Ionic transport in electrostatic Janus Membranes. An explicit solvent molecular dynamic simulation.

Montes De Oca, Joan Manuel; Dhanasekaran, Johnson; Cordoba, Andres; Darling, Seth; De Pablo, Juan J.

doi:10.48550/arXiv.2109.01278

Title: Ionic transport in electrostatic Janus Membranes. An explicit solvent molecular dynamic simulation.

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Abstract

Janus –or two-sided, charged membranes offer promise as ionic current rectifiers. In such systems, pores consisting of two regions of opposite charge can be used to generate a current from a gradient in salinity. The efficiency of nanoscale Janus pores increases dramatically as their diameter becomes smaller. However, little is known about the underlying transport processes, particularly under experimentally accessible conditions. In this work, we examine the molecular basis for rectification in Janus nanopores using an applied electric field. Molecular simulations with explicit water and ions are used to examine the structure and dynamics of all molecular species in aqueous electrolyte solutions. For several macroscopic observables, the results of such simulations are consistent with experimental observations on asymmetric membranes. Our analysis reveals a number of previously unknown features, including a pronounced local re-orientation of water molecules in the pores, and a segregation of ionic species that has not been anticipated by previously reported continuum analyses of Janus pores. Using these insights, a model is proposed for ionic current rectification in which electric leakage at pore entrance controls net transport.

Authors:

Montes De Oca, Joan Manuel ^[1]; Dhanasekaran, Johnson ^[1]; Cordoba, Andres ^[1]; Darling, Seth ^[1]; De Pablo, Juan J. ^[1]

Univ. of Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)

Publication Date:: Tue Mar 01 00:00:00 EST 2022

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1870121

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: ACS Nano

Additional Journal Information:: Journal Volume: 16; Journal Issue: 3

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ionic; janus; membranes

Citation Formats


                    Montes De Oca, Joan Manuel, Dhanasekaran, Johnson, Cordoba, Andres, Darling, Seth, and De Pablo, Juan J. Ionic transport in electrostatic Janus Membranes. An explicit solvent molecular dynamic simulation..  United States: N. p., 2022. 
Web.  doi:10.48550/arXiv.2109.01278.

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                    Montes De Oca, Joan Manuel, Dhanasekaran, Johnson, Cordoba, Andres, Darling, Seth, & De Pablo, Juan J. Ionic transport in electrostatic Janus Membranes. An explicit solvent molecular dynamic simulation..  United States.  https://doi.org/10.48550/arXiv.2109.01278

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                    Montes De Oca, Joan Manuel, Dhanasekaran, Johnson, Cordoba, Andres, Darling, Seth, and De Pablo, Juan J. Tue .  
"Ionic transport in electrostatic Janus Membranes. An explicit solvent molecular dynamic simulation.".  United States.  https://doi.org/10.48550/arXiv.2109.01278.  https://www.osti.gov/servlets/purl/1870121.

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@article{osti_1870121,

  title        = {Ionic transport in electrostatic Janus Membranes. An explicit solvent molecular dynamic simulation.},

  author       = {Montes De Oca, Joan Manuel and Dhanasekaran, Johnson and Cordoba, Andres and Darling, Seth and De Pablo, Juan J.},

  abstractNote = {Janus –or two-sided, charged membranes offer promise as ionic current rectifiers. In such systems, pores consisting of two regions of opposite charge can be used to generate a current from a gradient in salinity. The efficiency of nanoscale Janus pores increases dramatically as their diameter becomes smaller. However, little is known about the underlying transport processes, particularly under experimentally accessible conditions. In this work, we examine the molecular basis for rectification in Janus nanopores using an applied electric field. Molecular simulations with explicit water and ions are used to examine the structure and dynamics of all molecular species in aqueous electrolyte solutions. For several macroscopic observables, the results of such simulations are consistent with experimental observations on asymmetric membranes. Our analysis reveals a number of previously unknown features, including a pronounced local re-orientation of water molecules in the pores, and a segregation of ionic species that has not been anticipated by previously reported continuum analyses of Janus pores. Using these insights, a model is proposed for ionic current rectification in which electric leakage at pore entrance controls net transport.},

  doi          = {10.48550/arXiv.2109.01278},

  journal      = {ACS Nano},

  number       = 3,

  volume       = 16,

  place        = {United States},

  year         = {Tue Mar 01 00:00:00 EST 2022},

  month        = {Tue Mar 01 00:00:00 EST 2022}

}

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