Strong Coupling between Nanofluidic Transport and Interfacial Chemistry: How Defect Reactivity Controls Liquid–Solid Friction through Hydrogen Bonding

Joly, Laurent; Tocci, Gabriele; Mérabia, Samy; Michaelides, Angelos

doi:10.1021/acs.jpclett.6b00280

Cited by 44 publications

(52 citation statements)

References 61 publications

Supporting

Mentioning

Contrasting

Unclassified

Order By: Relevance

“…Various theoretical studies on band gap engineering using h-BN and graphene mixtures, [15][16][17][18][19][20][21][22][23] have revealed the tuneability of these materials through the mixture of atoms. Other studies have focused on exploiting this tuneability for catalysis of oxygen reduction reactions, [24][25][26][27][28][29][30][31][32][33] water transport, 34 and H 2 adsorption. [35][36][37] An important aspect to consider, if using graphene and h-BN based materials as catalysts, is their degree of selectivity.…”

Section: Introductionmentioning

confidence: 99%

Tuning dissociation using isoelectronically doped graphene and hexagonal boron nitride: Water and other small molecules

Al-Hamdani

Alfè

Lilienfeld

et al. 2016

The Journal of Chemical Physics

Self Cite

View full text Add to dashboard Cite

Novel uses for 2-dimensional materials like graphene and hexagonal boron nitride (h-BN) are being frequently discovered especially for membrane and catalysis applications. Still however, a great deal remains to be understood about the interaction of environmentally and industrially relevant molecules such as water with these materials. Taking inspiration from advances in hybridising graphene and h-BN, we explore using density functional theory, the dissociation of water, hydrogen, methane, and methanol on graphene, h-BN, and their isoelectronic doped counterparts: BN doped graphene and C doped h-BN. We find that doped surfaces are considerably more reactive than their pristine counterparts and by comparing the reactivity of several small molecules, we develop a general framework for dissociative adsorption. From this a particularly attractive consequence of isoelectronic doping emerges: substrates can be doped to enhance their reactivity specifically towards either polar or non-polar adsorbates. As such, these substrates are potentially viable candidates for selective catalysts and membranes, with the implication that a range of tuneable materials can be designed. Published by AIP Publishing. [http://dx

show abstract

Section: Introductionmentioning

confidence: 99%

Tuning dissociation using isoelectronically doped graphene and hexagonal boron nitride: Water and other small molecules

Al-Hamdani

Alfè

Lilienfeld

et al. 2016

The Journal of Chemical Physics

Self Cite

View full text Add to dashboard Cite

show abstract

“…3 illustrate the difficulty to obtain the liquid-solid FC through the evaluation of the Green-Kubo integral of the friction force autocorrelation function [3,45] given by equilibrium MD simulations. In the evaluation of the Green-Kubo integral in systems of finite size, it is often assumed that the mass of the fluid involved in the liquid-solid friction is a finite constant [46][47][48], but the present results show that it is actually frequency dependent.…”

Section: A Identification Of the Hydrodynamic Boundary Conditionmentioning

confidence: 61%

Full characterization of the hydrodynamic boundary condition at the atomic scale using an oscillating channel: Identification of the viscoelastic interfacial friction and the hydrodynamic boundary position

et al. 2019

Self Cite

View full text Add to dashboard Cite

Flows in nanofluidic systems are controlled by the hydrodynamic boundary condition (BC), involving the friction coefficient and the hydrodynamic wall position. Here we considered a liquid nanoslab confined between two walls, where we derived, from the Stokes equation and the Navier slip BC, analytical expressions for the liquid response to an oscillatory tangential motion of the walls in terms of the wall shear stress and mean fluid velocity. By fitting these expressions to molecular dynamics simulation results, we could extract both the viscoelastic friction coefficient and hydrodynamic wall position for walls with three different wettabilities, hence fully characterizing the frequency-dependent hydrodynamic boundary condition. The proposed method could be applied to a variety of liquid-solid interfaces of interest, e.g., for flows of complex fluids or fluids at a low temperature. It should also support methodological developments on the characterization of the hydrodynamic slip in general.

show abstract

“…In particular, AIMD can be used to compute vibrational spectra and non-linear optical response [147,[160][161][162][163][164], and as such is a key tool to help interpret experimental observations. Recently, liquid-solid friction has been characterized with AIMD [165,166], opening perspectives for the investigation of other transport properties with these methods. At present, however, ab initio methods are typically based on density functional theory, and take electronic exchange and correlations into account through an approximate functional.…”

Section: Latest Developments In Molecular Modelingmentioning

confidence: 99%

Measuring surface charge: Why experimental characterization and molecular modeling should be coupled

Hartkamp

Biance

et al. 2018

Current Opinion in Colloid & Interface Science

Self Cite

View full text Add to dashboard Cite

Surface charge controls many static and dynamic properties of soft matter and micro/nanofluidic systems, but its unambiguous measurement forms a challenge. Standard characterization methods typically probe an effective surface charge, which provides limited insight into the distribution and dynamics of charge across the interface, and which cannot predict consistently all surfacecharge-governed properties. New experimental approaches provide local information on both structure and transport, but models are typically required to interpret raw data. Conversely, molecular dynamics simulations have helped showing the limits of standard models and developing more accurate ones, but their reliability is limited by the empirical interaction potentials they are usually based on. This review highlights recent developments and limitations in both experimental and computational research focusing on the liquid-solid interface. Based on recent studies, we make the case that coupling of experiments and simulations is pivotal to mitigate methodological shortcomings and address open problems pertaining to charged interfaces.

show abstract

Strong Coupling between Nanofluidic Transport and Interfacial Chemistry: How Defect Reactivity Controls Liquid–Solid Friction through Hydrogen Bonding

Cited by 44 publications

References 61 publications

Tuning dissociation using isoelectronically doped graphene and hexagonal boron nitride: Water and other small molecules

Tuning dissociation using isoelectronically doped graphene and hexagonal boron nitride: Water and other small molecules

Full characterization of the hydrodynamic boundary condition at the atomic scale using an oscillating channel: Identification of the viscoelastic interfacial friction and the hydrodynamic boundary position

Measuring surface charge: Why experimental characterization and molecular modeling should be coupled

Contact Info

Product

Resources

About