How hydrophobic side chain design affects water cluster connectivity in model polymer electrolyte membranes: Linear versus Y-shaped side chains

Dorenbos, G.

doi:10.1016/j.ijhydene.2020.09.010

Cited by 5 publications

(12 citation statements)

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“…To systematically aid in elucidating general design rules in terms of the architecture of the backbones and side chains and also the chemistry of the pendant acidic or basic groups, Dorenbos and co-workers performed extensive studies on the hydrated morphology and the size and shape of ionic channels as a function of EW, hydrophilic site distribution, hydrophilic/hydrophobic side chain length and distribution, doping proton transport channels, and amphiphilic block architecture. − ,− …”

Section: Proton Exchange Membranesmentioning

confidence: 99%

Coarse-Grained Modeling of Ion-Containing Polymers

2022

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Ion-containing polymers have continued to be an important research focus for several decades due to their use as an electrolyte in energy storage and conversion devices. Elucidation of connections between the mesoscopic structure and multiscale dynamics of the ions and solvent remains incompletely understood. Coarse-grained modeling provides an efficient approach for exploring the structural and dynamical properties of these soft materials. The unique physicochemical properties of such polymers are of broad interest. In this review, we summarize the current development and understanding of the structure–property relationship of ion-containing polymers and provide insights into the design of such materials determined from coarse-grained modeling and simulations accompanying significant advances in experimental strategies. We specifically concentrate on three types of ion-containing polymers: proton exchange membranes (PEMs), anion exchange membranes (AEMs), and polymerized ionic liquids (polyILs). We posit that insight into the similarities and differences in these materials will lead to guidance in the rational design of high-performance novel materials with improved properties for various power source technologies.

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Section: Proton Exchange Membranesmentioning

confidence: 99%

Coarse-Grained Modeling of Ion-Containing Polymers

2022

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“…Given these challenges of unambiguously determining the morphology, theoretical approaches have been resorted to providing insight into the quantification of morphology for ion-containing membranes. Coarse grained MD and DPD simulations are widely utilized in modeling phase separations within membranes that typically requires long-time relaxation and a large length scale of 10-200 nm (Dorenbos, 2017a;Dorenbos, 2017b;Sepehr et al, 2017;Liu et al, 2018a;Dong et al, 2018b;Liu et al, 2018b;Wang R. et al, 2019;Clark et al, 2019;Dorenbos, 2019;Lee, 2019;Luo and Paddison, 2019;Zhu et al, 2019;Chen C. et al, 2020;Luo et al, 2020a;Dorenbos, 2020;Lee, 2020;Sevinis Ozbulut et al, 2020;Zhu et al, 2022). To further quantify the morphology including the size, shape, and connectivity of the ionic domains, which cannot be extracted from the peaks obtained by scattering methods, cluster analysis including distance-based and density-based algorithms is a powerful tool to provide a plethora of information on water domain size, shape, and connectivity from the trajectory of a MD or DPD simulation, which will be described in this section.…”

Section: Hydrated Pem Morphologymentioning

confidence: 99%

“…This suggests that for a low dopant content the small amount of high IEC dopants is situated near well-connected pores formed by the low IEC host polymers, implying that one can increase the overall IEC of the blended membrane without sacrificing the percolated networks by adding a dopant. To further study the influence of designs with hydrophobic side-chains on the connectivity of the water containing domains, Dorenbos correlated the pore connectivity to the average number of bonds separating A from the nearest C (N A−C bond ) and between nearest C beads (N C−C bond ) (Dorenbos, 2019;Dorenbos, 2020). It was determined that the connectivity of the water domains generally increases with increasing N C−C bond for the cases where N C−C bond > N A−C bond(max) and fixed IEC, while the opposite trend occurs for the cases where…”

Section: Hydrated Pem Morphologymentioning

confidence: 99%

“…There are two major directions: simulating the diffusion of ions and/or water in an equilibrium morphology Frontiers in Chemistry frontiersin.org obtained from DPD simulations; and incorporating local interactions into coarse-grained MD/DPD simulations. Dorenbos (Dorenbos, 2019;Dorenbos, 2020) performed grid-based Monte Carlo tracer diffusion calculations, which are capable of evaluating the diffusivity of water molecules based on equilibrium DPD morphologies but fails to describe proton transport behavior due to the lack of local interactions between the protons and the functional groups and solvent molecules. Another drawback is that the fixed pore networks cannot accurately represent the dynamical percolated watercontaining domains (i.e., "channels").…”

Section: In Hydrated Systemsmentioning

confidence: 99%

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Perspective: Morphology and ion transport in ion-containing polymers from multiscale modeling and simulations

Zhu

Paddison

2022

Front. Chem.

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Ion-containing polymers are soft materials composed of polymeric chains and mobile ions. Over the past several decades they have been the focus of considerable research and development for their use as the electrolyte in energy conversion and storage devices. Recent and significant results obtained from multiscale simulations and modeling for proton exchange membranes (PEMs), anion exchange membranes (AEMs), and polymerized ionic liquids (polyILs) are reviewed. The interplay of morphology and ion transport is emphasized. We discuss the influences of polymer architecture, tethered ionic groups, rigidity of the backbone, solvents, and additives on both morphology and ion transport in terms of specific interactions. Novel design strategies are highlighted including precisely controlling molecular conformations to design highly ordered morphologies; tuning the solvation structure of hydronium or hydroxide ions in hydrated ion exchange membranes; turning negative ion-ion correlations to positive correlations to improve ionic conductivity in polyILs; and balancing the strength of noncovalent interactions. The design of single-ion conductors, well-defined supramolecular architectures with enhanced one-dimensional ion transport, and the understanding of the hierarchy of the specific interactions continue as challenges but promising goals for future research.

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“…With the purpose to gain insight on how solely architecture design affects pore morphology a systematic series of DPD studies − has been performed at a fixed water content (16 vol % water, ϕ w = 0.16) for various graft type model polymers that are constructed solely from hydrophobic A and hydrophilic (functional) C beads. The backbones were fully hydrophobic with C beads centered on linear (A x C) or Y-shaped (A y [A x C][A x C]) side chains.…”

Section: Introductionmentioning

confidence: 99%

Simulated and Experimental Trends Regarding Water Uptake in Polymeric Electrolyte Membranes

Dorenbos

2023

J. Phys. Chem. B

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Polymeric membranes in an anion or a proton exchange membrane fuel cell need sufficient hydration in order to provide a high hydroxide ion or proton conductivity. The water uptake for six model ionomer membranes, all of the same ion exchange capacity, is modeled by dissipative particle dynamics. The architectures cover three types of families that are of potential interest in fuel cell membrane research. All architectures consist of connected hydrophobic backbone A beads, to which side chains are grafted. For the type I family, the hydrophilic (functional) C beads are pendent on (amphiphilic) [AxC] side chains. The type II architecture contains both hydrophobic [A 4 ] and short hydrophilic [C] side chains. For type III, the C beads are embedded along various locations within the [AxCAy] side chains (x + y = constant). For similar equilibrium time, the membrane water volume fraction increases with side chain length x for type I, and for type III, it increases with the distance x that C beads are separated from the backbone. Among the architectures (types I and III) for which the number of covalent C−A bonds are the same, the water uptake increases with the average number of A−A and A−C bonds (dpd springs) between A beads and the nearest C bead. A picture emerges in which for similar ion exchange capacity model membranes water uptake increases as a function of ⟨N bond phob-phyl ⟩.

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How hydrophobic side chain design affects water cluster connectivity in model polymer electrolyte membranes: Linear versus Y-shaped side chains

Cited by 5 publications

References 91 publications

Coarse-Grained Modeling of Ion-Containing Polymers

Coarse-Grained Modeling of Ion-Containing Polymers

Perspective: Morphology and ion transport in ion-containing polymers from multiscale modeling and simulations

Simulated and Experimental Trends Regarding Water Uptake in Polymeric Electrolyte Membranes

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