Klingler Sarah, Bagemihl Benedikt, Mengele Alexander K, Kaufhold Simon, Myllyperkiö Pasi, Ahokas Jussi, Pettersson Mika, Rau Sven, Mizaikoff Boris
Institute of Analytical and Bioanalytical Chemistry, Ulm University, Albert-Einstein-Allee 11, 89081, Ulm, Germany.
Institute of Inorganic Chemistry I, Ulm University, Albert-Einstein-Allee 11, 89081, Ulm, Germany.
Angew Chem Int Ed Engl. 2023 Oct 26;62(44):e202306287. doi: 10.1002/anie.202306287. Epub 2023 Aug 17.
Currently, most photosensitizers and catalysts used in the field of artificial photosynthesis are still based on rare earth metals and should thus be utilized as efficiently and economically as possible. While repair of an inactivated catalyst is a potential mitigation strategy, this remains a challenge. State-of-the-art methods are crucial for characterizing reaction products during photocatalysis and repair, and are currently based on invasive analysis techniques limiting real-time access to the involved mechanisms. Herein, we use an innovative in situ technique for detecting both initially evolved hydrogen and after active repair via advanced non-invasive rotational Raman spectroscopy. This facilitates unprecedently accurate monitoring of gaseous reaction products and insight into the mechanism of active repair during light-driven catalysis enabling the identification of relevant mechanistic details along with innovative repair strategies.
目前，人工光合作用领域中使用的大多数光敏剂和催化剂仍基于稀土金属，因此应尽可能高效且经济地加以利用。虽然修复失活的催化剂是一种潜在的缓解策略，但这仍然是一个挑战。先进的方法对于光催化和修复过程中反应产物的表征至关重要，而目前这些方法基于侵入性分析技术，限制了对相关机制的实时了解。在此，我们使用一种创新的原位技术，通过先进的非侵入性旋转拉曼光谱法检测最初产生的氢气以及活性修复后的氢气。这有助于以前所未有的精度监测气态反应产物，并深入了解光驱动催化过程中的活性修复机制，从而能够识别相关的机理细节以及创新的修复策略。
