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视角:超快激光光谱如何为化学和材料合成中新型有机光氧化还原催化剂的设计提供信息?

Perspective: How can ultrafast laser spectroscopy inform the design of new organic photoredox catalysts for chemical and materials synthesis?

作者信息

Orr-Ewing Andrew J

机构信息

School of Chemistry, University of Bristol, Cantock's Close, Bristol BS8 1TS, United Kingdom.

出版信息

Struct Dyn. 2019 Jan 23;6(1):010901. doi: 10.1063/1.5082620. eCollection 2019 Jan.

Abstract

Photoredox catalysis of chemical reactions, using light-activated molecules which serve as electron donors or acceptors to initiate chemical transformations under mild conditions, is finding widespread use in the synthesis of organic compounds and materials. The transition-metal-centred complexes first developed for these photoredox-catalysed applications are steadily being superseded by more sustainable and lower toxicity organic photocatalysts. While the diversity of possible structures for photoredox-active organic molecules brings benefits of design flexibility, it also presents considerable challenges for optimization of the photocatalyst molecular architecture. Transient absorption spectroscopy over timescales from the femtosecond to microsecond domains can explore the detailed mechanisms of activation and reaction of these organic photocatalysts in solution and, by linking their dynamical properties to their structures, has the potential to establish reliable design principles for future development of improved photocatalysts.

摘要

利用光活化分子作为电子供体或受体在温和条件下引发化学转化的光氧化还原催化化学反应,在有机化合物和材料的合成中得到了广泛应用。最初为这些光氧化还原催化应用开发的以过渡金属为中心的配合物正逐渐被更具可持续性和低毒性的有机光催化剂所取代。虽然光氧化还原活性有机分子可能结构的多样性带来了设计灵活性的好处,但它也给光催化剂分子结构的优化带来了相当大的挑战。从飞秒到微秒时间尺度的瞬态吸收光谱可以探索这些有机光催化剂在溶液中的活化和反应的详细机制,并且通过将它们的动力学性质与其结构联系起来,有潜力为改进的光催化剂的未来发展建立可靠的设计原则。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/21ef/6404927/93c61616b28c/SDTYAE-000006-010901_1-g001.jpg

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