Author, as appears in the article.: Lísal M; Larentzos JP; Avalos JB; Mackie AD; Brennan JK
Department: Enginyeria Química
URV's Author/s: Bonet Avalos, José / Mackie Walker, Allan Donald
Keywords: Equation-of-state simulations shock model mixtures high-temperature fluid conservation
Abstract: We present an extension of the generalized energy-conserving dissipative particle dynamics method (J. Bonet Avalos, et al., Phys Chem Chem Phys, 2019, 21, 24891-24911) to include chemical reactivity, denoted GenDPDE-RX. GenDPDE-RX provides a means of simulating chemical reactivity at the micro- and mesoscales, while exploiting the attributes of density- and temperature-dependent many-body force fields, which include improved transferability and scalability compared to two-body pairwise models. The GenDPDE-RX formulation considers intra-particle reactivity via a coarse-grain reactor construct. Extent-of-reaction variables assigned to each coarse-grain particle monitor the temporal evolution of the prescribed reaction mechanisms and kinetics assumed to occur within the particle. Descriptions of the algorithm, equations of motion, and numerical discretization are presented, followed by verification of the GenDPDE-RX method through comparison with reaction kinetics theoretical model predictions. Demonstrations of the GenDPDE-RX method are performed using constant-volume adiabatic heating simulations of three different reaction models, including both reversible and irreversible reactions, as well as multistep reaction mechanisms. The selection of the demonstrations is intended to illustrate the flexibility and generality of the method but is inspired by real material systems that span from fluids to solids. Many-body force fields using analytical forms of the ideal gas, Lennard-Jones, and exponential-6 equations of state are used for demonstration, although application to other forms of equation of states is possible. Finally, the flexibility of the GenDPDE-RX framework is addressed with a brief discussion of other possible adaptations and extensions of the method.
Thematic Areas: Química Physics, atomic, molecular & chemical Physical and theoretical chemistry Medicina i Materiais Matemática / probabilidade e estatística Interdisciplinar Farmacia Engenharias iii Computer science applications Ciências biológicas ii Ciências biológicas i Ciência da computação Chemistry, physical Chemistry, multidisciplinary Biotecnología Astronomia / física
licence for use: https://creativecommons.org/licenses/by/3.0/es/
Author's mail: josep.bonet@urv.cat allan.mackie@urv.cat
Author identifier: 0000-0002-7339-9564 0000-0002-1819-7820
Record's date: 2023-02-23
Papper version: info:eu-repo/semantics/acceptedVersion
Link to the original source: https://pubs.acs.org/doi/10.1021/acs.jctc.1c01294
Licence document URL: http://repositori.urv.cat/ca/proteccio-de-dades/
Papper original source: Journal Of Chemical Theory And Computation. 18 (4): 2503-2512
APA: Lísal M; Larentzos JP; Avalos JB; Mackie AD; Brennan JK (2022). Generalized Energy-Conserving Dissipative Particle Dynamics with Reactions. Journal Of Chemical Theory And Computation, 18(4), 2503-2512. DOI: 10.1021/acs.jctc.1c01294
Article's DOI: 10.1021/acs.jctc.1c01294
Entity: Universitat Rovira i Virgili
Journal publication year: 2022
Publication Type: Journal Publications
Repositori URV