Ionic current in nanochannels grafted with pH-responsive polyelectrolyte brushes modeled using augmented strong stretching theory

Sachar, Harnoor Singh; Sivasankar, Vishal Sankar; Etha, Sai Ankit; Chen, Guang; Das, Siddhartha

doi:10.1002/elps.201900248

Title: Ionic current in nanochannels grafted with pH-responsive polyelectrolyte brushes modeled using augmented strong stretching theory

Abstract

Here, we provide a theory to quantify the ionic current (i_ion) in nanochannels grafted with pH-responsive polyelectrolyte (PE) brushes. We consider the PE brushes to be modelled by our recently proposed augmented strong stretching theory (SST) model that improves the existing SST models by incorporating the effects of excluded volume interactions and an extended mass action law. Use of such augmented SST for this problem implies that this is the first study on computing i_ion in PE-brush-grafted nanochannels accounting for the appropriate coupled con guration-electrostatic description of the PE brushes. i_ion is obtained as functions of PE brush grafting density, medium pH and salt concentration (c_∞), and the density of polyelectrolyte chargeable sites (PECS). For large c_∞, i_ion increases linearly with c_∞ (as for such c_∞, i_ion becomes independent of the PE charge and is dominated by the bulk mobility and number density of the electrolyte ions), while iion is independent of c_∞ at small c_∞ (where the EDL electrostatics and the total number of ions in the system is dominated by the hydrogen ions). We further witness an enhancement of i_ion for smaller pH and larger grafting density at low and moderate c_∞, while there is little to nomore »« less

Authors:

Sachar, Harnoor Singh ^[1]; Sivasankar, Vishal Sankar ^[1]; Etha, Sai Ankit ^[1]; Chen, Guang ^[2];

^[1]

Univ. of Maryland, College Park, MD (United States)
Princeton Univ., NJ (United States)

Publication Date:: 2019-09-21

Research Org.:: Univ. of Maryland, College Park, MD (United States)

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

OSTI Identifier:: 1595335

Grant/Contract Number:: SC0017741

Resource Type:: Accepted Manuscript

Journal Name:: Electrophoresis

Additional Journal Information:: Journal Volume: 41; Journal Issue: 7-8; Journal ID: ISSN 0173-0835

Publisher:: Wiley

Country of Publication:: United States

Language:: English

Subject:: 42 ENGINEERING; ionic current; nanochannel; polyelectrolyte brush; strong stretching theory

Citation Formats


                    Sachar, Harnoor Singh, Sivasankar, Vishal Sankar, Etha, Sai Ankit, Chen, Guang, and Das, Siddhartha. Ionic current in nanochannels grafted with pH-responsive polyelectrolyte brushes modeled using augmented strong stretching theory.  United States: N. p., 2019. 
Web.  doi:10.1002/elps.201900248.

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                    Sachar, Harnoor Singh, Sivasankar, Vishal Sankar, Etha, Sai Ankit, Chen, Guang, & Das, Siddhartha. Ionic current in nanochannels grafted with pH-responsive polyelectrolyte brushes modeled using augmented strong stretching theory.  United States.  https://doi.org/10.1002/elps.201900248

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                    Sachar, Harnoor Singh, Sivasankar, Vishal Sankar, Etha, Sai Ankit, Chen, Guang, and Das, Siddhartha. Sat .  
"Ionic current in nanochannels grafted with pH-responsive polyelectrolyte brushes modeled using augmented strong stretching theory".  United States.  https://doi.org/10.1002/elps.201900248.  https://www.osti.gov/servlets/purl/1595335.

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@article{osti_1595335,

  title        = {Ionic current in nanochannels grafted with pH-responsive polyelectrolyte brushes modeled using augmented strong stretching theory},

  author       = {Sachar, Harnoor Singh and Sivasankar, Vishal Sankar and Etha, Sai Ankit and Chen, Guang and Das, Siddhartha},

  abstractNote = {Here, we provide a theory to quantify the ionic current (iion) in nanochannels grafted with pH-responsive polyelectrolyte (PE) brushes. We consider the PE brushes to be modelled by our recently proposed augmented strong stretching theory (SST) model that improves the existing SST models by incorporating the effects of excluded volume interactions and an extended mass action law. Use of such augmented SST for this problem implies that this is the first study on computing iion in PE-brush-grafted nanochannels accounting for the appropriate coupled con guration-electrostatic description of the PE brushes. iion is obtained as functions of PE brush grafting density, medium pH and salt concentration (c∞), and the density of polyelectrolyte chargeable sites (PECS). For large c∞, iion increases linearly with c∞ (as for such c∞, iion becomes independent of the PE charge and is dominated by the bulk mobility and number density of the electrolyte ions), while iion is independent of c∞ at small c∞ (where the EDL electrostatics and the total number of ions in the system is dominated by the hydrogen ions). We further witness an enhancement of iion for smaller pH and larger grafting density at low and moderate c∞, while there is little to no effect of the PECS density on the ionic current except for weakly grafted brushes at low c∞. We believe that this study will serve as a theoretical foundation for a large number of applications that are based on the brush-induced modification of the ionic current in a nanochannel.},

  doi          = {10.1002/elps.201900248},

  journal      = {Electrophoresis},

  number       = 7-8,

  volume       = 41,

  place        = {United States},

  year         = {2019},

  month        = {9}

}

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Title: Ionic current in nanochannels grafted with pH-responsive polyelectrolyte brushes modeled using augmented strong stretching theory

Abstract

Citation Formats

Rectification of ionic current in nanopores functionalized with bipolar polyelectrolyte brushes journal, April 2018

Single Conical Nanopores Displaying pH-Tunable Rectifying Characteristics. Manipulating Ionic Transport With Zwitterionic Polymer Brushes journal, February 2009

An improved model for predicting electrical conductance in nanochannels journal, January 2015

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Highly enhanced liquid flows via thermoosmotic effects in soft and charged nanochannels journal, January 2018

Massively Enhanced Electroosmotic Transport in Nanochannels Grafted with End-Charged Polyelectrolyte Brushes journal, March 2017

Electroosmotic transport in polyelectrolyte-grafted nanochannels with pH-dependent charge density journal, May 2015

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Ion transport and selectivity in biomimetic nanopores with pH-tunable zwitterionic polyelectrolyte brushes journal, January 2015

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Ionic Diffusoosmosis in Nanochannels Grafted with End-Charged Polyelectrolyte Brushes journal, July 2018

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Buffer effect on the ionic conductance in a pH-regulated nanochannel journal, February 2015

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Hydrogen Peroxide Sensing with Horseradish Peroxidase-Modified Polymer Single Conical Nanochannels journal, March 2011

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Rectification of ionic current in nanopores functionalized with bipolar polyelectrolyte brushes
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Single Conical Nanopores Displaying pH-Tunable Rectifying Characteristics. Manipulating Ionic Transport With Zwitterionic Polymer Brushes
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Highly enhanced liquid flows via thermoosmotic effects in soft and charged nanochannels
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Efficient electrochemomechanical energy conversion in nanochannels grafted with end-charged polyelectrolyte brushes at medium and high salt concentration
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Ion transport and selectivity in biomimetic nanopores with pH-tunable zwitterionic polyelectrolyte brushes
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Chiral recognition of l -tryptophan with beta-cyclodextrin-modified biomimetic single nanochannel
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Tunable Donnan Potential and Electrokinetic Flow in a Biomimetic Gated Nanochannel with pH-Regulated Polyelectrolyte Brushes
journal, August 2014

Alternating current electroosmotic flow in polyelectrolyte-grafted nanochannel
journal, November 2016

Electrokinetics in polyelectrolyte grafted nanofluidic channels modulated by the ion partitioning effect
journal, January 2016

Synthetic Proton-Gated Ion Channels via Single Solid-State Nanochannels Modified with Responsive Polymer Brushes
journal, July 2009

Ionic Diffusoosmosis in Nanochannels Grafted with End-Charged Polyelectrolyte Brushes
journal, July 2018

Self-consistent field theory of polyelectrolyte brushes with finite chain extensibility
journal, June 2017

Influence of salt valence on the rectification behavior of nanochannels
journal, December 2018

Efficient electrochemomechanical energy conversion in nanochannels grafted with polyelectrolyte layers with pH-dependent charge density
journal, January 2016

Structure and interaction of weakly charged polyelectrolyte brushes: Self-consistent field theory
journal, October 1997

Carbohydrate-actuated nanofluidic diode: switchable current rectification in a nanopipette
journal, January 2013

Buffer effect on the ionic conductance in a pH-regulated nanochannel
journal, February 2015

The effect of the surface functionalization and the electrolyte concentration on the electrical conductance of silica nanochannels
journal, May 2013

Electrokinetic energy conversion efficiency of viscoelastic fluids in a polyelectrolyte-grafted nanochannel
journal, August 2017

Electrokinetic ion and fluid transport in nanopores functionalized by polyelectrolyte brushes
journal, January 2012

Screening Effects in a Polyelectrolyte Brush: Self-Consistent-Field Theory
journal, June 2000

Transient alternating current electroosmotic flow of a Jeffrey fluid through a polyelectrolyte-grafted nanochannel
journal, January 2017

Hydrogen Peroxide Sensing with Horseradish Peroxidase-Modified Polymer Single Conical Nanochannels
journal, March 2011

Poisson–Boltzmann Theory of pH-Sensitive (Annealing) Polyelectrolyte Brush
journal, September 2011

Streaming potential and electroviscous effects in soft nanochannels beyond Debye–Hückel linearization
journal, May 2015

Field effect regulation of Donnan potential and electrokinetic flow in a functionalized soft nanochannel
journal, January 2013

Protein Biosensors Based on Biofunctionalized Conical Gold Nanotubes
journal, April 2005

pH-regulated ionic current rectification in conical nanopores functionalized with polyelectrolyte brushes
journal, January 2014

Analytical Self-Consistent-Field Model of Weak Polyacid Brushes
journal, May 1995

Ionic Current Rectification in a Conical Nanopore: Influences of Electroosmotic Flow and Type of Salt
journal, February 2017

Streaming potential and electroviscous effects in soft nanochannels: towards designing more efficient nanofluidic electrochemomechanical energy converters
journal, January 2014

Layer-by-Layer Assembly of Polyelectrolytes into Ionic Current Rectifying Solid-State Nanopores: Insights from Theory and Experiment
journal, June 2010

Voltage-controlled ion transport and selectivity in a conical nanopore functionalized with pH-tunable polyelectrolyte brushes
journal, March 2019

Electrokinetics in nanochannels
journal, September 2008

Gating of Single Synthetic Nanopores by Proton-Driven DNA Molecular Motors
journal, July 2008

Electrokinetic energy conversion in nanochannels grafted with pH-responsive polyelectrolyte brushes modelled using augmented strong stretching theory
journal, January 2019

Ionic Current Rectification in a pH-Tunable Polyelectrolyte Brushes Functionalized Conical Nanopore: Effect of Salt Gradient
journal, December 2015

Electrokinetics in nanochannels
journal, September 2008