Non-noble Metal Single-Molecule Photocatalysts for the Overall Photosynthesis of Hydrogen Peroxide

• Published in: Journal of the American Chemical Society 2024-12
• Main Authors: Fu, Fan, Liu, Yongxin, Liu, Mingliang, Li, Zhengguang, Zhong, Wanying, Li, Yaqin, Li, Kaixiu, Wang, Jun, Huang, Yongchao, Li, Yiming, Liu, Wei, Zhang, Yi, Xiang, Kaisong, Liu, Hui, Wang, Pingshan, Liu, Die
• Format: Article
• Language: English
• ISSN: 1520-5126; 1520-5126
• DOI: 10.1021/jacs.4c09445

Despite the great progress in molecule photocatalytic solar energy conversion, it is particularly challenging to realize a photocatalytic overall reaction in a non-noble metal complex, which represents a new paradigm for photosynthesis. In this study, a class of novel non-noble metal complexes with head-to-tail geometry were designed and readily synthesized via the coordination of triphenylamine-modified 2,2': 6',2″-terpyridine ligands with Zn . As expected, these complexes exhibited the desired through-space charge-transfer transition, generating both long-lived excited states (on the order of microseconds) and separate redox centers under visible-light irradiation. These complexes have particularly low exciton binding energies, which make them excellent heterogeneous single molecular photocatalysts for the overall photosynthetic production of H O . Remarkably, a high H O evolution rate (8862 μmol g h ) was achieved in pure H O under an air atmosphere via precise molecular tailoring, revealing the unparalleled advantages of molecular photocatalysts in improving the catalytic rate of H O production. This is the first time that single-molecule photocatalysts have been used to efficiently complete the photosynthesis of H O . This study presents a new paradigm for photocatalytic energy conversion and provides unique insights into the design of molecular photocatalysts.