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Creators/Authors contains: "Spasyuk, Denis M."

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  1. ; ; ; ; ; (, Chemical Communications)
    A rare redox-active Mn(0) dicarbene anion with solvent-dependent electrochemical behaviour has been synthesized and thoroughly characterized. 
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  2. ; ; ; (, Journal of the American Chemical Society)
    The scission of a C(sp3)−H bond to form a new metal−alkyl bond is a fundamental step in coordination chemistry and catalysis. However, the extent of C−H bond weakening when this moiety interacts with a transition metal is poorly understood and quantifying this phenomenon could provide insights into designing more efficient C−H functionalization catalysts. We present a nickel complex with a robust adamantyl reporter ligand that enables the measurement of C−H acidity (pKa) and bond dissociation free energy (BDFE) for a C(sp3)−H agostic interaction, showing a decrease in pKa by dozens of orders of magnitude and BDFE decrease of about 30 kcal/mol upon coordination. X-ray crystallographic data is provided for all molecules, including a distorted square planar NiIII metalloradical and “doubly agostic” NiII(κ2-CH2) complex. 
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