Combining scaling relationships overcomes rate versus overpotential trade-offs in O 2 molecular electrocatalysis

Martin, Daniel J.; Mercado, Brandon Q.; Mayer, James M.

doi:10.1126/sciadv.aaz3318

Title: Combining scaling relationships overcomes rate versus overpotential trade-offs in O ₂ molecular electrocatalysis

Journal Article · 13 March 2020 · Science Advances

DOI: https://doi.org/10.1126/sciadv.aaz3318 · OSTI ID:1626058

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Yale Univ., New Haven, CT (United States). Dept. of Chemistry

The development of advanced chemical-to-electrical energy conversions requires fast and efficient electrocatalysis of multielectron/multiproton reactions, such as the oxygen reduction reaction (ORR). Using molecular catalysts, correlations between the reaction rate and energy efficiency have recently been identified. Improved catalysis requires circumventing the rate versus overpotential trade-offs implied by such “scaling relationships.” Described here is an ORR system—using a soluble iron porphyrin and weak acids—with the best reported combination of rate and efficiency for a soluble ORR catalyst. This advance is achieved not by “breaking” scaling relationships but rather by combining two of them. Key to this behavior is a polycationic ligand, which enhances anionic ligand binding and changes the catalyst E_1/2. These results show how combining scaling relationships is a powerful way toward improved electrocatalysis.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Molecular Electrocatalysis (CME); Yale Univ., New Haven, CT (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-00ER41132

OSTI ID:: 1626058

Journal Information:: Science Advances, Vol. 6, Issue 11; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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