Institute of Inorganic Chemistry I, Ulm University, Albert-Einstein-Allee 11, 89081, Ulm, Germany.
Institute of Physical Chemistry, Friedrich Schiller University Jena, Helmholtzweg 4, 07743, Jena, Germany.
Chemistry. 2022 Nov 2;28(61):e202201931. doi: 10.1002/chem.202201931. Epub 2022 Sep 2.
The ambitious goal of artificial photosynthesis is to develop active systems that mimic nature and use light to split water into hydrogen and oxygen. Intramolecular design concepts are particularly promising. Herein, we firstly present an intramolecular photocatalyst integrating a perylene-based light-harvesting moiety and a catalytic rhodium center (Rh phenPer). The excited-state dynamics were investigated by means of steady-state and time-resolved absorption and emission spectroscopy. The studies reveal that photoexcitation of Rh phenPer yields the formation of a charge-separated intermediate, namely Rh phenPer⋅ , that results in a catalytically active species in the presence of protons.
人工光合作用的宏伟目标是开发模仿自然并利用光将水分解为氢气和氧气的活性系统。分子内设计概念尤其有前途。在此,我们首次提出了一种将基于苝的光捕获部分和催化铑中心(Rh phenPer)集成在一起的分子内光催化剂。通过稳态和时间分辨吸收和发射光谱研究了激发态动力学。研究表明,Rh phenPer 的光激发产生了电荷分离中间物 Rh phenPer⋅ ,在存在质子的情况下生成催化活性物质。