Evidence of Spin-Forbidden Excitation of [Ru(bpy)3]2+ and Application in Red-Light-Driven Photocatalysis

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-07-30 DOI:10.1021/acscatal.5c04437

Géraud Chacktas, Björn Pfund, Taline Kerackian, Polina Yaltseva, Maud Villeneuve, Didier Durand, Nicolas Fabre, Céline Fiorini-Debuisschert, Jean-Christophe Cintrat, Oliver S. Wenger* and Eugénie Romero*,

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Abstract

Red-light-driven catalysis presents a promising alternative to conventional blue light photocatalysis, offering enhanced light penetration, functional group tolerance, and energy efficiency. However, its widespread application remains underdeveloped, partly due to the lack of readily accessible photocatalysts capable of efficiently absorbing low-energy red photons. A promising, yet underexplored, strategy involves direct spin-forbidden singlet-to-triplet excitation. In this study, we demonstrate the experimental evidence that [Ru(bpy)₃]²⁺ can engage in photocatalysis through direct singlet-to-triplet excitation under red light irradiation. This finding, supported by optical and spectroscopic investigations, broadens the reactivity of [Ru(bpy)₃]²⁺ and offers broadly applicable design principles for robust Ru(II) photocatalysts suited for red-light-driven reactions.

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[Ru(bpy)3]2+自旋禁止激发的证据及其在红光驱动光催化中的应用

红光驱动的催化是传统蓝光光催化的一个很有前途的替代方案，具有增强的光穿透性、官能团耐受性和能源效率。然而，它的广泛应用仍然不发达，部分原因是缺乏易于获得的能够有效吸收低能红色光子的光催化剂。一个有希望的，但尚未开发的策略是直接自旋禁止的单重态到三重态激发。在本研究中，我们证明了在红光照射下[Ru(bpy)3]2+可以通过直接单重态到三重态激发进行光催化的实验证据。这一发现得到了光学和光谱研究的支持，拓宽了[Ru(bpy)3]2+的反应性，并为适合红光驱动反应的鲁棒Ru（II）光催化剂提供了广泛适用的设计原则。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.