Requirements for Lewis Acid-Mediated Capture and N-N Bond Cleavage of Hydrazine at Iron
Overview
Affiliations
An iron complex bearing a pyridine(dicarbene) pincer was designed to probe the requirements of Lewis acid-enabled NH capture and subsequent N-N bond cleavage. Appended boron Lewis acids were installed by two methods to circumvent the incompatibilities associated with Lewis acid/base quenching of free carbenes and boranes. NH capture by borane Lewis acids is dependent on both the Lewis acidity and the steric profile about boron. A substitutionally inert primary coordination sphere at iron prevents an Fe-NH interaction as well as N-N bond homolysis upon reduction.
Appended Lewis Acids Enable Dioxygen Reactivity and Catalytic Oxidations with Ni(II).
Beagan D, Rivera C, Szymczak N J Am Chem Soc. 2024; 146(18):12375-12385.
PMID: 38661576 PMC: 11148854. DOI: 10.1021/jacs.3c12399.
Beagan D, Kiernicki J, Zeller M, Szymczak N Angew Chem Int Ed Engl. 2023; 62(13):e202218907.
PMID: 36720708 PMC: 10023486. DOI: 10.1002/anie.202218907.
Wang B, Seo C, Zhang C, Chu J, Szymczak N J Am Chem Soc. 2022; 144(34):15793-15802.
PMID: 35973127 PMC: 10276360. DOI: 10.1021/jacs.2c06662.
Distinct Reactivity Modes of a Copper Hydride Enabled by an Intramolecular Lewis Acid.
Norwine E, Kiernicki J, Zeller M, Szymczak N J Am Chem Soc. 2022; 144(33):15038-15046.
PMID: 35960993 PMC: 10291504. DOI: 10.1021/jacs.2c02937.
Kiernicki J, Norwine E, Lovasz M, Zeller M, Szymczak N Chem Commun (Camb). 2020; 56(86):13105-13108.
PMID: 33016291 PMC: 7606458. DOI: 10.1039/d0cc05121g.