Kinetic model of the electrochemical oxidation of graphitic carbon in acidic environments
Literature Information
Kevin G. Gallagher
The electrochemical oxidation of graphitic carbon results in the performance decay of electrochemical systems such as aqueous, acidic fuel cells, redox-flow batteries, and supercapacitors. An electrochemical mechanism and numerical model is proposed to explain long-standing questions. The model predicts carbon weight loss and surface oxide growth as a function of time, temperature, and potential. Experimentally observed phenomena are discussed and analyzed using the numerical model. Three mechanisms are concluded to contribute to the current decay commonly observed during electrochemical oxidation: mass loss, reversible passive oxide formation, and irreversible oxide formation. Although reversible passive oxide formation governs the current decay under potentiostatic oxidation, a reduction in the equilibrium catalytic oxide is the most significant decay mechanism under potential cycling. Finally, the model is used to determine the change in active site concentration resulting from high-temperature heat treatment of carbon black.
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Physical Chemistry Chemical Physics

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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