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Creators/Authors contains: "Novas, Bryan T"

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  1. ; ; (, European Journal of Inorganic Chemistry)
    Abstract Hydrophosphination activity has been solicited from the parent and decamethyl zirconocene dichloride compounds, Cp2ZrCl2and Cp*2ZrCl2. Given recent reports of photocatalytic hydrophosphination, these compounds were irradiated in the near ultraviolet (UV) as precatalysts resulting in the successful hydrophosphination of styrene substrates and activated alkenes. Irradiation appears to induce homolysis of the Cp or Cp* ligand, resulting in radical hydrophosphination. Successful detection of this radical reactivity was achieved by monitoring for EPR signals within situirradiation, a methodology proving to be general for the determination of radical versus closed‐shell reactivity in transition‐metal photocatalysis. 
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  2. ; (, ChemCatChem)
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  3. ; ; ; (, Photochem)
    A comparative study of amino phenoxide zirconium catalysts in the hydrophosphination of alkenes with diphenylphosphine reveals enhanced activity upon irradiation during catalysis, with conversions up to 10-fold greater than reactions in ambient light. The origin of improved reactivity is hypothesized to result from substrate insertion upon an n→d charge transfer of a Zr–P bond in the excited state of putative phosphido (Zr–PR2) intermediates. TD-DFT analysis reveals the lowest lying excited state in the proposed active catalysts are dominated by a P 3p→Zr 4d MLCT, presumably leading to enhanced catalysis. This hypothesis follows from triamidoamine-supported zirconium catalysts but demonstrates the generality of photocatalytic hydrophosphination with d0 metals. 
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