Nanoconfined Water within Graphene Slit Pores Adopts Distinct Confinement-Dependent Regimes

Abstract

In view of the increasing importance of nanoconfined aqueous solutions for various technological applications, it has become necessary to understand how strong confinement affects the properties of water at the level of molecular and even electronic structure. By performing extensive ab initio simulations of two-dimensionally nanoconfined water lamellae between graphene sheets subject to different interlayer spacings, we find new regimes at interlayer distances of 10 Å and less where water can be described neither to behave like interfacial water nor to be bulklike at the level of its H-bonding characteristics and electronic structure properties. It is expected that this finding will offer new opportunities to tune both diffusive and reactive processes taking place in aqueous environments that are strongly confined by chemically inert hard walls.

Water Structure, Dynamics, and Sum-Frequency Generation Spectra at Electrified Graphene Interfaces

“…This interfacial water molecular arrangement is very similar to that found e.g. at the air/water interface and at extended hydrophobic interfaces 17,18 (see SI); it is also consistent with prior simulation results obtained with both classical and DFT-based molecular dynamics 8,[19][20][21] of water at an uncharged graphene interface.…”

Sulfate, Bisulfate, and Hydrogen Co-adsorption on Pt(111) and Au(111) in an Electrochemical Environment

“…To include van-der-Waals interactions we used the D3 correction scheme by Grimme et al ( 2010 ). It has been shown that the RPBE-D3 approach reliably yields properties of liquid water (Tonigold and Groß, 2012 ; Forster-Tonigold and Groß, 2014 ; Morawietz et al, 2016 ; Sakong et al, 2016 ; Schienbein and Marx, 2018 ), the interaction of water with surfaces (Tonigold and Groß, 2012 ; Forster-Tonigold and Groß, 2014 ; Sakong et al, 2016 ; Sakong and Groß, 2018 ; Mahlberg et al, 2019 ; Ruiz-Barragan et al, 2019 ), and the interaction of organic molecules with metal surfaces (Koslowski et al, 2013 ; Sakong and Groß, 2016 ). The electron-core interaction was described by the projector augmented wave method (PAW) (Blöchl, 1994 ), as constructed by Kresse and Joubert ( 1999 ).…”

Transparent proton transport through a two-dimensional nanomesh material

“…Although dispersion correction remedies the bad performance of DFT in describing water–carbon adsorption interactions 46,47 , relatively large variations are still found in interaction energies between a single water molecule and graphene predicted by different DFT models 49,50 . Despite these discrepancies, dispersion-corrected generalized gradient approximation (GGA) still gives rise to reasonable interfacial structures between liquid water and graphene 51,52 or carbon nanotubes 53 , and describes well the monolayer ice on graphite 54 .…”