Generalized Energy-Conserving Dissipative Particle Dynamics with Reactions br

We present an extension of the generalized energy-conservingdissipative particle dynamics method (J. Bonet Avalos, et al.,Phys Chem ChemPhys,2019,21, 24891-24911) to include chemical reactivity, denotedGenDPDE-RX. GenDPDE-RX provides a means of simulating chemical reactivityat the micro- and mesoscales, while exploiting the attributes of density- andtemperature-dependent many-body forcefields, which include improved trans-ferability and scalability compared to two-body pairwise models. The GenDPDE-RX formulation considers intra-particle reactivity via a coarse-grain reactorconstruct. Extent-of-reaction variables assigned to each coarse-grain particlemonitor the temporal evolution of the prescribed reaction mechanisms and kineticsassumed to occur within the particle. Descriptions of the algorithm, equations ofmotion, and numerical discretization are presented, followed by verification of theGenDPDE-RX method through comparison with reaction kinetics theoreticalmodel predictions. Demonstrations of the GenDPDE-RX method are performedusing constant-volume adiabatic heating simulations of three different reaction models, including both reversible and irreversiblereactions, as well as multistep reaction mechanisms. The selection of the demonstrations is intended to illustrate theflexibility andgenerality of the method but is inspired by real material systems that span fromfluids to solids. Many-body forcefields usinganalytical forms of the ideal gas, Lennard-Jones, and exponential-6 equations of state are used for demonstration, althoughapplication to other forms of equation of states is possible. Finally, theflexibility of the GenDPDE-RX framework is addressed with abrief discussion of other possible adaptations and extensions of the method