Photoinduced Electron Transfer in Donor-linked Fullerenes

供体连接的富勒烯中的光致电子转移

• 批准号: 13440190
• 负责人: IMAHORI Hiroshi
• 金额: $ 8.7万
• 依托单位: KYOTO UNIVERSITY (2002)Osaka University (2001)
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (B)
• 财政年份: 2001
• 资助国家: 日本
• 起止时间: 2001 至 2002
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-13440190/
• 关键词: Photosynthesis; Electron Transfer; Porphyrins; Fullerenes; Ferrocenes; Transient Absorption Spectroscopy; meso, meso-Linked Porphyrins; Donor-Acceptor Linked Systems; 時間分解過度吸収分光法; 電子スピン共鳴分光法; エネルギー移動

We have prepared ferrocene-porphyrin dimer-fullerene triad where meso, meso-linked porphyrindimer is incorporated successfully into a charge separation unit as photosynthetic multistep electron transfer model for the first time. The triad reveals photoinduced electron transfer from the porphyrin dimer excited singlet state to the C_<60>, followed by charge-shift from the ferrocene to the porphyrin dimer radical cation, to produce the ferricenium ion-C<60> radical ion pair with a high quantum yield (0.71-0.88) as well as a long-lived charge-separated lifetime (16-83 μs) depending on the solvent. It should be emphasized here that the charge-separated lifetime of the present triad has been prolonged by replacing porphyrin monomer with porphyrin dimer without reducing the quantum yield significantly. The charge-separated lifetime is governed by stepwise charge recombination rather than direct charge recombination.

我们制备了二茂铁-卟啉二聚体-富勒烯三联体，其中meso，meso连接的卟啉二聚体首次成功地被纳入一个电荷分离单元作为光合多步电子转移模型。该三联体揭示了光诱导电子从卟啉二聚体激发单重态转移到C_<60>，然后从二茂铁转移到卟啉二聚体自由基阳离子，产生<60>了高量子产率（0.71-0.88）和长寿命的电荷分离寿命（16-83 μs）的铁离子-C自由基离子对，取决于溶剂。这里应该强调的是，通过用卟啉二聚体代替卟啉单体，本三联体的电荷分离寿命已经延长，而不显著降低量子产率。电荷分离寿命是由逐步电荷复合，而不是直接电荷复合。

项目成果

Hiroshi Imahori et al.: "Concentration Effects of Porphyrin Monolayers on the Structure and Photoelectrochemical Properties of Mixed Self-Assembled Monolayers of Porphyrin and Alkanethiol on Gold Electrodes"Langmuir. 17・16. 2099-2108 (2001)

Hiroshi Imahori 等人：“卟啉单分子层对金电极上卟啉和烷硫醇混合自组装单分子层的结构和光电化学性能的影响”Langmuir 17・16。

今堀 博他: "分子太陽電池の展望"化学工業. 537-541 (2001)

Hiroshi Imahori 等人：“分子太阳能电池的前景”化学工业 537-541 (2001)。

Hiroshi Imahori, et al.: "Large Photocurrent Generation of Gold Eelectrodes Modified with [60]Fullerene-liked Oligothiophenes B earing a Tripodal Rigid Anchor"J. Am. Chem. Soc.. 124-4. 532-533 (2002)

Hiroshi Imahori 等人：“用带有三足刚性锚的[60]类富勒烯低聚噻吩修饰的金电极产生大光电流”J。

Hiroshi Imahori, et al.: "Stepwise Charge Separation and Charge Recombination in Ferrocene-meso,meso-Linked Porphyrin DimerFullerene Tetrad"J. Am. Chem. Soc. ,. 124-18. 5165-5174 (2002)

Hiroshi Imahori 等人：“二茂铁-内消旋、内消旋连接的卟啉二聚体富勒烯四分体中的逐步电荷分离和电荷重组”J。

今堀 博ほか: "ナノ連結系によるエネルギー・電子移動デバイス、化学フロンティア-分子ナノテクノロジー-(分担)"化学同人. 11 (2002)

Hiroshi Imahori 等人：“基于纳米耦合系统的能量/电子转移装置，化学前沿 - 分子纳米技术 -（分享）” Kagaku Doujin 11 (2002)。