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Study on the Synthesis and the Stability of Manganese-Oxo Corrole

Author: LiuJingJing
Tutor: LiuHaiYang
School: South China University of Technology
Course: Inorganic Chemistry
Keywords: Corrole Manganese Oxo Stability Axial ligand
CLC: O627.7
Type: Master's thesis
Year: 2011
Downloads: 46
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Abstract


Corrole is an 18-πelectron macrocycle having a direct pyrrole-pyrrole linkage. Its ring structure is in close resemblance to porphyrin. Reactive Mn oxo species have been implicated as intermediates in the oxidation of water to oxygen in Photosystem II as well as in certain catalases and oxygen atom transfer （OAT） reactions. MnV oxo complexes are an important mechanistic probe for OAT reactions in the catalytic oxidation of alkenes. Controlling the reactivity of Mn oxo complexes are not completely understood, and the current literature on Mn oxo chemistry is not without controversy. Some meaningful conclusions have been drawn according to experimental results and theoretical analysis, which are as follows: Free base of corrole, 5,10,15-tris（pentafluorophenyl）corrole, and its manganese complexes had been also successfully synthesized. They were well chracterized by MS, UV-Vis and NMR spectra.5,10,15-tris（pentafluorophenyl） Corrole （tpfc） manganese（V）-Oxo had been synthesized in different solvents including octanol, tetrahydrofuran, dimethyl sulfoxide , water, toluene, N’N-dimethyl formamide, ethyl acetate, ethanol, acetone. The stability of 5,10,15-tris（pentafluorophenyl） Corrole （tpfc） manganese（V）-Oxo in different solvents and in the presence of axial ligand were investigated. The results showed ethanol, octanol, ethyl ether, tetrahydrofuran, dimethyl sulfoxide and toluene could accelerate the decay of （tpfc）MnV≡O using dichloromethane as reference, and N’N-dimethyl formamide, water, ethyl acetate, acetone would slow down the decay of （tpfc）MnV≡O.The reaction of （tpfc）MnV≡O and hydrochloric acid and acetic acid yielded （tpfc）MnIVCl, （tpfc）MnIVAc respectively. The axial coordination of MnIII-tpfc by imidazole, 4-methylimidazole, pyridine gave 1:1 complexes. The association constants followed an order of imidazole >4-methylimidazole > pyridine. In the presence of these axial ligands, the stability of （tpfc）MnV≡O decreases significantly. The MnIII/MnIV half-wave potential of MnIII-tpfc moved negatively upon combination with axial ligand. XPS results showed that the binding energy of center manganese Mn2p3/2 decreased after axial coordination, and the extent of reduction depends on the electron-donor capacity of axial ligand.

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CLC: > Mathematical sciences and chemical > Chemistry > Organic Chemistry > Elements in organic compounds > The Ⅶ group elements, organic compounds ( except halogens )
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