Introducing a closed system approach for the investigation of chemical steps involving proton and electron transfer; as illustrated by a copper-based water oxidation catalyst

Literature Information

Publication Date 2016-12-21
DOI 10.1039/C6CP07454E
Impact Factor 3.676
Authors

Jessica M. de Ruiter, Francesco Buda


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Abstract

The investigation of the catalytic mechanism of homogeneous water oxidation catalysts remains an active field of research. When examining catalytic steps theoretically, it is often difficult to account for the transfer of protons and electrons from step to step. To this end, a closed system approach is proposed which includes both proton and electron acceptors in the simulation box to allow for the description of proton-coupled electron transfer processes. Using Car–Parrinello Molecular Dynamics, a mononuclear copper water oxidation catalyst Cu(bpy)(OH)2 was used as a model system to explore this closed system approach. The exploration of this model system shows that, compared to traditional methods, this approach offers extra insight into proposed catalytic steps and allows for the clear identification of preferred reaction paths.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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