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The mechanism of OsH6(PiPr3)2‐mediated fragmentation of a 4‐(2 pyridyl)‐2‐azetidinone has been investigated by DFT calculations. The addition of the C4H bond of the substrate to OsH2(PiPr3)2 allows the active participation of an osmium lone pair in the B‐type β‐lactam fragmentation process. This new mechanism makes the N1C4/C2C3 fragmentation of the lactamic core thermally accessible through a...
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