Post-Assembly Reactivity of N-Aryl Iminoboronates: Reversible Radical Coupling and Unusual B-N Dynamic Covalent Chemistry

N-芳基亚氨基硼酸酯的组装后反应性:可逆自由基偶联和不寻常的BN动态共价化学

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Abstract

Post-assembly reaction of a dynamic covalent iminoboronate system following addition of Cp(2) Co resulted in the formation of a series of new reductively coupled dianionic dimers via C-C bond formation. The dimers formed as a mixture of BN-containing isomeric products: diastereomers rac(5) and meso(5,) with coupled five-membered rings, and enantiomeric rac(6,) with a fused six-membered ring bicyclic system from C-C bond formation and rearrangement of the B-N bonds. Each isomer was identified using (1) H NMR spectroscopy in combination with single crystal X-ray structure determination. Interestingly, interconversion between the coupled five-membered rings (rac(5) ) and fused bicyclic systems (rac(6) ) was found to occur through an unprecedented breaking and reforming of the B-N covalent bond. Further, the coupled products could be converted quantitatively back to their iminoboronate precursors with addition of the electron abstractor Ph(3) C(+) .

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