Photoinduced hydrogen evolution in supramolecular devices with a rhenium photosensitizer linked to FeFe-hydrogenase model complexes.
Coordination of the pyridyl-attached diiron azadithiolate hexacarbonyl complexes (2 and 3) through the pyridyl nitrogen to the Re on 10-phenanthroline rhenium (5a) and 2,9-diphenyl-1,10-phenanthroline rhenium (5b) forms novel [Re-Fe] complexes 7a, 7b and 8 respectively. Under visible light illumination using triethylamine as a sacrificial electron donor and [Re-Fe] type complexes (7a, 7b or 8) as catalysts, remarkably increased efficiency was observed for photoinduced hydrogen production with a turnover number reaching 11.8 from complex 7a and 8.75 from 7b. To the best of our knowledge, these are the best values compared to other [Re-Fe] photocatalysts reported so far. In contrast to the parent molecules, the turnover number by the intermolecular combination of complexes 6a and 2 showed a value of 5.23, and that from 6b and 2 is 3.8, while no H(2) was detected from 8a and 3 under the same experimental conditions. Obviously, the intramolecular combination of rhenium(I) and [2Fe2S] as a catalyst is promising for efficient H(2) evolution, and it is better than the intermolecular multi-component system.
State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian, 116012, P. R. China. liujh@dlut.edu.cn
Jianhui
J
Liu
Weina
W
Jiang
D040761:Biomimetic Materials / Q000737:chemistry*; D002384:Catalysis; D056831:Coordination Complexes / Q000737:chemistry; D006859:Hydrogen / Q000737:chemistry*; D006864:Hydrogenase / Q000737:chemistry*; D007506:Iron-Sulfur Proteins / Q000737:chemistry*; D008027:Light; D010618:Phenanthrolines / Q000737:chemistry; D017319:Photosensitizing Agents / Q000737:chemistry*; D012211:Rhenium / Q000737:chemistry*
D056831:Coordination Complexes; D007506:Iron-Sulfur Proteins; D010618:Phenanthrolines; D017319:Photosensitizing Agents; D012211:Rhenium; D006859:Hydrogen; D006864:Hydrogenase; C025205:1,10-phenanthroline