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The homoleptic organocerium complex Ce{C(SiHMe2)3}3 (1) reacts with B(C6F5)3 to produce the zwitterionic bis(alkyl) hydridoborato Ce{C(SiHMe2)3}2HB(C6F5)3 (2). NMR and IR spectroscopy and X‐ray crystallography indicate that each alkyl ligand contains two bridging Ce↼H‐Si interactions in both 1 and 2. Compound 2 serves as a precatalyst for the hydrosilylation of acrylates to give α‐silyl esters at...
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