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Microscopic insights into poly- and mono-crystalline methane hydrate dissociation in Na-montmorillonite pores at static and dynamic fluid conditions

Fang, B. (author), Lü, Tao (author), Li, Wei (author), Moultos, O. (author), Vlugt, T.J.H. (author), Ning, Fulong (author)

Knowledge on the kinetics of gas hydrate dissociation in clay pores at static and dynamic fluid conditions is a fundamental scientific issue for improving gas production efficiency from hydrate deposits using thermal stimulation and depressurization respectively. Here, molecular dynamics simulations were used to investigate poly- and mono...

journal article 2024

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The impact of metal centers in the M-MOF-74 series on carbon dioxide and hydrogen separation

Wasik, Dominika O. (author), Vicent-Luna, José Manuel (author), Luna-Triguero, Azahara (author), Dubbeldam, David (author), Vlugt, T.J.H. (author), Calero, Sofía (author)

The series of metal–organic frameworks M-MOF-74 gained popularity in the field of capture and separation of CO₂ due to the presence of numerous, highly reactive open-metal sites. The description of effective interactions between guest molecules and open-metal sites without accounting for polarization effects is challenging but it...

journal article 2024

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Application of thermodynamics at different scales to describe the behaviour of fast reacting binary mixtures in vapour-liquid equilibrium

Lasala, Silvia (author), Samukov, Konstantin (author), Polat, H.M. (author), Lachet, Véronique (author), Herbinet, Olivier (author), Privat, Romain (author), Jaubert, Jean Noël (author), Moultos, O. (author), De Ras, Kevin (author), Vlugt, T.J.H. (author)

The use of reactive working fluids in thermodynamic cycles is currently being considered as an alternative to inert working fluids, because of the preliminarily attested higher energy-efficiency potential. The current needs to simulate their use in thermodynamic cycles, which may operate in liquid, vapour or vapour-liquid state, are an...

journal article 2024

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Scaling towards the critical point in the combined reaction/Gibbs ensemble

Polat, H.M. (author), Lasala, Silvia (author), De Meyer, Frédérick (author), Houriez, Céline (author), Moultos, O. (author), Vlugt, T.J.H. (author)

We explore the impact of force field parameters and reaction equilibrium on the scaling behavior towards the critical point in reactive binary systems, focusing on NO ₂/N ₂O ₄. This system can be considered as a special single-component system since NO ₂ and N ₂O ₄ are in...

journal article 2024

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Computing solubility and thermodynamic properties of H₂O₂ in water

Saji, Tijin H.G. (author), Vicent-Luna, José Manuel (author), Vlugt, T.J.H. (author), Calero, Sofía (author), Bagheri, Behnaz (author)

Hydrogen peroxide plays a key role in many environmental and industrial chemical processes. We performed classical Molecular Dynamics and Continuous Fractional Component Monte Carlo simulations to calculate thermodynamic properties of H₂O₂ in aqueous solutions. The quality of the available force fields for H₂O...

journal article 2024

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Enhancement of formic acid production from carbon dioxide hydrogenation using metal-organic frameworks: Monte Carlo simulation study

Wasik, Dominika O. (author), Martín-Calvo, Ana (author), Gutiérrez-Sevillano, Juan José (author), Dubbeldam, David (author), Vlugt, T.J.H. (author), Calero, Sofía (author)

Formic acid production from CO₂ allows the reduction of carbon dioxide emissions while synthesizing a product with a wide range of applications. CO₂ hydrogenation is challenging due to the cost of transition metal catalysts and the toxicity of the transition elements. In this work, the thermodynamic confinement effects...

journal article 2023

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Transport properties of mixtures of acid gases with aqueous monoethanolamine solutions: A molecular dynamics study

Polat, H.M. (author), de Meyer, Frédérick (author), Houriez, Céline (author), Coquelet, Christophe (author), Moultos, O. (author), Vlugt, T.J.H. (author)

We investigated the effect of temperature and monoethanolamine (MEA) concentration on the self-diffusivity of acid gases, CO₂, and H₂S in aqueous MEA solutions. For this purpose, we computed densities of pure MEA and 30 wt% MEA/water solutions while scaling the LJ energy (ϵ) parameter and point charges of MEA. Results...

journal article 2023

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Kinetics of zeolite-catalyzed heptane hydroisomerization and hydrocracking with CBMC-modeled adsorption terms: Zeolite Beta as a large pore base case

Agarwal, Umang (author), Rigutto, Marcello S. (author), Zuidema, Erik (author), Jansen, A. P.J. (author), Poursaeidesfahani, A. (author), Sharma, S. (author), Dubbeldam, David (author), Vlugt, T.J.H. (author)

A reactor model that deconvolutes thermodynamics of adsorption of hydrocarbon in the pores of zeolite Beta, obtained by Configurational-bias Monte Carlo simulations, from intrinsic, intraporous kinetics of hydroisomerization and hydrocracking reactions, provides a good quantitative description of all significant reactions in the kinetic...

journal article 2022

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Diffusivity of α-, β-, γ-cyclodextrin and the inclusion complex of β-cyclodextrin: Ibuprofen in aqueous solutions; A molecular dynamics simulation study

Erdös, M. (author), Frangou, Michalis (author), Vlugt, T.J.H. (author), Moultos, O. (author)

Cyclodextrins (CDs) are widely used in drug delivery, catalysis, food and separation processes. In this work, a comprehensive simulation study on the diffusion of the native α-, β- and γ-CDs in aqueous solutions is carried out using Molecular Dynamics simulations. The effect of the system size on the computed self-diffusivity is investigated...

journal article 2021

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Thermal conductivity of aqueous solutions of reline, ethaline, and glyceline deep eutectic solvents; a molecular dynamics simulation study

Celebi, A.T. (author), Vlugt, T.J.H. (author), Moultos, O. (author)

Accurate knowledge and control of thermal conductivities is central for the efficient design of heat storage and transfer devices working with deep eutectic solvents (DESs). The addition of water is a straightforward and cost-efficient way of tuning many properties of DESs. In this work, the thermal conductivities of aqueous solutions of...

journal article 2021

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In Silico Screening of Zeolites for High-Pressure Hydrogen Drying

Erdös, M. (author), Geerdink, Daan F. (author), Martin-Calvo, Ana (author), Pidko, E.A. (author), van den Broeke, L.J.P. (author), Calero, Sofia (author), Vlugt, T.J.H. (author), Moultos, O. (author)

According to the ISO 14687-2:2019 standard, the water content of H2 fuel for transportation and stationary applications should not exceed 5 ppm (molar). To achieve this water content, zeolites can be used as a selective adsorbent for water. In this work, a computational screening study is carried out for the first time to identify potential...

journal article 2021

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The adsorption mechanisms of organic micropollutants on high-silica zeolites causing S-shaped adsorption isotherms: An experimental and Monte Carlo simulation study

Jiang, N. (author), Erdös, M. (author), Moultos, O. (author), Shang, R. (author), Vlugt, T.J.H. (author), Heijman, Sebastiaan (author), Rietveld, L.C. (author)

The adsorption of organic micropollutants (OMPs) on high-silica zeolites is characterized by adsorption isotherms with various shapes. The occurrence of an S-shaped adsorption isotherm indicates the lack of adsorption affinity for OMPs at low, environmentally relevant equilibrium concentrations. In this study, S-shaped isotherms were observed...

journal article 2020

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Gibbs Ensemble Monte Carlo Simulation of Fluids in Confinement: Relation between the Differential and Integral Pressures

Erdös, M. (author), Galteland, O. (author), Bedeaux, Dick (author), Kjelstrup, Signe (author), Moultos, O. (author), Vlugt, T.J.H. (author)

The accurate description of the behavior of fluids in nanoporous materials is of great importance for numerous industrial applications. Recently, a new approach was reported to calculate the pressure of nanoconfined fluids. In this approach, two different pressures are defined to take into account the smallness of the system: the so-called...

journal article 2020

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Mechanical Response of Nanocrystalline Ice-Contained Methane Hydrates: Key Role of Water Ice

Cao, Pinqiang (author), Ning, Fulong (author), Wu, Jianyang (author), Cao, Boxiao (author), Li, Tianshu (author), Sveinsson, Henrik Andersen (author), Liu, Z. (author), Vlugt, T.J.H. (author), Hyodo, Masayuki (author)

Water ice and gas hydrates can coexist in the permafrost and polar regions on Earth and in the universe. However, the role of ice in the mechanical response of ice-contained methane hydrates is still unclear. Here, we conduct direct million-atom molecular simulations of ice-contained polycrystalline methane hydrates and identify a crossover...

journal article 2020

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Brick-CFCMC: Open Source Software for Monte Carlo Simulations of Phase and Reaction Equilibria Using the Continuous Fractional Component Method

Hens, R. (author), Rahbari, A. (author), Caro Ortiz, S.A. (author), Dawass, N. (author), Erdös, M. (author), Poursaeidesfahani, A. (author), Seyed Salehi, H. (author), Celebi, A.T. (author), Ramdin, M. (author), Moultos, O. (author), Dubbeldam, D. (author), Vlugt, T.J.H. (author)

We present a new molecular simulation code, Brick-CFCMC, for performing Monte Carlo simulations using state-of-the-art simulation techniques. The Continuous Fractional Component (CFC) method is implemented for simulations in the NVT/NPT ensembles, the Gibbs Ensemble, the Grand-Canonical Ensemble, and the Reaction Ensemble. Molecule transfers...

journal article 2020

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Multiple linear regression and thermodynamic fluctuations are equivalent for computing thermodynamic derivatives from molecular simulation

Rahbari, A. (author), Josephson, Tyler R. (author), Sun, Yangzesheng (author), Moultos, O. (author), Dubbeldam, D. (author), Siepmann, J. Ilja (author), Vlugt, T.J.H. (author)

Partial molar properties are of fundamental importance for understanding properties of non-ideal mixtures. Josephson and co-workers (Mol. Phys. 2019, 117, 3589–3602) used least squares multiple linear regression to obtain partial molar properties in open constant-pressure ensembles. Assuming composition-independent partial molar properties...

journal article 2020

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Kirkwood-Buff integrals from molecular simulation

Dawass, N. (author), Krüger, Peter (author), Schnell, Sondre K. (author), Simon, Jean Marc (author), Vlugt, T.J.H. (author)

The Kirkwood-Buff (KB) theory provides a rigorous framework to predict thermodynamic properties of isotropic liquids from the microscopic structure. Several thermodynamic quantities relate to KB integrals, such as partial molar volumes. KB integrals are expressed as integrals of RDFs over volume but can also be obtained from density...

journal article 2019

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Molecular simulation of the vapor-liquid equilibria of xylene mixtures: Force field performance, and Wolf vs. Ewald for electrostatic interactions

Caro Ortiz, S.A. (author), Hens, R. (author), Zuidema, Erik (author), Rigutto, Marcello (author), Dubbeldam, David (author), Vlugt, T.J.H. (author)

This article explores how well vapor-liquid equilibria of pure components and binary mixtures of xylenes can be predicted using different force fields in molecular simulations. The accuracy of the Wolf method and the Ewald summation is evaluated. Monte Carlo simulations in the Gibbs ensemble are performed at conditions comparable to...

journal article 2019

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Modeling the electrochemical conversion of carbon dioxide to formic acid or formate at elevated pressures

Morrison, A.R.T. (author), van Beusekom, Vincent (author), Ramdin, M. (author), van den Broeke, L.J.P. (author), Vlugt, T.J.H. (author), de Jong, W. (author)

In this work a model of an elevated pressure CO₂ electrolyzer producing primarily formate or formic acid is presented. It consists of three parts: A model of the bulk electrolyte, the diffusion layer, and the electrode surface. Data from the literature was used to validate both the bulk portion of the model, as well as the overall...

journal article 2019

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Computing solubility parameters of deep eutectic solvents from Molecular Dynamics simulations

Seyed Salehi, H. (author), Ramdin, M. (author), Moultos, O. (author), Vlugt, T.J.H. (author)

The solubility parameter (SP) of a solvent is a key property that measures the polarity and quantifies the ‘like-dissolves-like’ principle, which is an important rule in chemistry for screening solvents for separation processes. It is challenging to experimentally obtain solubility parameters of non-volatile solvents like ionic liquids (ILs),...

journal article 2019