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Oscillatory Reaction Induced Periodic C-Quadruplex DNA Gating of Artificial Ion Channels

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† Key Laboratory of Bio-inspired Materials and Interface Science, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, People’s Republic of China
‡ Department of Chemical Engineering, Monash University, Clayton, Victoria 3800, Australia
§ Beijing National Laboratory for Molecular Sciences, Key Laboratory of Green Printing, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, People’s Republic of China
∥ Key Laboratory of Organic Optoelectronics and Molecular Engineering, Department of Chemistry, Tsinghua University, Beijing 100084, People’s Republic of China
*E-mail (H. Zhang): [email protected]
*E-mail Y. Tian): [email protected]
Cite this: ACS Nano 2017, 11, 3, 3022–3029
Publication Date (Web):February 22, 2017
https://doi.org/10.1021/acsnano.6b08727
Copyright © 2017 American Chemical Society
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    Abstract

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    Many biological ion channels controlled by biochemical reactions have autonomous and periodic gating functions, which play important roles in continuous mass transport and signal transmission in living systems. Inspired by these functional biological ion channel systems, here we report an artificial self-oscillating nanochannel system that can autonomously and periodically control its gating process under constant conditions. The system is constructed by integrating a chemical oscillator, consisting of BrO3–, Fe(CN)64–, H+, and SO32–, into a synthetic proton-sensitive nanochannel modified with C-quadruplex (C4) DNA motors. The chemical oscillator, containing H+-producing and H+-consuming reactions, can cyclically drive conformational changes of the C4-DNA motors on the channel wall between random coil and folded i-motif structures, thus leading to autonomous gating of the nanochannel between open and closed states. The autonomous gating processes are confirmed by periodic high–low ionic current oscillations of the channel monitored under constant reaction conditions. The utilization of a chemical oscillator integrated with DNA molecules represents a method to directly convert chemical energy of oscillating reactions to kinetic energy of conformational changes of the artificial nanochannels and even to achieve diverse autonomous gating functions in artificial nanofluidic devices.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.6b08727.

    • SEM images of the cross section and the surface of the bullet-shaped nanochannel membrane, contact angles, XPS data and current–voltage measurements of the nanochannel before and after modification, C4-DNA molecular structure, experimental apparatus, original data of ionic currents, pH, ion conductivity, temperature, and redox potential oscillations of the reaction solution at 35 °C, pH and ionic current oscillation under conditions with and without peristaltic pumps, and dependence of on–off ratios on the channel size (PDF)

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