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首页> 外文期刊>Chemistry: A European journal >Functionalization of diameter-sorted semiconductive SWCNTs with photosensitizing porphyrins: Syntheses and photoinduced electron transfer
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Functionalization of diameter-sorted semiconductive SWCNTs with photosensitizing porphyrins: Syntheses and photoinduced electron transfer

机译：具有光敏性卟啉的直径排序半导体SWCNT的功能化：合成和光致电子转移

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摘要

Covalent functionalization of diameter sorted SWCNTs with porphyrins (MP), and photochemistry to establish nanotube diameter-dependent charge separation efficiencies are reported. The MP-SWCNT(n,m) [M=2 H or Zn, and (n,m)=(7,6) or (6,5)] nanohybrids are characterized by a variety of spectroscopic, thermogravimetric, TEM imaging techniques, and also by DFT MO calculations. The thermogravimetric, Raman and fluorescence studies reveal the presence of a moderate number of porphyrins on the SWCNT surface. The MO results suggest charge separation (CS) via the excited state of MP. Time-resolved fluorescence studies reveal quenching of the singlet excited state of the MP with SWCNT(n,m), giving the rate constants of charge separation (k_(CS)) in the range of (4-5)×10~9 s~(-1). Nanosecond transient absorption measurements confirm the charge-separated radical cation and the radical anion as [MP.~+-SWCNT.~-] with their characteristic absorption bands in the visible and near-IR regions. The charge separated states persist for about 70-100 ns thus giving an opportunity to utilize them to build photoelectrochemical cells, which allowed us to derive the structure-reactivity relationship between the nature of porphyrin and diameter of the employed nanotubes. Size matters! Diameter-dependent efficiencies of photoinduced electron transfer leading to charge stabilization, and photoelectrochemical response of solar cells is demonstrated in porphyrin covalently linked to (7,6)- and (6,5)-enriched single-wall carbon nanotube (SWCNT) donor-acceptor nanohybrids (see figure; MP=metalloporphyrin).
机译：报道了直径排序的SWCNT与卟啉（MP）的共价官能化以及建立纳米管直径依赖性电荷分离效率的光化学方法。 MP-SWCNT（n，m）[M = 2 H或Zn，并且（n，m）=（7,6）或（6,5）]纳米杂化物的特征在于多种光谱，热重，TEM成像技术，也可以通过DFT MO计算。热重，拉曼和荧光研究表明，SWCNT表面存在适量的卟啉。 MO结果表明通过MP的激发态进行电荷分离（CS）。时间分辨荧光研究表明，用SWCNT（n，m）淬灭了MP的单重激发态，使电荷分离的速率常数（k_（CS））在（4-5）×10〜9 s范围内〜（-1）。纳秒瞬态吸收测量结果证实了电荷分离的自由基阳离子和自由基阴离子为[MP。+-SWCNT.-]，它们在可见光和近红外区域具有特征吸收带。电荷分离状态持续约70-100 ns，从而提供了利用它们构建光电化学电池的机会，这使我们能够得出卟啉性质与所用纳米管直径之间的结构反应关系。大小事项！卟啉与富集（7,6）和（6,5）的单壁碳纳米管（SWCNT）供体-共价连接的卟啉证明了光诱导电子转移的直径依赖性效率导致电荷稳定，以及太阳能电池的光电化学反应。受体纳米杂化物（见图; MP =金属卟啉）。

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