Adsorption and diffusion of water on graphene from first principles

Ma, Jie; Michaelides, Angelos; Alfè, Dario; Schimka, Laurids; Kresse, Georg; Wang, Enge

doi:10.1103/physrevb.84.033402

Cited by 266 publications

(295 citation statements)

References 30 publications

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“…42 This functional was shown to describe with a good accuracy both liquid water 43 and soft layered materials such as graphite and BN. 44 As compared to reference quantum Monte Carlo data, [45][46][47] it slightly overbinds water to graphene and BN, but the relative energy differences between different sites (relevant to friction) are well described (see the SI of Ref. 14 ).…”

mentioning

confidence: 92%

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

Joly

Tocci

Mérabia

et al. 2016

J. Phys. Chem. Lett.

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Defects are inevitably present in nanofluidic systems, yet the role they play in nanofluidic transport remains poorly understood. Here, we report ab initio molecular dynamics (AIMD) simulations of the friction of liquid water on defective graphene and boron nitride sheets. We show that water dissociates at certain defects and that these "reactive" defects lead to much larger friction than the "nonreactive" defects at which water molecules remain intact. Furthermore, we find that friction is extremely sensitive to the chemical structure of reactive defects and to the number of hydrogen bonds they can partake in with the liquid. Finally, we discuss how the insight obtained from AIMD can be used to quantify the influence of defects on friction in nanofluidic devices for water treatment and sustainable energy harvesting. Overall, we provide new insight into the role of interfacial chemistry on nanofluidic transport in real, defective systems.

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confidence: 92%

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

Joly

Tocci

Mérabia

et al. 2016

J. Phys. Chem. Lett.

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“…Hydrogen production through the splitting of water at a metal surface is of great interest for solar cell devices [1], and generating hydrogen and oxygen gas has been proposed as a means to store energy [2]. Despite significant efforts both computationally [3][4][5][6][7][8][9][10][11][12][13][14][15][16] and experimentally [14,[17][18][19] to study electrode-water interfaces, to-date, there has yet to be an explicit treatment of liquid water next to a realistic, catalytic surface computed at the level of accurate, first principles molecular dynamics. Almost 10 years ago, Cicero et al [3] studied several liquid water-graphene interfaces as well as water confined in carbon nanotubes with differing radii using DFT with the PBE exchange correlation functional [20].…”

Section: Introductionmentioning

confidence: 99%

Structural characterization of water-metal interfaces

Ryczko

Tamblyn

2017

Phys. Rev. B

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We analyze and compare the structural, dynamical, and electronic properties of liquid water next to prototypical metals including Pt, graphite, and graphene. Our results are built on BornOppenheimer molecular dynamics (BOMD) generated using density functional theory (DFT) which explicitly include van der Waals (vdW) interactions within a first principles approach. All calculations reported use large simulation cells, allowing for an accurate treatment of the water-electrode interfaces. We have included vdW interactions through the use of the optB86b-vdW exchange correlation functional. Comparisons with the Perdew-Burke-Ernzerhof (PBE) exchange correlation functional are also shown. We find an initial peak, due to chemisorption, in the density profile of the liquid water-Pt interface not seen in the liquid water-graphite interface, liquid water-graphene interface, nor interfaces studied previously. To further investigate this chemisorption peak, we also report differences in the electronic structure of single water molecules on both Pt and graphite surfaces. We find that a covalent bond forms between the single water molecule and the Pt surface, but not between the single water molecule and the graphite surface. We also discuss the effects that defects and dopants in the graphite and graphene surfaces have on the structure and dynamics of liquid water.

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“…[17][18][19] Despite the growing number of studies for water on h-BN [20][21][22] and graphene 15,16,[23][24][25][26][27] there are no direct measurements of adsorption energies for the water monomer, and the theoretical adsorption energies for these systems vary significantly across different high accuracy methods. 25,[27][28][29] One can use smaller model systems for graphene 25,[29][30][31][32] and h-BN, such as benzene and the inorganic counterpart borazine (B 3 N 3 H 6 ), to help understand the interaction with water. With these small molecules, it is possible to use high accuracy methods to calculate benchmark interaction energies and binding conformations, [33][34][35][36][37] that would otherwise be infeasible for the extended surfaces.…”

Section: Introductionmentioning

confidence: 99%

Water on BN doped benzene: A hard test for exchange-correlation functionals and the impact of exact exchange on weak binding

Al-Hamdani

Alfè

Lilienfeld

et al. 2014

The Journal of Chemical Physics

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Density functional theory (DFT) studies of weakly interacting complexes have recently focused on the importance of van der Waals dispersion forces, whereas the role of exchange has received far less attention. Here, by exploiting the subtle binding between water and a boron and nitrogen doped benzene derivative (1,2-azaborine) we show how exact exchange can alter the binding conformation within a complex. Benchmark values have been calculated for three orientations of the water monomer on 1,2-azaborine from explicitly correlated quantum chemical methods, and we have also used diffusion quantum Monte Carlo. For a host of popular DFT exchange-correlation functionals we show that the lack of exact exchange leads to the wrong lowest energy orientation of water on 1,2-azaborine. As such, we suggest that a high proportion of exact exchange and the associated improvement in the electronic structure could be needed for the accurate prediction of physisorption sites on doped surfaces and in complex organic molecules. Meanwhile to predict correct absolute interaction energies an accurate description of exchange needs to be augmented by dispersion inclusive functionals, and certain non-local van der Waals functionals (optB88- and optB86b-vdW) perform very well for absolute interaction energies. Through a comparison with water on benzene and borazine (B3N3H6) we show that these results could have implications for the interaction of water with doped graphene surfaces, and suggest a possible way of tuning the interaction energy.

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Adsorption and diffusion of water on graphene from first principles

Cited by 266 publications

References 30 publications

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

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

Structural characterization of water-metal interfaces

Water on BN doped benzene: A hard test for exchange-correlation functionals and the impact of exact exchange on weak binding

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