| Summary: | 碩士 === 國立中興大學 === 化學系所 === 105 === This study demonstrated that the methane/ethane oxidation is able to be facilely mediated by the reaction of [CuICuICuI(7-Dipy)](ClO4)2 with hydrogen peroxide or oxygen. By means of combining ESI-MS (Electrospray Ionization Mass Spectrometry) with RFQ (Rapid Freeze Quench), we first successfully detected the highly acitve species [CuIICuII(μ-O)2CuII]4+ or [CuIICuIII(μ-O)2CuIII]4+, which are proposed to closely correlate with the active intermediate [CuIICuII(μ-O)2CuIII]3+ in pMMO hydroxylation. Moreover, for precisely quantifying the employed H2O2 in the catalytic reaction carried out by tricopper cluster, hydrogen peroxide (H2O2) concentration has been first determined by using absorption spectral titration of the CH2Cl2 solution containing Co(II)(OETTP) and imidazole with the ratio (1:2). In such reaction, H2O2 acts as one-electron oxidant. When Co(II)(OETTP) underwent one-electron oxidation, imidazole will rapidly coordinate to the Co(III) ion to give rise to clear changes of the absorption.
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