Segmental Dynamics of Ethylene Oxide-Containing Polymers with Diverse Backbone Chemistries

Bartels, Joshua; Wang, Jing Han Helen; Chen, Quan; Runt, James; Colby, Ralph H.

doi:10.1021/acs.macromol.5b02423

Cited by 15 publications

(20 citation statements)

References 64 publications

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“…The nonionic sample with 9 EO side chains was synthesized by RAFT polymerization, 15 while those with 2 and 5 EO side chains were made by free radical polymerization. 27 The neutral polymer with 20 EO side chains, synthesized from atom transfer radical polymerization, was kindly provided by Longcheng Gao from the School of Chemistry and Environment at Beihang University. The plasticizer with PEO central part and carbonate end groups was synthesized by Siwei Liang at Penn State University via a condensation reaction.…”

Section: Methodsmentioning

confidence: 99%

Morphological Evolution of Ionomer/Plasticizer Mixtures during a Transition from Ionomer to Polyelectrolyte

et al. 2017

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X-ray scattering data were used to examine the morphological evolution that accompanies the ionomer-to-polyelectrolyte transition. Bulk random ionomer based on methacryl diglyme side chains and sodium sulfonated styrene exhibits an amorphous halo, a backbone correlation peak, and an ionic aggregate spacing peak in X-ray scattering. The ionic peak intensifies as either polymer content or temperature increases due to enhanced aggregation, since the dielectric constant of the polar liquid decreases as temperature is raised. Addition of polar plasticizer into the ionomer softens the ionic interactions by raising the dielectric constant, which weakens the ionic peak, leading to more polyelectrolyte character at higher plasticizer content, with many dissociated Na counterions. There is a wide range of ion content and dielectric constant (gray region in graphic) within which these materials transition from ionomer to polyelectrolyte as the polar plasticizer is added, and both the ionic aggregation peak of the ionomer and the correlation length (interchain spacing) of polyelectrolyte solutions can be resolved. The complete transition to polyelectrolyte occurs when the average distance between the ions becomes larger than the Bjerrum length, so that many Na counterions dissociate, and the ionic aggregate spacing peak disappears.

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Section: Methodsmentioning

confidence: 99%

Morphological Evolution of Ionomer/Plasticizer Mixtures during a Transition from Ionomer to Polyelectrolyte

et al. 2017

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“…On the other hand, electrostatic cohesion enhances microphase separation when the volume fraction of the charged block is small (e.g., f < 0.3) but suppresses microphase separation when f is increased . The dielectric constant for neutral POEGMA is ε POEGMA ≈ 11, although the actual value is likely higher when the sodium sulfonate group is included; the dielectric constant for PS is ε PS ≈ 2.5. This significant difference in ε is expected to shift the phase boundaries toward lower χ eff N , compared to the neutral case, based solely on counterion solvation.…”

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Influence of Charge Fraction on the Phase Behavior of Symmetric Single-Ion Conducting Diblock Copolymers

et al. 2021

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A series of symmetric poly [(oligo(ethylene glycol) methyl ether methacrylate-co-oligo(ethylene glycol) propyl sodium sulfonate methacrylate)]-block-polystyrene (PsOEGMA-PS) diblock copolymers were synthesized as a model system to probe the effect of charge fraction on the phase behavior of charged-neutral single-ion conducting diblock copolymers. Small-angle X-ray scattering (SAXS) experiments showed that increasing the charge fraction does not alter the ordered phase morphology (lamellar) but increases the order− disorder transition temperature (T ODT ) significantly. Additionally, the effective Flory−Huggins interaction parameter (χ eff ) was found to increase linearly with the charge fraction, similar to the case of conventional salt-doped diblock copolymers. This indicates that the effect of counterion solvation, attributed to the significant mismatch between the dielectric constant of each block, provides the dominant effect in tuning the phase behavior of this charged diblock copolymer. We therefore infer that electrostatic cohesion (local charge ordering induced by Coulombic interactions), which is predicted to suppress microphase separation and lead to asymmetric phase diagrams, only plays a minor role in this model system.

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“…In these SBBCEs, (PPEGMEA- b -PS) 2 ( 3 ) acts like BAB triblock copolymers to form nano-assemblies in CH 3 O–PEG–PC, in which the two terminal solvophobic rigid polystyrene (PS) blocks form the bulk of nano-assemblies together or separately, and the middle solvophilic block of poly[poly(ethylene glycol) methyl ether acrylate] (PPEGMEA) bridges nano-assemblies to form the crosslinked network and therefore enhances mechanical strength of SBBCEs. Besides, the PEG side-brushes in the PPEGMEA block can coordinate with lithium to improve ionic conductivity. − Fumed SiO 2 improves interfacial compatibility between the electrodes and electrolytes, and therefore improves cells performance. The modified poly(ethylene glycol) of CH 3 O–PEG–PC acts as two roles.…”

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Star Brush Block Copolymer Electrolytes with High Ambient-Temperature Ionic Conductivity for Quasi-Solid-State Lithium Batteries

Guan

Qian

Guo

et al. 2019

ACS Materials Lett.

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We report high-performance star brush block copolymer electrolytes (SBBCEs) composed of 2-arm star polymer of [poly[poly(ethylene glycol) methyl ether acrylate]b-polystyrene] 2 . The physically crosslinked structure endows SBBCEs with excellent thermal stability and considerable mechanical strength, high ionic conductivity of 2.1 × 10 −4 S cm −1 at 28 °C, wide electrochemical stability window up to 5.6 V, and good interfacial compatibility with lithium anode. A s s e m b l e d L i F e P O 4 | S B B C E | L i a n d N i -r i c h L i -Ni 0.89 Co 0.09 Mg 0.02 O 2 |SBBCE|Li cells deliver superior ambienttemperature cycling performance with high reversible capacities, high Coulombic efficiency, and outstanding cyclic stability at considerable rate of 0.5 C. This proposed idea of employing physically crosslinked structure of brush block copolymer without any chemical crosslinker may broaden a new way to design high-performance polymer electrolytes.

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Segmental Dynamics of Ethylene Oxide-Containing Polymers with Diverse Backbone Chemistries

Cited by 15 publications

References 64 publications

Morphological Evolution of Ionomer/Plasticizer Mixtures during a Transition from Ionomer to Polyelectrolyte

Morphological Evolution of Ionomer/Plasticizer Mixtures during a Transition from Ionomer to Polyelectrolyte

Influence of Charge Fraction on the Phase Behavior of Symmetric Single-Ion Conducting Diblock Copolymers

Star Brush Block Copolymer Electrolytes with High Ambient-Temperature Ionic Conductivity for Quasi-Solid-State Lithium Batteries

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