Energetic Effects of a Closed System Approach Including Explicit Proton and Electron Acceptors as Demonstrated by a Mononuclear Ruthenium Water Oxidation Catalyst.

ABSTRACT: When considering water oxidation catalysis theoretically, accounting for the transfer of protons and electrons from one catalytic intermediate to the next remains challenging: correction factors are usually employed to approximate the energetics of electron and proton transfer. Here these energetics were investigated using a closed system approach, which places the catalytic intermediate in a simulation box including proton and electron acceptors, as well as explicit solvent. As a proof of principle, the first two catalytic steps of the mononuclear ruthenium-based water oxidation catalyst [Ru(cy)(bpy)(H₂O)]²⁺ were examined using Car-Parrinello Molecular Dynamics. This investigation shows that this approach offers added insight, not only into the free energy profile be

SUBMITTER: de Ruiter JM 

PROVIDER: S-EPMC6221022 | biostudies-literature | 2018 Oct

REPOSITORIES: biostudies-literature