O2 Activation by a Heterobimetallic Zr/Co Complex

Zhang, Hongtu; Hatzis, Gregory P.; Moore, Curtis E.; Dickie, Diane A.; Bezpalko, Mark W.; Foxman, Bruce M.; Thomas, Christine M.

doi:10.1021/jacs.9b04215

Title: O₂ Activation by a Heterobimetallic Zr/Co Complex

Journal Article · Mon Jun 03 00:00:00 EDT 2019 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.9b04215· OSTI ID:1524776

^[1]; Hatzis, Gregory P. ^[1];

^[1];

^[2]; Bezpalko, Mark W. ^[2];

^[2];

^[1]

The Ohio State Univ., Columbus, OH (United States). Dept. of Chemistry and Biochemistry
Brandeis Univ., Waltham, MA (United States). Dept. of Chemistry

Oxygen reduction is a critical half reaction in renewable fuel cell development and a key step in the development of aerobic oxidation reactions. We report rapid two-electron O₂ reduction by a d⁰ Zr^IV center with an appended redox-active Co^–I site serving as an electron reservoir. The early/late heterobimetallic Zr/Co complex (THF)Zr(MesNPⁱPr₂)₃CoCN^tBu (1) reacts readily with O₂ and O atom transfer reagents to generate reactive oxygenated species including terminal peroxo and oxo complexes, (O₂)Zr(MesNPⁱPr₂)₃CoCN^tBu (2) and O≡Zr(MesNPⁱPr₂)₃CoCN^tBu (3). The bimetallic Zr/Co complex provides a new cooperative synthetic pathway to promote multielectron redox processes such as oxygen reduction, with each metal playing a distinct role as a substrate binding site or redox mediator.

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Research Organization:: The Ohio State Univ., Columbus, OH (United States)

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

Grant/Contract Number:: SC0019179

OSTI ID:: 1524776

Journal Information:: Journal of the American Chemical Society, Vol. 141, Issue 24; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 32 works

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CCDC 1922509: Experimental Crystal Structure Determination Hongtu, Zhang,; P., Hatzis, Gregory; E., Moore, Curtis https://doi.org/10.5517/ccdc.csd.cc22jjfl The current record is supplemented by this dataset	dataset	January 2019
CCDC 1922510: Experimental Crystal Structure Determination Hongtu, Zhang,; P., Hatzis, Gregory; E., Moore, Curtis https://doi.org/10.5517/ccdc.csd.cc22jjgm The current record is supplemented by this dataset	dataset	January 2019
CCDC 1922511: Experimental Crystal Structure Determination Hongtu, Zhang,; P., Hatzis, Gregory; E., Moore, Curtis https://doi.org/10.5517/ccdc.csd.cc22jjhn The current record is supplemented by this dataset	dataset	January 2019
CCDC 1922512: Experimental Crystal Structure Determination Hongtu, Zhang,; P., Hatzis, Gregory; E., Moore, Curtis https://doi.org/10.5517/ccdc.csd.cc22jjjp The current record is supplemented by this dataset	dataset	January 2019
CCDC 1922513: Experimental Crystal Structure Determination Hongtu, Zhang,; P., Hatzis, Gregory; E., Moore, Curtis https://doi.org/10.5517/ccdc.csd.cc22jjkq The current record is supplemented by this dataset	dataset	January 2019
CCDC 1922514: Experimental Crystal Structure Determination Hongtu, Zhang,; P., Hatzis, Gregory; E., Moore, Curtis https://doi.org/10.5517/ccdc.csd.cc22jjlr The current record is supplemented by this dataset	dataset	January 2019
CCDC 1922508: Experimental Crystal Structure Determination Hongtu, Zhang,; P., Hatzis, Gregory; E., Moore, Curtis https://doi.org/10.5517/ccdc.csd.cc22jjdk The current record is supplemented by this dataset	dataset	January 2019

Title: O2 Activation by a Heterobimetallic Zr/Co Complex

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