Abstract
AbstractReduction of the {Co(NO)}8 cobalt–nitrosyl N‐confused porphyrin (NCP) [Co(CTPPMe)(NO)] (1) produced electron‐rich {Co(NO)}9 [Co(CTPPMe)(NO)][Co(Cp*)2] (2), which was necessary for NO‐to‐N2O conversion. Complex 2 was NO‐reduction‐silent in neat THF, but was partially activated to a hydrogen‐bonded species 2⋅⋅⋅MeOH in THF/MeOH (1:1, v/v). This species coupling with 2 transformed NO into N2O, which was fragmented from an [N2O2]‐bridging intermediate. An intense IR peak at 1622 cm−1 was ascribed to ν(NO) in an [N2O2]‐containing intermediate. Time–course ESI(−) mass spectra supported the presence of the dimeric [Co(NCP)]2(N2O2) intermediate. Five complete NO‐to‐N2O conversion cycles were possible without significant decay in the amount of N2O produced.
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