含鈷四苯基四苯卟啉的光譜鑑定及光氧化反應之探討

李柏逸

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含鈷四苯基四苯卟啉的光譜鑑定及光氧化反應之探討

Spectroscopic Properties and Photooxidation of Co(II)TPTBP (Tetraphenyltetrabenzoporphyrin)

李柏逸 , Masters　　Advisor：陳炳宇　　

繁體中文

鈷；卟啉光氧化； Cobalt ； porphyrin ； photooxidation

Abstract │ Reference (85) │ Times Cited (1) │ Altmetrics

Abstract 〈TOP〉

Parallel Abstract 〈TOP〉

A suspected photo-driven oxidation of hydroxyl anion (OH-), sourcing from N(Bu)4OH, into oxygen catalyzed by CoII(TPTBP) have been reported by means of X-ray crystallography, UV-vis, paramagnetic NMR and EPR spectroscopies.
In this study we have revealed that the catalytic oxidation of OH- is accompanied by the persistent converting of CoII(TPTBP) into one-electron oxidation product [CoII(TPTBP)]+ evidenced by the transforms of 1H NMR and UV-vis time course experiments. On the basis of the X-ray data of five-coordinate CoIII(Bu)(TPTBP) at the terminated catalysis, the cation N(Bu)4+ should accept an electron and simultaneously releases a Bu. radical when CoII(TPTBP) is presumably oxidized cobalt center, dimerization of two CoIII(OH)(TPTBP) and formation of cobalt(III) μ-1,2-peroxo dimers are proposed to be the active intermediates in the pathway of  evolving oxygen via 4-electron oxidation.
Although, the detailed mechanistic aspects remained more discusses, the light-triggered one-electron oxidation of CoII(TPTBP) was supported by continuous illumination adopting the light of 470 nm in the solution of acetone, showing evident converting toward one-electron oxidation product. In contrast, with rest in the dark the oxidized complex will almost return to the CoII(TPTBP). According to the crystal obtained by illuminated condition, a five-coordinate CoIII(CH2-C(O)-CH3)(TPTBP) structure revealed that the acetone is underwent one electron reduction to the enolate, coordinating on the cobalt center.

Reference ( 85 ) 〈TOP〉

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Times Cited (1) 〈TOP〉

吳函儒(2017)。含鈷四苯基四苯卟啉的光譜鑑定。中興大學化學系所學位論文。2017。1-146。

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