Gel Electrolyte Research Articles

A Comprehensive Review of Functional Gel Polymer Electrolytes and Applications in Lithium-Ion Battery.

The rapid expansion of flexible and wearable electronics has necessitated a focus on ensuring their safety and operational reliability. Gel polymer electrolytes (GPEs) have become preferred alternatives to traditional liquid electrolytes, offering enhanced safety features and adaptability to the design requirements of flexible lithium-ion batteries. This review provides a comprehensive and critical overview of recent advancements in GPE technology, highlighting significant improvements in its physicochemical properties, which contribute to superior long-term cycling stability and high-rate capacity compared with traditional organic liquid electrolytes. Special attention is given to the development of smart GPEs endowed with advanced functionalities such as self-protection, thermotolerance, and self-healing properties, which further enhance battery safety and reliability. This review also critically examines the application of GPEs in high-energy cathode materials, including lithium nickel cobalt manganese (NCM), lithium nickel cobalt aluminum (NCA), and thermally stable lithium iron phosphate (LiFePO4). Despite the advancements, several challenges in GPE development remain unresolved, such as improving ionic conductivity at low temperatures and ensuring mechanical integrity and interfacial compatibility. This review concludes by outlining future research directions and the remaining technical hurdles, providing valuable insights to guide ongoing and future efforts in the field of GPEs for lithium-ion batteries, with a particular emphasis on applications in high-energy and thermally stable cathodes.

Binary solvent-reinforced poly (vinyl alcohol)/sodium alginate double network hydrogel as a highly ion-conducting, resilient, and self-healing gel polymer electrolyte for flexible supercapacitors

We present a reliable approach for producing high-performance ion-conducting gel polymer electrolytes (GPEs) based on the sodium chloride (NaCl)-integrated dual network hydrogel of poly (vinyl alcohol)/sodium alginate (PVA/SA) using a binary solvent system of ethylene glycol (EG) and water, providing exceptional ionic conductivity, mechanical strength, and self-healing properties. Different GPEs were produced via the freezing-thawing method using different v/v% of EG and water (named PVA/SA/EG). The best PVA/SA/EG GPE provided a maximum ionic conductivity of 25 mS cm−1, astonishing mechanical strength of 0.42 MPa, exceptional stretchability of 462 %, and remarkable self-healing properties. The binary solvent system- and water-based GPEs were utilized in the construction of symmetric supercapacitors (SSCs) using carbon cloth electrodes and their electrochemical performance were compared. At a current density of 0.5 mA cm−2, the SSC prepared using the best PVA/SA/EG GPE demonstrated a high specific capacity of 577.21 mF cm−2, maintained 94.5 % capacitance after 5000 cycles at 1 mA cm−2, and provided an energy density of 80.14 mWh cm−2 while operating at a power density of 293.3 mW cm−2. The flexible SSC prepared based on this GPE demonstrated outstanding flexibility, while no significant decline in capacitive performance and ionic conductivity was detected when it was bent.

Tissue-like interfacing of planar electrochemical organic neuromorphic devices

Abstract Electrochemical organic neuromorphic devices (ENODes) are rapidly developing as platforms for computing, automation, and biointerfacing. Resembling short- and long-term synaptic plasticity is a key characteristic in creating functional neuromorphic interfaces that showcase spiking activity and learning capabilities. This potentially enables ENODes to couple with biological systems, such as living neuronal cells and ultimately the brain. Before coupling ENODes with the brain, it is worth investigating the neuromorphic behavior of ENODes when they interface with electrolytes that have a consistency similar to brain tissue in mechanical properties, as this can affect the modulation of ion and neurotransmitter diffusion. Here, we present ENODEs based on different PEDOT:PSS formulations with various geometries interfacing with gel-electrolytes loaded with a neurotransmitter to mimic brain-chip interfacing. Short-term plasticity and neurotransmitter-mediated long-term plasticity have been characterized in contact with diverse gel electrolytes. We found that both the composition of the electrolyte and the PEDOT:PSS formulation used as gate and channel material play a crucial role in the diffusion and trapping of cations that ultimately modulate the conductance of the transistor channels. It was shown that paired pulse facilitation can be achieved in both devices, while long-term plasticity can be achieved with a tissue-like soft electrolyte, such as agarose gel electrolyte, on spin-coated ENODes. Our work on ENODe-gel coupling could pave the way for effective brain interfacing for computing and neuroelectronic applications.

Urea-lactic acid as efficient lignin solvent and its practical utility in sustainable electrospinning

The development of lignin-based materials presents a promising avenue for advancing green chemistry and mitigating environmental impact. However, the key challenge lies in the processability of lignin, which significantly affects its practical applications. Addressing the issues related to lignin's complex structure, variability, and reactivity is crucial for optimizing its incorporation into high-performance materials. Therefore, in this study we explore the efficacy of a urea-lactic acid-based deep eutectic solvent (ULA) for the dissolution of kraft lignin, aiming to enhance its practical utility in sustainable electrospinning processes, for the first time. Results of elemental analysis, IR and 2D NMR spectroscopy, provide crucial insights into the structural properties of the regenerated material post-DES treatment. The findings confirm a high lignin recovery rate, reaching up to 96.6 % for samples dissolved at 100°C. Additionally, 2D NMR analysis indicates that the process leads to partial esterification of lignin with lactate ions. The ability of the studied DES to effectively solubilize lignin underscores its potential as an efficient lignin solvent and facilitates the fabrication of lignin-based nanofibers via electrospinning. The incorporation of this DES in electrospinning processes promises significant advancements in the development of sustainable, lignin-derived materials and offers a green alternative for production of high-performance nanofibers. Preliminary results of electrochemical impedance spectroscopy and galvanostatic charge/discharge measurements confirm that the EDLC with prepared hydrogel electrolyte demonstrates attractive electrochemical properties (specific capacitance, CSP = 95 F g–1; series resistance RS = 2.2 Ω; charge transfer resistance, RCT = 1.6 Ω), which are comparable with the reference cell based on a commercial glass fibre separator. Hence, the DES-assisted-electrospinned lignin membrane can be viewed as a potential gel electrolyte matrix for practical use in construction of sustainable energy storage devices.

Improving the Cyclic Stability of Electrochromic Mirrors Composed of Gel Electrolyte

Improving the Cyclic Stability of Electrochromic Mirrors Composed of Gel Electrolyte

Tailored Cellulose Gel Electrolytes with Dual Pores, Aligned Channels, and Dendrite Mitigation for Improved K/Zn Dual-Ion Battery

Tailored Cellulose Gel Electrolytes with Dual Pores, Aligned Channels, and Dendrite Mitigation for Improved K/Zn Dual-Ion Battery

Nickel sulfide nanoparticles decorated on carbon spheres derived from Verbena officinalis for high-performance asymmetric all-solid-state flexible supercapacitors

The crafting and development of electrode materials possessing extensive energy storage capacities, alongside their adherence to environmental and economic principles, along with their outstanding capacitive behaviors, stand as pivotal elements in propelling the technological progress of supercapacitors. In this study, we utilized discarded Verbena officinalis (VOCs) as a carbon substrate and successfully synthesized porous hollow carbon spheres through an in-situ hydrothermal method, subsequently depositing NiS nanoparticles to form a shell-like structured material. The optimized VOCs/NiS-3 composite material exhibited an exceptional specific capacitance of 202.8 mAh g−1 at a current density of 1.0 A g−1; it maintained 71 % of its capacitance even at a high current density of 10 A g−1 (144.2 mAh g−1). After enduring 10,000 charge-discharge iterations, the preservation of charge storage capacity was 81.7 %, highlighting the material's outstanding performance in terms of rapid charge-discharge rates and enduring stability. Furthermore, within a PVA/KOH gel electrolyte, we fabricated an asymmetric all-solid-state supercapacitor device that delivered an energy density of 32.58 Wh k g−1 at a power density of 800 W k g−1. The device sustained a capacitance loss rate of 9.9 % and a coulombic efficiency of 96.8 % after 5000 cycles. Even after 3000 repeated bending at 120°, the capacitance retention reached 88.3 %, indicating the device's exceptional specific capacitance, flexibility and longevity. This research offers a renewable and waste-resource recycling design strategy for synthesizing outstanding-performance, flexible, all-solid-state supercapacitor electrode materials with NiS deposited on discarded biomass carbon, unveiling considerable potential for enhancing energy storage efficiency.

Fabrication of functional laser-induced graphene using gelatin-2,6-diaminoanthraquinone coating for high-performance micro-supercapacitor

In this investigation, we develop a procedure in which gelatin and 2,6-diaminoanthraquinone (ANQ) are combined and then applied as a coating on laser-induced graphene (LIG). The resulting materials are subjected to laser irradiation, which facilitates the introduction of nitrogen doping and the integration of oxygenated functional groups onto the LIG surface. The gelatin polymer played a pivotal role in introducing oxygenated functional groups, while ANQ molecules contributed to both doping with nitrogen and the inclusion of additional oxygenated groups on the LIG surface. The electrode material's performance was enhanced by these functional groups. When evaluated in a three-electrode setup, the ANQ-LIG configuration exhibited a significantly high areal capacitance of 32.4 mF cm−2 at 0.2 mA cm−2, which is five times that of pristine LIG (6.3 mF cm−2) and three times that of gelatin-LIG (9.0 mF cm−2). When integrated into a micro-supercapacitor using a polyvinyl alcohol (PVA)-sulfuric acid (H2SO4) gel electrolyte, ANQ-LIG demonstrated superior areal capacitance (16.0 mF cm−2 at 0.1 mA cm−2) compared to gelatin-LIG (5.3 mF cm−2) at the same current. Additionally, ANQ-LIG displayed favorable capacitance retention (83.8 % after 10,000 cycles) and coulombic efficiency (98.1 % after 10,000 cycles).

Weakened functional group activity enables the uniform distribution of the gel electrolyte to achieve the high-performance of Li-ion batteries

Electrolyte gelation is considered to be one of the main routes to solve the safety problem of liquid electrolytes. However, the distribution of gel polymer electrolyte (GPE) on the surface of electrodes and the mechanism of their effect on the performance of battery are still unknown. Here, methyl methacrylate (MMA) containing methyl (-CH3) and methyl-2-cyanoacrylate (MCA) containing cyanide (-CN) are employed as representative monomers to explore the relationship between gel distribution and battery performance. Due to the stronger electron-withdrawing properties, PMCA gel has shorter chain length and greater shrinkage, showing many cracks on the electrode surface, while PMMA gel can evenly cover the surfaces of electrodes. As a result, the capacity retention rate of 1.4 Ah NCM811/Gr pouch cells with PMMA is 93.5% for 500 cycles at 25 °C and 91.5% for 600 cycles at 60 °C, which these of the cells with PMCA are 58.8% for 266 cycles at 25 °C and 69.1% for 327 cycles at 60 °C. XPS analysis of the electrode sheets before and after cycling reveal that the PMCA-electrode has a large number of rzero valent lithium element precipitation, whereas the PMMA-electrode has the more stable interface film. This study indicates that the uniform distribution of gel electrolyte with -CH3 functional group on the electrode surface can improve the electrochemical performance of NCM811/Gr battery, which has the guiding significance.

The role of polymer gel electrolyte infiltration for enhancement of capacitance and cycle stability

With the increasing application of electronic materials in various fields such as flexible electronic textiles, wearable and portable gadgets, aerospace and aircraft systems etc., the demand for clean high-power energy storage devices is also increasing rapidly. To date, the application of market available supercapacitors has not met the energy expectations in the range of market leading Li-ion batteries (LIBs) due to their unreliable mechanical flexibility, electrolyte leakage, low voltage application, low capacity, low cycle stability and moderate rate-capability. Inappropriate utilization of the maximum porosity of the electrode material and inefficient activities of the electrode/electrolyte interface are major challenges for present supercapacitor development. In this work, for the first time, the role of polymer gel electrolyte infiltration to improve the electrochemical performance of a supercapacitor has been explicitly studied and investigated. It has been observed that 1-Ethyl-3- Methylimidazolium bis(trifluoromethylsulfonyl)imide [EMIM][TFSI] ionic liquid electrolyte embedded in Polypropylene Carbonate (PPC) and Polycarbonate (PC) polymer matrix polymer gel electrolyte (PGE) showed excellent supercapacitive performance at high voltage window 2.6 V by delivering maximum total capacitance of 5.81 F and maximum energy density 10.9 Wh kg-1 at 30 mA current (0.06 A g-1). Regular infiltration of the polymer gel electrolyte inside the electrode material is also observed during long cycle operation of 10,000 cycles. Infiltration of electrolyte ions into the pores of electrode materials plays a significant role in increasing capacitance and cycle Stability. These results highlight the potential of this novel high-voltage polymer gel electrolyte for future high-power energy storage device applications.

Tough and self-healing all-in-one supercapacitor enabled by triple-network redox carrageenan and sodium carboxymethylcellulose reinforcing gel polymer electrolyte

Flexible supercapacitors have recently gained great attention in the field of wearable electronics due to their long cycle life, and high efficiency. Herein, an all-in-one flexible supercapacitor is fabricated by in-situ polymerization of PANI on the surface of a fully physical cross-linking polyacrylamide/κ-carrageenan-K+/sodium carboxymethylcellulose-Al3+ triple network gel polymer electrolyte (GPE). By designing multiple interpenetrating networks and bimetallic ions cross-linking, the GPE displays outstanding mechanical performance. Meanwhile, owing to the dynamic interactions (hydrogen bond, ion coordination and thermoreverisible transition of KC) among different polymer chains, the GPE exhibits remarkable self-healing properties. Additionally, the all-in-one configuration accelerates ion transport at electrode-electrolyte interface and provides extremely low interface resistance, which endows the supercapacitor with excellent capacitance performance (254.58 mF/cm2) and energy density (59.81 μWh/cm2). Thanks to the unique integrated structure, the device avoids the slippage among multilayers and shows splendid electrochemical stability even under various physical deformations. More importantly, the all-in-one supercapacitor displays superior safety, self-healing and low temperature properties (85 % capacitance retention after 8 cutting/healing cycles even at −20 °C) due to the multi-function GPE. This simple and versatile strategy for constructing the all-in-one supercapacitors will offer broad prospects for designing energy storage devices in wearable electronics.

CdS/CuInS2 Quantum Dots Cosensitized Solar Cells Using Functionalized Polyurethane Gel Electrolytes

CdS/CuInS2 Quantum Dots Cosensitized Solar Cells Using Functionalized Polyurethane Gel Electrolytes

MIL-125 (Ti) and porous dielectric polymer substrate introducing composite gel polymer electrolyte with enhanced mechanical property, thermal stability and electrochemical property

Lithium metal batteries have potentially high energy density, but severe uncontrolled lithium dendrites and unstable side reactions prevent large-scale applications. Serial three-dimensional porous poly (vinylidene fluoride) and copolymer membrane-based composite gel electrolytes are designed by introducing MIL-125 (Ti) and ethylene carbonate. Abundant lithium-ion transportation channels and homogeneous ion transport microregion are provided the new type porous fluoropolymer substrate. We also find that crystalline phase and dielectric properties of serial polymer membrane have significant impact on electrochemical performance for composite gel electrolytes. The mechanical and dielectric property of composite electrolyte enhanced by incorporating uniform and well distribution MIL-125 (Ti), which improve the electrolyte/electrode interface charge distribution and promote uniform lithium deposition, leading to lithium dendrite suppression. MIL-125 (Ti)/P(VDF-TrFE-CTFE) composite membrane shows the enhanced maximum strain of 181 %, thermal stability (188 °C) and corresponding composite gel electrolyte reflects higher ionic conductivity of 1.7 × 10–3 S cm-1 and wider electrochemical window at room temperature than PVDF and PVDF-HFP composite electrolytes. Expectedly, quasi-solid state lithium metal battery of MIL-125 (Ti)/P(VDF-TrFE-CTFE) composite gel electrolyte exhibits higher discharge capacity (152.8 mAh g-1) at 240th cycle and 1 C, longer cycling life and better rate performance under large current density than PVDF and PVDF-HFP composite electrolytes.

Simple construction of molybdate anions-intercalated NiCo-based layered double hydroxides nanosheet arrays on carbon fibers for enhanced flexible fiber-shaped supercapacitors

As the energy supply devices for miniaturized, wearable, portable and intellectualized electronic products, flexible fiber-shaped supercapacitors (FSCs) have attracted great attention by virtue of their peculiar superiorities such as ultra-fast charge/discharge ability, ultra-high output power, ideal service life, outstanding mechanical flexibility, and superior compatibility with the human body. The performance enhancement of FSCs is highly dependent on the high-performance active electrode materials. In this work, a series of molybdate anions-intercalated NiCo based layered double hydroxides (NiCoMo-LDHs) have been synthesized on flexible carbon fiber (CF) by a simple electrodeposition strategy by regulating the Mo content and the growth time. It turns out that the intercalation of molybdate anions can significantly widen the interlayer spacing and reduce the crystallinity of the synthesized LDH materials. The morphological differences between the LDHs with different Ni/Co/Mo ratios are analyzed, and the morphological evolution process of the materials with the specific Ni/Co/Mo ratio of 1:3:0.2 are systematically investigated. The well-developed NiCoMo-LDH nanosheets electrode with appropriate Ni/Co/Mo ratio (NCM2–500) delivers the best electrochemical performances among all the synthesized LDHs. In particular, the synthesized NCM2–500 fiber electrode exhibits excellent specific capacitance, superior electrical conductivity and favourable cycling stability. Additionally, the assembled parallel type NCM2–500//AC FSC device using NCM2–500 and activated carbon (AC) as the cathode and anode with the assistance of PVA/KOH gel electrolyte demonstrates a brilliant specific energy of 36 Wh cm−1 at 845 W cm−1 (nearly 17 Wh kg−1 at about 400 W kg−1) and a high cycle lifespan of maintaining 103 % of the pristine capacity after 5000 cycles. This FSC device is an ideal candidate for next-generation applications due to its remarkable electrochemical properties.

Real-time monitoring the formation of polymer double network for gel polymer electrolyte by means of dielectric spectroscopy

A non-destructive method of detecting the internal information of the system is attempted in a polymer double network for gel polymer electrolyte in lithium-ion battery. The real-time monitoring for polymerization of 1,3-dioxolane (DOL) and cross-linking of cyanoethyl poly(vinyl alcohol) (PVA-CN) is carried out in a coin cell at 0–80 ℃ by means of dielectric spectrum. A widely distributed dielectric relaxation varying with monitoring time and temperature is observed in the frequency range of 3–103 kHz, and the relaxation parameters of the three sub-relaxations are obtained by fitting the dielectric spectrum with the HN equation. It is found that the relaxation intensity Δε and relaxation time τ are obviously dependent on the monitoring time and temperature: Δε and τ change obviously near the respective gel points of DOL and PVA-CN (DOL at 25 ℃, PVA-CN at 60 ℃), suggesting gelation at two gel points respectively. The different structural changes of the system before and after gelling temperature are speculated, and the possible microstructure of the system in each temperature range is proposed after analyzing the relaxation parameters. The applicability of the real-time dielectric monitoring in the study of the structure of gel polymer electrolytes is preliminarily concluded.

Calcination synthesized and self-assembled “rough bark-like” cobalt pyrophosphate for the high-performance hybrid supercapacitor as cathode materials

Transition-metal phosphate/pyrophosphate always exhibits promising theoretical electrochemical performance and has essential prospects in supercapacitors. In this study, “rough bark-like” Co2P2O7 is successfully synthesized via calcination method using ammonium cobalt phosphate as raw material. By investigating the effect of calcination temperature on the morphology of Co2P2O7, the pure cobalt pyrophosphate piece could be prepared at 600 °C (CPO-600). Due to the unique morphology and mesoporous presence, the CPO-600 exhibits a good affinity and infiltration interface with the electrolyte and displays a specific capacitance of 544 F g−1 at 1 A g−1 in 3 M KOH, which has excellent rate performance. After 10,000 cycles at 20 A g−1, it still maintains the good cycle stability with 81.48 % initial specific capacitance. Furthermore, the hybrid asymmetric aqueous supercapacitor of CPO-600//AC delivers remarkable energy densities of 10.6 Wh kg−1 at power densities of 559 W kg−1. And its gel electrolyte device also provides higher electrochemical properties and good comprehensive performance.

An in situ gel electrolyte for the facile preparation of high‐safety Li‐S battery

AbstractLithium‐sulfur (Li‐S) battery shows promising development potential in secondary lithium‐ion batteries. However, the shuttle effect of polysulfides, uncontrollable lithium dendrite growth, and safety hazards in conventional liquid electrolytes limit the popularity of Li‐S batteries in the future commercial market. In this work, a high‐performance gel electrolyte (GPE) was prepared in situ by initiating the ring‐opening polymerization of 1,3‐dioxolane (DOL) with aluminum trifluoromethanesulfonate (Al(OTf)3) and using diethylene glycol dimethyl ether (DME) as a plasticizer, which can effectively improve the interfacial compatibility between sulfur cathode and the electrolyte, as well as the stability of lithium anode. The electrochemical performance of the poly‐DOL (PDOL) GPE was optimized by adjusting the concentration ratio of the initiator. When the concentration of Al(OTf)3 is 4 mM, the PDOL GPE has a high ionic conductivity up to 3.81 × 10−4 S cm−1 and a lithium ion migration number of 0.57. The assembled quasi‐solid‐state Li‐S batteries shows an initial discharge specific capacity of 908.1 mAh g−1 at 0.1 C with a capacity retention of 68% after 240 cycles, and its average Coulombic efficiency is maintained at 96.1%. This gel electrolyte design provides a feasible practical idea in quasi‐solid‐state Li‐S batteries.

Optimized Nb‐Doped TiO2/rGO Nanocomposites for Assessment of Photovoltaic Performance With Metal‐Free Dye and Polymer Gel Electrolyte

AbstractThis research presents the development of niobium (Nb)‐doped titania (TiO2)/reduced graphene oxide (rGO) nanocomposites (NTR NCs) for dye‐sensitized solar cells (DSSCs). The novelty lies in two aspects: introducing Nb (V) ions into TiO2/rGO nanocomposites via an in‐situ sol‐gel method with doping concentrations from 1.0 to 3.0 mol %, and fabricating photoanodes using the doctor blade technique, sensitized with a Co2+/Co3+‐based PEO‐PEG polymer gel electrolyte‐assisted D‐π‐A carbazole metal‐free (SK3) dye. Detailed investigations into the optoelectrical, structural, and morphological properties were conducted using various spectral and analytical tools. Notably, DSSCs based on Nb‐doped TiO2/rGO nanocomposites with 2.0 mol % Nb (NTR‐2) achieved a remarkable solar efficiency (η) of 5.48 % under AM 1.5 solar simulation, significantly outperforming devices based on bare TiO2 nanoparticles and undoped TiO2/rGO NCs by factors of 4.15 and 2.97, respectively. The substantial enhancement in photovoltaic performance is attributed to superior charge transfer properties and higher carrier density, as revealed by electrochemical impedance spectroscopy (EIS) and Mott‐Schottky (M–S) analysis. Nb‐doping results in an energetic surface nature, improved optical absorption, and reduced charge transfer resistance, collectively boosting the overall efficiency of DSSCs. This work underscores the potential of Nb‐doped TiO2/rGO NCs as effective photoanode materials in enhancing DSSC performance.

A polysaccharide extracted from guar beans-based gel polymer electrolytes for efficient dye-sensitized solar cells

Liquid electrolytes in dye-sensitized solar cells (DSSCs), while effective in minimizing recombination of TiO2 conduction band with redox couple (I−/I3−), suffer from leakage and evaporation issues, hindering commercialization. Although solid-state electrolytes were introduced as an alternative, their performance is constrained by poor electrode contact. To solve these issues, gel polymer electrolytes (GPE) have been formulated based on guar gum (GG) crosslinked with poly (ethylene glycol) (PEG 200) incorporating potassium iodide (KI) as the doping salt. The incorporation of PEG 200 into the GPE allows a stable gel polymer electrolyte to form by using dimethyl sulfoxide (DMSO) as the organic solvent. The GPE boasts a structure free from leakage, showcases captivating ionic conductivity and thermal stability. Comprehensive structural and thermal analyses, including Fourier Transform Infrared spectroscopy (FTIR), Differential Scanning Calorimeter (DSC), and Thermogravimetric Analysis (TGA) have been carried out. The electrochemical properties of the GPE were also studied via Electrical Impedance Spectroscopy (EIS) and are significantly enhanced with higher concentration of KI introduced into the GPE. The highest ionic conductivity (σ) value of 9.76 × 10−3 S cm−1 is obtained in the GPE contained 40 wt% KI, with an efficiency of 5.65 %. Importantly, this study introduces a better and effective approach for designing electrolyte materials with high ionic conductivity, efficiency, and stability in DSSC.

Biscrolled hierarchical hybrid structure of PEDOT:PSS/CNTs-NMP yarn based solid state linear supercapacitor for wearable e-textile

The environmental friendly flexible solid state linear supercapacitor (FSLSc) based on the hierarchical hybrid yarn with core-shell type structure of poly(3,4-ethylenedioxythiophene): polystyrenesulfonate (PEDOT:PSS) and hydrophilic carbon nanotubes (CNTs) sheet, fabricated using novel biscrolling technique is proposed. The hierarchical hybrid yarn structure of the electrode establishes the improved electrochemical interface of PEDOT:PSS with the both the hydrophilic CNTs and an aqueous PVA/H3PO4 gel electrolyte. The exterior surface of the yarn electrode rich in PEDOT:PSS which interact with ions from electrolyte and stores charges faradaically while the core region with dense CNTs yarn contributes with its multifunctional capabilities such as EDLC type capacitor, current collector and mechanical support. The observed two-fold decrease in ESR value (∼49Ω) and two-fold increase in capacitance (∼112.76 F/g) for hybrid yarn electrode with N-methyl-2-pyrrolidone (NMP) treated hydrophilic CNTs compared to the one with pristine CNTs, confirms the improved interface of PEDOT:PSS formed with hydrophilic CNTs and aqueous electrolyte. The FSLSc devices with NMP treated CNTs hybrid yarn electrodes exhibited excellent electrochemical performance in terms of the maximum power and energy density of 980 W/kg and 3.799 Wh/kg, respectively. The FSLSc displayed remarkable cycling performance upto 5000 cycles of charge-discharge and a robust bending stability after 1000 bending cycles, making it promising for practical application of the next-generation flexible solid state electrochemical energy storage in e-textiles.