Size-dependent electronic structure controls activity for ethanol electro-oxidation at Ptn/indium tin oxide (n = 1 to 14)

Literature Information

Publication Date 2015-05-19
DOI 10.1039/C5CP01824B
Impact Factor 3.676
Authors

Alexander von Weber, Eric T. Baxter, Sebastian Proch, Matthew D. Kane, Michael Rosenfelder, Henry S. White, Scott L. Anderson


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Abstract

Understanding the factors that control electrochemical catalysis is essential to improving performance. We report a study of electrocatalytic ethanol oxidation – a process important for direct ethanol fuel cells – over size-selected Pt centers ranging from single atoms to Pt14. Model electrodes were prepared by soft-landing of mass-selected Ptn+ on indium tin oxide (ITO) supports in ultrahigh vacuum, and transferred to an in situ electrochemical cell without exposure to air. Each electrode had identical Pt coverage, and differed only in the size of Pt clusters deposited. The small Ptn have activities that vary strongly, and non-monotonically with deposited size. Activity per gram Pt ranges up to ten times higher than that of 5 to 10 nm Pt particles dispersed on ITO. Activity is anti-correlated with the Pt 4d core orbital binding energy, indicating that electron rich clusters are essential for high activity.

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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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