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An arene interaction can mask a low‐valent and low‐coordinate VII complex, [(nacnac)V(Ntol2)] (see structure), which allows for facile coordination of terminal ligands on the vanadium center. Small‐molecule activation by this S=3/2 complex provides facile access to a wide range of ligand frameworks such as terminal VIV imido, VIV cyclopropene, VV nitride, and the first VVcyclo‐P3 complex (see scheme).
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