Project Details
Projekt
A multi-scale non-equilibrium molecular dynamics strategy to investigate electrochemical flow cells
Subject Area
Statistical Physics, Nonlinear Dynamics, Complex Systems, Soft and Fluid Matter, Biological Physics
Term
since 2023
Project identifier
Deutsche Forschungsgemeinschaft (DFG) - Project number 413163866
In this project, we propose tuning and validating the adaptive resolution (AdResS) method into an open-boundary non-equilibrium molecular dynamics tool to simulate electro-organic flow cells at an exceptional degree of complexity and detail. In the AdResS method, an atomistic representation of a physical system coexists with an ideal gas in terms of temperature and chemical potentials within one simulation box. Appropriate periodic boundaries enable us to investigate diverse non-equilibrium conditions impacting the atomistic region, trivially enforced on the ideal gas reservoirs. Our plan initially focuses on simulating a prototypical flow cell that includes graphite electrodes and acetonitrile-based electrolytes. This system, which has been thoroughly investigated in experiments, allows us to connect to the simulation results of the previous funding period. We consider the domino-oxidation-reduction sequence in this setting to synthesise nitriles from aldoximes. Classical empirical force fields (OPLS) prevent us from considering chemical reactions explicitly. However, we plan to investigate implicit effects by including oxime, nitrile oxide and nitrile at various concentrations and understand the role of diffusion of different species with respect to the electrodes. Our research plan will follow close interactions with the group of Prof. Kremer at the Max Planck Institute for Polymer Research, whose pioneering work forms the basis of this proposal. Moreover, we intend to interact with UNODE experimental partners, Prof. Waldvogel at the JGU to tailor the simulation setup and comprehensively understand chemical flow cells; Prof. Ferdi Schüth at the Max-Planck-Institut für Kohlenforschung to investigate at a later stage of the project novel reactions with the method we proposed; and theoretical partner, Prof. Kai S. Exner at the University Duisburg-Essen to rationalise results and share knowledge at the electrode interface. The main goal of this project is to establish a framework for simulating realistic electro-organic flow cells using a non-equilibrium multi-scale approach to identify the combined role of the anode, electrolyte, reactants and products on the structural, thermodynamic, electrical and dynamic properties of the system. We will focus on a graphite anode, and a prototypical electrolyte consisting on acetonitrile, water and methyl-tri-propylammonium methylsulfate. We will include explicitly elements of a domino-oxidation-reduction reaction for the synthesis of nitriles from aldoximes, namely oxime, nitrile oxide and nitrile.
DFG Programme
Research Units
Subproject of
FOR 2982:
UNODE - Unusual Anode Reactions
