Ion Conducting Polymer Electrolyte Research Articles

Preparation and characterization of lithium ion conducting polymer electrolytes based on a blend of poly(vinylidene fluoride-co-hexafluoropropylene) and poly(methyl methacrylate).

Ion conducting polymer electrolytes composed of poly(vinylidene fluoride-co-hexafluoropropylene) (PVdF-HFP), poly(methyl methacrylate) (PMMA) and lithium triflate (LiTf) were prepared using the solution casting method. Structural change and complex formation in the blend electrolyte systems were confirmed from the X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy and scanning electron microscopy (SEM) studies. Thermal properties of the samples were investigated by the differential scanning calorimetry (DSC) technique. The ionic conductivity of these polymer electrolytes was studied by impedance spectroscopy at various temperatures ranging from 303–393 K. The results reveal that the ionic conductivity of the polymer blend electrolytes depends on the PVdF-HFP:PMMA composition as well as the temperature. Maximum room temperature conductivity of S cm−1 was achieved with 22.5 wt.% PMMA. The blending of PVdF-HFP with PMMA improved the thermal stability and ionic conductivity of the polymer electrolyte. Estimated transference numbers suggest the charge transport is predominantly ionic.

A simple route toward next-gen green energy storage concept by nanofibres-based self-supporting electrodes and a solid polymeric design

A novel, unique, truly-solid Li-ion cell structural design, based on LiFePO4/graphite electrodes and profoundly ionic conducting polymer electrolyte, is fabricated by exploiting, for the first time, carbonised cellulose nanofibrils as both the conductive binder and the current collector substrate. Moreover, cellulose nanofibrils are used as reinforcing additive for the preparation of the unconventional composite polymer electrolyte separator. The resulting solid polymeric lab-scale Li-ion cell, assembled in a “pouch cell” envelop, shows remarkably stable characteristics upon prolonged cycling at ambient temperature even at high current regimes. By the way, a simple procedure, easily scalable, is optimized for the spray coating and water-based papermaking. As a result, all components can be fully recovered at the end of the cell operational life by taking advantage of a simple water-based paper recycling technique, opening new horizons for the manufacture of sustainable electrochemical energy storage devices.

Correlation Between Solvation Structure and Ion-Conductive Properties of Highly-Concentrated Poly(ethylene carbonate)-Based Electrolytes

Ion-conductive solid polymer electrolytes (SPEs) are of great interest as key materials to realizing safe and flexible rechargeable batteries, particularly Li batteries. Since the discovery of ionic conductions in poly(ethylene oxide) (PEO)/metal salt complexes, numerous efforts have been made to improve their electrochemical properties. However, it is difficult to increase Li-ion conductivity that is the product of overall conductivity and Li transference number (t +). This drawback mainly arises from excessively tight complex structures between polar polymers and Li ion. To overcome the drawback and create all-solid-state batteries based on SPEs, we specifically focus on poly(alkylene carbonate)s derived from CO2/epoxide copolymerization as SPE polymer hosts [1,2]. Consequently, we have found an unusual ion-conductive behavior of poly(ethylene carbonate) (PEC)-based electrolyte, including high ionic conductivity of highly-concentrated electrolytes and extremely high t +, which in some cases is above 0.8 [3,4]. In this PEC-based electrolyte system, ionic conductivity continues to increase with increasing salt concentration, which is a behavior scarcely shown in conventional electrolyte systems. In addition, we have already confirmed operations of prototype Li/LiFePO4 cells based on PEC-based electrolytes combined with plasticizing and reinforcing additives [5,6]. In this context, we considered that elucidation of salt solvation structure is a key to better understanding the origin of the particular ion-conductive behavior, and improving the performance further. In the present study, we adopted spectroscopic studies including FT-IR, Raman spectroscopy, and solid-state 7Li magic angle spinning (MAS) NMR for PEC/lithium bis(fluorosulfonyl)imide (LiFSI) electrolytes with varying concentration. The FT-IR and Raman spectroscopy indicate that most FSI ions interact with more than one Li ion at high concentration region, which is referred to as aggregates, while C=O groups dissociates the salt. The 7Li MAS NMR suggested that a relatively weak contact between Li ions and FSI ions withdraws Li ions from a strong interaction with C=O groups. We conclude that this moderate complex structure, where C=O groups allows the highly concentrated ions to remain amorphous and mobile, leads to reasonable conductivity with extremely high t +. We believe that this finding will provide a new insight for developing SPEs having both high conductivity and high t + simultaneously.

A Single-Lithiun-Ion Conductor Coordinated Porous Pvfm-Peg Based Membrane and Plasticizer As Electrolyte for Lithium Ion Batteries

Polymer electrolyte comprised of lithium dissolved in polymer matrix has draw great attention due to its safety as well as processability, flexibility and lightweight. The dissociation of binary lithium salt in polar polymer matrix gives rise to so called bi-ionic conductors in which both cations and anions migrate as charge carriers. But unfortunatelly, a serious concentration polarization takes place in bi-ionic conductors due to the buildup of the anions at the electrode/electrolyte interface[1]. In order to solve the above problem, a single ion conductive polymer electrolyte has been proposed, in which the counter anions are tethered to the polymer backbone or immobilized in a matrix, eliminating polarization loss and enabling the passage of larger currents through the cells[2]. Until recently, single ion polymer electrolytes reported show low ambient temperature ionic conductivities (<10-6S·cm-1) due to the strong interaction between cations and their immobile matrixes[3]. A single-ion conductive hybrid electrolyte of porous PVFM-PEG based membrane and the optimized PC/EC (1/1, vol) mixed solvent as plasticizer was fabricated. The membrane and its electrolyte were characterized using scanning electron microscopy (SEM), stress-stain test, linear sweep voltammetry (LSV), ionic conductivity and lithium ion transference number measurement. The results indicate the combination of optimized PC/EC (1/1 in vol) plasticizer and porous PVFM-PEG based membranes[4] contributes to a considerable enhancement of room-temperature conductivity to 1.59×10-4S/cm. At the same time, lithium ion transference number of hybrid electrolyte based on the porous PVFM-PEG electrolyte membranes increased to 0.76. The assembled cells from the hybrid electrolyte also show wide electrochemical stability window and excellent cyclability.Reference [1] Bouchet R, Maria S, Meziane R, et al. Single-ion BAB triblock copolymers as highly efficient electrolytes for lithium-metal batteries[J]. Nature materials, 2013, 12(5): 452-457. [2] Sinha K, Wang W, Winey K I, et al. Dynamic Patterning in PEO-Based Single Ion Conductors for Li Ion Batteries[J]. Macromolecules, 2012, 45(10): 4354-4362. [3] Kobayashi N, Uchiyama M, Tsuchida E. Poly [lithium methacrylate-co-oligo (oxyethylene) methacrylate] as a solid electrolyte with high ionic conductivity[J]. Solid State Ionics, 1985, 17(4): 307-311. [4] Fang Lian, Hong-yan Guan, Yan Wen, Xiao-rong Pan, Polyvinyl formal based single-ion conductor membranes as polymer electrolyte for lithium ion batteries, Journal of membrane science 2014, 469, 67-72

Computer Simulations of Ion Transport in Polymer Electrolyte Membranes

Understanding the mechanisms and optimizing ion transport in polymer membranes have been the subject of active research for more than three decades. We present an overview of the progress and challenges involved with the modeling and simulation aspects of the ion transport properties of polymer membranes. We are concerned mainly with atomistic and coarser level simulation studies and discuss some salient work in the context of pure binary and single ion conducting polymer electrolytes, polymer nanocomposites, block copolymers, and ionic liquid-based hybrid electrolytes. We conclude with an outlook highlighting future directions.

Electrochemical and mechanical properties of polyolefin hard segment with polyethylene oxide conductive phase block copolymers

A high lithium ion conductivity polymer electrolyte with excellent mechanical properties was developed in a polyolefin hard segment with a polyethylene oxide conducting phase block copolymer (OEO) and tetraethylene glycol dimethyl ether (G4) composite polymer with lithium bis(fluorosulfonyl)imide (LiFSI). The effect of the modulus of polymers on the ionic conductivity is generally controversial; high ion conducting polymer electrolyte typically exhibit poor mechanical properties. The composite polymer electrolytes developed in this study have ion conductivities in the range of 10−5 to 4×10−4Scm−1 and tensile strengths in the range of 1 to 12MPa at room temperature. 10OEO-1.4LiFSI-2.5G4, where OEO is based on ethylene oxide (EO) units, has ionic conductivity of 1.3×10−4Scm−1 and tensile strength of 5.1MPa at room temperature. The high G4 content composite of 10OEO-3.0LiFSI-4.0G4 has a high ion conductivity of 4.0×10−4Scm−1, but a low tensile strength of 1.0MPa at room temperature. The OEO-LiFSI-G4 composite polymer with high conductivity and high tensile strength is an attractive candidate for the electrolyte in lithium polymer batteries.

A study of structural, electrical and electrochemical properties of PVdF-HFP gel polymer electrolyte films for magnesium ion battery applications

New magnesium ion conducting polymer electrolyte films are developed and their experimental investigations are reported. The polymer electrolyte films are composed of various poly(vinylidene fluoride-co-hexafluoropropylene):magnesium trifluoromethanesulfonate compositions (PVdF-HFP:Mg(Tf)2 in weight ratio) with different quantities of 1-ethyl-3-methylimidazolium trifluoromethanesulfonate ionic liquid (EMITf). X-ray diffraction reveals that the pristine PVdF-HFP polymer film possesses a semi-crystalline structure and its amorphicity increases with increasing Mg(Tf)2 and EMITf concentrations. From thermal analysis, the melting temperature (Tm), relative crystallinity (χc) and thermal stability of the 90PVdF-HFP:10Mg(Tf)2 gel polymer electrolyte film doped with 40wt.% EMITf are obtained as 112°C, 21.8% and 355°C, respectively. The room-temperature ionic conductivity of the gel polymer electrolyte film increases with increasing EMITf concentration and reaches a high value of approximately 4.63×10−3Scm−1 at 40wt.% EMITf due to its amorphicity increase and interconnected pore structure. For the 40wt.% EMITf electrolyte film, the temperature dependence of ionic conductivity follows the Arrhenius relation with an activation energy of 0.35eV. The electrochemical stability window of the 40wt.% EMITf electrolyte film is determined as ∼4.8V. The findings from this study are promising and have great potential for practical ionic device applications, particularly in rechargeable magnesium ion batteries.

Structural, electrical conductivity, and transport analysis of PAN–NH4Cl polymer electrolyte system

Poly (acrylonitrile) (PAN) and ammonium chloride (NH4Cl)-based proton conducting polymer electrolytes with different compositions have been prepared by solution casting technique. The amorphous nature of the polymer electrolytes has been confirmed by XRD analysis. The FTIR analysis confirms the complex formation of the host polymer (PAN) with the salt (NH4Cl). DSC measurements show a decrease in Tg with the increase in salt concentration. The conductivity analysis shows that the 25 mol% ammonium chloride doped polymer electrolyte has a maximum ionic conductivity, and it has been found to be 6.4 × 10−3 Scm−1, at room temperature. The temperature dependence of conductivity of the polymer electrolyte complexes appears to obey the Arrhenius nature. The activation energy (Ea = 0.23 eV) has been found to be low for 25 mol% salt doped polymer electrolyte. The dielectric behavior has been analyzed using dielectric permittivity (e*), and the relaxation frequency (τ) has been calculated from the loss tangent spectra (tan δ). Using this maximum ionic conducting polymer electrolyte, the primary proton conducting battery with configuration Zn + ZnSO4·7H2O/75 PAN:25 NH4Cl/PbO2 + V2O5 has been fabricated and their discharge characteristics have been studied.

A mechanically robust porous single ion conducting electrolyte membrane fabricated via self-assembly

A polymer elctrolyte with high porosity and good mechanical strength plays a critical role in improving the compatibility between the electrolyte and the electrodes in a battery device by raising the ionic conductivity and enhancing the cyclic performance. Here, we present a facile self-assembly technique to fabricate a single ion conducting polymer electrolyte membrane with appropriate porosity and strong mechanical strength by taking advantage of the poor physical compatibility between the rigid aromatic backbone of the polymer electrolyte and the flexible aliphatic poly(vinylidene fluoride-hexafluoropropylene) used as a binder. The influence of membrane porosity on ionic conductivity and interfacial contacts between the polymer electrolyte and electrodes was investigated. Excellent battery performance at both room temperature and 60°C was demonstrated.

High rate lithium-sulfur battery enabled by sandwiched single ion conducting polymer electrolyte.

Lithium-sulfur batteries are highly promising for electric energy storage with high energy density, abundant resources and low cost. However, the battery technologies have often suffered from a short cycle life and poor rate stability arising from the well-known “polysulfide shuttle” effect. Here, we report a novel cell design by sandwiching a sp3 boron based single ion conducting polymer electrolyte film between two carbon films to fabricate a composite separator for lithium-sulfur batteries. The dense negative charges uniformly distributed in the electrolyte membrane inherently prohibit transport of polysulfide anions formed in the cathode inside the polymer matrix and effectively blocks polysulfide shuttling. A battery assembled with the composite separator exhibits a remarkably long cycle life at high charge/discharge rates.

AC Impedance Studies on Magnesium Ion Conducting Polymer Electrolyte System with Ethylene Carbonate as Plasticizer and MgO as Nanofiller

AC Impedance Studies on Magnesium Ion Conducting Polymer Electrolyte System with Ethylene Carbonate as Plasticizer and MgO as Nanofiller

Enhanced performance of dye-sensitized solar cell using 2-mercaptobenzothiazole-doped poly(vinylidinefluoride-co-hexafluoropropylene) polymer electrolyte

The effect of 2-mercaptobenzothiazole (2-MCBT) on the performance of poly(vinylidinefluoride-co-hexafluoropropylene)/KI/I2 (PVDF-HFP/KI/I2) electrolyte in dye-sensitized solar cell (DSSC) was studied. The pure and 2-MCBT-doped PVDF-HFP/KI/I2 electrolytes were prepared by solution casting technique using N,N-dimethyl formamide (DMF) as a solvent. The characteristic properties of the as-prepared polymer electrolyte films were examined using various techniques such as Fourier transform infrared (FTIR) spectroscopy, X-ray diffractometer (XRD), AC-impedance analysis, and scanning electron microscopy (SEM) analysis. The ionic conductivity of polymer electrolytes was determined using AC-impedance analysis. The room temperature ionic conductivity of pure and 2-MCBT-doped PVDF-HFP/KI/I2 electrolytes were found to be 7.08 × 10−6 and 5.96 × 10−5 Scm−1, respectively. The increase in ionic conductivity of 2-MCBT-doped electrolyte may be due to the increase of both amorphous nature and iodide ion mobility of the polymer electrolyte. The photovoltaic studies, using pure and 2-MCBT-doped PVDF-HFP/KI/I2 electrolyte in DSSC showed an increase of power conversion efficiency from 1.74 to 3.46 % under the light intensity of 60 mW/cm2. Thus, the 2-MCBT-doped polymer electrolyte has been found to be a suitable material for DSSC applications.

Structural and Electrical Conductivity studies of pure PVA and PVA doped with Succinic acid polymer electrolyte system

An ion conducting polymer electrolyte based on poly (vinyl alcohol) PVA complexed with Succinic acid is prepared using solution cast technique. The structural properties of PVA and complexed electrolytes are studied using XRD and FTIR techniques. The results of XRD reveal that with the increase of Succinic acid concentration, the amorphous nature of PVA Polymer matrix increases. FTIR spectra studies for pure and complexed electrolytes reveal the vibrational changes that occur due to the effect of dopant in the polymer. The dc conductivity of these composite electrolytes has been studied. The dc conductivity of PVA is found to be increasing as the concentration of Succinic acid increases.

Bifunctional Ion-Conducting Polymer Electrolyte for the Vanadium Redox Flow Battery with High Selectivity

The need for electrochemical energy storage increases along with the growing share of fluctuating renewables for power generation. The all-vanadium redox flow battery (VRB) has experienced increasing attention in this context. Its electrolyte membrane is a key component, yet currently perfluorinated materials (e.g., Nafion) are mainly used in VRBs, which have neither been designed for this particular application, nor are they cost-effective. The cross-over of redox active vanadium species impairs cell efficiency, in particular in case of thin Nafion membranes with low ohmic resistance. Here, we present a potentially generic concept of a bifunctional ion-conducting membrane prepared by radiation grafting with sulfonic acid proton exchange sites and amidoxime moieties. The crossover of vanadium-ions is reduced four-fold in the presence of amidoxime groups without markedly impairing the conductivity of the membrane. A VRB cell containing such membrane shows increased energy efficiency and negligible capacity fading over 122 charge / discharge cycles compared to cells with Nafion membrane, which showed a loss of discharge capacity of around 35% after 35 cycles and considerable electrolyte imbalance.

Investigation of ionic liquid-doped ion conducting polymer electrolytes for carbon-based electric double layer capacitors (EDLCs)

Ionic liquid-based poly(vinyl alcohol) (PVA)/ammonium acetate (CH3COONH4) ion conducting polymer electrolytes are prepared by solution casting technique. Ionic liquid, 1-butyl-3-methylimidazoliumtrifluoromethanesulfonate (BmImTf) is then added to increase the ionic conductivity of polymer electrolytes by reducing the glass transition temperature (Tg).It is found that ionic conductivity of polymer electrolytes increases with temperature. The polymer electrolytes are found to obey the Vogel–Tamman–Fucher (VTF) rule in the conduction mechanism which is related to free volume model. Subsequently, two symmetrical electrodes containing activated carbon, carbon black and carbon nanotubes (CNT) are prepared through the dip coating method. Electric double layer capacitors (EDLCs) are then assembled using these electrodes and polymer electrolytes. Excellent electrochemical properties such as higher specific capacitance were obtained for EDLC comprising ionic liquid–doped polymer electrolytes. Power density of 18.37kWkg−1 was obtained for the EDLC containing the most conducting ionic liquid–added polymer electrolyte.

Toward ambient temperature operation with all-solid-state lithium metal batteries with a sp3 boron-based solid single ion conducting polymer electrolyte

The ionic conductivity decay problem of poly(ethylene oxide) (PEO)-based solid polymer electrolytes (SPEs) when increase the lithium salt of the SPEs up to high concentration is here functionally overcome by the incorporation of a charge delocalized sp3 boron based single ion conducting polymer electrolyte (SIPE) with poly(ethylene oxide) to fabricate solid-state sp3 boron based SIPE membranes (S-BSMs). By characterizations, particularly differential scanning calorimeter (DSC) and ionic conductivity studies, the fabricated S-BSMs showed decreased melting points and increased ionic conductivity as steadily increase the content of sp3 boron based SIPE, which significantly improved the low temperature performance of the all-solid-state lithium batteries. The fabricated Li | S-BSMs | LiFePO4 cells exhibit highly electrochemical stability and excellent cycling at temperature below melting point of PEO, which has never been reported so far for SIPEs based all-solid-state lithium batteries.

Hematite Fe&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;3&lt;/sub&gt; Nanoparticles Incorporated Polyvinyl Alcohol Based Polymer Electrolytes for Dye-Sensitized Solar Cells

Influence of hematite iron oxide nanoparticles (α-Fe2O3 NPs) on ionic conductivity of polyvinyl alcohol/KI/I2 (PVA/KI/I2) polymer electrolytes was investigated in this work. The pure and different weight percentage (wt %) ratios (2, 3, 4 and 5 % with respect to PVA) of α-Fe2O3 NPs incorporated PVA/KI/I2 polymer electrolyte films were prepared by solution casting method using DMSO as solvent. The prepared polymer electrolyte films were characterized by Fourier transform infrared (FT-IR) spectroscopy, X-ray diffractometer (XRD) and alternating current (AC)-impedance analysis. The AC-impedance studies revealed a significant increase in the ionic conductivity of α-Fe2O3 NPs incorporated PVA/KI/I2 polymer electrolytes than compared to pure PVA/KI/I2. This incorporated polymer electrolytes reduces the crystallinity of the polymer and enhance the mobility of I-/I3- redox couple, thereby increasing the ionic conductivity of polymer electrolytes. The highest ionic conductivity of 1.167 × 10-4 Scm-1 was observed for 4 wt % of α-Fe2O3 NPs incorporated PVA/KI/I2 polymer electrolyte. Also, the dye sensitized solar cell (DSSC) fabricated with this electrolyte showed an enhanced power conversion efficiency of 3.62 % than that of pure PVA/KI/I2 electrolyte (1.51 %). Thus, the synthesized α-Fe2O3 NPs added polymer electrolyte can be serve as a suitable material for dye sensitized solar cell application studies.

Multiscale Model of Proton Transport in Perfluorosulfonic-Acid Membrane

To optimize polymer-electrolyte-fuel-cell performance, it is critical to improve transport properties of the polymer membrane. The typical fuel-cell membrane is a perfluorosulfonic-acid ionomer that consists of a hydrophobic backbone with hydrophilic side chains terminated by a sulfonic acid group. The polymer phase separates into hydrophilic domains that are on the order of nanometers and enables water and proton transport around the surrounding hydrophobic matrix that provides structural integrity. Although there have been concerted efforts to use molecular-level theory and simulations to understand ion and water transport inside a single pore, there is a need to develop a robust multiscale methodology to bridge molecular descriptors through mesoscale structures to macroscopic properties. In this poster, we present a methodology for such an approach. Building on previous multiscale modeling efforts1, we use a resistor-network paradigm to describe ionomers as a network of conductive nodes and throats. The effective network resistance is a function of the connectivity of the network and transport resistance between each neighboring node. We use common imaging methods to extract the network geometry from direct imaging of the ionomer2. Molecular theory and simulations are used to describe and calculate the proton conductivity in throats as a function of size. Kirchhoff's circuit laws are applied on each node in the system and the effective resistance across the membrane is determined for ion conduction. Once designed, a poroelastic model is used to change node and throat sizes and subsequent network connectivity with water content and swelling. Acknowledgements This work was funded by the Assistant Secretary for Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office, of the U. S. Department of Energy under contract number DE-AC02-05CH11231 and by a National Science Foundation Graduate Research Fellowship under Grant No. DGE 1106400 Citations [1] J. T. Gostick and A. Z. Weber, “Resistor-Network Modeling of Ionic Conduction in Polymer Electrolytes,” Electrochimica Acta. [2] F. I. Allen, L. R. Comolli, A. Kusoglu, M. A. Modestino, A. M. Minor, and A. Z. Weber, “Morphology of Hydrated As-Cast Nafion Revealed through Cryo Electron Tomography,” ACS Macro Lett., vol. 4, no. 1, pp. 1–5, Jan. 2015. Figure 1. 3D projection of pore-network generated from skeletonization of cryo-TEM tomography image of Nafion ionomer. The green cylinders show throats of the hydrophilic network connecting nodes, shown as red balls. The background is a cutaway of the network where blue is the hydrophilic domain and black the hydrophobic backbone. Figure 1

Electrical and structural studies of ionic liquid-based poly(vinyl alcohol) proton conductors

Ionic liquid-based proton conducting polymer electrolytes containing poly(vinyl alcohol) (PVA), ammonium acetate (CH3COONH4) and 1-butyl-3-methylimidazolium bromide (BmImBr) are prepared and investigated in this present work. The ionic conductivity of polymer electrolytes increases with temperature as shown in temperature dependent-ionic conductivity study. All the polymer electrolytes follow Vogel–Tamman–Fulcher (VTF) relationship. This principle infers the coupling effect of ionic hopping mechanism and free volume theory. The pseudo-activation energy of all the polymer electrolytes is also determined by fitting the plots with VTF empirical equation. The complexation between PVA, CH3COONH4 and BmImBr is verified in Attenuated Total Reflectance–Fourier Transform Infrared (ATR–FTIR) study. Addition of ionic liquid reduces the crystallinity of polymer electrolytes as proven in x-ray diffraction (XRD) by calculating the degree of crystallinity of polymer electrolytes. The crystallite sizes of polymer electrolytes are also determined using XRD. Proton nuclear magnetic resonance (H-NMR) spectrum reveals the rapid conduction mechanism in the polymer electrolyte by determining the ion diffusion coefficient.

Newly Elaborated Multipurpose Polymer Electrolyte Encompassing RTILs for Smart Energy-Efficient Devices.

Profoundly ion-conducting, self-standing, and tack-free ethylene oxide-based polymer electrolytes encompassing a room-temperature ionic liquid (RTIL) with specific amounts of lithium salt are successfully prepared via a rapid and easily upscalable process including a UV irradiation step. All prepared materials are thoroughly characterized in terms of their physical, chemical, and morphological properties and eventually galvanostatically cycled in lab-scale lithium batteries (LIBs) exploiting a novel direct polymerization procedure to get intimate electrode/electrolyte interfacial characteristics. The promising multipurpose characteristics of the newly elaborated materials are demonstrated by testing them in dye-sensitized solar cells (DSSCs), where the introduction of the iodine/iodide-based redox mediator in the polymer matrix assured the functioning of a lab-scale test cell with conversion efficiency exceeding 6% at 1 sun. The reported results enlighten the promising prospects of the material to be successfully implemented as stable, durable, and efficient electrolyte in next-generation energy conversion and storage devices.