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PubMed2002

Reagentless biosensors based on co-entrapment of a soluble redox polymer and an enzyme within an electrochemically deposited polymer film.

A novel biosensor architecture, which is based on the combination of a manual and a non-manual deposition technique for sensor components on the electrode surface is reported. A water-soluble Os-poly(vinyl-imidazole) redox hydrogel is deposited on a graphite electrode by drop-coating (i.e. manually) followed by the electrochemically-induced deposition of an enzyme-containing non-conducting polymer film. The local polymer deposition is initiated by electrochemical generation of H(3)O(+) exclusively at the electrode surface causing a pH-shift to be established in the diffusion zone around the electrode (i.e. non-manually). This pH-shift leads to the protonation of a dissolved polyanionic polymer which in consequence changes significantly its solubility and is hence precipitating on the electrode surface. In the presence of a suitable enzyme, such as quinohemoprotein alcohol dehydrogenase (QH-ADH), the polymer precipitation leads to an entrapment of the redox enzyme within the polymer film. Simultaneously, the water-soluble Os-poly(vinyl-imidazole) redox hydrogel, which is slowly dissolving from the electrode surface after addition of the electrolyte, is co-entrapped within the precipitating polymer layer. This provides the pre-requisite for an efficient electron-transfer pathway from the redox enzyme via the polymer-bound redox centres to the electrode surface. The sensor preparation protocol has been optimised aiming on a high mediator concentration in the polymer film and an effective electron transfer.

Alcohol Oxidoreductases↗
PubMed2007

pH-controlled, polymer-mediated assembly of polymer micelle nanoparticles.

We describe pH-controlled, polymer-mediated assembly of polymer micelles in aqueous media based on reversible complexation between the micelles of pyrene-labeled poly(epsilon-caprolactone)-b-poly(carboxylic acid) copolymers and proton-accepting water-soluble polymers such as poly(ethylene glycol) (PEG), poly(2-ethyl-2-oxazoline) (PEtOz), and poly(1-vinylpyrrolidone) (PVP). The key factor determining assembly phenomena was identified as the modulation of hydrogen-bonding interaction between ionizable anionic micellar shells and the proton-accepting polymers by the pH control. As pH decreased from 7.4 to 2.0, the mixture of the polymer micelles and polymers underwent assembly and formed solid hybrids at specific pH values. The micelles assembled in the hybrid could be reversibly dispersed as micelles above specific pH ranges. The assembly/disassembly behavior as well as phase transitions of the micelle/proton-accepting polymer could be precisely controlled by adjusting pH. This assembling behavior depended on the rationally designed parameters such as the chemical structure and length of micellar shell-forming poly(carboxylic acid)s and the class of proton-accepting polymers.

Chemistry, Physical↗
PubMed2000

Antithrombogenic polymer alloy composed of 2-methacryloyloxyethyl phosphorylcholine polymer and segmented polyurethane.

To evaluate the antithrombogenicity of a new polymeric biomaterial in vivo, a polymer alloy tube composed of poly[2-methacryloyloxyethyl phosphorylcholine(MPC)-co-2-ethylhexyl methacrylate](PMEH) polymer and a segmented polyurethane (SPU) was prepared by a solvent evaporation method on a Teflon rod from a homogeneous solution containing both the PMHE and SPU. The composition of the PMEH vs the SPU was 10 wt%. The inner and outer surfaces of the polymer alloy tubing were characterized by X-ray electron spectroscopic (XPS) measurements. The MPC units were located on the inner surface of the polymer alloy tubing rather than the outer surface. After immersion in aqueous media, a higher concentration of the MPC units was observed on both surfaces. Selective staining of the MPC units with osmium tetraoxide was carried out to observe the morphology of the PMEH domain on the surface of the polymer alloy. There were large-sized PMEH domains on the inner surface of the tubing but small-sized domains were found on the outer surface. This result was in good agreement with the XPS results. Blood compatibility of the polymer alloy was evaluated by observation of fibrinogen adsorption and platelet adhesion from human plasma. A lot of fibrinogen was adsorbed and many platelets adhered to the inner surface of the original SPU tubing. On the other hand, the PHEH/SPU polymer alloy tubing suppressed these adsorptions and adhesions. When the PMEH/SPU polymer alloy tubing was implanted into a rabbit's artery, thrombus could not be observed even after a 7-day implantation but the original SPU tubing was almost totally occluded only after a 90-min implantation due to serious thrombus deposition on the surface. These results clearly indicated that the PMEH in the SPU matrix acted as an antithrombus reagent by suppression of protein adsorption and platelet adhesion and activation. Particularly, the MPC units played a significant role in this function.

Adsorption↗
PubMed2002

Polymer depletion-induced instability of silica suspensions in the presence of flexible and semiflexible polymers.

Polymer depletion-induced instability of silica suspensions in dilute toluene solutions of flexible polystyrene (PS) or semiflexible poly(hexyl isocyanate) (PHIC) was investigated by direct observation and oscillatory moduli measurements as functions of silica volume fraction and polymer molecular weight. Addition of the respective polymers to the gelled silica suspensions induces a gel settling. Below the silica volume fraction phi=4 vol%, PS chains compress the volume of the sediment silica phase, whereas PHIC chains expand it and play a role in swelling agents. Thus, PHIC chains lead to the formation of aggregates in the silica suspensions that are larger and less compact than those formed by the PS chains. On the other hand, above phi=4 vol% where the silica suspension occurs gelation, the effect of nonadsorbing polymers on changes in the volume of the silica phase is opposite. Moreover, polymer depletion interaction results in a mechanically stronger gelled phase, leading to the storage modulus G' values larger than those without polymer, but the effects of polymer concentration and polymer molecular weight on the G' values are not clear.

Journal Article↗
PubMed2006

Ion and polymer dynamics in polymer electrolytes PPO-LiClO4. I. Insights from NMR line-shape analysis.

We investigate ion and polymer dynamics in polymer electrolytes PPO-LiClO4 performing 2H and 7Li NMR line-shape analysis. Comparison of temperature dependent 7Li and 2H NMR spectra gives evidence for a coupling of ion and polymer dynamics. 2H NMR spectra for various salt concentrations reveal a strong slowdown of the polymer segmental motion when the salt content is increased. The 2H NMR line shape further indicates that the segmental motion is governed by dynamical heterogeneities. While the width of the distribution of correlation times G(log tau) is moderate for low and high salt content, an extremely broad distribution exists for an intermediate salt concentration of 15:1 PPO-LiClO4. For the latter composition, a weighted superposition of two spectral components, reflecting the fast and the slow polymer segments of the distribution, describes the 2H NMR line shape over a broad temperature range. Analysis of the temperature dependent relative intensity of both spectral components indicates the existence of a continuous rather than a discontinuous distribution G(log tau). Such continuous distribution is consistent with gradual fluctuations of the local salt concentration and, hence, of the local environments of the polymer segments, whereas it is at variance with the existence of large salt-depleted and salt-rich domains featuring fast and slow polymer dynamics, respectively. Finally, for all studied PPO-LiClO4 mixtures, the 2H NMR line shape strongly depends on the echo delay in the applied echo-pulse sequence, indicating that the structural relaxation of the polymer segments involves successive rotational jumps about small angles gamma < 20 degrees .

Journal Article↗
PubMed1994

Cell partitioning in two-polymer aqueous phase systems and cell electrophoresis in aqueous polymer solutions. Human and rat young and old red blood cells.

It has recently been found that electrophoresis in solutions of appropriately selected polymers in phosphate-buffered saline (PBS) can differentiate between some closely related cell populations which have identical electrophoretic mobilities (EPM) in PBS (e.g., human young and old red blood cells (RBC); RBC from Alzheimer patients and normal individuals). The EPM differences detected in polymer solutions are most likely a consequence of cell- and polymer-specific interactions. Aspects of the relation between the electrophoresis in aqueous polymer solutions of native and in vitro treated young and old RBC (from human and rat) and their partitioning in a charge-sensitive dextran-poly(ethylene glycol) (PEG) aqueous phase system (i.e., a system with a Donnan potential between the phases, top phase positive) have been examined further and are discussed. Unlike the behavior of RBC from Alzheimer patients and normal individuals in which an EPM difference can be detected in PEG solutions but not in dextran, differences in EPM between human young and old RBC are detectable in solutions of either polymer. Selected enzyme treatments of human young and old RBC or their fixation with aldehyde eliminates the EPM differences in dextran; while neuraminidase treatment or formaldehyde fixation of rat young and old RBC retains EPM differences in dextran between these cells. In these latter cases partitioning differences are also in evidence and are in the same direction as the cells' relative EPM (i.e., old RBC < young RBC). The earlier hypothesis that cell partitioning is 'more sensitive' than cell electrophoresis in detecting differences in surface charge between cells bears reexamination because human young and old RBC, which cannot be differentiated by single-tube partitioning in a charge-sensitive phase system, have different EPM in polymer solutions. The difference between these cells can be detected by partitioning but only by use of a multiple-extraction procedure. It is then found to be in a direction similar to the cells' relative EPM in dextran (i.e., human old RBC > young RBC). Rat young and old RBC have different partitions (rat old RBC < young RBC) and different EPM (also rat old RBC < young RBC). Thus, while cell partitioning in a charge-sensitive dextran-PEG aqueous phase system and cell electrophoresis in polymer solution seem to reflect, at least with these cell subpopulations, qualitatively analogous differences in surface properties (in that increasing partitions and EPM are concomitant), there are instances in which either of these physical measurements discerns surface differences which escape detection by the other.

Aging↗
PubMed1987

Effect of polymer structure on affinity partitioning of lactate dehydrogenase in polymer-water two-phase systems.

Lactate dehydrogenase from rabbit muscle (EC 1.1.1.27) was partitioned between the liquid phases of aqueous two-phase systems containing two kinds of polymers. The partition was influenced by the use of a dye ligand, Procion Yellow HE-3G, bound to a polymer. The ligand-carrying polymers were poly(ethyleneglycol), poly(vinyl alcohol), ethylhydroxyethylcellulose, hydroxypropyl-starch, Ficoll and dextran. Their influence on the partition of lactate dehydrogenase was studied in systems composed of the following pairs of polymers: dextran-poly(ethylene glycol), dextran-poly(vinyl alcohol), dextran-Ficoll and hydroxypropyl-starch-poly (ethylene glycol). The ratio between the change in the logarithmic partition coefficient of the enzyme, delta log K, caused by the ligand and the logarithm of the partition coefficient of the ligand-polymer, log KL-polymer, was used as a measure of the number of ligand polymers bound per enzyme molecule under saturation conditions. Possible explanations for the observed effects are discussed.

Animals↗
PubMed2007

Blends of reverse enteric polymer with Enteric and pH-independent polymers: mechanistic investigations for tailoring drug release.

Blends of conventional reverse enteric polymer with enteric polymers result in insoluble polyelectrolyte complexes and hence cannot be used in film coatings. We report a new set of miscible blends of a new reverse enteric polymer (NREP) synthesized by us with enteric and pH-independent polymers. The nature of interactions between polymers in the blends has been established by analyzing Fourier transform infrared (FTIR) spectra. The extent of interaction has been investigated by thermal analysis and quantified in terms of parameters K1 and K2 in the Schneider equation. Based on these values, the interactions between NREP and these polymers have been ranked in the order EC (ethylcellulose) < ES (Eudragit S) < HPMCP (hydroxypropyl methylcellulose phthalate). The quantification of interactions in blends helps explain the release pattern of cefuroxime axetil (CA) at gastric pH and tailor the release of other drugs according to their pharmacokinetic characteristics. The understanding also provides a more rational approach for selection of polymers and their content in the coating compositions, rather than an empirical approach.

Cellulose↗
PubMed2000

Aqueous polymer two-phase systems formed by new thermoseparating polymers.

A set of new polymers that can be used as phase forming components in aqueous two-phase systems is presented. All polymers studied have thermoseparating properties i.e. form one separate polymer enriched phase and one aqueous solution when heated above the critical temperature. This property makes the polymers attractive alternatives to the polymers used in traditional aqueous two-phase systems such as poly(ethylene glycol) (PEG) and dextran. The thermal phase separation simplifies recycling of the polymers, thus making the aqueous two-phase systems more cost efficient and suitable for use in large scale. Thermoseparating polymers studied have been copolymers of ethylene oxide and propylene oxide (EO-PO), poly (N-isopropylacrylamide) (poly-NIPAM), poly vinyl caprolactam (poly-VCL) and copolymers of N-isopropylacrylamide and vinyl caprolactam with vinyl imidazole (poly(NIPAM-VI) and poly(VCL-VI), respectively). In addition, the copolymer poly(NIPAM-VI) has the property to be uncharged at pH above 7.0 and positively charged at lower pH. This allows the partitioning of protein to be directed by changing the pH in the system instead of the traditional addition of salt to direct the partitioning. Hydrophobically modified EO-PO copolymer (HM-(EO-PO)) with alkyl groups (C14) at both ends forms two-phase system with for example poly(NIPAM-VI). The phase diagram for poly(NIPAM-VI)/HM-(EO-PO) was determined and the model proteins lysozyme and BSA were partitioned in this system. For BSA in poly(NIPAM-VI)/HM-(EO-PO) system a change in pH from 8.0 to 5.4 results in a change of partition coefficient from K = 0.8 to K = 5.1, i.e. BSA could be transferred from the HM-(EO-PO) phase to the poly(NIPAM-VI) phase. BSA partitioning in poly(NIPAM-VI)/HM-(EO-PO) system allows quantitative BSA recovery, and recoveries of poly(NIPAM-VI) and HM-(EO-PO) were 53% and 92%, respectively, after the thermoseparation step.

Animals↗
PubMed1997

The influence of polymer structure on the interactions of cationic polymers with DNA and morphology of the resulting complexes.

Four cationic polymers used to deliver DNA into cultured cells: polylysine, intact polyamidoamine dendrimer, fractured polyamidoamine dendrimer and polyethylenimine, are examined for their ability to interact with DNA. Complexes between the polymers and DNA were examined using electron microscopy. Similar toroidal structures with diameters of 55 +/- 12 nm were formed from all of the cationic polymers with DNA. The DNA complexes of the fractured dendrimer and polyethylenimine were observed as single, distinct units; their apparent diameters in solution as measured by dynamic light scattering ranged from 90 to 130 nm. The DNA complexes of polylysine and intact dendrimer generally appeared as clusters in electron micrographs; their diameters in solution were larger than 1000 nm, which suggests that their toroidal complexes aggregate in solution. The cationic polymers bind to DNA in a stoichiometry that is nearly 1:1 in primary amines to DNA phosphates. The apparent binding of all cationic polymers to DNA decreases linearly with increasing ionic strength, up to 0.8 M NaCl. Thus, at the concentrations studied, these polymers interact electrostatically with DNA forming a unit structure with toroidal morphology; the extent of aggregation of the unit structures in solution depends upon the characteristics of the individual polymer.

Animals↗
PubMed1980

A two-step synthesis of new water-soluble polymers of NAD+ and ADP. The biological properties of these polymers.

Alkylation at the N-1 position of the adenine moiety of NAD+, ADP or ATP with 2,3-epoxypropyl acrylate, followed by polymerization with or without acrylamide at pH 8, gave water-soluble polymers of NAD+ and ADP where the alkyl chain was located at the exocyclic adenine C-6 amino group. Cofactor incorporations were good to high: 145-447 mumol NAD+/g polymer and 667 mumol ADP/g polymer. About 30% of the bound NAD+ could be reduced with rabbit muscle lactae dehydrogenase, yeast alcohol dehydrogenase and Bacillus subtilis alanine dehydrogenase; 84% of the bound ADP was phosphorylated with rabbit muscle creatine kinase. High cofactor activities were obtained with polymerized NAD+ with alcohol dehydrogenase as enzyme: the initial rate of NAD+ polymer reduction was 35-81% that of free NAD+. These values remained substantially high with agarose-immobilized alcohol dehydrogenase (15-36%) and should eventually allow their use in continuous enzymatic reactors. Enzymatic phosphorylation of ADP polymer by creatine kinase gave an ATP polymer with high biological activity: 480 mumol ATP/g polymer were transformed with yeast hexokinase.

Acrylic Resins↗
PubMed1976

Enzymatic attack on side chains of synthetic polymers. Chymotrypsin-catalyzed hydrolysis of specific substrate groups attached to acrylamide or acrylic acid co-polymers.

Three vinyl monomers, M-1, M-3, and M-5, in which L-phenylalanine p-nitroanilide was acylated with CH2==CHCONH(CH2)nCO--(n = 1, 3, 5) were synthesized. They were co-polymerized with a large excess of acrylamide (co-polymers PAm-1, PAm-3, and PAm-5) and with a large excess of acrylic acid (co-polymers PAc=1, PAc-3, and PCc-5). In addition, M-5 was co-polymerized with acrylamide containing 2.8 mol % of the hydrophobic monomer N-acrylyl-1-naphthylamine (co-polymer PAm-5N). The rates of the chymotrypsin-catalyzed hydrolysis of the nitroanilide groups of M-5 and the various co-polymers were determined over a range of pH. For some of the systems data were also obtained over a range of substrate concentrations to derive values for Vmax and Km. Results obtained with PAm-5 were found to be independent of the chain length of the co-polymer. At pH 7, 25 degrees and with 2.7 X 10(-6) M enzyme, Vmax values for M-5, PAm-k, PAm-5N, and PAc-5 were 5.5, 5.5, 10, and 3.6 X 10(-8) M/S, while Km values were 8.5, 16.5, 10, and 2.2 X 10(-5),respectively, With PAc-5, the pH activity profile was shifted to higher acidities as compared to the profiles obtained with M-5 and PAm-5. The susceptibility of the co-polymers to chymotrypsin attack decreases sharply with a decreasing spacing of the L-phenylalanine p-nitroanilide residue from the backbone of the polymer chains.

Acrylamides↗
PubMed2001

Preservation of platelet function on 2-methacryloyloxyethyl phosphorylcholine-graft polymer as compared to various water-soluble graft polymers.

The chemical structures of water-soluble polymers grafted onto PE surfaces affect platelet function when the platelets contact the polymer surfaces. To improve our understanding of this effect, this study sought to control the blood/materials interaction on the surfaces of polyethylene (PE) by grafting with various water-soluble polymers. Such polymers as poly(2-methacryloyloxyethyl phosphorylcholine) (PMPC), poly(acrylamide) (PAAm), poly(N-vinylpyrrolidone) (PVPy), and poly[monomethacryloyl poly(ethylene glycol)] (PMPEG) were grafted on low-density PE sheets by photoinduced graft polymerization. Both the PE bags modified with water-soluble polymers and those nonmodified were prepared by heat processing. Activation of platelets after storage in the PE bags was evaluated by measuring the cytoplasmic free calcium ion concentration ([Ca(2+)]i). The concentration of [Ca(2+)]i of platelets in contact with the PE surface grafted with PMPC was the same as that of native platelets and significantly less than that in contact with other PE surfaces grafted with water-soluble polymers. The number of adherent platelets was effectively decreased on PE surfaces grafted with PMPC and PMPEG, as compared with nontreated PE. The aggregation ability of platelets was also measured after storage of platelet-rich plasma in the PE bags. The PE surface grafted with PMPC effectively maintained aggregation ability as compared with both the nontreated PE and with PE grafted with PAAm, PVPy, and PMPEG. It was concluded that for preserving platelet function, PMPC was the most effective of these water-soluble polymers used for surface modification.

Animals↗
PubMed2006

A detailed discussion of the influence of the amount of deposited polymer on the retention properties of polymer-coated silicas.

Problems of the modification of the surface of micro-spherical silica gel with layers of polymer and the influence of the quantity of the coated polymer on the chromatographic properties of the resulting sorbents have been considered. The polymer modification of the surface of wide-pore micro-spherical silica gel obtained by means of hydrothermal treatment of the meso-porous silica gel under autoclave conditions is described. The polymer layer itself is formed by an octadecylmethacrylate-methylmethacrylate co-polymer. As a result, packings for RP-HPLC were obtained. An increase of the capacity factor (k) has been observed with an increase of the quantity of the polymer deposited during the polymer modification process. The indicated phenomenon depends on the increase of the number of C18 groups in the packing.

Journal Article↗
PubMed2001

Lipid membrane expansion and micelle formation by polymer-grafted lipids: scaling with polymer length studied by spin-label electron spin resonance.

Spin-label electron spin resonance (ESR) spectroscopy and auxiliary optical density measurements are used to study lipid dispersions of N-poly(ethylene glycol)-dipalmitoyl phosphatidylethanolamine (PEG:5000-DPPE) mixed with dipalmitoyl phosphatidylcholine (DPPC). PEG:5000-DPPE bears a large hydrophilic polymer headgroup (with approximately 114 oxyethylene monomers) and is commonly used for steric stabilization of liposomes used in drug delivery. Comparison is made with results from mixtures of DPPC with polymer lipids bearing shorter headgroups (approximately 45 and 8 oxyethylene monomers). ESR spectra of phosphatidylcholine spin-labeled on the 5-C atom position of the sn-2 chain are shown to reflect the area expansion of the lipid membranes by the lateral pressure exerted in the polymer brush, in a way that is consistent with theory. The lipid chain packing density at the onset of micelle formation is the same for all three PEG-lipids, although the mole fraction at which this occurs differs greatly. The mole fraction at onset scales inversely with the size of the polymer headgroup, where the experimental exponent of 0.7 is close to theoretical predictions (viz. 0.55-0.6). The mole fraction of PEG-lipid at completion of micelle formation is more weakly dependent on polymer size, which conforms with theoretical predictions. At high mole fractions of PEG:5000-DPPE the dependence of lipid packing density on mole fraction is multiphasic, which differs qualitatively from the monotonic decrease in packing density found with the shorter polymer lipids. Lipid spin-label ESR is an experimental tool that complements theoretical analysis using polymer models combined with the lipid equation of state.

1,2-Dipalmitoylphosphatidylcholine↗
PubMed1998

Biologically active polymers: synthesis and antimicrobial activity of modified glycidyl methacrylate polymers having a quaternary ammonium and phosphonium groups.

Polymers with antibacterial activity have been synthesized by chemical modification of poly(glycidyl methacrylate). The glycidyl methacrylate was polymerized by the free radical polymerization technique. The poly(glycidyl methacrylate) was hydrolyzed and was chloroacetylated using chloroacetyl chloride. The chloroacetylated product was modified to yield polymers with either quaternary ammonium or phosphonium salts. The antimicrobial activity of the modified glycidyl methacrylate polymers has been examined against a variety of test microorganisms by the cut plug and the viable cell counting methods using shake flask of ten times diluted nutrient broth medium. All three polymers obtained were inhibitory to the growth of Gram negative bacteria (Escherichia coli, Pseudomones aeruginosa, Shigella sp. and Salmonella typhae) and Gram positive bacteria (Bacillus subtilis and B. cereus) as well as the fungus (Trichophytun rubrum). It was found that the growth inhibitory effect varied according to the structure of the polymer and the composition of the active group and increased with increasing the concentration of the polymer. The tested polymers showed more antimicrobial activity against Gram negative bacteria and the fungus, whereas were less active against Gram positive bacteria.

Anti-Bacterial Agents↗
PubMed2006

Supramolecular self-assembly of dendronized polymers: reversible control of the polymer architectures through acid-base reactions.

Acid-base switchable supramolecular dendronized polyacetylenes (DPAs) with increasing steric bulk on going from generation one [G1] to three [G3], were constructed using multiple self-assembly processes between Fréchet-type [G1]-[G3]-dendritic dialkylammonium salts and a dibenzo[24]crown-8-containing polymer. The formation of the supramolecular systems is acid-base switchable to either an ON (rodlike dendronized polymers) or an OFF (flexible polymers) state. Thus, by controlling the superstructures of the supramolecular polymers with the [G1]-[G3] dendrons, it is possible to induce conformational changes within the polymer backbones. The supramolecular dendronized polymers, as well as their threading-dethreading properties, were characterized by (1)H NMR and UV absorption spectroscopies, gel permeation chromatography (GPC) and light scattering (LS). Independent measures of molecular weight (GPC, LS) indicate that DPAs behave as increasingly rigid macromolecules with each generation in solution. Molecular dynamics simulations of each DPA suggest that the lengths of the polymer backbones increase accordingly. Atomic force microscopy of the [G3]-dendronized polystyrene (DPS), as well as the DPAs, reveal surface morphologies indicative of aggregated superstructures.

Journal Article↗
PubMed2005

Distinct difference in ionic transport behavior in polymer electrolytes depending on the matrix polymers and incorporated salts.

Two different electrolyte salts, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), and a room temperature ionic liquid, 1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide (EMITFSI), were incorporated into network polymers to obtain ion-conductive polymer electrolytes. Network polymers of poly(ethylene oxide-co-propylene oxide) (P(EO/PO)) and poly(methyl methacrylate) (PMMA) were chosen as matrixes for LiTFSI and EMITFSI, respectively. Both of the polymer electrolytes were single-phase materials and were completely amorphous. Ionic conductivity of the polymer electrolytes was measured over a wide temperature range, with the lowest temperatures close to or below the glass transition temperatures (Tg). The Arrhenius plots of the conductivity for both of the systems exhibited positively curved profiles and could be well fit to the Vogel-Tamman-Fulcher (VTF) equation. The conductivity of the PMMA/EMITFSI electrolytes was higher at most by 3 orders of magnitude than that of the LiTFSI/P(EO/ PO) electrolytes at ambient temperature. When the ideal glass transition temperature, T0 (one of the VTF fitting parameters), was compared with the Tg, a difference in the ionic conduction was apparent in these systems. In the P(EO/PO)/LiTFSI electrolytes, the T0 and Tg increased in parallel with salt concentration and the T0 was lower than the Tg by ca. 50 degrees C. On the contrary, the difference between the T0 and the Tg increased with increasing content of PMMA in the PMMA/EMITFSI electrolytes, with the observed difference in the concentration range studied reaching up to ca. 100 degrees C. The conductivity at the Tg, sigma(Tg), for the LiTFSI/P(EO/PO) electrolytes was on the order of 10(-14-)10(-13) S cm(-1) and increased with increasing salt concentration, whereas that for the PMMA/EMITFSI polymer electrolytes reached 10(-7) S cm(-1) when the concentration of PMMA was high. The ion transport mechanism was discussed in terms of the concepts of coupling/decoupling and strong/fragile for the two different polymer electrolytes.

Journal Article↗