent non-selective voids are unavoidable, resulting in poor carbon dioxide (CO2) separation performances. In addition, the agglomeration makes it challenging to fabricate thin-film nanocomposite (TFN) membranes. In this study, zeolitic imidazolate framework (ZIF)-8- and ZIF-67-based TFN membranes were fabricated via a facile one-pot in situ synthesis protocol. The ZIF particles were synthesized in the polymeric solution, then the TFN membranes were fabricated by a dip coating method. With a casting solution concentration of 1.5 wt.%, a selective layer with a thickness of ∼300 nm can be prepared on the porous polyacrylonitrile (PAN) support. The results of thermogravimetric analysis (TGA), differential scanning calorimeter (DSC), Fourier Transform Infrared (FT-IR) spectroscopy, and X-ray diffraction (XRD) showed that ZIFs were successfully synthesized in the casting solution. At 35 °C and 2 bar, the membrane containing 5 wt.% ZIF-67 had a CO2 permeance of 223.35 gas permeation unit (GPU), which was 16.55 % higher than that of pure Pebax.

HBN/PVDF‐HFP and BNNS/PVDF‐HFP nanocomposites as flexible and lightweight dielectric capacitors: High energy storage performance via electrically insulating nanoparticles

AbstractAs the energy demand continuously increases, polymer‐based materials have attracted much attention for energy storage systems as dielectric capacitors due to their higher power density and charge–discharge rate than lithium‐ion batteries and supercapacitors. However, it is necessary to increase the energy density of dielectric capacitors. In this context, poly(vinylidene fluoride‐co‐hexafluoropropylene), PVDF‐HFP, matrix nanocomposites are produced by solution casting method reinforced with hexagonal boron nitride (hBN) nanoparticles and silane‐modified boron nitride nanosheets ‐BNNSs‐ (BNNS‐VTS) up to 10 wt.% filler content. The effects of filler content and surface modification of hBN/BNNSs on PVDF‐HFP matrix nanocomposites' microstructure, phase evolution, crystalization behavior, dielectric properties, and energy storage performance are discussed. 4% hBN/PVDF‐HFP nanocomposite demonstrates 641 MV·m−1 of breakdown strength and 23.2 J·cm−3 of discharged energy density due to hexagonal boron nitride's excellent electrical insulating behavior. The achieved values are 3.0 and 10.5 times superior to the values of the neat thin film, respectively, and they are noteworthy among hBN‐ or BNNS‐reinforced PVDF‐based nanocomposites, even in multi‐layered structures. Furthermore, 4% hBN/PVDF‐HFP presents a giant charge–discharge energy efficiency (92%). It is thus demonstrated that hBN/PVDF‐HFP nanocomposites hold a great potential to be used in energy storage applications as flexible and lightweight dielectric capacitors.Highlights PVDF‐HFP matrix nanocomposites for electrical energy storage as flexible dielectric capacitors hBN NPs and silane‐modified BNNSs are reinforced into the matrix by 0–10 wt.%. The effects of filler content and surface modification of hBN/BNNSs are discussed. 4% hBN loading results in 23.2 J·cm−3 energy density and 92% efficiency at 641 MV·m−1 breakdown strength. Those metrics are relatively high in hBN‐ or BNNS‐reinforced PVDF‐based nanocomposites.

Performance of high sulfonated poly(ether ether ketone) improved with microcrystalline cellulose and 2,3-dialdehyde cellulose for proton exchange membranes

Sulfonated poly (ether ether ketone) (SPEEK) has received substantial attention for its potential to improve the electrochemical behavior and thermomechanical capabilities of direct methanol fuel cells. This study examines how the integration by solution casting of microcrystalline cellulose (MCC) and 2,3-dialdehyde cellulose (DAC) onto highly sulfonated PEEK (with a sulfonation degree of 80%) affects its physicochemical properties and morphological structures. The mechanical attributes and proton conductivity of the polymer matrix are impacted by MCC and DAC inclusion into SPEEK membrane. The maximum proton conductivity was seen in the SPEEK/MCC membranes at 70 °C (up to 0.1 S cm−1). The proton conductivity in methanol vapor was increased by SPEEK/DAC membranes at high temperatures as opposed to pristine SPEEK and SPEEK/MCC membranes.

Electrospun Nano-Porous Cellulose Acetate Membrane Casted with Chitosan for Solid-State Sodium-Ion Batteries

Emerging as a safe and economically viable alternative to lithium-ion batteries, the solid-state sodium ion battery (ss-SIB) has captured increasing attention as a transformative technology for realizing a decarbonized economy and ensuring a sustainable energy supply. Here we report a nanoarchitecture strategy of biodegradable, biocompatible, and naturally abundant cellulose derivative (cellulose acetate, CA) and chitosan (CH) biopolymer-based nano-porous electrospun composite electrolyte (ECE) for flexible and wearable ss-SIBs. A simple combination of electrospinning and solution casting was utilized to fabricate mechanically robust (13.76 MPa), thin-film (0.067 mm), highly flexible, and high room temperature Na-ion conductive (1.04 x 10-4 S.cm-2) ECE. Lower activation energy (Ea = 0.13 eV) indicates easy charge carrier diffusion ability of as prepared ECE. The electrochemical stability window (ESW = 3.45 V) of ECE is studied by the linear sweep voltammetry (LSV) with respect to stainless steel and sodium metal electrodes. Uniform galvanostatic Na plating and stripping at room temperature is observed over 900 hrs at 0.5 mA•cm-2 current density in symmetric (Na|ECE|Na) cell performance, this underscores impressive electrochemical stability and compatibility with sodium metal. Using Na3V2(PO4)3 (NVP) as cathode, ECE, and Na metal as anode in the full cell, specific discharge capacity of 83 mA×h×g-1 at room temperature was attained at 0.1 C rate, highlighting the practical applicability of the nanostructured electrospun composite electrolyte for flexible and wearable ss-SIBs. Keywords Cellulose acetate, chitosan, electrospun, solid-state sodium-ion battery, specific discharge capacity.

Advancing Structural Supercapacitors with Hydrated Polymer

Structural supercapacitors, capable of bearing mechanical loads while storing electrical energy, hold great promise for enhancing mobile system efficiencies. However, developing practical structural supercapacitors often involves a challenging balance between mechanical and electrochemical performance, particularly in their electrolytes. Traditional research has focused on bi-continuous phase electrolytes (BPEs), which typically comprise high liquid content that weakens mechanical strength, and inert solid phases that hinder ion conduction and block electrode surfaces. Our previous work introduces a novel approach with a hydrated polymer electrolyte, demonstrating enhanced multifunctionality. This electrolyte, derived from controlled hydration of PET-LiClO4, forms a trihydrate (LiClO4∙3H2O) structure, where water molecules bond with ions without forming a liquid phase, thereby improving ion mobility while maintaining the base polymer's mechanical properties. This new design also promotes better electrochemical interfaces with electrodes, a significant advancement over traditional BPEs.In this study, we further enhance the performance and processability of such hydrated polymer electrolytes by incorporating polylactic acid (PLA) as the base polymer and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) as the salt. The electrolyte, prepared through solution casting and subsequent controlled hydration, consistently remains an amorphous solid solution in both dry and hydrated states, as confirmed by DSC, XRD, and FTIR analyses. Our tests on ionic conductivity and mechanical properties reveal that adding water to the polymer electrolyte substantially increases ionic conductivity while retaining mechanical properties. A specific composition demonstrated a remarkable increase in ionic conductivity coupled with superior toughness surpassing the base polymer. Furthermore, we successfully fabricated and tested structural supercapacitor devices made of composites of carbon fibers and these new electrolytes. The prototypes presented enhanced toughness with significant energy storage performance, demonstrating their vast application potential due to their outstanding multifunctionality.

Organic Ionic Plastic Crystal/Polymer Composite Electrolyte Prepared By Solution Casting Method for Solid-State Lithium Batteries

Solid-state electrolytes have been considered as a promising candidate to address the safety issues for next-generation lithium batteries. Organic ionic plastic crystals (OIPCs) are attracting increasing interests as solid electrolyte materials due to their unique advantages, such as plasticity, nonflammability, good thermal and electrochemical stability. In this study, an OIPC-based composite electrolyte consisting of the OIPC 1-ethyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide (Pyr12TFSI), lithium bis(trifluoromethylsulfonyl)imide (LiTFSI) and the polymer polyvinylidene fluoride (PVDF) has been developed by a facile solution casting strategy. A free-standing and flexible OIPC/polymer composite membrane was fabricated by the solution casting method, which not only provides flexibility and better electrode/electrolyte contact, but also is more compatible with current battery processing methods. The composite membrane used in Li/Li symmetric cell was cycled stably over 900 h at a current density of 0.1 mA cm−2 at 50 °C, demonstrating that the OIPC/polymer composite electrolyte enabled the reversible and stable lithium plating and stripping behaviors. Further tests of the OIPC/polymer composite as solid electrolyte in LiFePO4/Li cell presented a high specific capacity of 149 mAh g−1 at 0.1 C and a long cycle life of over 440 cycles with capacity retention of 89% at 0.5 C at 50 °C, which showed improved rate capability and cycling stability in comparison with the composites with similar compositions but obtained by powder pressing method. This study demonstrated the potential of the OIPC/polymer composite solid electrolyte prepared by solution casting method and will promote the development of high-performance OIPC-based composite electrolytes for solid-state batteries.

High‐Temperature Polymer Electrolyte Fuel Cells Based on Protic Ionic Liquids

ABSTRACTA hydrogen‐based energy system will be the backbone of a future energy grid using renewable energies. It is widely accepted that polymer electrolyte membrane fuel cells (PEMFCs) are promising converters of chemical energy stored as hydrogen into electrical energy. An increase of the operation temperature from below 80°C to above about 160°C is considered beneficial, as it would allow for much simpler water management and the use of waste heat. Here, we are investigating protic ionic liquids (PILs) immobilized in a polybenzimidazole polymer as electrolytes for high‐temperature PEMFCs. Ionic liquids are promising for fuel cell applications as they provide high thermal and chemical stability and high proton conductivity. In contrast to aqueous electrolytes, ionic liquids form a dense layered structure at the electrode–electrolyte interface that depends on the potential and on the content of residual water in the electrolyte. We investigate how PILs interact with the host polymer of the membrane revealing that porous polymer structures can be formed by solution casting, which allows for an encapsulation of the ionic liquid within the pores. After doping the polymer with small amounts of phosphoric acid, the membranes showed reasonable conductivity and fuel cell performance.

Enhanced performance in a NASICON-incorporated solid polymer electrolyte

In the present work, a novel ‘doped ceramic-polymer composite’-based solid polymer electrolytes (SPEs) has been synthesized using Zr (LAZTP) and Nb (LANbTP)-doped LATP as a ceramic filler and polyacrylonitrile (PAN) as a host polymer via the solution cast method. A series of SPEs with different ceramic loadings ranging from 10, 20, 30, 40, and 80 wt. % have been investigated using XRD, SEM, and impedance analysis. XRD spectra show the presence of crystalline ceramic peaks in composite solid polymer electrolyte. Further, the homogeneous distribution of the filler has been confirmed by SEM images. For SPEs, the highest conductivity of 5.31 × 10−5 S cm−1 has been obtained for PAN + LANbTP30 at room temperature. Whereas, the optimized conductivity for LATP-incorporated PAN shows 1.79 × 10−5 S cm−1, and the LAZTP-incorporated sample shows a conductivity of 3.03 × 10−5 S cm−1 at room temperature. Also, LANbTP-contained SPE shows excellent voltage stability of 4.90 V w.r.t. pure PAN.