Cooperative H2 Activation across a Metal–Metal Multiple Bond and Hydrogenation Reactions Catalyzed by a Zr/Co Heterobimetallic Complex

Gramigna, Kathryn M.; Dickie, Diane A.; Foxman, Bruce M.; Thomas, Christine M.

doi:10.1021/acscatal.8b04390

Title: Cooperative H₂ Activation across a Metal–Metal Multiple Bond and Hydrogenation Reactions Catalyzed by a Zr/Co Heterobimetallic Complex

Journal Article · Fri Mar 01 00:00:00 EST 2019 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.8b04390· OSTI ID:1524777

Gramigna, Kathryn M. ^[1];

^[1];

^[2]

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

In the quest for active and selective catalysts featuring nonprecious metals, bimetallic cooperativity poses a unique opportunity to promote catalytic reactions and influence selectivity. While examples of stoichiometric H2 activation across metal–metal bonds have been reported, there have been limited advances toward the incorporation of a well-defined cooperative bimetallic H2 activation process into a catalytic cycle for the hydrogenation of unsaturated hydrocarbons. Herein, we demonstrate that facile activation of H2 by two nonprecious metals is facilitated by metal–metal cooperativity in the coordinatively unsaturated Zr/Co bis(phosphinoamide) complexes (THF)(I)Zr(XylNPiPr2)2CoPR3 (3-PMe3 and 3-PMePh2, Xyl =3,5-dimethylphenyl), which feature highly polar Zr–Co triple bonds. Owing to the stabilizing nature of the metal–metal bond, the H2 activation products (THF)(I)Zr(μ-H)(XylNPiPr2)2Co(H)(PR3) (4-PMe3 and 4-PMePh2), which feature one terminally bound Co hydride and one hydride bridging the two metals, have been isolated and crystallographically characterized. The Zr/Co bimetallic complex 3-PMePh2 is an active catalyst for the hydrogenation of alkenes and semihydrogenation of alkynes, and relevant intermediates including 4-PMePh2 and alkene (5) and alkyne (6) adducts have been identified spectroscopically in situ and isolated and characterized through independent synthesis. The alkyne semihydrogenation reaction catalyzed by 3-PMePh2 exhibits high selectivity for alkene over alkane products and generates an unselective distribution of (E)- and (Z)-alkenes via direct formation of both stereoisomers. These findings lend insight into the roles that metal–metal bonding and cooperativity play in the activation of small molecules and the promotion and selectivity of subsequent catalytic transformations.

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Research Organization:: Brandeis Univ., Waltham, MA (United States)

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

Contributing Organization:: Ohio State University

Grant/Contract Number:: SC0014151

OSTI ID:: 1524777

Alternate ID(s):: OSTI ID: 1575199

Journal Information:: ACS Catalysis, Vol. 9, Issue 4; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 56 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
heterobimetallic
dihydrogen activation
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CCDC 1917805: Experimental Crystal Structure Determination M., Gramigna, Kathryn; A., Dickie, Diane; M., Foxman, Bruce https://doi.org/10.5517/ccdc.csd.cc22cmps The current record is supplemented by this dataset	dataset	January 2019
CCDC 1917806: Experimental Crystal Structure Determination M., Gramigna, Kathryn; A., Dickie, Diane; M., Foxman, Bruce https://doi.org/10.5517/ccdc.csd.cc22cmqt The current record is supplemented by this dataset	dataset	January 2019
CCDC 1917803: Experimental Crystal Structure Determination M., Gramigna, Kathryn; A., Dickie, Diane; M., Foxman, Bruce https://doi.org/10.5517/ccdc.csd.cc22cmmq The current record is supplemented by this dataset	dataset	January 2019
CCDC 1917804: Experimental Crystal Structure Determination M., Gramigna, Kathryn; A., Dickie, Diane; M., Foxman, Bruce https://doi.org/10.5517/ccdc.csd.cc22cmnr The current record is supplemented by this dataset	dataset	January 2019
CCDC 1917807: Experimental Crystal Structure Determination M., Gramigna, Kathryn; A., Dickie, Diane; M., Foxman, Bruce https://doi.org/10.5517/ccdc.csd.cc22cmrv The current record is supplemented by this dataset	dataset	January 2019
CCDC 1917808: Experimental Crystal Structure Determination M., Gramigna, Kathryn; A., Dickie, Diane; M., Foxman, Bruce https://doi.org/10.5517/ccdc.csd.cc22cmsw The current record is supplemented by this dataset	dataset	January 2019

Title: Cooperative H2 Activation across a Metal–Metal Multiple Bond and Hydrogenation Reactions Catalyzed by a Zr/Co Heterobimetallic Complex

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