Synthetic hydrogenases: Incorporation of an iron carbonyl thiolate into a designed peptide

被引:93
作者
Jones, Anne K. [1 ]
Lichtenstein, Bruce R.
Dutta, Arnab
Gordon, Gwyneth
Dutton, P. Leslie
机构
[1] Univ Penn, Sch Med, Johnson Res Fdn, Dept Biochem & Biophys, Philadelphia, PA 19104 USA
[2] Arizona State Univ, Sch Earth & Space Explorat, Dept Chem & Biochem, Tempe, AZ 85287 USA
关键词
D O I
10.1021/ja075116a
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
[FeFe] hydrogenases catalyze reversible hydrogen oxidation at an unusual organometallic active site. Neither enzymatic studies nor synthesis of small molecule models has managed to elucidate the mechanisms of these enzymes. In this paper, we demonstrate the incorporation of an iron carbonyl thiolate mimic of the hydrogenase active site into a de novo artificial peptide, creating the first peptide-based model system for hydrogenases. Copyright © 2007 American Chemical Society.
引用
收藏
页码:14844 / +
页数:3
相关论文
共 22 条
[11]  
Lyon EJ, 1999, ANGEW CHEM INT EDIT, V38, P3178, DOI 10.1002/(SICI)1521-3773(19991102)38:21<3178::AID-ANIE3178>3.3.CO
[12]  
2-W
[13]   Coordination sphere flexibility of active-site models for Fe-only hydrogenase: Studies in intra- and intermolecular diatomic ligand exchange [J].
Lyon, EJ ;
Georgakaki, IP ;
Reibenspies, JH ;
Darensbourg, MY .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2001, 123 (14) :3268-3278
[14]   UNUSUALLY STABLE HELIX FORMATION IN SHORT ALANINE-BASED PEPTIDES [J].
MARQUSEE, S ;
ROBBINS, VH ;
BALDWIN, RL .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 1989, 86 (14) :5286-5290
[15]   Probing metallopeptide folding mechanisms using de novo design peptides [J].
Pecoraro, VL ;
Farrer, B ;
Matzepetakis, M ;
Ghosh, D .
JOURNAL OF INORGANIC BIOCHEMISTRY, 2003, 96 (01) :30-30
[16]   X-ray crystal structure of the Fe-only hydrogenase (Cpl) from Clostridium pasteurianum to 1.8 angstrom resolution [J].
Peters, JW ;
Lanzilotta, WN ;
Lemon, BJ ;
Seefeldt, LC .
SCIENCE, 1998, 282 (5395) :1853-1858
[17]   Toward the synthesis of a photosynthetic reaction center maquette: A cofacial porphyrin pair assembled between two subunits of a synthetic four-helix bundle multiheme protein [J].
Rabanal, F ;
DeGrado, WF ;
Dutton, PL .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1996, 118 (02) :473-474
[18]   On the electronic structure of the hydrogenase H-cluster [J].
Schwab, David E. ;
Tard, Cedric ;
Brecht, Eric ;
Peters, John W. ;
Pickett, Christopher J. ;
Szilagyi, Robert K. .
CHEMICAL COMMUNICATIONS, 2006, (35) :3696-3698
[19]   Studies on the condensation pathway to and properties of diiron azadithiolate carbonyls [J].
Stanley, Jane L. ;
Rauchfuss, Thomas B. ;
Wilson, Scott R. .
ORGANOMETALLICS, 2007, 26 (08) :1907-1911
[20]   Synthesis of the H-cluster framework of iron-only hydrogenase [J].
Tard, C ;
Liu, XM ;
Ibrahim, SK ;
Bruschi, M ;
De Gioia, L ;
Davies, SC ;
Yang, X ;
Wang, LS ;
Sawers, G ;
Pickett, CJ .
NATURE, 2005, 433 (7026) :610-613