On the physisorption of water on graphene: Sub-chemical accuracy from many-body electronic structure methods

Abstract

Molecular adsorption on surfaces plays a central role in catalysis, corrosion, desalination, and many other processes of relevance to industry and the natural world. Few adsorption systems are more ubiquitous or of more widespread importance than those involving water and carbon, and for a molecular level understanding of such interfaces water monomer adsorption on graphene is a fundamental and representative system. This system is particularly interesting as it calls for an accurate treatment of electron correlation effects, as well as posing a practical challenge to experiments. Here, we employ many-body electronic structure methodologies that can be rigorously converged and thus provide faithful references for the molecule-surface interaction. In particular, we use diffusion Monte-Carlo (DMC), coupled cluster (CCSD(T)), as well as the random phase approximation (RPA) to calculate the strength of the interaction between water and an extended graphene surface. We establish excellent, sub-chemical, agreement between the complementary high-level methodologies, and an adsorption energy estimate in the most stable configuration of approximately -100\,meV is obtained. We also find that the adsorption energy is rather insensitive to the orientation of the water molecule on the surface, despite different binding motifs involving qualitatively different interfacial charge reorganisation. In producing the first demonstrably accurate adsorption energies for water on graphene this work also resolves discrepancies amongst previously reported values for this widely studied system. It also paves the way for more accurate and reliable studies of liquid water at carbon interfaces with cheaper computational methods, such as density functional theory and classical potentials.

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• Interaction between water and carbon nanostructures: How good are current density functional approximations?
• Nanoconfinement Facilitates Reactions of Carbon Dioxide in Supercritical Water
• A new scheme for fixed node diffusion quantum Monte Carlo with pseudopotentials: improving reproducibility and reducing the trial-wave-function bias
• Osmotic transport at the aqueous graphene and hBN interfaces: scaling laws from a unified, first principles description
• A QM/MD coupling method to model the ion-induced polarization of graphene
• Hydration of NH${}_4^{+}$ in Water: Bifurcated Hydrogen Bonding Structures and Fast Rotational Dynamics
• Surface science using coupled cluster theory via local Wannier functions and in-RPA-embedding: the case of water on graphitic carbon nitride
• Periodic Local Coupled-Cluster Theory for Insulators and Metals
• Efficient and accurate description of adsorption in zeolites
• A comparative study using state-of-the-art electronic structure theories on solid hydrogen phases under high pressures
• Machine learning density functionals from the random-phase approximation
• Diffusion Monte Carlo Study on Relative Stabilities of Boron Nitride Polymorphs
• Dynamical correlation energy of metals in large basis sets from downfolding and composite approaches
• Random Phase Approximation Applied to Many-Body Noncovalent Systems
• Error Cancellation in Diffusion Monte Carlo Calculations of Surface Chemistry
• How do interfaces alter the dynamics of supercooled water?
• Computational investigations of dispersion interactions between small molecules and graphene-like flakes
• Systematic discrepancies between reference methods for non-covalent interactions within the S66 dataset
• Interaction of water with nitrogen-doped graphene
• Coupled interactions at the ionic graphene/water interface
• New insights into the 1D carbon chain through the RPA
• Approaching the basis-set limit of the dRPA correlation energy with explicitly correlated and Projector Augmented-wave methods
• Raman and IR spectra of water under graphene nanoconfinement at ambient and extreme pressure-temperature conditions: a first-principles study
• Unveiling the hidden reaction kinetic network of carbon dioxide in supercritical aqueous solutions
• Understanding the wetting of transition metal dichalcogenides from an ab initio perspective
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• The binding of atomic hydrogen on graphene from density functional theory and diffusion Monte Carlo calculations
• Single-Molecule Water Motion on h-BN and Graphene: A Paradigm Shift in Understanding the Behaviour of Water on 2D Material Interfaces