Developing force field parameters for water interacting with graphene and graphene-like materials

Confined water can have properties dramatically different from bulk water, and these properties can be used to develop unique functionality at the nanoscale. For example, fast water transport, rotation-translation coupling, and fast rotationalmotion have been observed in graphitic carbon-based nano structures, which enables various applications like energy storage and seawater desalination. The explosive studies on graphene have sparked new interests towards graphene-analogous materials including hexagonal boron nitride (hBN) and molybdenum disulfide (MoS2). Compared to graphene, the graphene-analogous materials possess non-zero bandgap, chemical inertness, and biological compatibility. The graphene-analogous materials are promising materials, complementary to graphene, for high-temperature, biomedical and nanofluidic applications. We would like to understand and optimize graphene and graphene-analogous materials in these applications. The study of graphene and graphene-analogous materials at the atomic level requires accurate force field parameters to describe the water-surface interaction. We begin with benchmark quality first principles quantum Monte Carlo (QMC) calculations on the interaction energy between water and surface, which are used to validate random phase approximation (RPA) calculations. We then proceed with RPA to derive force field parameters, which are used to simulate properties like water contact angle on the surface, attaining a value within the experimental uncertainties. This work demonstrates that end-to-end multiscale modeling, starting at detailed many-body quantum mechanics, and ending with macroscopic properties, with the approximations controlled along the way, is feasible for these systems.

Name thesis:degree_name

Ph.D.

Level thesis:degree_level

Dissertation

Discipline thesis:degree_discipline

Mechanical Engineering

Grantor

University of Illinois at Urbana-Champaign

Year dc:date

2016

Author dc:creator

• Wu, Yanbin

Contributors dc:contributor

• Aluru, Narayana R.
• Ceperley, David
• Wagner, Lucas K.
• Nam, SungWoo

• Force field
• graphene
• water
• first principles
• multiscale
• hexagonal boron nitride (hBN)
• Molybdenum disulfide (MoS2)
• Diffusion Monte Carlo (DMC)
• Random phase approximation (RPA)
• Møller-Plesset perturbation theory (MP2)

Statement dc:rights

• Copyright 2016 Yanbin Wu

Language dc:language

en

Handle dc:identifier

http://hdl.handle.net/2142/93025

OAI identifier oai:identifier

oai:www.ideals.illinois.edu:2142/93025