Gel Polymer Electrolyte System Research Articles

A thermostable ionic liquid-methacrylate-based polymer electrolyte for energy storage application

In recent years, gel polymer electrolytes (GPEs) incorporating ionic liquids (ILs) have been explored extensively for lithium-ion batteries due to their favourable thermal stability and high ionic conductivity. Gel polymer electrolytes can also improve the safety of lithium-ion batteries by eliminating the flammable organic solvents which are often used in traditional electrolyte systems. Herein, we report an efficient synthesis of a thermostable ionic liquid-methacrylate-based polymer gel electrolyte via a photo-initiated phase separation (PIPS) process in an inert environment. Anionic liquid phase of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMIMTFSI), coupled with a low molecular weight polyethylene glycol dimethyl ether (PEGDME), was combined with a solid phase of bisphenol A ethoxylate dimethacrylate (BEMA) at varying solid to liquid ratios to produce a thermally stable gel electrolyte. The highest ionic conductivity of 1.9 × 10−3 S cm−1 (at 30 °C) was achieved for the electrolyte with a solid-to-liquid ratio of 1:3 by weight. The Lithium metal cells utilizing these electrolytes and LiFePO4 as cathode active material exhibited the initial discharge capacity of 144 mAh g−1 with capacity retention of 85 % over 100 cycles in ambient temperature. The thermal stability of the cells was significantly improved upon increasing the EMIMTFSI content. This study illustrates the potential application of the IL-methacrylate gel polymer electrolyte system in enhancing the safety of Li-ion batteries through careful tuning of the composition. Their versatile properties also make them suitable for quasi-solid-state batteries with high energy density and safety.

Gel Polymer Electrolytes for Lithium-Ion Batteries Enabled by Photo Crosslinked Polymer Network.

We demonstrate a gel polymer electrolyte (GPE) featuring a crosslinked polymer matrix formed by poly(ethylene glycol) diacrylate (PEGDA) and dipentaerythritol hexaacrylate (DPHA) using the radical photo initiator via ultraviolet (UV) photopolymerization for lithium-ion batteries. The two monomers with acrylate functional groups undergo chemical crosslinking, resulting in a three-dimensional structure capable of absorbing liquid electrolytes to form a gel. The GPE system was strategically designed by varying the ratios between the main polymer backbone (PEGDA) and the crosslinker (DPHA) to achieve an optimal gel polymer electrolyte network. The resulting GPE exhibited enhanced thermal stability compared to conventional liquid electrolytes (LE) and demonstrated high ionic conductivity (1.40 mS/cm) with a high lithium transference number of 0.65. Moreover, the obtained GPE displayed exceptional cycle performance, maintaining a higher capacity retention (85.2%) comparable to the cell with LE (79.3%) after 200 cycles.

Effect EMIMCl on electrochemical properties based PMMA-PLA hybrid gel polymer electrolyte

The formulation of a hybrid gel polymer electrolyte (HGPE) system comprising of polymethyl methacrylate (PMMA) and polylactic acid (PLA) as a hybrid host polymer doped with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) has been successfully prepared in this study with the introduction of an ionic liquid, namely 1-Ethyl-3-methylimidazolium chloride (EMIMCl). Fourier transform infrared (FTIR) spectroscopy and X-ray diffraction (XRD) were used to investigate the structural features of HGPEs. The FTIR analysis revealed that the complexation changes the peak intensity at region C = O stretching, CH2 bending, and C-O stretching. Meanwhile, XRD showed that the addition of EMIMCl altered the HGPE properties and formed an amorphous structure. The prepared HGPE sample was examined for ionic conduction properties through electrical impedance spectroscopy (EIS). It shows that by adding an EMIMCl to the PMMA-PLA-LiTFSI HGPE has decreased the activation energy (Ea ) and increased the ionic conductivity. The sample containing 15 wt.% has the lowest Ea value of 0.057 eV and the highest ionic conductivity at room temperature of 3.20 10−3 S cm−1. The itemperature dependence was studied in the temperature range from 303 K to 393 K, the HGPE systems were found to follow Arrhenius behavior. The effect of EMIMCl content had decreased the viscosity of HGPEs which led to the gel-like type behavior. The potential windows stability analysis revealed that the highest conducting sample was electrochemically stable up to 3.3 V versus Li/Li+, thus showing that the present electrolytes are promising to be applied as in Li-ions battery.

Progress in Gel Polymer Electrolytes for Sodium‐Ion Batteries

Sodium‐ion battery is a potential application system for large‐scale energy storage due to the advantage of higher nature abundance and lower production cost of sodium‐based materials. However, there exist inevitably the safety problems such as flammability due to the use of the same type of organic liquid electrolyte with lithium‐ion battery. Gel polymer electrolytes are being considered as an effective solution to replace conventional organic liquid electrolytes for building safer sodium‐ion batteries. In this review paper, the authors present a comprehensive overview of the research progress in electrochemical and physical properties of the gel polymer electrolyte‐based sodium batteries. The gel polymer electrolytes based on different polymer hosts namely poly(ethylene oxide), poly(acrylonitrile), poly(methyl methacrylate), poly(vinylidene fluoride), poly(vinylidene fluoride‐hexafluoro propylene), and other new polymer networks are summarized. The ionic conductivity, ion transference number, electrochemical window, thermal stability, mechanical property, and interfacial issue with electrodes of gel polymer electrolytes, and the corresponding influence factors are described in detail. Furthermore, the ion transport pathway and ion conduction mechanism are analyzed and discussed. In addition, the advanced gel polymer electrolyte systems including flame‐retardant polymer electrolytes, composite gel polymer electrolytes, copolymerization, single‐ion conducting polymer electrolytes, etc. with more superior and functional performance are classified and summarized. Finally, the application prospects, development opportunities, remaining challenges, and possible solutions are discussed.

Lamellar agarose/graphene oxide gel polymer electrolyte network for all-solid-state supercapacitor

The application of gel polymer electrolyte (GPE) in solid state supercapacitor (SSC) has attracted much attention due to its excellent mechanical properties and chemical stability. However, traditional polymer substrates have high crystallinity, resulting in sluggish lithium migration and low ionic conductivity. In this work, density functional theory calculations (DFT) firstly reveal that agarose molecules (a natural marine polysaccharide) can be assembled to highly-ordered lamellar network structure by hydrogen bonds forming (d’ = 0.454 nm) as GPE matrix combining with graphene oxide (GO) addictive. Specifically, radial distribution functions (RDFs) show that intensities of peaks (gLi-O(r)) at 0.189 nm are 45.2 and 54.8 for agarose and agarose/GO, respectively. This finding indicates an optimized agarose molecular configuration and a rapid lithium migration in agarose/GO GPE (Ag/GO-GPE) system. When Ag/GO-GPE was prepared, SSC assembled with Ag/GO2-GPE and activated carbon electrode has high ionic conductivity (73.8 mS cm−1) and a specific capacitance as high as 791.67 mF cm−2 at a current density of 5 mA cm−2. Moreover, the electrochemical performance of SSC based Ag/GO2-GPE is stable at a bending condition of 180°, resulted from the hydrogen bonds between agarose matrix and GO. In addition, Ag/GO2-GPE has an excellent mechanical strength (0.115 MPa) and flame retardant performance (heat release rates (HRR) of 11.08 kw/m2 and total heat release (THR) of 0.79 MJ m2). This research opens up a novel avenue to develop safe and efficient flexible wearable SSCs.

Effect of Glycerin on Electrical and Thermal Properties of PVA/Copper Sulphate Gel Polymer Electrolytes

Copper-ion conducting gel polymer electrolyte (GPE) systems based on polymer poly(vinyl alcohol) (PVA) and copper sulphate salt doped with glycerin as plasticizer have been synthesized by using solution casting technique. Differential scanning calorimetry (DSC) is used to examine the thermal effect of glycerin on a polymer electrolyte. With the addition of various quantities of glycerin, as a plasticizer in pure PVA and PVA + 20 wt% CuSO4 polymer electrolyte shows a decrease in the values of melting temperature, glass transition temperature and percentage of crystallinity. From TGA curves, it is observed that thermal degradation of the glycerin doped polymer electrolyte is shifted towards lower temperature when compared to pristine PVA and the weight loss of the polymer electrolyte increases with increase of glycerin concentration. From DTG analysis, the temperature of maximum decomposition for PVA is 283.4 °C and it is decreased by the addition of 20 wt% CuSO4 and upon increased concentration of the plasticizer from 1 to 3 mL of glycerin. For pure PVA and PVA + 20 wt% CuSO4, ε′ decreases with increasing glycerin concentration and is lowest at 3 mL glycerin concentration. The maximum ionic conductivity obtained was 9.39 × 10− 4 S/cm for PVA + 20 wt% CuSO4 + 3 mL glycerin gel polymer electrolyte. The above results suggested that, the optimum conducting sample is suitable as separator in rechargeable batteries.

Plasticizers and Salt Concentrations Effects on Polymer Gel Electrolytes Based on Poly (Methyl Methacrylate) for Electrochemical Applications.

This work describes the electrochemical properties of a type of PMMA-based gel polymer electrolytes (GPEs). The gel polymer electrolyte systems at a concentration of (20:80) % w/w were prepared from poly (methyl methacrylate), lithium perchlorate LiClO4 and single plasticizer propylene carbonate (PMMA-Li-PC) and a mixture of plasticizers made by propylene carbonate and ethylene carbonate in molar ratio 1:1, (PMMA-Li-PC-EC). Different salt concentrations (0.1 M, 0.5 M, 1 M, 2 M) were studied. The effect of different plasticizers (single and mixed) on the properties of gel polymer electrolytes were considered. The variation of conductivity versus salt concentration, thermal properties using DSC and TGA, anodic stability and FTIR spectroscopy were used in this study. The maximum ionic conductivity of σ = 0.031 S/cm were obtained for PMMA-Li-PC-EC with a salt concentration equal to 1 M. Ion-pairing phenomena and all ion associations were observed between lithium cations, plasticizers and host polymers through FTIR spectroscopy. The anodic stability of the PMMA-based gel polymer electrolytes was recorded up to 4 V. The glass temperatures of these electrolytes were estimated. We found they were dependent on the plasticization effect of plasticizers on the polymer chains and the increase of the salt concentration. Unexpectedly, it was determined that an unreacted PMMA monomer was present in the system, which appears to enhance ion conduction. The presence and possibly the addition of a monomer may be a technique for increasing ion conduction in other gel systems that warrants further study.

Electrical conduction of PMMA/PLA doped lithium bis(oxalato) borate based hybrid gel polymer electrolyte

The present work highlights the investigation of electrical conduction properties of gel polymer electrolyte (GPE) based poly(methyl) methacrylate (PMMA) and poly(lactic) acid (PLA) blend doped with various compositions of lithium bis(oxalato) borate. The impedance analysis revealed the GPE systems exhibit maximum ionic conductivity of 1.37 × 10−3 S cm−1 for sample PLi20. The electrical properties based on the dielectric permittivity of entire samples decreased with increasing frequency and followed the trend of ionic conductivity. Further analysis was carried out to determine the dielectric response at different temperatures, focusing on the most conducting sample (PLi20). Both dielectric constant and loss increase with the increasing temperature, which suggested that total polarization has occurred. In conclusion, the samples with 20 wt% composition of LiBOB exhibit the highest conducting properties which significantly provides good electrical performance for the application in energy storage devices.

Effect on 1-Butyl-3 Methylimidazolium Iodide Ionic Liquid in Nonedible Jatropha Oil-Based Polyurethane Acrylate. Tetrabutylammonium Iodide: Lithium Iodide-Based Gel Polymer Electrolyte for Dye-Sensitized Solar Cell Application

Improvement of the electrolyte ionic conductivity in DSSCs application is important as it contributes higher solar conversion efficiency. In this article, the polyurethane acrylate (PUA) gel polymer electrolyte (GPE) system was further improved with the addition of an ionic liquid in terms of ionic conductivity and also photovoltaic performance. The PUA GPE system enhanced with 6 wt % of 1-butyl-3-methylimidazolium iodide (BMII) ionic liquid was found to produce the highest improvement (ionic conductivity) compared to the different content of BMII. Ionic conductivity of (4.17 ± 0.01) × 10–4 S cm–1 was observed at room temperature with the addition of 6 wt % BMII in the GPE system. Moreover, the DSSC utilizing the GPE with 6 wt % BMII produces the highest solar conversion efficiency of (5.72 ± 0.14)% corresponding with the Jsc of (23.03 ± 0.2) mA cm–2 and Voc of (0.54 ± 0.01) V.

Effect of the potassium iodide in tetrapropyl ammonium iodide-polyvinyl alcohol based gel polymer electrolyte for dye-sensitized solar cells

Low ionic conductivity in gel polymer electrolytes with large cations is undoubtedly a critical issue. This research’s main objective was to explore potassium iodide influences on the conductivity in gel polymer electrolytes. PVA-based gel polymer electrolytes (GPEs), including tetrapropyl ammonium iodide and potassium iodide have been prepared. The GPEs have been characterized by X-ray diffraction (XRD) and electrical impedance spectroscopy (EIS). The GPEs prepared haves been recognized as an amorphous region through the X-ray diffraction analysis. The GPE sample’s conductivity (100 wt% of tetrapropyl ammonium iodide) of 6.24 × 10−3 S cm−1 was the lowest. The existence of potassium iodide in the GPE system improves the conductivity. The conductivity of 9.72 × 10−3 S cm−1 of GPE containing 30 wt% of tetrapropyl ammonium iodide and 70 wt% of potassium iodide was the highest derived from the EIS analysis. All prepared GPEs have the potential to be used for dye-sensitized solar cell applications. The dye-sensitized solar cell efficiency has been improved by ~30% if potassium iodide exists in the GPE system.

Studies on ionic liquid based nanocomposite gel polymer electrolyte and its application in sodium battery

A nanocomposite gel polymer electrolyte system comprising porous membrane of poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)/TiO2 immobilizing a liquid electrolyte of sodium trifluoromethanesulfonate (NaCF3SO3) in 1-butyl-3-methylimidazolium trifluoromethanesulfonate (BMImCF3SO3) ionic liquid is reported in the paper. The porous gel polymer electrolyte membranes are prepared by phase-inversion technique. The electrolyte membranes are characterized by various physical and electrochemical techniques. The TiO2 nanoparticles display interaction with the anion (CF3SO3−) of the liquid electrolyte and enhance amorphicity in the polymer network. The optimized membrane displays maximum room temperature ionic conductivity as ~0.4 mS cm−1 with improved electrochemical stability window of ~4.3 V and Na+ ion transport number as ~0.27. A proto-type sodium battery using the optimized membrane is fabricated and characterized. The battery delivers a stable open circuit potential of ~2.2 V and shows a discharge capacity ~200 mA h g−1 at 25 mA g−1 drain current.

Swift heavy ion beam modified MoS2- PVA nanocomposite free-standing electrodes for polymeric electrolyte based asymmetric supercapacitor

Swift heavy ion (SHI) beam irradiation technique is one of the sophisticated techniques used for modifying material properties to design efficient devices. In this report, the casted MoS2- PVA nanocomposite films have been irradiated with 80 MeV C6+, 100 MeV Si9+, and 120 A g9+ ion beams to achieve enhanced conductivity and have been exploited as an electrode material for asymmetric supercapacitor. PVDF-HFP: TPAI gel polymer electrolyte having 3 wt.% TPAI content showed the highest conductivity and was chosen for the iodide redox gel polymer electrolyte system. The pristine MoS2-PVA nanocomposite films having an electrical conductivity of 2.5E-5 S/cm exhibited specific capacitance of 65.27 F/g whereas the films irradiated with 120 MeV Ag9+ ion beams showed an electrical conductivity of 9.7E-3 S/cm and enhanced specific capacitance of 186.67 F/g. The enhanced capacitance is attributed to the high current density generated due to the increased conductivity of the electrodes.

Magnesium (II) bis(trifluoromethanesulfonimide) doped PVdC-co-AN gel polymer electrolytes for rechargeable batteries

Gel polymer electrolytes (GPEs) containing poly(vinylidene chloride-co-acrylonitrile) (PVdC-co-AN) as the polymer host and plastic crystal succinonitrile (SN) as plasticizer were prepared with varied concentrations of 5 to 30 wt.% of magnesium (II) bis(trifluoromethanesulfonimide) Mg(TFSI)2 salt. The highest room temperature ionic conductivity of 1.61 × 10−6 S cm−1 was obtained from the sample containing 20 wt.% of Mg(TFSI)2. The conductivity temperature dependence studies of the GPE system was found to obey the VTF relation. To study the interaction among the constituents in the GPEs as well as to confirm the complexation between them, Fourier transform infrared spectroscopy. (FTIR) was carried out. The analysis of FTIR spectra was further investigated by deconvolution of the FTIR spectra to prove the dependability of ionic conductivity with the presence of free ions, ion pairs, and ion aggregates in the GPEs. The amorphous nature of the GPEs were confirmed by X-ray diffraction (XRD) analysis while DSC studies revealed the relationship between the thermal stability of GPEs and ionic conductivity. The electrochemical study was also performed by linear sweep voltammetry (LSV) to verify the maximum withstand voltage of the electrolyte to be used in magnesium battery application.

Dendrite-free, wide temperature range lithium metal batteries enabled by hybrid network ionic liquids

Replacing liquid electrolytes with solid-state electrolytes is a promising approach to achieving practical applications of lithium metal batteries (LMBs). In this work, ionic liquid N-methyl-N-propyl-pyrrolidinium bis(fluorosulfonyl)imide (Pyr13FSI) was introduced into a hybrid network to obtain a series of gel polymer electrolytes (GPEs). Mechanical and electrochemical properties of the GPEs were tuned through controlling the network structure and ionic liquid contents, and ionic conductivity higher than 1 ​mS ​cm-1 at room temperature was achieved. The newly developed GPEs are flame-retardant and show excellent thermal and electrochemical stability as well as ultra-stability with lithium metal anode. Symmetrical lithium cells with the GPEs exhibit a stable cycling over 6800 ​h ​at a current density of 0.1 ​mA ​cm-2 and stable lithium stripping-plating at 1 ​mA ​cm-2, the highest current density reported for ionic liquid-based GPEs. Detailed correlation between mechanical properties, ionic conductivity and cell short-circuit time is discussed. Moreover, Li/LiFePO4 batteries with the obtained GPEs exhibit desirable cycling stability and rate performance over a wide temperature range from 0 ​°C to 90 ​°C, further suggesting that this new hybrid-network/ionic liquid GPE system has great potential for practical applications in next generation LMBs.

Role of Multiferroic Filler on the AC Response of Bi1‐xBaxFeO3 doped PVA:NH4CH3COO Nanocomposite Gel Polymer Electrolytes

AbstractThe frequency dependent AC conductivity and dielectric studies of multiferroic filler (Bi1‐xBaxFeO3) doped nanocomposite gel polymer electrolyte (NCGPEs) based on PVA:(NH4CH3COO) are investigated in the present work. The nano composite gel polymer electrolyte systems are synthesized for various filler concentrations by solution cast method. The effect of filler concentration on ionic conductivity is studied using AC impedance technique in the frequency range 1–106 Hz. X‐ray diffraction studies reveal the formation of nanocomposite gel polymer electrolyte. The low frequency dispersion in the dielectric response of electrolytes shows the relaxation contribution is superimposed with electrode polarization effects. The relaxation peaks in the NCGPEs are found to shift toward higher frequency side with increasing filler concentration and are suitably correlated to change in morphology of the gel electrolyte system. The variation of AC conductivity with frequency is seen to obey Jonscher's universal power law with the exception of small deviation in the low frequency regime. Modulus formalism of dielectric response suggests that the ion transport is strongly coupled to the polymer segmental motion.

Gel Polymer Electrolytes Based on Polymerizable Lithium Salt and Poly(ethylene glycol) for Lithium Battery Applications.

Here, a polymerizable lithium salt, lithium (trifluoromethanesulfonyl)(vinylsulfonyl)imide, was synthesized and used to prepare cross-linked gel polymer electrolyte systems with poly(ethylene glycol) methyl ether methacrylate as an ion-conducting moiety, poly(ethylene glycol) dimethacrylate as a cross-linker, and propylene carbonate as a liquid electrolyte without adding any conventional inorganic lithium salt. The gel polymer electrolytes prepared in this study exhibited a reasonably high ionic conductivity (6.7 × 10-4 S cm-1 at 25 °C and 1.8 × 10-3 S cm-1 at 60 °C) and lithium-ion transference number (0.52), and the lithium battery prepared using the gel polymer electrolyte showed a stable cycling performance over 50 cycles.

Effect of Al2O3 nanoparticles on ionic conductivity of PVdF-HFP/PMMA blend-based Na+-ion conducting nanocomposite gel polymer electrolyte

In the present work, the effect of dispersion of Al2O3 nanoparticles on ionic conductivity of non-aqueous PVdF-HFP/PMMA blend-based nanocomposite gel polymer electrolyte system comprising liquid electrolyte of sodium trifluoromethanesulfonate is investigated. The ionic conductivity of the electrolyte increases maximum to ∼ 1.5 × 10−3 S cm−1 for the composition with 6 wt% Al2O3 nanoparticles. The optimized composition retains Vogel-Tamman-Fulcher (VTF) behavior in the temperature range from − 50 to 95 °C. The scanning electron micrography and x-ray diffraction studies reveal the uniform dispersion of Al2O3 nanoparticles in the porous structure of the nanocomposite gel polymer electrolyte and enhanced amorphicity of polymer matrix. The optimized electrolyte composition owns a sufficiently large electrochemical stability window of ~ 3.6 V with good sodium ion transference number. The optimized electrolyte is used in a prototype sodium battery cell, which shows an open circuit potential of ~ 2.5 V and first discharge capacity ~ 400 mA h g−1 followed by a capacity decline with cycling.

Influence of crystalline and amorphous microscopic morphology on the capacitance performance and electrochromic phenomenon of triazine-based polyimides

In this paper, two series of polyimides TPI-Ns and TPI-Ds containing triazines were prepared using NMP and DMF as precursor solvents respectively. Through the characterization of XRD, FT-IR and SEM, it was found that the secondary structures of the two types of TPIs were significantly different. The former shows a higher crystallinity while the latter shows an amorphous state. The two types of polyimides were respectively prepared into gel polymer electrolytes (GPEs) and applied to capacitor devices with ITO as the electrode. It was shown that the charge–discharge rate of the two types of devices differed significantly with the concentration of TPI added in GPEs system. Compared with the former, the latter showed a stronger linear correlation, and the equation of the relationship between charge and discharge time t and TPI addition quantity c was fitted. In addition, it was found that the electrochromic device prepared with TPI-D-2 as the active layer could change the color between white, amaranth (coloring state) and green (fading state) with additional voltage (< 4.5 V) was applied. All the above indications show that the short-range ordered structure of TPIs can affect its microscopic morphology and is directly related to its capacitance performances and electrochromic activity.

Effect of PC:DEC plasticizers on structural and electrical properties of PVDF–HFP:PMMA based gel polymer electrolyte system

A gel polymer electrolyte based on poly(vinylidene fluoride–hexafluoropropylene) (PVDF–HFP) and poly(methyl methacrylate) (PMMA) as host polymers, lithium perchlorate ( $${\hbox {LiClO}}_{{4}}$$ ) as salt has been prepared with different concentrations of mixture of propylene carbonate (PC) and diethyl carbonate (DEC) (1:1) as plasticizers by using solution casting technique. Changes in structural properties have been studied by X-ray diffraction. Surface morphology has been analyzed using atomic force microscope studies. Electrical conductivity has been carried out by electrochemical impedance spectroscopy in the temperature range 303 K to 343 K. Addition of plasticizers to polymer blend electrolyte has been found to result in an enhancement of the ionic conductivity. A maximum electrical conductivity of $$1.03 \times 10^{-3}$$ S cm $$^{-1}$$ at 303 K has been achieved for the polymer blend gel electrolyte containing 60 wt $$\%$$ of PC:DEC plasticizers. The temperature dependence of the ionic conductivity exhibits Vogel–Tammann–Fulcher type behavior indicating a strong coupling between the ionic conductivity and the polymer chain segmental motions. AC conductivity has been analyzed using Jonscher’s power law. A relaxation phenomenon is studied with modulus formalism.

3D mesoporous reduced graphene oxide with remarkable supercapacitive performance

Chemical reduction of graphene oxide (GO) to reduced graphene oxide (rGO) is an important process in view of the development of graphene-based supercapacitors on industrial level. We report an in situ chemical reduction of GO by copper(I) salt (CuCl) and isolation of semiconducting rGO material with three-dimensional (3D) mesoporous structure. Fabricated all-solid-state supercapacitors of our rGO exhibited specific capacitance and energy density values as high as 310 F/g at a current density of 1 A/g and 10 Wh/kg, respectively in an eco-friendly aqueous gel polymer electrolyte (GPE) system. Furthermore, increasing the mass loading of rGO boosted the areal capacitance to a record value of about 580 mF/cm2 at 1 mA/cm2 current density. More than 80% capacitance was retained beyond 100,000 continued charge-discharge (CD) cycles. Also, sustainability of our rGO supercapacitor over switching current densities in the CD cycles was excellent resembling the rate performance in battery-like energy storing devices. The use of organic electrolyte boosted the energy density of rGO to very high level of ∼22 Wh/kg.