Wang Ping, Guo Song, Wang Hong-Juan, Chen Kai-Kai, Zhang Nan, Zhang Zhi-Ming, Lu Tong-Bu
International Joint Research Laboratory of Materials Microstructure, Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science & Engineering, Tianjin University of Technology, 300384, Tianjin, China.
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, 510275, Guangzhou, China.
Nat Commun. 2019 Jul 17;10(1):3155. doi: 10.1038/s41467-019-11099-8.
Developing broadband and strong visible-light-absorbing photosensitizer is highly desired for dramatically improving the utilization of solar energy and boosting artificial photosynthesis. Herein, we develop a facile strategy to co-sensitize Ir-complex with Coumarins and boron dipyrromethene to explore photosensitizer with a broadband covering ca. 50% visible light region (Ir-4). This type of photosensitizer is firstly introduced into water splitting system, exhibiting significantly enhanced performance with over 21 times higher than that of typical Ir(ppy)(bpy), and the turnover number towards Ir-4 reaches to 115840, representing the most active sensitizer among reported molecular photocatalytic systems. Experimental and theoretical investigations reveal that the Ir-mediation not only achieves a long-lived boron dipyrromethene-localized triplet state, but also makes an efficient excitation energy transfer from Coumarin to boron dipyrromethene to trigger the electron transfer. These findings provide an insight for developing broadband and strong visible-light-absorbing multicomponent arrays on molecular level for efficient artificial photosynthesis.
开发宽带且强可见光吸收的光敏剂对于大幅提高太阳能利用效率和促进人工光合作用非常必要。在此，我们开发了一种简便策略，将铱配合物与香豆素和硼二吡咯亚甲基共敏化，以探索覆盖约50%可见光区域的宽带光敏剂（Ir-4）。这种类型的光敏剂首次被引入到水分解系统中，表现出显著增强的性能，比典型的Ir(ppy)(bpy)高出21倍以上，并且Ir-4的周转数达到115840，是已报道的分子光催化系统中活性最高的敏化剂。实验和理论研究表明，铱介导不仅实现了长寿命的硼二吡咯亚甲基局域三重态，还实现了从香豆素到硼二吡咯亚甲基的高效激发能量转移以触发电子转移。这些发现为在分子水平上开发用于高效人工光合作用的宽带且强可见光吸收的多组分阵列提供了见解。
