期刊
CHEMICAL PHYSICS
卷 393, 期 1, 页码 65-73出版社
ELSEVIER
DOI: 10.1016/j.chemphys.2011.11.027
关键词
Photocatalysis; Ultrafast dynamics; Molecular photocatalyst; Impact of water on the catalytic properties; Hydrogen
资金
- Wenner-Gren Foundation
- Deutsche Bundesstiftung Umwelt (DBU)
- Fonds der Chemischen Industrie (FCI)
- Thuringer Ministerium fur Bildung, Wissenschaft und Kultur (PhotoMIC) [B 514-09049]
Molecular photocatalysts allow for selectively tuning their function on a molecular level based on an in-depth understanding of their chemical and photophysical properties. This contribution reports the synthesis and photophysical characterization of the novel molecular photocatalyst [(tbbpy)(2)Ru(tpac)PdCl2](2+) RutpacPd (with tpac = tetrapyrido[3,2-a:2',3'-c:3 '',2 ''-h:2''',3'''-j]acridine) and its mononuclear building block. Furthermore, detailed photocatalytic activity measurements of RutpacPd are presented. The introduction of the tpac-ligand into the molecular framework offers a potential route to reduce the impact of water as compared to the well-studied class of RutpphzPd (with tpphz = tetrapyrido[3,2-a:2',3'-c:300,2 ''-h: 2''',3'''-j] phenazine) complexes. The distinct impact of water on the electron-transfer processes in tpphz-ligands stems from the possibility of water to form hydrogen bonds to the phenazine nitrogen atoms and will potentially reduced when replacing the phenazine by the acridine unit. The effect of this structural variation on the catalytic properties and the underlying ultrafast intramolecular charge transfer behavior will be discussed in detail. (C) 2011 Elsevier B. V. All rights reserved.
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