Capturing charge and size effects of ions at the graphene–electrolyte interface using polarizable force field simulations

Haridas, Hemanth; Mewada, Rohan; Mallajosyula, Sairam S.

doi:10.1039/d2na00733a

Cited by 2 publications

(6 citation statements)

References 47 publications

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“…However, in Drude polarizable FF simulations, the graphene surface is able to respond to changes in the local environment, specifically the negative charge on the phosphate, leading to the accurate capture of both vdW and electrostatic interactions between the dimethyl phosphate molecule and the graphene surface. Drude polarizable simulations were able to capture similar interactions between the negatively charged Cl – ion and the graphene surface, which could not be captured by additive (nonpolarizable) simulations . Using batch adsorption experiments, Vasudevan and Lakshmi have shown that graphene has excellent phosphate adsorption properties .…”

Section: Resultsmentioning

confidence: 99%

“…Drude polarizable simulations were able to capture similar interactions between the negatively charged Cl − ion and the graphene surface, which could not be captured by additive (nonpolarizable) simulations. 39 Using batch adsorption experiments, Vasudevan and Lakshmi have shown that graphene has excellent phosphate adsorption properties. 66 They observed that the interaction of phosphate with the graphene surface was highly endothermic and a spontaneous process.…”

Section: ■ Computational Methodsmentioning

confidence: 99%

“…Herein, in the low surface loading concentration (0.25 M) limit, the simulations were able to capture ordered self-assemblies that were consistent with the experimental assemblies of cytosine nucleobases adsorbed at 1-octanol/HOPG solid–liquid interfaces and on Au(111) surfaces , observed via HR-STM imaging. Additionally, the developed parameters were also used to capture the solvation dynamics of ions at the graphene electrolyte interface . The polarizable simulations were able to capture both the size- and charge-dependent ion–graphene interactions.…”

Section: Introductionmentioning

confidence: 99%

“…Additionally, the developed parameters were also used to capture the solvation dynamics of ions at the graphene electrolyte interface. 39 The polarizable simulations were able to capture both the size-and chargedependent ion−graphene interactions. In particular, the Drude parameters were able to reliably capture anion−graphene interactions.…”

Section: ■ Introductionmentioning

confidence: 99%

“…We note that all these effects which were captured by polarizable simulations are severely underestimated in the additive (nonpolarizable) simulations. 32,37,39 Polarizable force fields have also been found to accurately describe the thermodynamics of ion permeation in biological nanopores which could not be described by additive (nonpolarizable) simulations. 40 In this study, we use polarizable simulations for the first time to study the translocation dynamics of ssDNA through a graphene nanopore.…”

Section: ■ Introductionmentioning

confidence: 99%

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Unveiling DNA Translocation in Pristine Graphene Nanopores: Understanding Pore Clogging via Polarizable Simulations

H.,

Mallajosyula

2023

ACS Appl. Mater. Interfaces

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Graphene has garnered remarkable attention in recent years as an attractive nanopore membrane for rapid and accurate sequencing of DNA. The inherent characteristics of graphene offer exquisite experimental control over pore dimensions, encompassing both the width (pore diameter) and height. Despite these promising prospects, the practical deployment of pristine graphene nanopores for DNA sequencing has encountered a formidable challenge in the form of pore clogging, which is primarily attributed to hydrophobic interactions. However, a comprehensive understanding of the atomistic origins underpinning this clogging phenomenon and the nuanced impact of individual nucleobase identities on clogging dynamics remain an underexplored domain. Elucidating the atomistic intricacies governing pore clogging is pivotal to devising strategies for its mitigation and advancing our understanding of graphene nanopore behavior. We harness Drude polarizable simulations to systematically dissect the nucleobase-dependent mechanisms that play a pivotal role in nanopore clogging. We unveil nucleobase-specific interactions that illuminate the multifaceted roles played by both hydrophobic and electrostatic forces in driving nanopore clogging events. Notably, the Drude simulations also unveil the bias-dependent translocation dynamics and its pivotal role in alleviating pore clogging�a facet that remains significantly underestimated in conventional additive (nonpolarizable) simulations. Our findings underscore the indispensability of incorporating polarizability to faithfully capture the intricate dynamics governing graphene nanopore translocation phenomena, thus deepening our insights into this crucial field.

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Section: Resultsmentioning

confidence: 99%

Section: ■ Computational Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Unveiling DNA Translocation in Pristine Graphene Nanopores: Understanding Pore Clogging via Polarizable Simulations

H.,

Mallajosyula

2023

ACS Appl. Mater. Interfaces

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Molecular modeling study on the water-electrode surface interaction in hydrovoltaic energy

Serdaroğlu,

Kariper,

Kariper

2023

Sci Rep

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The global energy problem caused by the decrease in fossil fuel sources, which have negative effects on human health and the environment, has made it necessary to research alternative energy sources. Renewable energy sources are more advantageous than fossil fuels because they are unlimited in quantity, do not cause great harm to the environment, are safe, and create economic value by reducing foreign dependency because they are obtained from natural resources. With nanotechnology, which enables the development of different technologies to meet energy needs, low-cost and environmentally friendly systems with high energy conversion efficiency are developed. Renewable energy production studies have focused on the development of hydrovoltaic technologies, in which electrical energy is produced by making use of the evaporation of natural water, which is the most abundant in the world. By using nanomaterials such as graphene, carbon nanoparticles, carbon nanotubes, and conductive polymers, hydrovoltaic technology provides systems with high energy conversion performance and low cost, which can directly convert the thermal energy resulting from the evaporation of water into electrical energy. The effect of the presence of water on the generation of energy via the interactions between the ion(s) and the liquid–solid surface can be enlightened by the mechanism of the hydovoltaic effect. Here, we simply try to get some tricky information underlying the hydrovoltaic effect by using DFT/B3LYP/6-311G(d, p) computations. Namely, the physicochemical and electronic properties of the graphene surface with a water molecule were investigated, and how/how much these quantities (or parameters) changed in case of the water molecule contained an equal number of charges were analyzed. In these computations, an excess of both positive charge and negative charge, and also a neutral environment was considered by using the Na+, Cl−, and NaCl salt, respectively.

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Capturing charge and size effects of ions at the graphene–electrolyte interface using polarizable force field simulations

Abstract: We present a systematic investigation capturing the charge and size effects of ions interacting with the graphene surface using polarizable simulations. Our results utilizing the Drude polarizable force field (FF)...

Cited by 2 publications

References 47 publications

Unveiling DNA Translocation in Pristine Graphene Nanopores: Understanding Pore Clogging via Polarizable Simulations

Unveiling DNA Translocation in Pristine Graphene Nanopores: Understanding Pore Clogging via Polarizable Simulations

Molecular modeling study on the water-electrode surface interaction in hydrovoltaic energy

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