The reaction between TpOs (N) Cl2 (1)[Tp= hydrotris (1-pyrazolyl) borate] and aqueous (nBu4N)(OH) in THF-d8 forms the nitrosyl complex TpOs (NO) Cl2 (5) among other products, suggesting an initial hydroxide attack at the nitrido ligand. In contrast, the reaction of the acetate complex TpOs (N)(OAc) 2 (2) with NaOH in Me2CO/H2O yields the osmium bis- hydroxide complex TpOs (N)(OH) 2 (3), which has been structurally characterized by ...