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Easy‐to‐prepare η2‐coordinated phosphine‐borane ligands are demonstrated to liberate hydrogen upon treatment with different σ‐donor/π‐acceptor ligands (CO, tBuNC, CN−). Depending on the utilized ancillary ligand, different reaction pathways are observed, ranging from simple hydride protonation to iron–boron bond formation and subsequent rearrangement to pincer‐type ligands based on a tricoordinate...
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