Dataset Information

Dissipative Particle Dynamics Modeling of Polyelectrolyte Membrane-Water Interfaces.

ABSTRACT: Previous experiments of water vapor penetration into polyelectrolyte membrane (PEM) thin films have indicated the influence of the water concentration gradient and polymer chemistry on the interface evolution, which will eventually affect the efficiency of the fuel cell operation. Moreover, PEMs of different side chains have shown differences in water cluster structure and diffusion. The evolution of the interface between water and polyelectrolyte membranes (PEMs), which are used in fuel cells and flow batteries, of three different side-chain lengths has been studied using dissipative particle dynamics (DPD) simulations. Higher and faster water uptake is usually beneficial in the operation of fuel cells and flow batteries. The simulated water uptake increased with the increasing side chain length. In addition, the water uptake was rapid initially and slowed down afterwards, which is in agreement with the experimental observations. The water cluster formation rate was also found to increase with the increasing side-chain length, whereas the water cluster shapes were unaffected. Water diffusion in the membranes, which affects proton mobility in the PEMs, increased with the side-chain length at all distances from the interface. In conclusion, side-chain length was found to have a strong influence on the interface water structure and water penetration rates, which can be harnessed for the better design of PEMs. Since the PEM can undergo cycles of dehydration and rehydration, faster water uptake increases the efficiency of these devices. We show that the longer side chains with backbone structure similar to Nafion should be more suitable for fuel cell/flow battery usage.

SUBMITTER: Sengupta S

PROVIDER: S-EPMC7240515 | biostudies-literature | 2020 Apr

REPOSITORIES: biostudies-literature

ACCESS DATA

Publications

Dissipative Particle Dynamics Modeling of Polyelectrolyte Membrane-Water Interfaces.

Sengupta Soumyadipta S Lyulin Alexey A

Polymers 20200414 4

Previous experiments of water vapor penetration into polyelectrolyte membrane (PEM) thin films have indicated the influence of the water concentration gradient and polymer chemistry on the interface evolution, which will eventually affect the efficiency of the fuel cell operation. Moreover, PEMs of different side chains have shown differences in water cluster structure and diffusion. The evolution of the interface between water and polyelectrolyte membranes (PEMs), which are used in fuel cells a ...[more]

PMID: 32295222

Similar Datasets

Project description:Lipid membranes are more than just barriers between cell compartments; they provide molecular environments with a finely tuned balance between hydrophilic and hydrophobic interactions that enable proteins to dynamically fold and self-assemble to regulate biological function. Characterizing dynamics at the lipid-water interface is essential to understanding molecular complexities from the thermodynamics of liquid-liquid phase separation down to picosecond-scale reorganization of interfacial hydrogen-bond networks.Ultrafast vibrational spectroscopy, including two-dimensional infrared (2D IR) and vibrational sum-frequency generation (VSFG) spectroscopies, is a powerful tool to examine picosecond interfacial dynamics. Two-dimensional IR spectroscopy provides a bond-centered view of dynamics with subpicosecond time resolutions, as vibrational frequencies are highly sensitive to the local environment. Recently, 2D IR spectroscopy has been applied to carbonyl and phosphate vibrations intrinsically located at the lipid-water interface. Interface-specific VSFG spectroscopy probes the water vibrational modes directly, accessing H-bond strength and water organization at lipid headgroup positions. Signals in VSFG arise from the interfacial dipole contributions, directly probing headgroup ordering and water orientation to provide a structural view of the interface.In this Account we discuss novel applications of ultrafast spectroscopy to lipid membranes, a field that has experienced significant growth over the past decade. In particular, ultrafast experiments now offer a molecular perspective on increasingly complex membranes. The powerful combination of ultrafast, interface-selective spectroscopy and simulations opens up new routes to understanding multicomponent membranes and their function. This Account highlights key prevailing views that have emerged from recent experiments: (1) Water dynamics at the lipid-water interface are slow compared to those of bulk water as a result of disrupted H-bond networks near the headgroups. (2) Peptides, ions, osmolytes, and cosolvents perturb interfacial dynamics, indicating that dynamics at the interface are affected by bulk solvent dynamics and vice versa. (3) The interfacial environment is generally dictated by the headgroup structure and orientation, but hydrophobic interactions within the acyl chains also modulate interfacial dynamics. Ultrafast spectroscopy has been essential to characterizing the biophysical chemistry of the lipid-water interface; however, challenges remain in interpreting congested spectra as well as designing appropriate model systems to capture the complexity of a membrane environment.

Dataset Information

Dissipative Particle Dynamics Modeling of Polyelectrolyte Membrane-Water Interfaces.

Publications

Dissipative Particle Dynamics Modeling of Polyelectrolyte Membrane-Water Interfaces.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets