Ion Gating in Nanopore Electrode Arrays with Hierarchically Organized pH-Responsive Block Copolymer Membranes

Baek, Seol; Kwon, Seung-Ryong; Fu, Kaiyu; Bohn, Paul W.

doi:10.1021/acsami.0c12926

Title: Ion Gating in Nanopore Electrode Arrays with Hierarchically Organized pH-Responsive Block Copolymer Membranes

Abstract

Inspired by biological ion channels, artificial nanopore-based architectures have been developed for smart ion/molecular transport control with potential applications to iontronics and energy conversion. Advances in nanofabrication technology enable simple, versatile construction methods, and post-fabrication functionalization delivers nanochannels with unique ion transport-control attributes. Here, we characterize a pH-responsive, charge-selective dual-gating block copolymer (BCP) membrane composed of polystyrene-b-poly(4-vinylpyridine) (PS₄₈₄₀₀-b-P4VP₂₁₃₀₀), capable of self-organizing into highly ordered nanocylindrical domains. Because the PS-b-P4VP membrane exhibits pH-dependent structural transitions, it is suitable for designing intelligent pH-gated biomimetic channels, for example, exhibiting on–off transport switching at pH values near the pK_a of P4VP with excellent anion permselectivity at pH < pK_a. Introducing the BCP membrane onto nanopore electrode arrays (BCP@NEAs) allows the BCP to serve as a pH-responsive gate controlling ion transfer into the NEA nanopores. Such selectively transported and confined ions are detected by using a 100 nm gap dual-ring nanoelectrode structure capable of enhancing current output by efficient redox cycling with an amplification factor >10². In addition, BCP@NEAs exhibit extraordinary pH-gated ion selectivity, resulting in a 3380-fold current difference between anion and cation probes at pH 3.0. Furthermore, this hierarchically organized BCP-gated NEA system can serve as a template for the development of othermore »« less

Authors:

Baek, Seol ^[1];

^[1];

^[2];

^[1]

Univ. of Notre Dame, IN (United States)
Stanford Univ., CA (United States)

Publication Date:: Sat Nov 21 00:00:00 EST 2020

Research Org.:: Univ. of Notre Dame, IN (United States)

Sponsoring Org.:: USDOE Office of Science (SC); National Science Foundation (NSF)

OSTI Identifier:: 1737368

Grant/Contract Number:: FG02-07ER15851

Resource Type:: Accepted Manuscript

Journal Name:: ACS Applied Materials and Interfaces

Additional Journal Information:: Journal Volume: 12; Journal Issue: 49; Journal ID: ISSN 1944-8244

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Nanopore electrode arrays; block copolymers; redox cycling; ion channels; pH gates; permselectivity; redox reactions; electrodes; ions; membranes; nanopores

Citation Formats


                    Baek, Seol, Kwon, Seung-Ryong, Fu, Kaiyu, and Bohn, Paul W. Ion Gating in Nanopore Electrode Arrays with Hierarchically Organized pH-Responsive Block Copolymer Membranes.  United States: N. p., 2020. 
Web.  doi:10.1021/acsami.0c12926.

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                    Baek, Seol, Kwon, Seung-Ryong, Fu, Kaiyu, & Bohn, Paul W. Ion Gating in Nanopore Electrode Arrays with Hierarchically Organized pH-Responsive Block Copolymer Membranes.  United States.  https://doi.org/10.1021/acsami.0c12926

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                    Baek, Seol, Kwon, Seung-Ryong, Fu, Kaiyu, and Bohn, Paul W. Sat .  
"Ion Gating in Nanopore Electrode Arrays with Hierarchically Organized pH-Responsive Block Copolymer Membranes".  United States.  https://doi.org/10.1021/acsami.0c12926.  https://www.osti.gov/servlets/purl/1737368.

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@article{osti_1737368,

  title        = {Ion Gating in Nanopore Electrode Arrays with Hierarchically Organized pH-Responsive Block Copolymer Membranes},

  author       = {Baek, Seol and Kwon, Seung-Ryong and Fu, Kaiyu and Bohn, Paul W.},

  abstractNote = {Inspired by biological ion channels, artificial nanopore-based architectures have been developed for smart ion/molecular transport control with potential applications to iontronics and energy conversion. Advances in nanofabrication technology enable simple, versatile construction methods, and post-fabrication functionalization delivers nanochannels with unique ion transport-control attributes. Here, we characterize a pH-responsive, charge-selective dual-gating block copolymer (BCP) membrane composed of polystyrene-b-poly(4-vinylpyridine) (PS48400-b-P4VP21300), capable of self-organizing into highly ordered nanocylindrical domains. Because the PS-b-P4VP membrane exhibits pH-dependent structural transitions, it is suitable for designing intelligent pH-gated biomimetic channels, for example, exhibiting on–off transport switching at pH values near the pKa of P4VP with excellent anion permselectivity at pH < pKa. Introducing the BCP membrane onto nanopore electrode arrays (BCP@NEAs) allows the BCP to serve as a pH-responsive gate controlling ion transfer into the NEA nanopores. Such selectively transported and confined ions are detected by using a 100 nm gap dual-ring nanoelectrode structure capable of enhancing current output by efficient redox cycling with an amplification factor >102. In addition, BCP@NEAs exhibit extraordinary pH-gated ion selectivity, resulting in a 3380-fold current difference between anion and cation probes at pH 3.0. Furthermore, this hierarchically organized BCP-gated NEA system can serve as a template for the development of other stimulus-responsive ion gates, for example, those based on temperature and ligand gating, thus exploiting the intrinsic advantages of NEAs, such as enhanced sensitivity based on redox cycling, which may lead to technological applications such as engineered biosensors and iontronic devices.},

  doi          = {10.1021/acsami.0c12926},

  journal      = {ACS Applied Materials and Interfaces},

  number       = 49,

  volume       = 12,

  place        = {United States},

  year         = {Sat Nov 21 00:00:00 EST 2020},

  month        = {Sat Nov 21 00:00:00 EST 2020}

}

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Title: Ion Gating in Nanopore Electrode Arrays with Hierarchically Organized pH-Responsive Block Copolymer Membranes

Abstract

Citation Formats

The Structure of the Potassium Channel: Molecular Basis of K+ Conduction and Selectivity journal, April 1998

Principles of Selective Ion Transport in Channels and Pumps journal, December 2005

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Fundamental studies and practical applications of bio-inspired smart solid-state nanopores and nanochannels journal, February 2016

Solid-state nanopore based biomimetic voltage gated ion channels journal, November 2017

Biomimetic potassium-selective nanopores journal, February 2019

Recent Advances in Solid Nanopore/Channel Analysis journal, December 2017

Thermo- and pH-responsive graphene oxide membranes with tunable nanochannels for water gating and permeability of small molecules journal, October 2019

Electric-field-induced wetting and dewetting in single hydrophobic nanopores journal, October 2011

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Polydispersity and block copolymer self-assembly journal, September 2008

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Voltage-Gated Hydrophobic Nanopores
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Voltage Gating of a Biomimetic Nanopore: Electrowetting of a Hydrophobic Barrier
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Counterion Binding in Aqueous Solutions of Poly(vinylpyridines) as Assessed by Potentiometric Titration
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The influence of cations on the electrode kinetics of ferricyanide-ferrocyanide system on the rotating gold electrode
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A microelectrode study of the mechanism and kinetics of the ferro/ferricyanide couple in aqueous media: The influence of the electrolyte and its concentration
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pH-Sensitive nano-systems for drug delivery in cancer therapy
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Iontronics: A Decade of Iontronic Delivery Devices (Adv. Mater. Technol. 5/2018)
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Endeavor of Iontronics: From Fundamentals to Applications of Ion‐Controlled Electronics
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