Visible Light-Driven Hydrogen Evolution from Water Catalyzed by A Molecular Cobalt Complex
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  • 作者:Lianpeng Tong ; Ruifa Zong ; Randolph P. Thummel
  • 刊名:Journal of the American Chemical Society
  • 出版年:2014
  • 出版时间:April 2, 2014
  • 年:2014
  • 卷:136
  • 期:13
  • 页码:4881-4884
  • 全文大小:298K
  • 年卷期:v.136,no.13(April 2, 2014)
  • ISSN:1520-5126
文摘
An approximately planar tetradentate polypyridine ligand, 8-(1鈥?10鈥?phenanthrol-2鈥?yl)-2-(pyrid-2鈥?yl)quinoline (ppq), has been prepared by two sequential Friedl盲nder condensations. The ligand readily accommodates Co(II) bearing two axial chlorides, and the resulting complex is reasonably soluble in water. In DMF the complex shows three well-behaved redox waves in the window of 0 to 鈭?.4 V (vs SHE). However in pH 7 buffer the third wave is obscured by a catalytic current at 鈭?.95 V, indicating hydrogen production that appears to involve a proton-coupled electron-transfer event. The complex [Co(ppq)Cl2] (6) in pH 4 aqueous solution, together with [Ru(bpy)3]Cl2 and ascorbic acid as a sacrificial electron donor, in the presence of blue light (位max = 469 nm) produces hydrogen with an initial TOF = 586 h鈥?.

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