Complex Reaction Network Thermodynamic and Kinetic Autoconstruction Based on Ab Initio Statistical Mechanics: A Case Study of O2 Activation on Ag4 Clusters

An approach based on ab initio statistical mechanics is demonstrated for autoconstructing complex reaction networks. Ab initio molecular dynamics combined with Markov state models are employed to study relevant transitions and corresponding thermodynamic and kinetic properties of a reaction. To explore the capability and flexibility of this approach, we present a study of oxygen activation on Ag-4 as a model reaction. Specifically, with the same sampled trajectories, it is possible to study the structural effects and the reaction rate of the cited reaction. The results show that this approach is suitable for automatized construction of reaction networks, especially for non-well-studied reactions, which can benefit from this ab initio molecular dynamics based approach to construct comprehensive reaction networks with Markov state model without prior knowledge about the potential energy landscape.

Automated summary

An approach based on ab initio statistical mechanics is demonstrated for autoconstructing complex reaction networks, with oxygen activation on Ag-4 as a model reaction. It has been shown that this method is suitable for automatized construction of reaction networks and can be used for studying structural effects and reaction rates, especially for non-well-studied reactions.