3 years ago

Design of Multifunctional Nanogate in Response to Multiple External Stimuli Using Amphiphilic Diblock Copolymer

Design of Multifunctional Nanogate in Response to Multiple External Stimuli Using Amphiphilic Diblock Copolymer
Igal Szleifer, Kai Huang
Nature uses the interplay between hydrophobic and electrostatic interactions of disordered proteins to orchestrate complicated molecular gates such as the nuclear pore complex to control the transport of biological masses. Inspired by nature, we here theoretically show that well-defined gate shape, sensitive response to pH and salt concentration, and selectivity in cargo transport can be simultaneously achieved by grafting amphiphilic diblock copolymers made of sequence-controlled hydrophobic and ionizable monomers on the inner surface of solid-state nanopore. As a result, multiple functions such as ionic gating and molecular filtering can be implemented into one single copolymer nanogate. The gate structure and thermodynamics is a result of the self-assembly of the sequence-designed copolymer in the confined geometry that minimizes the free energy of the system. Our theory further predicts a phase transition and discontinuous charge regulation of the confined copolymer that allows logical gating in biosensors and nanofluidic devices. As an example of application, a nanolocker with the potential of molecular pumping has also been designed with the cooperation of two amphiphilic copolymer gates. Our results highlight the importance of polymer sequence in nanogating, and these insights can be used to guide the rational design of polymer-coated smart nanopores.

Publisher URL: http://dx.doi.org/10.1021/jacs.7b02057

DOI: 10.1021/jacs.7b02057

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