Directed Electron Transfer

定向电子转移

• 批准号: EP/D032946/1
• 负责人: Anthony Harriman
• 金额: $ 41.78万
• 依托单位: Newcastle University
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2006
• 资助国家: 英国
• 起止时间: 2006 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FD032946%2F1
• 关键词: Directed; Electron; Transfer

Electron-transfer processes play key roles in chemical reactions, energy-storage systems and contemporary devices for information transfer. Such reactions are driven by thermodynamics and, given the choice between several partners, electron transfer will generate a thermodynamically stable distribution of products. Selectivity is acquired only by way of proximity and reduction potential. Here, we set out to devise rational ways to direct an electron along one particular pathway when several seemingly identical routes are available. In this case, selectivity is obtained by the choice of excitation wavelength. Low energy excitation of the main chromophore causes electron transfer to a proximal acceptor. Higher energy excitation into the same chromophore causes energy transfer to a secondary chromophore, which subsequently transfers an electron to a distal acceptor. The redox products differ in terms of spin and/or chemical identity. The ultimate achievement within this programme refers to directed electron transfer around a ring. Thus, low energy excitation causes clockwise electron flow but higher energy illumination causes electrons to move around the ring in an anti-clockwise direction.

电子转移过程在化学反应、能量储存系统和现代信息传递装置中起着关键作用。此类反应由热力学驱动，并且如果在几个伙伴之间进行选择，电子转移将产生热力学稳定的产物分布。选择性仅通过接近性和还原电位获得。在这里，我们开始设计合理的方法来引导电子沿着一个特定的路径，当几个看似相同的路线是可用的。在这种情况下，通过选择激发波长来获得选择性。主发色团的低能量激发导致电子转移到邻近受体。进入相同发色团的较高能量激发导致能量转移到次级发色团，其随后将电子转移到远端受体。氧化还原产物在自旋和/或化学特性方面不同。该计划的最终成就是围绕环的定向电子转移。因此，低能量激发导致顺时针电子流，但较高能量照射导致电子以逆时针方向围绕环移动。

项目成果

Selective triplet-state formation during charge recombination in a fullerene/Bodipy molecular dyad (Bodipy=borondipyrromethene).

• DOI: 10.1002/chem.200900440
• 发表时间: 2009-07
• 期刊: Chemistry
• 作者: R. Ziessel;Ben D. Allen;D. B. Rewinska;A. Harriman

Bidirectional electron transfer in molecular tetrads.

• DOI: 10.1021/ja908865k
• 发表时间: 2010-01
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: A. Benniston;A. Harriman;Peiyi Li

Redox-controlled fluorescence modulation in a BODIPY-quinone dyad

• DOI: 10.1002/ejoc.200800191
• 发表时间: 2008-06-01
• 期刊: EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
• 影响因子: 2.8
• 作者: Benniston, Andrew C.;Copley, Graeme;Clegg, William
• 通讯作者: Clegg, William

Boron dipyrrin dyes exhibiting "push-pull-pull" electronic signatures.

硼二吡啉染料表现出“推-拉-拉”电子特征。

• DOI: 10.1002/chem.200901725
• 发表时间: 2009
• 期刊: Chemistry (Weinheim an der Bergstrasse, Germany)
• 作者: Ziessel R

Thermoresponsive fluorescent polymers based on a quaterthiophene-containing boron dipyrromethene (Bodipy) dyad dispersed in silicone rubber

• DOI: 10.1039/c0jm03351k
• 发表时间: 2011-01-01
• 期刊: JOURNAL OF MATERIALS CHEMISTRY
• 作者: Benniston, Andrew C.;Copley, Graeme;Ryan, Ruth
• 通讯作者: Ryan, Ruth