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Small modifications on the co‐ligands of complexes containing two coordinated hydrogen atoms can determine the elongated dihydrogen versus compressed dihydride nature of these species and therefore their chemical behavior. 2,6‐diphenylpyridine favors the formation of the osmium(IV) cation [OsH2(C6H4pyPh)(PiPr3)2]+, whereas 2‐phenoxy‐6‐phenylpyridine, which contains an oxygen atom between the heterocycle...
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