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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Cobalt Porphyrin Catalyzed Reduction of CO↓(2). Radiation Chemical, Photochemical, and Electrochemical Studies
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Cobalt Porphyrin Catalyzed Reduction of CO↓(2). Radiation Chemical, Photochemical, and Electrochemical Studies

机译：钴卟啉催化还原CO↓（2）。辐射化学，光化学和电化学研究

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摘要

Several cobalt porphyrins (CoP) have been reduced by radiation chemical, photochemical, and electrochemical methods, in aqueous and organic solvents. In aqueous solutions, the Co↑(I)p state is stable at high pH but is shorter lived in neutral and acidic solutions. Stable Co↑(I)p is also observed in organic solvents and is unreactive toward CO↓(2). One-electron reduction of Co↑(I)p leads to formation of a species that is observed as a transient intermediate by pulse radiolysis in aqueous solutions and as a stable product following reduction by Na in tetrahydrofuran solutions. The spectrum of this species is not the characteristic spectrum of a metalloporphyrin π-radical anion and is ascribed to Co↑(0)P. This species binds and reduces CO↓(2). Catalytic formation of CO and HCO O↓(2)- is confirmed by photochemical experiments in acetonitrile solutions containing triethylamine an a reductive quencher. Catalytic reduction of CO↓(2) is also confirmed by cyclic voltammetry in acetonitrile and butyronitrile solutions and is shown to occur at the potential at which Co↑(I)p is reduced to Co↑(0)P. As compared with CoTPP, fluorinated derivatives are reduced, and catalyze C O↓(2) reduction, at less negative potentials.
机译：在水性和有机溶剂中，通过辐射化学，光化学和电化学方法已还原了几种钴卟啉（CoP）。在水溶液中，Co↑（I）p状态在高pH下稳定，但在中性和酸性溶液中的寿命较短。在有机溶剂中也观察到稳定的Co↑（I）p，对CO↓（2）无反应。 Co↑（I）p的单电子还原导致形成一种物质，该物质可通过在水溶液中进行脉冲辐解而作为瞬时中间体观察到，并在四氢呋喃溶液中被Na还原后作为稳定产物观察到。该物种的光谱不是金属卟啉π自由基阴离子的特征光谱，归因于Co↑（0）P。该物种结合并降低了CO↓（2）。通过光化学实验在含有三乙胺的乙腈溶液（还原性淬灭剂）中的光化学实验证实了CO和HCO O↓（2）-的催化形成。循环伏安法在乙腈和丁腈溶液中也证实了CO↓（2）的催化还原作用，并显示在Co↑（I）p还原为Co↑（0）P的电位下发生。与CoTPP相比，氟化衍生物被还原，并以较低的负电势催化C O↓（2）的还原。

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