Stimuli-Responsive Polymer Brushes for Flow Control through Nanopores

Adiga, Shashishekar P.; Brenner, Donald W.

doi:10.3390/jfb3020239

Cited by 67 publications

(54 citation statements)

References 46 publications

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“…For instance, grafting nanocarriers with polymers improves their bio-compatibility and stability, making them a promising candidate for drug transport [4,5]. Channels coated with polymers regulate flows and enable “smart” functionalities in sieving, separation, and remote control [6,7,8]. Such wide-spread applications have stimulated the fundamental research on transport phenomena involving polymer-grafted surfaces [9,10,11,12,13].…”

Section: Introductionmentioning

confidence: 99%

Hydrodynamic Properties of Polymers Screening the Electrokinetic Flow: Insights from a Computational Study

Sun

Jiang

et al. 2019

Polymers

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Understanding the hydrodynamic properties of polymeric coatings is crucial for the rational design of molecular transport involving polymeric surfaces and is relevant to drug delivery, sieving, molecular separations, etc. It has been found that the hydrodynamic radius of a polymer segment is an order of magnitude smaller than its physical size, but the origin of this effect does not seem to be well understood. Herein, we study the hydrodynamic properties of polymeric coatings by using molecular dynamics simulations, navigated by the continuous Navier-Stokes-Brinkman model. We confirm that the averaged hydrodynamic radius of a polymer bead is about one order of magnitude smaller than its physical radius, and, in addition, we show that it exhibits a strong dependence on the degree of polymerization. We relate this variation of the hydrodynamic radius to the structural properties and hydrodynamic shielding by surrounding polymer beads. This is done by separating the effects originating from near and far beads. For the near beads, shielding is mainly due to the two nearest beads (of the same polymer) and leads to about a 5-fold reduction in the hydrodynamic radius. Assuming the additivity of the hydrodynamic shielding by far beads, we suggest a simple model, which captures correctly the qualitative behaviour of the hydrodynamic radius with the degree of polymerization. The revealed shielding effects provide important insights relevant to the advanced modelling of hydrodynamic properties of polymeric coatings.

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Section: Introductionmentioning

confidence: 99%

Hydrodynamic Properties of Polymers Screening the Electrokinetic Flow: Insights from a Computational Study

Sun

Jiang

et al. 2019

Polymers

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“…[15][16][17][18] Solid-state nanopores grafted with polymers are also suggested as a possible flow control mechanism in microfluidic systems, responding to stimuli such as temperature or pH. 19,20 A fascinating example of a polymer-coated nanopore can be found in the living cell, where the nuclear pore complex (NPC) is responsible for all macromolecular transport between the cell nucleus and the cytoplasm. 21,22 The walls of the NPC are lined with natively unfolded proteins, which are intrinsically disordered and rich in the phenylalanine-glycine (FG) repeat amino-acid sequence.…”

Section: Introductionmentioning

confidence: 99%

Effects of rotational symmetry breaking in polymer-coated nanopores

Osmanović

Kerr-Winter

Eccleston

et al. 2015

The Journal of Chemical Physics

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The statistical theory of polymers tethered around the inner surface of a cylindrical channel has traditionally employed the assumption that the equilibrium density of the polymers is independent of the azimuthal coordinate. However, simulations have shown that this rotational symmetry can be broken when there are attractive interactions between the polymers. We investigate the phases that emerge in these circumstances, and we quantify the effect of the symmetry assumption on the phase behavior of the system. In the absence of this assumption, one can observe large differences in the equilibrium densities between the rotationally symmetric case and the non-rotationally symmetric case. A simple analytical model is developed that illustrates the driving thermodynamic forces responsible for this symmetry breaking. Our results have implications for the current understanding of the polymer behavior in cylindrical nanopores.

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“…Some polymer brushes are environment-sensitive, with specific changes in solvent conditions triggering their expansion or collapse. These materials can be used to exert dynamic control over the spatial presentation of regulatory peptides and are under investigation for many applications 4,5 , including sensors 6 , flow valves 7 and controlled drug release systems 8 . However, because these brushes are almost universally constructed from synthetic polymers, they are frequently somewhat heterogeneous and are challenging to modify at specific monomeric positions along the chain.…”

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confidence: 99%

Stimuli-sensitive intrinsically disordered protein brushes

et al. 2014

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Grafting polymers onto surfaces at high density to yield polymer brush coatings is a widely employed strategy to reduce biofouling and interfacial friction. These brushes almost universally feature synthetic polymers, which are often heterogeneous and do not readily allow incorporation of chemical functionalities at precise sites along the constituent chains. To complement these synthetic systems, we introduce a biomimetic, recombinant intrinsically disordered protein that can assemble into an environment-sensitive brush. This macromolecule adopts an extended conformation and can be grafted to solid supports to form oriented protein brushes that swell and collapse dramatically with changes in solution pH and ionic strength. We illustrate the value of sequence specificity by using proteases with mutually orthogonal recognition sites to modulate brush height in situ to predictable values. This study demonstrates that stimuli-responsive brushes can be fabricated from proteins and introduces them as a new class of smart biomaterial building blocks.

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Stimuli-Responsive Polymer Brushes for Flow Control through Nanopores

Cited by 67 publications

References 46 publications

Hydrodynamic Properties of Polymers Screening the Electrokinetic Flow: Insights from a Computational Study

Hydrodynamic Properties of Polymers Screening the Electrokinetic Flow: Insights from a Computational Study

Effects of rotational symmetry breaking in polymer-coated nanopores

Stimuli-sensitive intrinsically disordered protein brushes

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