Noncovalent assembly of a metalloporphyrin and an iron hydrogenase active-site model:: Photo-induced electron transfer and hydrogen generation

被引：133

作者：

Li, Xueqiang ^{[1
]}

Wang, Mei ^{[1
]}

Zhang, Suping ^{[1
]}

Pan, Jingxi ^{[1
]}

Na, Yong ^{[1
]}

Liu, Jianhui ^{[1
]}

Akermark, Bjorn ^{[2
]}

Sun, Licheng ^{[1
,3
]}

机构：

[1] Dalian Univ Technol, State Key Lab Fine Chem, DUT KTH Joint Educ & Res Ctr Mol Devices, Dalian 116012, Peoples R China

[2] Stockholm Univ, Arrhenius Lab, Dept Organ Chem, S-10691 Stockholm, Sweden

[3] Royal Inst Technol KTH, KTH Sch Chem Sci & Engn, Dept Chem, S-10044 Stockholm, Sweden

来源：

JOURNAL OF PHYSICAL CHEMISTRY B | 2008年 / 112卷 / 27期

关键词：

D O I：

10.1021/jp710498v

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

A noncovalent assembly of a pyridyl-functionalized hydrogenase active-site model complex and zinc tetraphenylporphyrin has been obtained and characterized. Upon light irradiation, fluorescence quenching by electron transfer was observed from the singlet excited state of the porphyrin to the diiron center, and the mechanism was verified by fluorescence lifetime and transient absorption spectroscopic measurements. In contrast to molecular dyads linked by covalent bonds, the assembled system was designed to avoid charge recombination via complex dissociation after photo-induced electron transfer. Visible light-driven hydrogen generation was observed from this self-assembled system. The assembling strategy employed in this study has the potential to be used for any other hydrogenase models in the future.

引用

页码：8198 / 8202

页数：5

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