Photoredox catalysis's relevance in organic synthesis research and innovation will increase in the coming decades. However, the processes rely almost exclusively on expensive noble metal complexes, most notably iridium complexes, to absorb light and transfer a single charge to a substrate or a catalyst to initiate cascade transformations. Light-triggered plasmon resonances generate a non-Fermi-Dirac energy distribution with many hot carriers that decay in ∼1 ps. Their ultrafast relaxation makes performing single electron transfer (SET) transformations challenging. Herein, a novel photosystem is proposed based on surface-modified gold nanoparticles (aka plasmon "molecularization"), which improved charge separation and, more importantly, enabled SET reactions, expanding the portfolio of photocatalysts available for photoredox catalysis. The photosystem was made into an electrode, permitting its use in photoelectrochemical arrangements that leverage electro- and photo-chemical approaches' benefits and chemical engineering solutions, helping the synthetic chemistry efforts towards greener synthesis and synthesis of more complex structures on a scale.

未来几十年，光氧化还原催化在有机合成研究和创新中的相关性将会增加。然而，这些过程几乎完全依赖昂贵的贵金属配合物，尤其是铱配合物，来吸收光并将单个电荷转移到基材或催化剂上以引发级联转化。光触发的等离子体共振产生非费米-狄拉克能量分布，其中许多热载流子在〜1 ps内衰变。它们的超快弛豫使得执行单电子转移 (SET) 转换具有挑战性。在此，提出了一种基于表面改性金纳米粒子（又名等离子体“分子化”）的新型光系统，它改善了电荷分离，更重要的是，实现了SET反应，扩大了可用于光氧化还原催化的光催化剂组合。该光系统被制成电极，允许其在光电化学装置中使用，利用电化学和光化学方法的优点和化学工程解决方案，帮助合成化学努力实现更绿色的合成和大规模合成更复杂的结构。