Li NMR, ionic conductivity and self-diffusion coefficients of lithium ion and solvent of plasticized organic-inorganic hybrid electrolyte based on PPG-PEG-PPG diamine and alkoxysilanes

Organic-inorganic hybrid electrolytes based on poly(propylene glycol)-block-poly(ethylene glycol)-block-poly(propylene glycol) bis(2-aminopropyl ether) (D2000) complexed with LiClO₄ via the co-condensation of an epoxy trialkoxysilane and tetraethoxysilane have been prepared and plasticized by a solution of ethylene carbonate (EC)/propylene carbonate (PC) mixture (1:1 by weight). The cross-linked hybrid network shows no solvent exudation and retains a large amount of plasticizer over 70 wt.% in stable state. The in situ built in silica network provides the hybrid electrolytes with good mechanical properties. The ionic conductivity of the dry hybrid electrolyte films was enhanced by two orders of magnitude via plasticization, reaching a maximum conductivity value of 4.0 × 10⁻³ S/cm at 30 °C. Variable temperature ⁷Li-{¹H} magic angle spinning (MAS) NMR demonstrated that the Li⁺ cations can be complexed by the polymer network as well as by the plasticizing solvents, but not with the incorporated silica network. Furthermore, the ⁷Li chemical shift change indicated a progressive change in the lithium coordination from lithium-polymer to lithium-solvent with increasing temperatures. The role of the solvents and the mobility of the lithium ions were investigated by pulsed gradient spin echo (PGSE) NMR measurements to elucidate the behavior of the ionic conductivity.     

Effect of surface modified porous inorganic-organic hybrid polyphosphazene nanotubes on the properties of polyethylene oxide based solid polymer electrolytes

2-(2-methyloxyethoxy)ethanol modified poly (cyclotriphosphazene-co-4,4′-sufonyldiphenol) (PZS) nanotubes were synthesized and solid composite polymer electrolytes based on the surface modified polyphosphazene nanotubes added to PEO/LiClO₄ model system were prepared. Differential Scanning Calorimetry (DSC) and Scanning Electron Microscopy (SEM) were used to investigate the characteristics of the composite polymer electrolytes (CPE). The ionic conductivity, lithium ion transference number and electrochemical stability window can be enhanced after the addition of surface modified PZS nanotubes. The electrochemical investigation shows that the solid composite polymer electrolytes incorporated with PZS nanotubes have higher ionic conductivity and lithium ion transference number than the filler SiO₂. Maximum ionic conductivity values of 4.95 × 10⁻⁵ S cm⁻¹ at ambient temperature and 1.64 × 10⁻³ S cm⁻¹ at 80 °C with 10 wt % content of surface modified PZS nanotubes were obtained and the lithium ion transference number was 0.41. The good chemical properties of the solid state composite polymer electrolytes suggested that the inorganic-organic hybrid polyphosphazene nanotubes had a promising use as fillers in solid composite polymer electrolytes and the PEO₁₀-LiClO₄-PZS nanotubes solid composite polymer electrolyte can be used as a candidate material for lithium polymer batteries.     

NMR, conductivity and DSC study of Li transport in ethylene glycol/citric acid polymer gel

In this present paper the influence of viscosity on the ionic dynamics of polymer gel electrolytes prepared by the Pechini polymeric precursor method is investigated by impedance spectroscopy, differential scanning calorimetric (DSC) and NMR techniques. Polymer gel electrolytes are formed by ethylene glycol (EG) and citric acid (CA) and lithium perchlorate. Room temperature conductivity of the order of 2.3 × 10⁻⁴ S/cm was obtained for the sample of EG/CA:LiClO₄ with lower viscosity (η = 197 cP). The results show that the ionic conductivity of the electrolytes increases for decreasing viscosity. Proton (¹H) and Lithium (⁷Li) NMR lineshapes and spin-lattice relaxation times were measured as a function of temperature and viscosity (197-868 cP). The ⁷Li relaxation process was found to be dominated by quadrupolar couplings. The activation energy extracted from the ¹H and ⁷Li relaxation data (∼0.23 eV) was found to be independent of the viscosity of the gel electrolyte. The ⁷Li NMR relaxation results indicate an increase of the lithium ion mobility with decreasing viscosity.     

Influence of molecular weight of PEG on the property of polymer gel electrolyte and performance of quasi-solid-state dye-sensitized solar cells

A new kind of polymer gel electrolyte based on poly(acrylic acid)-poly(ethylene glycol) (PAA-PEG) hybrid was synthesized. The factor of molecular weight of PEG in the hybrid plays an important role in determining the liquid electrolyte absorbency of the hybrid and ionic conductivity of the polymer gel electrolyte, sequentially affects the photovoltaic performance of quasi-solid-state dye-sensitized solar cells. Using the hybrid with PEG molecular weight of 20,000, a polymer gel electrolyte with liquid electrolyte absorbency of 6.9 g g⁻¹ and ionic conductivity of 5.35 mS cm⁻¹ was obtained. Based on the polymer gel electrolyte, a quasi-solid-state dye-sensitized solar cell with conversion efficiency of 5.25% was achieved under irradiation of AM 1.5, 100 mW cm⁻².     

The study on the conductivity and morphology of polyurethaneurea electrolytes based on poly(ethylene glycol) 2000 and LiClO4

Polyurethaneureas (PUU), which were synthesized from 4,4′-diphenylmethane diisocyanate (MDI), poly(ethylene glycol) (PEG, MW=2000), and 3,5-diaminobenzoic acid, were used as the matrix of the polyelectrolytes in this study. Differential scanning calorimetry (DSC), Fourier-transform infrared spectroscopy (FT-IR), and ⁷Li magic angle spinning (MAS) solid-state NMR were used to monitor changes in the morphology of PUU electrolytes corresponding to the concentration of lithium perchlorate (LiClO₄) dopants. The results of DSC and FT-IR indicate the different polymer complexes formed by the interaction of the Li⁺ ions with the different coordination sites of PUU. The ⁷Li MAS solid-state NMR investigation of the PUU electrolytes points out that two different Li⁺ environments exist at lower temperature. The results of DSC and the ⁷Li MAS solid-state NMR show that Li⁺ ions are preferentially coordinated to the ether oxygen of the PEG soft-segment when the salt concentration is below 0.1 mmol LiClO₄(gPUU)⁻¹. Impedance spectroscopy measurements show that the conductivity behavior followed the Arrhenius equation and was influenced by the hard-segment T_g. One of the PUU electrolytes under the investigation has an ionic conductivity as high as 3.0×10⁻⁵ S cm⁻¹ at 30 °C.     

Influence of ionic additives NaI/I2 on the properties of polymer gel electrolyte and performance of quasi-solid-state dye-sensitized solar cells

The ionic additives NaI/I₂ in polymer gel electrolyte not only provide cations, but also affect the liquid electrolyte absorbency of the poly(acrylic acid)-poly(ethylene glycol) hybrid, which results in the change of ionic conductivity of polymer gel electrolyte and the photovoltaic performance of quasi-solid-state dye-sensitized solar cell. With the optimized components of liquid electrolyte containing 0.5 M NaI, 0.05 M I₂, 0.4 M pyridine, 70 vol.% γ-butyrolactone and 30 vol.% N-methylpyrrolidone, a 4.74% power conversion efficiency of quasi-solid-state dye-sensitized solar cell was obtained under 100 mW cm⁻² (AM 1.5) irradiation.     

Preparation and characterization of gel polymer electrolytes based on acrylonitrile-methoxy polyethylene glycol (350) monoacrylate-lithium acrylate terpolymers

The acrylonitrile (AN)-methoxy polyethylene glycol (350) monoacrylate (MPGA)-lithium acrylate (LiAc) copolymers (PAMGLiAc) was synthesized by emulsion polymerization. Phase inversion technique was used to prepare the PAMGLiAc microporous membrane. The gel polymer electrolytes (GPEs) with the PAMGLiAc were obtained by the copolymer microporous membrane soaking liquid electrolyte. The component and structure of the PAMGLiAc were characterized by IR, NMR and TGA/DSC measurement. The electrochemical characteristics of the PAMGLiAc gel electrolytes were investigated in terms of different composition. The ionic conductivity exceeded 2.0 × 10⁻³ S/cm at ambient temperature, and this system also showed good mechanical properties and a sufficient electrochemical stability with a decomposition voltage as much as 5 V vs. Li to allow far wider operation in the rechargeable lithium-ion polymer batteries.     

Increasing ionic conductivity and mechanical strength of a plastic electrolyte by inclusion of a polymer

In this contribution we present a soft matter solid electrolyte which was obtained by inclusion of a polymer (polyacrylonitrile, PAN) in LiClO₄/LiTFSI-succinonitrile (SN), a semi-solid organic plastic electrolyte. Addition of the polymer resulted in considerable enhancement in ionic conductivity as well as mechanical strength of LiX-SN (X = ClO₄, TFSI) plastic electrolyte. Ionic conductivity of 92.5%-[1 M LiClO₄-SN]:7.5%-PAN (PAN amount as per SN weight) composite at 25 °C recorded a remarkably high value of 7 × 10⁻³ Ω⁻¹ cm⁻¹, higher by few tens of order in magnitude compared to 1 M LiClO₄-SN. Composite conductivity at sub-ambient temperature is also quite high. At −20 °C, the ionic conductivity of (100 − x)%-[1 M LiClO₄-SN]:x%-PAN composites are in the range 3 × 10⁻⁵-4.5 × 10⁻⁴ Ω⁻¹ cm⁻¹, approximately one to two orders of magnitude higher with respect to 1 M LiClO₄-SN electrolyte conductivity. Addition of PAN resulted in an increase of the Young's modulus (Y) from Y → 0 for LiClO₄-SN to a maximum of 0.4 MPa for the composites. Microstructural studies based on X-ray diffraction, differential scanning calorimetry and Fourier transform infrared spectroscopy suggest that enhancement in composite ionic conductivity is a combined effect of decrease in crystallinity and enhanced trans conformer concentration.     

Hybrid inorganic-organic polymer electrolytes: synthesis, FT-Raman studies and conductivity of {Zr[(CH2CH2O)8.7]ρ/(LiClO4)z}n network complexes

This paper describes the synthesis and characterization of three-dimensional hybrid inorganic-organic networks prepared by a polycondensation reaction between Zr(O(CH₂)₃CH₃)₄ and polyethylene glycol 400 (PEG400). Eleven hybrid networks doped with varying concentrations of LiClO₄ salt were prepared. On the basis of analytical data and FT-Raman studies it was concluded that these polymer electrolytes consist of inorganic-organic networks with zirconium atoms bonded together by PEG400 bridges. These polymers are transparent with a solid rubber consistency and are very stable under inert atmosphere. Scanning electron microscopy revealed a smooth glassy surface. X-ray fluorescence microanalysis with energy dispersive spectroscopy demonstrated that all the constituent elements are homogeneously distributed in the materials. Thermogravimetric measurements revealed that these materials are thermally stable up to 262 °C. Differential Scanning Calorimetry measurements indicated that the glass transition temperature T_g of these inorganic-organic hybrids varies from −43 to −15 °C with increasing LiClO₄ concentration. FT-Raman investigations revealed the TGT (T=trans, G=gauche) conformation of polyether chains and allowed characterization of the types of ion-ion and ion-polymer host interactions in the bulk materials. The conductivity of the materials at different temperatures was determined by impedance spectroscopy over the 20 Hz-1 MHz frequency range. Results indicated that the materials conduct ionically and that their ionic conductivity is strongly influenced by the segmental motion of the polymer network and the type of ionic species distributed in the bulk material. Finally, it is to be highlighted that the hybrid network with a n_Li/n_O molar ratio of 0.0223 shows a conductivity of ca. 1×10⁻⁵ S cm⁻¹ at 40 °C.     

Li NMR spectroscopy and ion conduction mechanism of composite gel polymer electrolyte: A comparative study with variation of salt and plasticizer with filler

Microporous composite gel polymer electrolyte (CGPE) has been prepared by incorporating the home-made silica aerogel (SAG) particles into the poly(vinylidene fluoride-co-hexafluoropropylene) (PVdF-HFP) copolymer/LiClO₄ matrix. The ionic transport behavior of the electrolyte is studied with various experimental techniques such as AC impedance, X-ray diffraction (XRD), infrared (IR) spectra, nuclear magnetic resonance (NMR), scanning electron microscopy (SEM), differential scanning calorimetry (DSC) and thermogravimetric analyzer (TGA), etc. The results reveal that the SAG particles are well dispersed in the electrolytes and incorporate with the other components of the CGPEs. The solid-state ⁷Li NMR study has confirmed the interactions of lithium ion with SAG, polymer and plasticizers, causing to form the microporous structure and reduce the glass transition temperature and crystallinity, resulting in an increase in ionic conductivity of the CGPE. The best ionic conductivity (1.04 × 10⁻² S/cm at room temperature) is obtained from the composite polymer electrolyte containing 4 wt% of SAG, which is approximately four times higher than the ionic conductivity of the electrolyte without the filler.     

Polymer electrolytes based on poly(ethylene glycol) dimethyl ether and the ionic liquid 1-butyl-3-methylimidazolium hexafluorophosphate: Preparation, physico-chemical characterization, and theoretical study

Polymer electrolytes based on poly(ethylene glycol) dimethyl ether (PEGdME) and the ionic liquid (IL) 1-butyl-3-methylimidazolium hexafluorophosphate ([bmim]PF₆) have been prepared and characterized by different techniques. Coordination of the IL by the polymer occurs mainly in the amorphous phase. This finding was correlated with previous theoretical investigations of a similar model for polymer electrolytes based on poly(ethylene oxide), PEO, and IL. It has been obtained ionic conductivity σ ∼ 10⁻³ S cm⁻¹ for the polymer electrolyte with 35 wt% of IL at 100 °C. The same order of magnitude for σ was obtained by molecular dynamics simulation of PEO/IL. This work demonstrates consistency between experimental and theoretical results for polymer electrolytes containing ionic liquids.     

A microporous gel electrolyte based on poly(vinylidene fluoride-co-hexafluoropropylene)/fully cyanoethylated cellulose derivative blend for lithium-ion battery

A gel polymer electrolyte based on the blend of poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) and fully cyanoethylated cellulose derivative (DH-4-CN) was prepared and characterized. Thermal, mechanical, swelling, liquid electrolyte retention and electrochemical properties, as well as microstructures of the prepared polymer electrolytes, were investigated using thermogravimetric analysis, electrochemical impedance spectroscopy, linear sweep voltammetry, and scanning electron microscopy. The results showed that the addition of DH-4-CN could obviously improve the conductivity of PVDF-HFP based electrolyte. The maximum ionic conductivity of 4.36 mS cm⁻¹ at 20 °C can be obtained for PVDF-HFP/DH-4-CN 14:1 in the presence of 1 M LiPF₆ in EC and DMC (1:1, w/w). The dry blend membranes exhibit excellent thermal behavior. All the blend electrolytes are electrochemically stable up to about 4.8 V vs. Li/Li⁺ for all compositions. The results reveal that the composite polymer electrolyte qualifies as a potential application in lithium-ion battery.     

Ternary polymer electrolytes with 1-methylimidazole based ionic liquids and aprotic solvents

New polymer gel electrolytes containing ionic liquids were developed for modern chemical power sources—supercapacitors and lithium-ion batteries. Ternary systems polymer-ionic liquid-aprotic solvent as well as materials containing also lithium salts (LiClO₄ or LiPF₆) were prepared by direct, thermally initiated polymerisation. Poly(2-ethoxyethyl methacrylate) PEOEMA was combined with various ionic liquids based on 1-methylimidazole. Only 1-butyl-3-methylimidazolium hexafluorophosphate BMIPF₆ formed a homogenous and slightly translucent polymer electrolyte, where aprotic solvents—propylene carbonate and ethylene carbonates were used as plasticisers. Materials were studied using the electrochemical and thermogravimetric methods and exhibit high ionic conductivity up to 0.94 mS cm⁻¹ at 25 °C together with high electrochemical stability: the accessible potential window on the glassy carbon was found ca. 4.3 V. Prepared non-volatile materials are long-term and thermally stable up to 150 °C.     

Ionic conductivity in polyethylene-b-poly(ethylene oxide)/lithium perchlorate solid polymer electrolytes

The ionic conductivity and phase arrangement of solid polymeric electrolytes based on the block copolymer polyethylene-b-poly(ethylene oxide) (PE-b-PEO) and LiClO₄ have been investigated. One set of electrolytes was prepared from copolymers with 75% of PEO units and another set was based on a blend of copolymer with 50% PEO units and homopolymers. The differential scanning calorimetry (DSC) results, for electrolytes based on the copolymer with 75% of PEO units, were dominated by the PEO phase. The PEO block crystallinity dropped and the glass transition increased with salt addition due to the coordination of the cation by PEO oxygen. The conductivity for copolymers 75% PEO-based electrolyte with 15 wt% of salt was higher than 10⁻⁵ S/cm at room temperature and reached to 10⁻³ S/cm at 100 °C on a heating measurement. The blend of PE-b-PEO (50% PEO)/PEO/PE showed a complex thermal behavior with decoupled melting of the blocks and the homopolymers. Upon salt addition the endotherms associated with PEO domains disappeared and the PE crystals remained untouched. The conductivity results were limited at 100 °C to values close to 10⁻⁴ S/cm and at room temperature values close to 3 × 10⁻⁶ S/cm were obtained for the 15 wt% salt electrolyte. Raman study showed that the ionic association of the highly concentrated blend electrolytes at room temperature is not significant. Therefore, the lower values of conductivity in the case of the blend with 50% PEO can be assigned to the higher content of PE domains leading to a morphology with lower connectivity for ionic conduction both in the crystalline and melted state of the PE domains.     

The conductivity and characterization of the plasticized polymer electrolyte based on the P(AN-co-GMA-IDA) copolymer with chelating group (II): The effect of free ion in the plasticized polymer electrolyte

A new gel-type polymer electrolyte (GPE) was made by the copolymerizing acrylonitrile (AN) and (2-methylacrylic acid 3-(bis-carboxymethylamino)-2-hydroxy-propyl ester) (GMA-IDA). The copolymer mixed with a plasticizer—propylene carbonate (PC) and lithium salt to form GPE. The lithium salts are LiCF₃SO₃, LiBr and LiClO₄. FT-IR spectra show that the lithium ion in the LiClO₄ system has the strongest interaction with the group based on the plasticized polymer. FT-IR spectra also indicate that CF₃SO₃⁻ prefers producing anion-cation association. Moreover, the ¹³C solid state NMR spectra for the carbons attached to the PC of GPE exhibited different level of chemical shift (158.5 ppm) when the different lithium salts were added to the electrolyte. The results of differential scanning calorimeter (DSC) also indicate that the LiClO₄ system has more free lithium ions; therefore, it has the maximum conductivity. In this study, the highest conductivity 2.98 × 10⁻³ S cm⁻¹ exists in AG2/PC = 20/80 wt.% system which contain 3 mmole (g-polymer)⁻¹ LiClO₄. Additionally, the polymer electrolytes, which contain GMA-IDA have better interfacial resistance stability with lithium electrode.     

Composite alkaline polymer electrolytes and its application to nickel-metal hydride batteries

In order to enhance the ionic conductivity of polyethylene oxide (PEO)-KOH based alkaline polymer electrolytes, three types of nano-powders, i.e., TiO₂, β-Al₂O₃ and SiO₂ were added to PEO-KOH complex, respectively, and the corresponding composite alkaline polymer electrolytes were prepared. The experimental results showed that the prepared polymer electrolytes exhibited higher ionic conductivities at room temperature, typically 10⁻³ S cm⁻¹ as measured by ac impedance method, and good electrochemical stability. The electrochemical stability window of ca. 1.6 V was determined by cyclic voltammetry with stainless steel blocking electrodes. The influence of the film composition such as KOH, H₂O and nano-additives on ion conductivity was investigated and explained. The temperature dependence of conductivity was also determined. In addition, polyvinyl alcohol (PVA)-sodium carboxymethyl cellulose (CMC)-KOH alkaline polymer electrolytes were obtained using solvent casting method. The properties of the polymer electrolytes were characterized by ac impedance, cyclic voltammetry and differential thermal analysis methods. The ionic conductivity of the prepared PVA-CMC-KOH-H₂O electrolytes can reach the order of 10⁻² S cm⁻¹. The effect of CMC addition on the alkaline polymer electrolytes was also explained. The experimental results demonstrated that the PVA-CMC-KOH-H₂O polymer electrolyte could be used in Ni/MH battery.     

1-Alkyl-2,3-dimethylimidazolium bis(trifluoromethanesulfonyl)imide ionic liquids as highly safe electrolyte for Li/LiFePO4 battery

Several 1-alkyl-2,3-dimethylimidazolium bis(trifluoromethanesulfonyl)imide ionic liquids (alkyl-DMimTFSI) were prepared by changing carbon chain lengths and configuration of the alkyl group, and their electrochemical properties and compatibility with Li/LiFePO₄ battery electrodes were investigated in detail. Experiments indicated the type of ionic liquid has a wide electrochemical window (−0.16 to 5.2 V vs. Li⁺/Li) and are theoretically feasible as an electrolyte for batteries with metallic lithium as anode. Addition of vinylene carbonate (VC) improves the compatibility of alkyl-DMimTFSI-based electrolytes towards lithium anode and LiFePO₄ cathode, and enhanced the formation of solid electrolyte interface to protect lithium anodes from corrosion. The electrochemical properties of the ionic liquids obviously depend on carbon chain length and configuration of the alkyl, including ionic conductivity, viscosity, and charge/discharge capacity etc. Among five alkyl-DMimTFSI-LiTFSI-VC electrolytes, Li/LiFePO₄ battery with the electrolyte-based on amyl-DMimTFSI shows best charge/discharge capacity and reversibility due to relatively high conductivity and low viscosity, its initial discharge capacity is about 152.6 mAh g⁻¹, which the value is near to theoretical specific capacity (170 mAh g⁻¹). Although the battery with electrolyte-based isooctyl-DMimTFSI has lowest initial discharge capacity (8.1 mAh g⁻¹) due to relatively poor conductivity and high viscosity, the value will be dramatically added to 129.6 mAh g⁻¹ when 10% propylene carbonate was introduced into the ternary electrolyte as diluent. These results clearly indicates this type of ionic liquids have fine application prospect for lithium batteries as highly safety electrolytes in the future.     

Synthesis and characterization of a new hyperbranched organic–inorganic solid polymer electrolyte with cyanuric chloride as a core element

A new hyperbranched organic–inorganic hybrid electrolyte based on the use of 2,4,6-trichloro-1,3,5-triazine (cyanuric chloride, CC) as the coupling core to couple with oligo(oxyalkylene)-amines, followed by condensation with (3-glycidoxypropyl)-trimethoxysilane (GLYMO) and complexed with LiClO₄, has been prepared and characterized. The Vogel–Tamman–Fulcher (VTF) like conductivity behavior is observed in the present organic–inorganic hybrid electrolytes with a maximum ionic conductivity value of 4.4 × 10⁻⁵ S cm⁻¹ at 30 °C. Multinuclear NMR techniques are used to provide a microscopic view for the specific interaction between the polymer chains and Li⁺ cations and their dynamic behaviors. The results of 2D ¹H–¹³C wide-line separation (WISE) and ⁷Li static line NMR width measurements divulge that the mobility of the ⁷Li cations is strongly related to a dynamic environment created by the polymer motion in the amorphous phase. The combined results of conductivity and ⁷Li pulse-gradient spin-echo (PGSE) NMR self-diffusion coefficient measurements reveal that the conductivity enhancement at low salt concentrations is mainly caused by the high mobility of the lithium cations.     

Synthesis and electrochemical characterization of PEO-based polymer electrolytes with room temperature ionic liquids

New gel polymer electrolytes containing 1-butyl-4-methylpyridinium bis(trifluoromethanesulfonyl)imide (BMPyTFSI) ionic liquid are prepared by solution casting method. Thermal and electrochemical properties have been determined for these gel polymer electrolytes. The addition of BMPyTFSI to the P(EO)₂₀LiTFSI electrolyte results in an increase of the ionic conductivity, and at high BMPyTFSI concentration (BMPy⁺/Li⁺ = 1.0), the ionic conductivity reaches the value of 6.9 × 10⁻⁴ S/cm at 40 °C. The lithium ion transference numbers obtained from polarization measurements at 40 °C were found to decrease as the amount of BMPyTFSI increased. However, the lithium ionic conductivity increased with the content of BMPyTFSI. The electrochemical stability and interfacial stability for these gel polymer electrolytes were significantly improved due to the incorporation of BMPyTFSI.     

Preparation of a microporous polymer electrolyte based on poly(vinyl chloride)/poly(acrylonitrile-butyl acrylate) blend for Li-ion batteries

Poly(acrylonitrile-co-butyl acrylate) (P(AN-co-BuA))/poly(vinyl chloride) (PVC) blend-based gel polymer electrolyte (BGPE) was prepared for lithium-ion batteries. The P(AN-co-BuA)/PVC BGPE consists of an electrolyte-rich phase, which is mainly composed of P(AN-co-BuA) and liquid electrolyte, acting as a conducting channel and a PVC-rich phase that provides mechanical strength. The dual phase was just simply developed by the difference of miscibility properties in solvent, PC, between P(AN-co-BuA) and PVC. The mechanical strength of this new blend electrolyte was found to be much higher, with a fracture stress as high as 29 MPa in dry membrane and 21 MPa in gel state, than that of a previously reported P(AN-co-BuA)-based gel polymer electrolyte. The blended gel polymer electrolyte showed ionic conductivity of higher than 1.5 × 10⁻³ S cm⁻¹ and electrochemical stability up to at least 4.8 V. The results showed that the as-prepared gel polymer electrolytes were promising materials for lithium-ion batteries.