Electrochemically induced oxygen spillover and diffusion on Pt(111): PEEM imaging and kinetic modelling

Literature Information

Publication Date 2011-06-20
DOI 10.1039/C1CP20361D
Impact Factor 3.676
Authors

Eva Mutoro, Christian Hellwig, Bjoern Luerssen, Sebastian Guenther, Jürgen Janek


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Abstract

Electrochemically induced oxygen spillover and diffusion in the Pt(O2)|YSZ system is investigated in a combined experimental and theoretical study. The spreading of spillover oxygen is imaged by photoelectron emission microscopy (PEEM) on dense and epitaxial Pt(111) thin film electrodes prepared by pulsed laser deposition (PLD). Two different models are used to obtain surface diffusion coefficients from the experimental data, (i) an analytical solution of Fick's 2nd law of diffusion, and (ii) a numerical reaction-diffusion model that includes recombinative desorption of O2 into the gas phase. The resulting diffusion coefficient has an activation energy of 50 kJ mol−1 and a preexponential factor of 0.129 cm2 s−1 with an estimated uncertainty of ±20% for the activation energy and ±50% for the absolute value. The Fickian model slightly overpredicts diffusion coefficients due to the neglect of oxygen desorption. Experimental and theoretical results and limitations are discussed and compared to previous work.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
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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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