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首页> 外文期刊>Chemistry: A European journal >Supramolecular triad and pentad composed of zinc-porphyrin(s), oxoporphyrinogen, and fullerene(s): Design and ellectron-transfer studies
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Supramolecular triad and pentad composed of zinc-porphyrin(s), oxoporphyrinogen, and fullerene(s): Design and ellectron-transfer studies

机译：由锌卟啉，氧气卟啉代和富勒烯和富勒烯组成的超分子三合会和五边形：设计和埃尔考科转移研究

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摘要

By adopting a "covalent-coordinate" bonding approach, novel supramolecular pentad and triad molecules composed of zinc-porphyrin(s), fullerene(s), and oxoporphyrinogen redox-/photoactive entities have been constructed, and also characterized by means of spectral and electrochemical techniques. The geometry and electronic structures of the pentad and the triad were deduced by means of DFT calculations. Free-energy calculations suggested that the photoinduced electron/energy transfer from the zinc-porphyrin (ZnP) singlet-excited state to the imidazole modified fullerene (IMC60) acceptor and oxoporphyrinogen (00) entities is feasible for both the triad and the pentad. The charge-separation rates (k(CS)) determined from picosecond time-resolved emission studies were higher for pentad (C(60)Im:ZnP)(2)-OxP than for the corresponding triad, C(60)Im:ZnP-OxP. A comparison of the k(CS) values previously reported for the covalently linked bis(zinc-porphyrin)-oxoporphyrinogen triad suggests that employing a fullerene acceptor improves the electron-transfer rates. Nanosecond transient absorption studies provide evidence for the occurrence of electron-transfer processes. Lifetimes of the radical ion pairs (tau(RIP)) are in the range of hundreds of nanoseconds, which indicates that there is charge stabilization in the supramolecular systems.
机译：通过采用“共价坐标”粘合方法，已经构建了由锌 - 卟啉，富勒序和氧气卟啉氧化钠氧化氧/光学固体组成的新型超分子五分子和三合会分子，并且还通过光谱和电化学技术。通过DFT计算推断出五角体和三合会的几何形状和电子结构。自由能量计算表明，从吡啶卟啉（ZnP）单次激发态的光诱导的电子/能量转移到咪唑改性的富勒烯（IMC60）受体和氧气卟啉（00）实体对于TRIAD和PENTAD都是可行的。从PIC秒时间分辨排放研究中确定的电荷分离速率（K（CS））对于PENTAD（C（60）IM：ZnP）（2）-OxP而不是相应的三合会，C（60）IM：ZnP -oxp。先前报道了共价连接的双（锌 - 卟啉）-Oxoporphyrinogen三合会的K（CS）值的比较表明，使用富勒烯受体提高了电子传递率。纳秒瞬态吸收研究提供了电子转移过程的证据。自由基离子对（Tau（RIP））的寿命在数百纳秒的范围内，这表明在超分子系统中存在电荷稳定。

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