Graphite-Conjugated Pyrazines as Molecularly Tunable Heterogeneous Electrocatalysts
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Author(s) • • •
Fukushima, Tomohiro
Drisdell, Walter
Yano, Junko
Surendranath, Yogesh
Date Issued
August 2015
Journal
Journal of the American Chemical Society
Publisher
American Chemical Society (ACS)
Citation
Fukushima, Tomohiro, Walter Drisdell, Junko Yano, and Yogesh Surendranath. “Graphite-Conjugated Pyrazines as Molecularly Tunable Heterogeneous Electrocatalysts.” Journal of the American Chemical Society 137, no. 34 (September 2, 2015): 10926–10929.
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Author's final manuscript
Abstract
Condensation of ortho-phenylenediamine derivatives with ortho-quinone moieties at edge planes of graphitic carbon generates graphite-conjugated pyrazines (GCPs) that are active for oxygen reduction electrocatalysis in alkaline aqueous electrolyte. Catalytic rates of oxygen reduction are positively correlated with the electrophilicity of the active site pyrazine unit and can be tuned by over 70-fold by appending electron-withdrawing substituents to the phenylenediamine precursors. Discrete molecular analogs containing pyrazine moieties display no activity above background under identical conditions. This simple bottom up method for constructing molecularly well-defined active sites on ubiquitous graphitic solids enables the rational design of tunable heterogeneous catalysts.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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DOI of Published Version
https://doi.org/10.1021/jacs.5b06737