Styrene Sulfonic Acid Research Articles

Flexible free-standing BixSey@C/PEDOT:PSS thermoelectric composite film with high-performance electromagnetic interference shielding

Due to the component advantages and structural features, poly(3,4-ethylenedioxythiophene):poly(styrenesulfonic acid) (PEDOT:PSS) based inorganic–organic composite films shows huge application potential in various fields. However, there are few reports on the bi-functions of thermoelectric (TE) and electromagnetic interference (EMI) shielding for the PEDOT:PSS-based functional films. Herein, metal–organic frameworks (MOFs)-derived BixSey@C sheets with average size about ∼ 7.32 μm are obtained via the solvothermal reaction and selenization pyrolysis treatment, and then flexible free-standing BixSey@C/PEDOT: PSS (BSCP) composite films are obtained by a feasible vacuum filtration combined with cold pressing treatment, using different contents of BixSey@C content as inorganic component. Micrometer BixSey@C sheets are uniformly dispersed in the PEDOT:PSS matrix constructing bi-functional composite films with unique layered structure. When the MOFs-derived BixSey@C content is 70%, BSCP-70 composite film gets a power factor of 11.23 μW m−1 K−2 at 340 K. Meanwhile, the BSCP-70 composite film reaches the highest average total EMI shielding effectiveness (SET) value of 45.0 dB at only 41.9 μm thickness at X-band. Based on multi-physical properties of MOF-derived BixSey@C and PEDOT:PSS, flexible BixSey@C/PEDOT:PSS composite films display good application potentiality in the flexible TE devices and EMI shielding protection.

Monitoring the salt stability and solvent swelling behavior of PAH‐based polyelectrolyte multilayers by quartz crystal microbalance with dissipation

AbstractThis contribution is aimed to examine the layer stability and solvent swelling behavior of polyelectrolyte multilayers (PEMs) obtained from poly(allylamine hydrochloride) (PAH), poly(styrene sulfonic acid sodium salt) (PSS), and poly(acrylic acid) against different salt solutions using Quartz Crystal Microbalance with Dissipation in terms of the solution concentration, charge type of the top layer, and PEM structure. In general, all multilayers remain stable against MgCl2 and NaCl, phosphate buffer saline, ionic liquid, and solvents, namely methanol and heptane, while 4.5‐bilayered PAH‐PSS film displays partial layer decomposition against 1 M NaOCl. Additionally, it is found that the stability of Layer‐by‐Layer (LbL) films remains unaffected by the surface charge type, although variations in the adsorbed and desorbed amounts, as well as the viscoelastic properties, occur during the salt passage and rinsing steps. Along the salt exposure, changes in dissipation (ΔD) significantly increase because of the fast diffusion of ions through the multilayers but return to their initial value after washing. Especially high and reversible ΔD values of the PEMs against methanol are evaluated as swelling in methanol without chemical disintegration. This behavior can be attractive for solvent‐induced release behavior for the LbL‐assembled films or microcapsules.Highlights Multilayer stability and solvent swelling of PEMs are discussed using QCM‐D. PAH‐PSS films have the highest stability against salt solutions. PAH‐PAA films exhibited significant changes in dissipation values. PEMs did not show multilayer stability against NaOCl solution. (PAH‐PSS)5 film was stable and had swelling/de‐swelling capability against methanol.

Modified polymer electrolyte membrane for microbial fuel cell: Performance analysis, investigation on anti-biofouling effect, and microbial community analysis on biofouled membrane

Sulphonation is limited in Sulphonated Polyether Ether Ketone (SPEEK) due to its solubility in water beyond an extent. However, to enhance performance of polymer electrolyte membrane (PEM) in microbial fuel cell (MFC), more functional groups are required. To facilitate effective proton transfer, styrene sulphonic acid (SSA) is grafted onto SPEEK, resulting in SPEEK/SSA, to increase the number of functional groups. Based on membrane properties, 5 wt% SSA is found to be the optimum grafting for further filler addition. Copper oxide doped reduced graphene oxide (CuO@rGO) is used as membrane filler at various concentrations to enhance anti-biofouling effect. Swelling is excessive in SPEEK/SSA (30.2%), whereas it is only 17.3% in SPEEK/SSA+1.5 wt%CuO@rGO. As evidenced by the zone of inhibition assay, biofilm inhibition test, and Bradford protein assay, the membrane's anti-biofouling impact is improved by the inherent hydrophilicity of SPEEK/SSA and antibacterial activity of CuO@rGO. The MFC with 1.5 wt% CuO@rGO membrane shows highest maximum power density of 186 ± 5 mW m−2 and Chemical Oxygen Demand removal of 81.23%. Phylogenetic analysis on biofouled membrane shows the predominance of Pseudomonas, Acidovorax and Flavobacterium. The research demonstrates that despite biofouling, the synthesized grafted PEM exhibits high resistance to it and hence performs better.

Novel dry EEG electrode with composite filler of PEDOT:PSS and carbon particles.

We have developed a novel composite filler with Poly(3,4-ethylenedioxythiophene) : poly(styrenesulfonic acid) (PEDOT:PSS), a biocompatible organic conductive polymer, adsorbed on carbon particles for biological electrodes. This composite filler enables to fabricate high-performance biological electrodes simply by adding it to resin in the same way as conventional conductive fillers. The fabricated electrodes achieve ion exchange properties similar to those of PEDOT:PSS polymers and therefore low skin and electrode contact impedance. Electroencephalogram (EEG) measurements show that these electrodes capture various brain activities and exhibit high correlation (≥ 0.9) to commercially available wet and AgCl electrodes. Additionally, each electrode can be molded into various shapes and structures while retaining its electrode characteristics. Therefore, the proposed electrode is promising for EEG measurement, which requires high comfort and signal quality.

Highly Conductive and Reusable Cellulose Hydrogels for Supercapacitor Applications.

We report Na-Alginate-based hydrogels with high ionic conductivity and water content fabrication using poly (3,4-ethylene dioxythiophene) (PEDOT): poly (4-styrene sulfonic acid) (PSS) and a hydrogel matrix based on dimethyl sulfoxide (DMSO). DMSO was incorporated within the PEDOT:PSS hydrogel. A hydrogel with higher conductivity was created through the in-situ synthesis of intra-Na-Alginate, which was then improved upon by H2SO4 treatment. Field emission scanning electron microscopy (FESEM) was used to examine the surface morphology of the pure and synthetic hydrogel. Structural analysis was performed using Fourier-transform infrared spectroscopy (FTIR). Thermogravimetric analysis (TGA), which examines thermal properties, was also used. A specific capacitance of 312 F/g at 80 mV/s (energy density of 40.58 W/kg at a power density of 402.20 W/kg) at 100 DC mA/g was achieved by the symmetric Na-Alginate/PEDOT:PSS based flexible supercapacitor. The electrolyte achieved a higher ionic conductivity of 9.82 × 10-2 and 7.6 × 10-2 Scm-1 of Na-Alginate and a composite of Na-Alginate/PEDOT:PSS at 25 °C. Furthermore, the supercapacitor Na-Alginate/PEDOT:PSS//AC had excellent electrochemical stability by showing a capacity retention of 92.5% after 3000 continuous charge-discharge cycles at 10 mA current density. The Na- Alginate/PEDOT:PSS hydrogel displayed excellent flexibility and self-healing after re-contacting the two cut hydrogel samples of electrolyte for 90 min because of the dynamic cross-linking network efficiently dissipated energy. The illumination of a light-emitting diode (LED) verified the hydrogel's capacity for self-healing.

The Composite Material of (PEDOT-Polystyrene Sulfonate)/Chitosan-AuNPS-Glutaraldehyde/as the Base to a Sensor with Laccase for the Determination of Polyphenols.

The described research aimed to develop the properties of the conductive composite /poly(3,4-ethylenedioxy-thiophene-poly(4-lithium styrenesulfonic acid)/chitosan-AuNPs-glutaraldehyde/ (/PEDOT-PSSLi/chit-AuNPs-GA/) and to develop an electrochemical enzyme sensor based on this composite material and glassy carbon electrodes (GCEs). The composite was created via electrochemical production of an /EDOT-PSSLi/ layer on a glassy carbon electrode (GCE). This layer was covered with a glutaraldehyde cross-linked chitosan and doped with AuNPs. The influence of AuNPs on the increase in the electrical conductivity of the chitosan layers and on facilitating the oxidation of polyphenols in these layers was demonstrated. The enzymatic sensor was obtained via immobilization of the laccase on the surface of the composite, with glutaraldehyde as the linker. The investigation of the surface morphology of the GCE/PEDOT-PSSLi/chit-AuNPs-GA/Laccase sensor was carried out using SEM and AFM microscopy. Using EDS and Raman spectroscopy, AuNPs were detected in the chitosan layer and in the laccase on the surface of the sensor. Polyphenols were determined using differential pulse voltammetry. The biosensor exhibited catalytic activity toward the oxidation of polyphenols. It has been shown that laccase is regenerated through direct electron transfer between the sensor and the enzyme. The results of the DPV tests showed that the developed sensor can be used for the determination of polyphenols. The peak current was linearly proportional to the concentrations of catechol in the range of 2-90 μM, with a limit of detection (LOD) of 1.7 μM; to those of caffeic acid in the range of 2-90 μM, LOD = 1.9 μM; and to those of gallic acid in the range 2-18 μM, LOD = 1.7 μM. Finally, the research conducted in order to determine gallic acid in a natural sample, for which white wine was used, was described.

Fluorinated Sulfonated Poly(ether sulfone)‐Based Poly(3,4‐ethylenedioxythiophene) Dispersion: A Hole Transport Layer Material in Organic Solar Cells

AbstractHere the synthesis of poly(3,4‐ethylenedioxythiophene) (PEDOT) aqueous dispersion using sulfonated poly(ether sulfone) (SPES) with hydrophobic fluorinated groups to improve the weather and water stability of the conductive film is reported. The conductivity and surface morphology of the fabricated PEDOT:SPES conductive thin films are investigated. The PEDOT:SPES film after the N,N‐dimethylformamide (DMF) treatment showed a 200 times increase in the conductivity and the transmittance is over 96.5%. Raman spectroscopy indicates conformational changes in PEDOT chains due to the solvent treatment. The PEDOT:SPES film shows better water and weather stability performance in terms of dimensional stability in comparison to the commercial PEDOT:poly(styrene sulfonic acid) (PSS). Further, the organic solar cells performance is tested using PEDOT:SPES as hole transport layer and poly(3‐hexylthiophene) (P3HT):[6,6]‐phenyl C71‐butyric acid methyl ester (PC71BM) as active material. The PEDOT:SPES achieves a good power conversion efficiency (=3.36%), comparable with the conventional PEDOT:PSS (AI 4083).

Nylon fabric supported poly (styrene sulfonic acid) brush catalyst: A superior heterogeneous Brønsted acid catalyst with stable performance and facile recyclability

The development of highly efficient and easily recyclable heterogeneous catalysts is of great significance for green synthesis. By adopting a facile photoinduced grafting strategy, we have successfully developed fabric nylon-supported poly (styrene sulfonic acid) brush catalyst which can serve as efficient and recyclable Brønsted acid catalyst. The fabric-supported catalyst was prepared from commercially available nylon nonwoven fabric, and characterized by XPS, FTIR, EA, SEM and Hammett acidity. Results obtained indicate that the fabric catalyst possesses high catalytic activity for the condensation of anthranilamide with aldehydes or ketones in ethanol (15 examples yields 90–97%), as well as the advantage to be easily recycled and reused, with superior stability and catalytic activity even after 15 runs. What's more, application of the fabric catalyst for scale-up synthesis of pharmaceutical molecule NSC-145669 further demonstrated its promising potential in industrial production. Attractively, this method could be easily extended to various olefin-containing monomers and thus provided a general strategy for designing textile catalysts.

Engineering of Solvation Entropy by Poly(4-styrenesulfonic acid) Additive in an Aqueous Electrochemical System for Enhanced Low-Grade Heat Harvesting.

The thermally regenerative electrochemical cycle (TREC) is a reliable and efficient approach to converting low-grade heat into electricity. A high temperature coefficient (α) is the key to maximize the energy conversion efficiency of the TREC system. In this study, we present significant improvement of α of a Prussian blue analogue (PBA)-based electrochemical cell by adding poly(4-styrenesulfonic acid) (PSS) to the electrolyte. Raman spectra showed that water-soluble charged polymers strongly affect the ion hydration structure and increase the entropy change (ΔS) during ion intercalation in PBA. A large α of -2.01 mV K-1 and high absolute heat-to-electricity conversion efficiency up to 1.83% was achieved with a TREC cell in the temperature range 10-40 °C. This study provides a fundamental understanding of the origin of α and a facile method to boosting the temperature coefficient for building a highly efficient low-grade heat harvesting system.

Desalination performance of fabric-structured charged mosaic membrane prepared from poly(vinyl alcohol)-based charged fibers

Charged mosaic (CM) membranes were prepared from fabric structures using two types of poly(vinyl alcohol) (PVA)-based fibers. The fibers were fabricated using anionic and cationic block-type PVA, poly(vinyl alcohol-b-sodium styrene sulfonic acid), and poly(vinyl alcohol-b-vinylbenzyl trimethylammonium chloride). The fabrics were heat pressed to form a nonporous film and crosslinked with glutaraldehyde (GA) to produce fabric-structured CM membranes. Volume flux experiments indicated that the CM membrane exhibited negative osmosis, whereas the uncharged PVA membrane showed positive osmosis. The CM membrane made from the fabric exhibited sufficient mechanical strength for performing a piezodialysis experiment under a pressure of 0.3 MPa. The analytical results of piezodialysis experiments for the CM membrane indicated that the salt flux increased, whereas the water flux remained constant with an increasing initial NaCl concentration. Therefore, the salt-to-water flux ratio increased with increasing NaCl concentration. The CM membrane was desalinated with up to 1500 ppm of NaCl at a pressure of 0.3 MPa. Consequently, the fabricated CM membranes demonstrated the potential for desalinating low-salinity solutions.

Vaterite-nanosilver hybrids with antibacterial properties and pH-triggered release

Silver nanoparticles (AgNPs) have been used for over a century in various applications due to their distinctive properties. Nonetheless, the poor stability of AgNPs and adverse effects on living organisms have driven the search for materials able to protect and better control their release. Vaterite CaCO3 crystals have been studied in the last two decades as carriers for different drugs due to their biocompatibility, easy synthesis and pH-sensitive properties. Herein, AgNPs were loaded into vaterite to protect, store, and control their release, resulting in CaCO3/AgNPs hybrids. To tune the release of the AgNPs, the recrystallization of the hybrids into thermodynamically more stable calcite was studied and modulated with carboxymethyl–dextran (DexCM) and poly(4-styrenesulfonic acid) sodium salt (PSS), with the last one being able to stabilise the hybrids and prevent a premature release of the AgNPs at low contents (2%, w/w). The release of AgNPs from the hybrids was studied at pH 5 to 9, showing a pH-dependent release suppression for PSS-stabilised hybrids. Various mathematical models were applied to clarify the release mechanism, confirming the role of PSS in stabilising and targeting the release of AgNPs. The antibacterial studies demonstrated that the hybrids protect the AgNPs without affecting their activity, with the released nanoparticles being effective against Escherichia coli, methicillin-resistant Staphylococcus aureus and Pseudomonas aeruginosa. Overall, this work sheds light on the release mechanisms of AgNPs from the inorganic hybrids helping to foresee the release profiles of other compounds from vaterite.

Poly(styrene sulfonic acid)-Grafted Carbon Black Synthesized by Surface-Initiated Atom Transfer Radical Polymerization.

Owing to their excellent electrical conductivity and robust mechanical properties, carbon-based nanocomposites are being used in a wide range of applications and devices, such as electromagnetic wave interference shielding, electronic devices, and fuel cells. While several approaches have been developed for synthesizing carbon nanotubes and carbon-black-based polymer nanocomposites, most studies have focused on the simple blending of the carbon material with a polymer matrix. However, this results in uncontrolled interactions between the carbon filler and the polymer chains, leading to the agglomeration of the carbon filler. Herein, we report a new strategy for synthesizing sulfonated polystyrene (PSS)-grafted carbon black nanoparticles (NPs) via surface-initiated atom-transfer radical polymerization. Treatments with O2 plasma and H2O2 result in the effective attachment of the appropriate initiator to the carbon black NPs, thus allowing for the controlled formation of the PSS brushes. The high polymeric processability and desirable mechanical properties of the PSS-grafted carbon black NPs enable them suitable for use in nonfluorinated-hydrocarbon-based polymer electrolyte membranes for fuel cells, which must exhibit high proton conductivity without interrupting the network of channels consisting of ionic clusters (i.e., sulfonic acid moieties).

ТЕРМООКИСЛИТЕЛЬНАЯ УСТОЙЧИВОСТЬ ПРОТОНООБМЕННЫХ МЕМБРАН НА ОСНОВЕ СОПОЛИМЕРОВ СТИРОЛСУЛЬФОКИСЛОТЫ И N-ВИНИЛИМИДАЗОЛА

The differential scanning colorimetry (DSC) thermooxidative stability of new copolymers of styrene-sulfonic acid and N-vinylimidazole obtained by radical copolymerization in a DMF solution in an argon atmosphere has been studied

Optical and electrical properties of poly(4-styrenesulfonic acid)-polyacrylic acid polyelectrolyte brushes incorporating with potassium permanganate

In this work, the effect of potassium permanganate (KMnO4) on the optical and electrical properties of poly(4-styrenesulfonic acid)-polyacrylic acid polyelectrolyte brushes (PSS-PAA PEBs) was investigated. In addition, PSS-PAA/KMnO4 PEBs were modified by connecting a fraction of carboxylic groups with thiol functional groups that bind to the substrate with covalent bonds. IR vibrational bands confirm the formation of thiolated PSS-PAA/KMnO4 PEBs into the ITO substrate. In addition, introducing KMnO4 into the PSS-PAA matrix leads to converting the stretched brushes to collapsed brushes and increasing the roughness from 0.36 to 0.58 nm upon increasing KMnO4 from 0 to 4 wt.%. Introducing KMnO4 into PSS-PAA PEBs decreases the transmittance values as well as increases the extinction coefficient values within the visible region. The bandgap energy of PSS-PAA/KMnO4 PEBs decreases from 3.82 to 3.54 eV as KMnO4 concentration increases from 0 to 4 wt.%. In addition, increasing KMnO4 concentration in PSS-PAA/KMnO4 PEBs changes the PEBs from stretched to collapsed brushes and consequently increases the Urbach energy values from 0.20 to 0.35 eV. Finally, the electrical conductivity of PSS-PAA/KMnO4 PEBs increases gradually from 4.05 × 10−6 S.cm−1 to 5.81 × 10−4 S.cm−1 as KMnO4 concentration increases from 0 to 4 wt.%.

Efficient method for fabrication of reusable printed organic electrochemical transistors for liquid sensors based on the complex of poly(3,4-ethylenedioxythiophene) with poly(styrenesulfonic acid)

Efficient method for fabrication of reusable printed organic electrochemical transistors for liquid sensors based on the complex of poly(3,4-ethylenedioxythiophene) with poly(styrenesulfonic acid)

Polyvinyl alcohol/poly(3,4-ethylenedioxythiophene): poly(styrenesulfonic acid)/copper (II) oxide nanocomposites as high performance dielectric materials for energy storage applications

Polyvinyl alcohol/poly(3,4-ethylenedioxythiophene): poly(styrenesulfonic acid)/copper (II) oxide nanocomposites as high performance dielectric materials for energy storage applications

Rapid, Highly-Efficient and Selective Removal of Anionic and Cationic Dyes from Wastewater Using Hollow Polyelectrolyte Microcapsules

Herein, poly (allylamine hydrochloride) (PAH)/ poly (styrene sulfonic acid) sodium salt (PSS) microcapsules of (PAH/PSS)2PAH (P2P MCs) and (PAH/PSS)2 (P2 MCs) were obtained by a layer-by-layer method. The P2 MCs show high adsorption capacity for Rhodamine B (642.26 mg/g) and methylene blue (909.25 mg/g), with an extremely low equilibrium adsorption time (~20 min). The P2P MCs exhibited high adsorption capacities of reactive orange K-G (ROKG) and direct yellow 5G (DY5G) which were 404.79 and 451.56 mg/g. Adsorption processes of all dyes onto microcapsules were best described by the Langmuir isotherm model and a pseudo-second-order kinetic model. In addition, the P2P MCs loaded with reactive dyes (P2P-ROKG), could further adsorb rhodamine B (RhB) dye, and P2 MCs that had adsorbed cationic MB dyes could also be used for secondary adsorption treatment of direct dye waste-water, respectively. The present work confirmed that P2P and P2 MCs were expected to become an excellent adsorbent in the water treatment industry.

Microscopic Determination of the Local Hydration Number of Polymer Electrolyte Membranes Using SANS Partial Scattering Function Analysis.

The conventional hydration number, λ, of a polymer electrolyte membrane (PEM) is estimated by the gravimetric measurement of the total water uptake in the membrane. This is the overall water molecules divided by the number of ionic groups covering the water distribution from the macroscale to the molecular level. For a more precise evaluation of the local ion-water interactions and ion transport efficiency in hydrophilic channels, in contrast to λ, we here propose an index, local hydration number (λlocal), defined as the number of water molecules located adjacent to and interacting with ionic groups in a PEM, per ionic group in the hydrophilic channels. We introduce an experimental method using partial scattering function analysis through a contrast-variation small-angle neutron scattering technique to precisely determine λlocal at the micro- (nano-) scale to the molecular level for PEMs. When applied to the benchmark material Nafion and the well-studied radiation-grafted PEM, consisting of poly(styrene sulfonic acid) grafted onto poly(ethylene-co-tetrafluoroethylene) (ETFE-g-PSSA), the obtained λlocal was close to the conventional λ. This means all water molecules interacted with sulfonic acid groups, which is much different from the case of anion-type grafted PEMs. Comparing the λlocal value obtained in this study with the conventional λ value confirmed that water existed only in nanostructured hydrophilic channels in these PEMs. The result of this work provides a route to understand local molecular structures of high-performing PEMs for energy conversion applications.

Hydroxypropyl methyl cellulose reinforced conducting polymer hydrogels with ultra-stretchability and low hysteresis as highly sensitive strain sensors for wearable health monitoring

Conducting polymer hydrogels have emerged as promising materials to fabricate highly sensitive strain sensors. However, due to weak bindings between conducting polymer and gel network, they usually suffer from limited stretchability and large hysteresis, failing to achieve wide-range strain sensing. Herein, we combine hydroxypropyl methyl cellulose (HPMC), poly (3,4-ethylenedioxythiophene):poly (styrene sulfonic acid) (PEDOT: PSS) with chemically cross-linked polyacrylamide (PAM) to prepare a conducting polymer hydrogel for strain sensors. Owing to abundant hydrogen bonds between HPMC, PEDOT:PSS and PAM chains, this conducting polymer hydrogel exhibits high tensile strength (166 kPa), ultra-stretchability (>1600 %) and low hysteresis (<10 % at 1000 % cyclic tensile strain). The resultant hydrogel strain sensor shows ultra-high sensitivity, wide strain sensing ranges of 2–1600 %, and excellent durability and reproducibility. Finally, this strain sensor can be used as wearable sensor to monitor vigorous human movement and fine physiological activity, and services as bioelectrodes for electrocardiograph and electromyography monitoring. This work provides new horizons to design conducting polymer hydrogels for advanced sensing devices.

Ion‐Conducting Non‐Flammable Liquid Crystal–Polymer Composites for High‐Frequency Soft Actuators

AbstractHigh‐frequency actuators are reported based on non‐flammable lithium‐ion conducting phosphate liquid crystal–polymer composite electrolytes, which exhibit a bending response at frequencies up to 80 Hz under an AC voltage of 2 V, owing to its high ionic conductivity reaching 10−4 S cm−1 at room temperature. An equimolar complex of a phosphate‐containing mesogenic molecule and lithium bis(trifluoromethylsulfonyl)imide through the ion‐dipole interactions induced a room‐temperature smectic A liquid‐crystalline (LC) phase forming 2D ion‐transport pathways comprising the 2D array of the phosphate moieties. A blend of 80 wt% LC electrolyte and 20 wt% polymers (poly(vinyl chloride) and poly(vinylidene fluoride‐co‐hexafluoropropylene)) formed a flexible, mechanically robust LC–polymer composite film. Scanning electron microscopy and white light interference microscopy revealed a microphase‐segregated structure consisting of a continuous LC phase and a porous polymer matrix. In addition, the continuity of porous structure across the film is confirmed by permeation experiments of solvents thorough the membrane with a homemade filter in a dead‐end filtration mode. The LC–polymer composite film sandwiched between two poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonic acid) electrodes is found to simultaneously exhibit high bending strain (0.63%) and high output force (0.35 mN), owing to the high ion migration into the composite electrolyte and electrode.