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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 469 records · Page 26
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Poly(ionic liquid)s with Dicationic Pendants as Gas Separation Membranes

Poly(norbornene)s and poly(ionic liquid)s are two different classes of attractive materials, which are known for their structural tunability and thermal stabilities, and have been extensively studied as gas separation membranes. The incorporation of ionic liquids (ILs) into the poly(norbornene) through post-polymerization has resulted in unique materials with synergistic properties. However, direct polymerization of norbornene-containing IL monomers as gas separation membranes are limited. To this end, a series of norbornene-containing imidazolium-based mono- and di-cationic ILs (NBM-mIm and NBM-DILs) with different connectivity and spacer lengths were synthesized and characterized spectroscopically. Subsequently, the poly(NBM-mIm) with bistriflimide [Tf2N−] and poly([NBM-DILs][Tf2N]2) comprising homo-, random-, and block- (co)polymers were synthesized via ring-opening metathesis polymerization using the air-stable Grubbs second-generation catalyst. Block copolymers (BCPs), specifically, [NBM-mIM][Tf2N] and [NBM-ImCnmIm] [Tf2N]2 (n = 4 and 6) were synthesized at two different compositions, which generated high molecular weight polymers with decent solubility relative to homo- and random (co)polymers of [NBM-DILs] [Tf2N]2. The prepared BCPs were efficiently analyzed by a host of analytical tools, including 1H-NMR, GPC, and WAXD. The successfully BCPs were cast into thin membranes ranging from 47 to 125 μm and their gas (CO2, N2, CH4, and H2) permeations were measured at 20 °C using a time-lag apparatus. These membranes displayed modest CO2 permeability in a non-linear fashion with respect to composition and a reverse trend in CO2/N2 permselectivity was observed, as a usual trade-off behavior between permeability and permselectivity.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

Electrospun Separator Based on Sulfonated Polyoxadiazole with Outstanding Thermal Stability and Electrochemical Properties for Lithium-Ion Batteries

Traditional polyolefin separators used in lithium-ion batteries (LIBs) are seriously limited by the issues of inferior security and poor electrolyte wettability. Most of the very promising candidate separators based on heat-resistant polymers are, however, inherently difficult to process. Herein, a unique sulfonated aromatic heterocyclic polymer, lithiated poly(diphenyl ether oxadiazole) sulfonate (Li-SPEOD), was synthesized through a simple one-pot method and further electrospun to act as a novel separator (es-Li-SPEOD) for LIBs. In this work, the prepared Li-SPEOD possesses a high degree of sulfonation with a high molecular weight (M w = 4.31 × 10 5 ). The es-Li-SPEOD separator exhibits excellent mechanical and fire-resistance properties and is able to maintain dimensional stability at a temperature of even up to 400 °C in air. The ionic conductivity (3.57 mS cm –1 ) and lithium-ion transference number (0.37) of the es-Li-SPEOD with an electrochemical stability window of 4.5 V vs Li + /Li can be improved by 382.4 and 32.1%, respectively, compared to those of Celgard-2500 in the LiPF 6 electrolyte. The enhanced rate capability and cycle performance of the LiFePO 4 –Li half-cell are therefore obtained. Moreover, the es-Li-SPEOD displays an outstanding dendrite-suppressing effect for the lithium metal anode. This research proves that the Li-SPEOD-based separator has a broad application perspective in next-generation lithium batteries.

25 ENERGY STORAGE↗
DOE OSTI2022

Proton Conducting Sulfonated Poly(Ionic Liquid) Block Copolymers

Herein, we report the synthesis of proton-conducting sulfonated poly(ionic liquid) block copolymers (S-PILBCPs) containing one block with sulfonic acid (sulfonated styrene, SS) and the other with an IL moiety (vinylbenzylmethylimidazolium bis(trifluoromethylsulfonyl)imide, VBMIm-TFSI) using reversible addition–fragmentation chain-transfer (RAFT) polymerization and post-polymerization modifications (i.e., functionalization, anion exchange reactions, and sulfonation). The S-PILBCPs uniquely conjoin the SS block with mobile protons (H + ) and the PIL block with mobile anions (TFSI – ), where multiple highly desired properties, including high proton conductivity (from the SS block), and high IL-philicity and oxygen solubility (from the PIL block) can exist compartmentally within a microphase separated morphology (evidenced by differential scanning calorimetry (DSC) and small-angle X-ray scattering (SAXS)). High ion conductivity of 79.7 mS/cm at a PIL block composition of 21.6 mol % was observed at 80 °C and 90% relative humidity (RH) (comparable to the benchmark Nafion ionomer). This work successfully demonstrates the design of S-PILBCPs as a new material platform and showcases its promise as an ionomer for proton exchange membrane fuel cells (PEMFCs) as they simultaneously and compartmentally combine proton conductivity and oxygen solubility. Furthermore, these benefits have recently been leveraged to achieve substantial improvement in oxygen reduction reaction (ORR) activity and subsequently fuel cell performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Polyacrylonitrile-based electrolytes: How processing and residual solvent affect ion transport and stability

Polyacrylonitrile (PAN) is one of the alternative candidate polymer hosts to form solid polymer electrolytes (SPEs) besides the widely used poly(ethylene oxide). In this study, we systematically investigate the processing of PAN based SPEs containing lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt, using dimethylformamide (DMF) as the solvent. The effects of PAN processing procedure including solution mixing, casting, and drying on the morphology, ion transport, solvation structure, Li and oxidative stability of PAN electrolytes are thoroughly examined. In particular, four drying conditions are investigated and the amount of residual DMF is accurately determined using infrared (IR) spectroscopy. Varying the drying conditions can lead to five orders of magnitude decrease in the ionic conductivity. As DMF content decreases, the SPE's stability again Li metal dramatically improves. The practical oxidative stability is also strongly affected by the residual DMF content, ranging from 2.5 V to 3.5 V, much lower than reported values. Finally, the role of the residual DMF solvent is elucidated. DMF content vitally influences ion solvation structure at different concentration regimes, which ultimately dictates the ion conduction mechanism and oxidative stability of PAN based SPEs. In conclusion, this thorough study lays the groundwork for future development of PAN based electrolytes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Interconnected cathode-electrolyte double-layer enabling continuous Li-ion conduction throughout solid-state Li-S battery

All-solid-state lithium (Li) batteries with high energy density are a promising solution for the next-generation energy storage systems in large-scale devices. To simultaneously overcome the challenges of poor ionic conduction of solid electrolytes and shuttling of active materials, here we introduce a functional electrolyte-cathode bilayer framework with interconnected LLAZO channels from the electrolyte into the cathode for advanced solid-state Li-S batteries. Differing from the traditional solid-state batteries with separated layer compositions, the introduced bilayer framework provides ultrafast and continuous ion/electron conduction. Instead of transferring Li+ across the polymer and garnet phases which involve huge interfacial resistance, Li+ is directly conducted through the LLAZO channels created continuously from the cathode layer to the solid electrolyte layer, significantly shortening the diffusion distance and facilitating the redox reaction of sulfur and sulfides. A stable cycle life is demonstrated in the prototype Li-S solid-state batteries assembled with the introduced LLAZO-LLAZO@CNF interconnected bilayer framework. High capacity is obtained at room temperature, indicating the superior electrochemical properties of the bilayer framework that result from the unique design of the interconnected LLAZO garnet phase.

25 ENERGY STORAGE↗
DOE OSTI2022

Electrochemical Probing of Steric, Electrostatic and Hydrophobic Interactions of Large Cations in Polymers of Intrinsic Microporosity

Porous membranes have been used for many applications, including separations in biotechnology, the food industry, water purification, and even energy storage devices. The benefit of polymers of intrinsic microporosity (PIMs) is their consistently sized nanopore channels. Inherent functionalities of the PIM structure not only create these channels but are also available for further modifications that can change the interactions of ions and molecules inside of the pore. Here we design solid state nanopores on which are drop-casted two different PIMs, functionalized with either a cyano group or a carboxylic acid. Ionic transport through the membranes is investigated based on pore size and charge-charge interactions, as well as steric and hydrophobic interactions. Achieving specific ion selectivity with easily processable porous membranes opens new avenues for water purification strategies and energy storage.

25 ENERGY STORAGE↗
DOE OSTI2023

Modeling Nanoscale Ohmics in Carbon Supports of Fuel Cell Cathodes

Here, reducing platinum (Pt) loading in polymer electrolyte fuel cells (PEFCs) while meeting performace requirements is critical to their widespread deployment. However, significant polarization losses manifest at higher current densities in cathodes with lower Pt content. The morphology of the carbon supports in PEFC cathodes affects the location of Pt deposition into the micropits or onto the surface of the carbon support, translating into different kinetic and transport resistances. In this work, we derive an agglomerate scale model that differentiates the sink terms for Pt on the surface and in the pits of carbon supports. We develop an approach to assess the impact of nanoscale ohmic resistance to Pt in the micropits arising from weakly ionic solution in the carbon support on PEFC performance. Effectiveness factors relating the actual reaction rate to the maximum reaction rate (had all the Pt been exposed) are derived and embedded into a one-dimensional catalyst layer model. Parameters in the catalyst layer model are tuned based on experimental local oxygen transport resistances. Subsequently, we estimate bounds for the micropore resistances based on geometric and physical arguments. Lastly, polarization curves are simulated to assess the effect of the micropore resistance in fully-humidified and oxygen-rich environments.

25 ENERGY STORAGE↗
DOE OSTI2022

Ionic Liquid Facilitated Solvent‐Phase Polymerization of Ultrasmooth Coatings of Polycatecholamines

Mussel-inspired polycatecholamine coatings and films have proven to be versatile materials for surface modification. However, the progress of chemically modified coatings with tailored properties has been slow due to the lack of definitive evidence of their polymeric structure. Polycatecholamines form aggregates during polymerization, and their formation mechanism has been a subject of debate owing to their insolubility in traditional molecular solvents. Exploiting the capability of ionic liquids (ILs) to exhibit strong electrostatic interactions, herein, the first solution-phase polymerization approach is reported to achieve polymerization of four catecholamines – dopamine (DA), norepinephrine (NE), L-3,4-dihydroxyphenylalanine (L-DOPA), and adrenaline (AD). Kinetic control over the polymerization process in the solution phase enabled it to follow the process with 1 H NMR spectroscopy, revealing the formation of structural features of resulting complex heterogeneous and soluble polymers. The polymers are both covalent and associative in nature. Solution phase polymerization prevented the formation of large aggregates in the solution, thus facilitating the formation of coatings that are ultra-smooth and have root mean square roughness of the order of sub-nm to nm scale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Ion Correlations and Partial Ionicities in the Lamellar Phases of Block Copolymeric Ionic Liquids

Recently, significant interest has arisen on the impact of dynamical ion correlations on the conductivity and transport properties of polymeric electrolyte materials. It has been hypothesized that confining ion motion to narrow channels may reduce such ion correlations and enhance the resulting ionic conductivity. Motivated by such considerations, in this study we used a multiscale simulation framework to study the dynamical ion correlations in the microphase-separated lamella phase of block copolymeric ionic liquids and compare with the corresponding results for homopolymeric systems. We probed the influence of ion correlations through the partial ionicity, Δ, which quantifies the ratio of true conductivity to the ideal, Nernst–Einstein conductivity for the anion-related contributions. Consistent with our original hypothesis, our results demonstrate that the partial ionicity relating to the mobile anions is much larger in the lamella phases of block copolymers compared to that in homopolymers. Analysis of the distinct conductivity contributions demonstrates that such results arise as a result of an intricate compensation among the nonideal dynamical correlations relating to anions in lamella phases. Overall, our results suggest that self-assembled phases of block copolymers may provide an avenue to tune the dynamical ion correlations in polymer electrolyte systems.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Covalent adaptable networks for electrolyte–binder integration in recyclable lithium metal batteries

Lithium-metal batteries (LMBs) are considered a promising next-generation energy storage technology due to their exceptionally high energy density. However, the development of solid polymer electrolytes and cathode binders for LMBs faces critical challenges, including interfacial instability, poor recyclability, and growing environmental concerns. In particular, current systems often rely on non-recyclable components featuring permanently crosslinked networks and polyfluoroalkyl substances (PFAS), such as poly(vinylidene fluoride) (PVDF), which cause battery waste and environmental harm. Herein, we introduce a multifunctional covalent adaptable network (CAN) platform based on thermally reversible Diels–Alder (DA) chemistry, designed for dual functionality as a CAN-based electrolyte (CAE) and a CAN-based cathode binder. The CAE achieves high ionic conductivity and strong storage modulus (1.4 mS cm −1 and ∼ 10 5 Pa at room temperature, respectively) and enables stable long-term cycling in symmetric Li||Li cells for over 2000 h with low overpotential. When it is applied as a cathode binder in LiFePO 4 (LFP) composite electrodes (C-LFP), the CAN matrix significantly reduces interfacial resistance and enhances discharge capacity compared to conventional PVDF-based systems. Thermal treatment induces self-healing at the cathode–electrolyte interface, further improving contact and yielding a discharge capacity of 150 mAh g −1 at 0.5 C. Moreover, the dynamic CAN architecture allows efficient recovery and reuse of lithium salts from spent electrolytes through retro-DA reactions under mild conditions (∼80 °C), establishing a low-energy, cost-effective recycling pathway. In conclusion, this work presents a scalable and sustainable strategy for high-performance LMBs by integrating recyclability, interfacial healing, and PFAS-free design, offering a holistic solution aligned with circular economy principles and next-generation battery demands.

Diels–Alder↗
DOE OSTI2020

Morphology and Transport of Multivalent Cation-Exchanged Ionomer Membranes Using Perfluorosulfonic Acid–Ce Z+ as a Model System

Perfluorosulfonic acids (PFSAs) are commonly used as solid polymer electrolyte membranes (PEMs) in electrochemical energy devices, where they are vulnerable to attack by radical species during operation. A popular strategy to combat this problem is to introduce radical scavengers like cerium (Ce) ions that neutralize these species before they attack the PFSA. Such cation doping creates a multi-ion system, in which understanding the mechanisms of cation solvation and transport becomes important for the effective design and utilization of PFSA–cation systems. Ce ions also provide a representative model system for multication-exchanged ionomers in electrochemical systems. In this study, hydration and conductivity measurements, along with X-ray fluorescence and scattering, are employed to elucidate how Ce ion exchange alters PFSA’s ionic solvation, as well as nano- and mesoscale morphologies, which ultimately control its ion transport properties. A molecular transport model is used to deconvolute the impact of Ce ions on the local solvation structure of water in the membrane from mesoscale changes of the transport pathways. The combined experimental and theoretical analysis reveals a nonlinear decrease in conductivity driven by cation solvation at the molecular level and morphological changes at longer length scales. Migration–diffusion coupling, its nonlinear dependence on ion exchange and hydration, and its overall implications for ionomer performance are also discussed. Finally, these findings have the potential to be translated into other mixed cation–ionomer systems for a wide range of energy and environmental devices.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Solvent Dynamics in Gel Polymer Electrolytes for Lithium–Sulfur Batteries

Li−sulfur (Li−S) batteries are promising as the next-generation energy storage technology but face challenges due to sluggish sulfur redox reaction (SRR) kinetics and a sulfur shuttling effect. While many studies have explored polycaprolactone (PCL)-based gel polymer electrolytes (GPEs) to address these issues, the influence of solvent properties, including dielectric constant (ϵ) and donor and acceptor numbers (DN and AN), remain unexplored despite their critical impact on performance and full-scale implementation. This study systematically compares three distinct electrolytes, dimethoxyethane (DME), dimethyl sulfoxide (DMSO), and tetraethylene glycol dimethyl ether (TEGDME)-paired with PCL, to correlate the varied solvent properties and their effects on the physical properties of the GPE, in terms of Li + transport and solvation, and polysulfide’s confinement. Among them, the DME-based GPE, with an intermediate DN, exhibited the lowest crystallinity (2.31%), highest ionic conductivity (7.49 mS/cm), and high Li + transference number (0.77). As a result, it achieved a specific capacity of 795 mAh/g sulfur and an average Coulombic efficiency of 97.5% after 120 cycles at C/5, outperforming its competitors. Operando Raman and UV−vis spectroscopy confirmed that PCL effectively confines long-chain polysulfides within its network, mitigating the shuttle effect and facilitating reversible polysulfide conversion. These findings demonstrate that GPEs with moderate DN values and balanced ϵ significantly enhance stability, extend cycle life, and improve rate performance for Li−S batteries. This work provides valuable insights into the design of advanced electrolyte systems for practical energy storage applications.

25 ENERGY STORAGE↗
DOE OSTI2024

Selective ion transport through hydrated micropores in polymer membranes

Abstract Ion-conducting polymer membranes are essential in many separation processes and electrochemical devices, including electrodialysis 1 , redox flow batteries 2 , fuel cells 3 and electrolysers 4,5 . Controlling ion transport and selectivity in these membranes largely hinges on the manipulation of pore size. Although membrane pore structures can be designed in the dry state 6 , they are redefined upon hydration owing to swelling in electrolyte solutions. Strategies to control pore hydration and a deeper understanding of pore structure evolution are vital for accurate pore size tuning. Here we report polymer membranes containing pendant groups of varying hydrophobicity, strategically positioned near charged groups to regulate their hydration capacity and pore swelling. Modulation of the hydrated micropore size (less than two nanometres) enables direct control over water and ion transport across broad length scales, as quantified by spectroscopic and computational methods. Ion selectivity improves in hydration-restrained pores created by more hydrophobic pendant groups. These highly interconnected ion transport channels, with tuned pore gate sizes, show higher ionic conductivity and orders-of-magnitude lower permeation rates of redox-active species compared with conventional membranes, enabling stable cycling of energy-dense aqueous organic redox flow batteries. This pore size tailoring approach provides a promising avenue to membranes with precisely controlled ionic and molecular transport functions.

Science & Technology - Other Topics↗
DOE OSTI2024

Structure Development in Cross-Linked, Soybean Oil-based Waterborne Polyurethanes

Development of waterborne polyurethanes (WPU) using bio-based sources represents a step towards sustainable materials science and industry. We synthesized bio-based cationic water-dispersed crosslinked polyurethanes from high oleic soybean oil (HOSO) polyol, isophorone diisocyanate, and methyldiethanol amine, with varying ionic group contents after neutralization with acetic acid. Our primary objective was to analyze how crosslinking affects the dispersion process and film properties in multifunctional systems. The synthesis-structure-property relationship is elucidated through comprehensive analyses of the products at different stages of the synthesis. The dispersion of the WPU particles in water must occur prior to gelation during the final preparation, leading to incomplete conversion and the formation of imperfect networks. Insight into the synthesis process and polymer structure was gained by simulating polymer network parameters. Morphological analyses using synchrotron-based X-ray scattering and atomic force microscopy revealed a hierarchical structure within the WPU films. Importantly, all the films prepared in this study, without using coalescence agents, have low water absorption and high water contact angles, demonstrating their potential for textile and leather coatings and other applications.

bio-based polymers↗
DOE OSTI2021

Ready Access to Anhydrous Anionic Lanthanide Acetates by Using Imidazolium Acetate Ionic Liquids as the Reaction Medium

Abstract Access to lanthanide acetate coordination compounds is challenged by the tendency of lanthanides to coordinate water and the plethora of acetate coordination modes. A straightforward, reproducible synthetic procedure by treating lanthanide chloride hydrates with defined ratios of the ionic liquid (IL) 1‐ethyl‐3‐methylimidazolium acetate ([C 2 mim][OAc]) has been developed. This reaction pathway leads to two isostructural crystalline anhydrous coordination complexes, the polymeric [C 2 mim] n [{Ln 2 (OAc) 7 } n ] and the dimeric [C 2 mim] 2 [Ln 2 (OAc) 8 ], based on the ion size and the ratio of IL used. A reaction with an IL : Ln‐salt ratio of 5 : 1, where Ln=Nd, Sm, and Gd, led exclusively to the polymer, whilst for the heaviest lanthanides (Dy−Lu) the dimer was observed. Reaction with Eu and Tb resulted in a mixture of both polymeric and dimeric forms. When the amount of IL and/or the size of the cation was increased, the reaction led to only the dimeric compound for all the lanthanide series. Crystallographic analyses of the resulting salts revealed three different types of metal‐acetate coordination modes where η 2 μκ 2 is the most represented in both structure types.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Interfacial Adhesion Mechanism of Anionic Polyelectrolyte Brushes Induced by Oppositely Charged Macromolecular Counterions

Abstract Polyelectrolyte brushes are widely used as model systems for investigating electrostatic interactions at soft interfaces and to achieve exceptional lubrication properties. Previous studies have primarily focused on their behavior in the presence of multivalent counterions, which induce brush collapse, ionic crosslinking, and pronounced changes in interfacial structures. However, interactions between polyelectrolyte brushes and oppositely charged macromolecular counterions, such as polycations, remain poorly understood. Here, we prepare well-defined polystyrene sulfonate (PSS) brushes fabricated via surface-initiated grafting and employ surface forces apparatus measurements to investigate their interactions with oppositely charged polycations. In contrast to multivalent ions, polycations do not induce noticeable brush collapse, but instead generate significant adhesion between symmetric PSS brush layers. This adhesion increases with both contact time and applied load, eventually reaching a steady plateau, indicating that the interaction is governed not simply by electrostatic screening but by the gradual formation of polycation-mediated bridging under confinement. Furthermore, the introduction of monovalent Na+ ions disrupts the adhesive interaction even at very low concentrations, suggesting that the bridging function of the adsorbed polycation is highly sensitive to competitive ionic screening. In comparison, measurements with trivalent counterions reveal the expected brush collapse behavior but minimal dependence of adhesion on contact time, highlighting a clear mechanistic distinction from the polymeric counterion case. Collectively, these results demonstrate that molecular size, configurational restriction, and confinement-induced rearrangement, rather than charge valency alone, govern the interaction behavior of macromolecular counterions at brush interfaces. This work provides new insight into the molecular origins of adhesion and the regulation of interfacial interactions in charged polymer brush systems.

Park, Jinwoo [Argonne National Laboratory , , , ,;↗
DOE OSTI2026

Design Trade-Offs in Composite Fuel Cell Membranes: Effects of Reinforcement and Chemical Additives

Perfluorosulfonic acid (PFSA) membranes are critical components in proton exchange membrane fuel cells, where performance depends on balancing ionic conductivity, mechanical durability, and chemical stability. This study characterizes a composite membrane (NC700) featuring PFSA-impregnated expanded polytetrafluoroethylene (ePTFE) reinforcement and cerium-based radical scavengers, benchmarked against unreinforced NR211. Complementary techniques, including electron microscopy, X-ray scattering, infrared spectroscopy, thermogravimetric analysis, and dynamic mechanical analysis, identify the structural and compositional strategies employed in NC700. Water sorption isotherms reveal lower water uptake for NC700 across all conditions, attributed to reinforcement and cerium incorporation. Reinforcement reduces in-plane swelling from 11% to 2.1% at 90% RH, confirming strong swelling anisotropy, while maintaining mechanical properties at elevated temperatures. While the ionic conductivity of NC700 is approximately 10% lower than that of NR211, the reduced thickness yields a 40% decrease in calculated area-specific resistance, suggesting the composite architecture can favorably shift the conductivity-stability trade-off. The composite structure also reduces gas permeability, indicating potential for improved separator function alongside favorable transport properties. Systematic deconvolution of reinforcement and additive contributions shows that conductivity losses from cerium incorporation are largely offset by gains from the lower equivalent-weight polymer, providing quantitative relationships that may guide composite membrane design for fuel cells and other electrochemical applications.

25 ENERGY STORAGE↗
DOE OSTI2023

Mixed-Polarity Copolymers Based on Ethylene Oxide and Cyclic Carbonate: Insights into Li-Ion Solvation and Conductivity

Here, this study investigates the relationship between polarity and ionic conductivity in random and block copolymer electrolytes comprising highly flexible oligo(ethylene oxide) methyl ether methacrylate (OEM) and highly polar but glassy glycerol carbonate methacrylate (GCMA) monomers, blended with either lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) or lithium triflate. Interestingly, the high polarity of GCMA did not significantly enhance ionic dissociation, and the random copolymers (POEM-r-PGCMA) showed similar or lower ionic conductivities than the POEM homopolymer. Further analysis revealed that Li + only interacts with OEM and its counterion, not with GCMA. The less-intermixed and weakly phase-separated block copolymer (POEM-b-PGCMA) exhibited even lower conductivities than the random copolymer. Our results suggest that Li + solvation occurs only in the POEM-rich phase and that the larger PGCMA regions, depleted of Li + , disrupt long-range ion transport. These findings provide valuable insights into the design of polymer electrolytes and how segmental mobility and functional groups with contrasting polarities affect ion transport.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗