Phosphate‐Responsive Biomimetic Nanofluidic Diodes Regulated by Polyamine–Phosphate Interactions: Insights into Their Functional Behavior from Theory and Experiment

Pérez-Mitta, Gonzalo; Marmisollé, Waldemar A.; Albesa, Alberto G.; Toimil-Molares, María Eugenia; Trautmann, C.; Azzaroni, Omar

doi:10.1002/smll.201702131

Cited by 60 publications

(51 citation statements)

References 57 publications

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“…A large set of conformations of these polymer chains are generated using a Rotational Isomeric State (RIS) model (Flory 1969), where each polymer segment can assume one out of three iso-energetic relative orientations. The pKa of the allylamine group is 9.86 (Pérez-Mitta et al 2018).…”

Section: Methodsmentioning

confidence: 99%

Molecular theory of glyphosate adsorption to pH-responsive polymer layers

2019

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By means of a molecular-level theory we investigate glyphosate adsorption from aqueous solutions to surface-grafted poly(allylamine) layers. Our molecular model of glyphosate and the polymeric material includes description of size, shape, conformational freedom, and state of protonation of both components. The composition of the bulk solution (pH, salt concentration and glyphosate concentration) plays a critical role to determine adsorption. Adsorption is a non-monotonic function of the solution pH, which can be explained in terms of the pH-dependent protonation behavior of both adsorbate and adsorbent material. Lowering the solution salinity is an efficient way to enhance glyphosate adsorption. This is because glyphosate and salt anions compete for adsorption to the polymer layer. In this competition, glyphosate deprotonation, to increase its negative charge upon entering the polymer layer, plays an critical role to favor its adsorption under a variety of solution conditions. This deprotonation is the result of the higher pH that establishes inside the polymer. Our results show that such pH increase can be controlled, while achieving significant glyphosate adsorption, through varying the grafting density of the material. This result is important since glyphosate degradation by microbial activity is pH-dependent. These polymeric systems are excellent candidates for the development functional materials that combine glyphosate sequestration and in situ biodegradation.

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Section: Methodsmentioning

confidence: 99%

Molecular theory of glyphosate adsorption to pH-responsive polymer layers

2019

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“…7(a)(iii)-(v)). 34,36,[143][144][145][146][147][148] For nanosized channels, the channel shape (cylindrical or conical) has a strong inuence on the I-V curve, e.g. leading to a diodelike behavior.…”

Section: Diffusio-osmotic Mechanismmentioning

confidence: 99%

Nanofluidic osmotic power generators – advanced nanoporous membranes and nanochannels for blue energy harvesting

et al. 2021

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“…In recent years, the modification of solid‐state nanopores via polyelectrolyte assembly/adsorption has gained increasing interest . The LbL assembly of polyelectrolytes represents a very simple and versatile chemical method to create functional thin films with nanoscale precision .…”

Section: Functionalization Of Solid‐state Nanoporesmentioning

confidence: 99%

Molecular Design of Solid‐State Nanopores: Fundamental Concepts and Applications

et al. 2019

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Solid‐state nanopores are fascinating objects that enable the development of specific and efficient chemical and biological sensors, as well as the investigation of the physicochemical principles ruling the behavior of biological channels. The great variety of biological nanopores that nature provides regulates not only the most critical processes in the human body, including neuronal communication and sensory perception, but also the most important bioenergetic process on earth: photosynthesis. This makes them an exhaustless source of inspiration toward the development of more efficient, selective, and sophisticated nanopore‐based nanofluidic devices. The key point responsible for the vibrant and exciting advance of solid nanopore research in the last decade has been the simultaneous combination of advanced fabrication nanotechnologies to tailor the size, geometry, and application of novel and creative approaches to confer the nanopore surface specific functionalities and responsiveness. Here, the state of the art is described in the following critical areas: i) theory, ii) nanofabrication techniques, iii) (bio)chemical functionalization, iv) construction of nanofluidic actuators, v) nanopore (bio)sensors, and vi) commercial aspects. The plethora of potential applications once envisioned for solid‐state nanochannels is progressively and quickly materializing into new technologies that hold promise to revolutionize the everyday life.

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Phosphate‐Responsive Biomimetic Nanofluidic Diodes Regulated by Polyamine–Phosphate Interactions: Insights into Their Functional Behavior from Theory and Experiment

Cited by 60 publications

References 57 publications

Molecular theory of glyphosate adsorption to pH-responsive polymer layers

Molecular theory of glyphosate adsorption to pH-responsive polymer layers

Nanofluidic osmotic power generators – advanced nanoporous membranes and nanochannels for blue energy harvesting

Molecular Design of Solid‐State Nanopores: Fundamental Concepts and Applications

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