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N–H Bond Activation of Ammonia Using Intramolecular cAAC-Borane Lewis Pairs

https://doi.org/10.1021/acs.inorgchem.5c02533

Song, Hayoung; Szymczak, Nathaniel K (August 2025, Inorganic Chemistry)

Free, publicly-accessible full text available August 25, 2026
Tuning Secondary-Sphere Lewis Acidity via Late-Stage Modification of an Appended Borane

https://doi.org/10.1021/acs.inorgchem.4c03056

Atkins, Alice L; Zeller, Matthias; Szymczak, Nathaniel K (December 2024, Inorganic Chemistry)

To develop synthetic strategies to construct ligands containing secondary sphere acids, we demonstrate that an appended borane of low Lewis acidity (–BPin) can be upgraded to a strong Lewis acid (–BF2). Using a pyridine-pyrazole ligand coordinated to Mo(CO)4, we show that a pendent –BPin group undergoes exhaustive fluorination to –BF3K, a precursor to a highly acidic –BF2 unit (acceptor number ~15x greater than –BPin).
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Free, publicly-accessible full text available December 2, 2025
Additive Effects in Metal/Lewis Acid Cooperativity Assessed in a Tetrahedral Copper Hydrazine Complex Featuring an Appended Borane

https://doi.org/10.1021/acs.inorgchem.4c02865

Norwine, Emily E; Kiernicki, John J; Zeller, Matthias; Szymczak, Nathaniel K (October 2024, Inorganic Chemistry)

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Lewis Acid‐Tethered (cAAC)–Copper Complexes: Reactivity for Hydride Transfer and Catalytic CO2 Hydrogenation

https://doi.org/10.1002/anie.202411099

Song, Hayoung; Szymczak, Nathaniel Kolnik (July 2024, Angewandte Chemie International Edition)

We present a series of borane‐tethered cyclic (alkyl)(amino)carbene (cAAC)‐copper complexes, including a borane‐capped Cu(I) hydride. This hydride is unusually hydridic and reacts rapidly with both CO2 and 2,6‐dimethylphenol at room temperature. Its reactivity is distinct from variants without a tethered borane, and the underlying principles governing the enhanced hydricity were evaluated experimentally and theoretically. These stoichiometric results were extended to catalytic CO2 hydrogenation, and the borane‐tethered (intramolecular) system exhibits ~3‐fold enhancement relative to an intermolecular system.
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