1. Neutral Cyclometalated Ir(III) Complexes with Pyridylpyrrole Ligand for Photocatalytic Hydrogen Generation from Water
- Author
-
Piao He, Xiu-Fang Mo, Xiao-Yi Yi, Chao Liu, Hai-Xia Tong, Zhi-Liang Gan, and Yi Zhou
- Subjects
Quenching (fluorescence) ,010405 organic chemistry ,Ligand ,Ionic bonding ,chemistry.chemical_element ,010402 general chemistry ,Electrochemistry ,01 natural sciences ,0104 chemical sciences ,Catalysis ,Inorganic Chemistry ,chemistry.chemical_compound ,chemistry ,Triethanolamine ,Polymer chemistry ,Pyridine ,medicine ,Iridium ,Physical and Theoretical Chemistry ,medicine.drug - Abstract
To explore structure-activity relationships with respect to light-harvesting behavior, a family of neutral iridium complexes [Ir(ppy)2(LR)] 1-4 (where ppy = 2-phenylpyridine, and NN = 2-(1H-pyrrol-2-yl)pyridine and its functionalized derivatives) were designed and synthesized. The structural modifications in metal complexes are accomplished through the attributions of electron-donating CH3 in 2, OCH3 in 3, and electron-withdrawing CF3 in 4. The structural analysis displays that the pyridylpyrrole acts as one-negative charged bidentated ligand to chelate the iridium center. The electrochemical and photophysical properties of these complexes were systematically studied. The neutral 1-4 as well as the ionic structurally analogous [Ir(ppy)2(bpy)](PF6) (5) were utilized as PSs in photocatalytic hydrogen generation from water with [Co(bpy)3](PF6)2 as catalyst and triethanolamine (TEOA) as electron sacrificial agent in the presence of salt LiCl. Complex 1 maintains activity for more than 144 h under irradiation, and the total turnover number is up to 1768. The electrochemical properties and the quenching reaction indicate the H2 generation by neutral complexes 1-4 is involved exclusively in the oxidative quenching process.
- Published
- 2021