Directing protonation in [FeFe] hydrogenase active site models by modifications in their second coordination sphere

被引：74

作者：

Ezzaher, Salah ^{[1
]}

Gogoll, Adolf ^{[2
]}

Bruhn, Clemens ^{[3
]}

Ott, Sascha ^{[1
]}

机构：

[1] Uppsala Univ, Angstrom Labs, Dept Photochem & Mol Sci, S-75120 Uppsala, Sweden

[2] Uppsala Univ, Dept Biochem & Organ Chem, S-75123 Uppsala, Sweden

[3] Univ Kassel, Dept Chem, D-34132 Kassel, Germany

来源：

CHEMICAL COMMUNICATIONS | 2010年 / 46卷 / 31期

基金：

瑞典研究理事会;

关键词：

IRON HYDROGENASE; ELECTRONIC-PROPERTIES; ONLY HYDROGENASE; COMPLEXES; HYDRIDE; LIGANDS;

D O I：

10.1039/c0cc00724b

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Subtle changes in the second coordination sphere of [Cl(2)bdtFe(2)-(CO)(4)(Ph(2)P-CH(2)-X-CH(2)-PPh(2))] (bdt = benzene-1,2-dithiolate, X = NCH(3), NCH(2)CF(3), CH(2)) that do not influence the electronic character of the Fe(2) center can however direct protonation to three different sites: the N in the bis-phosphane, the Fe-Fe bond or the bdt-S.

引用

页码：5775 / 5777

页数：3

共 25 条

[1] Aza- and Oxadithiolates Are Probable Proton Relays in Functional Models for the [FeFe]-Hydrogenases [J].

Barton, Bryan E. ;

Olsen, Matthew T. ;

Rauchfuss, Thomas B. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (50) :16834-+

[2] FLUORINE-CONTAINING NITROGEN COMPOUNDS .1. TRIFLUOROETHYLAMINES [J].

BISSELL, ER ;

FINGER, M .

JOURNAL OF ORGANIC CHEMISTRY, 1959, 24 (09) :1256-1259

[3] DFT investigation of structural, electronic, and catalytic properties of diiron complexes related to the [2Fe]H subcluster of Fe-only hydrogenases [J].

Bruschi, M ;

Fantucci, P ;

De Gioia, L .

INORGANIC CHEMISTRY, 2002, 41 (06) :1421-1429

[4] An insight into the protonation property of a diiron azadithiolate complex pertinent to the active site of Fe-only hydirogenases [J].

Dong, WB ;

Wang, M ;

Liu, XY ;

Jin, K ;

Li, GH ;

Wang, FJ ;

Sun, LC .

CHEMICAL COMMUNICATIONS, 2006, (03) :305-307

[5] Ligand versus metal protonation of an iron hydrogenase active site mimic [J].

Eilers, Gerriet ;

Schwartz, Lennart ;

Stein, Matthias ;

Zampella, Giuseppe ;

de Gioia, Luca ;

Ott, Sascha ;

Lomoth, Reiner .

CHEMISTRY-A EUROPEAN JOURNAL, 2007, 13 (25) :7075-7084

[6] Evidence for the formation of terminal hydrides by protonation of an asymmetric iron hydrogenase active site mimic [J].

Ezzaher, Salah ;

Capon, Jean-Francois ;

Gloaguen, Frederic ;

Petillon, Francois Y. ;

Schollhammer, Philippe ;

Talarmin, Jean .

INORGANIC CHEMISTRY, 2007, 46 (09) :3426-3428

[7] Influence of a Pendant Amine in the Second Coordination Sphere on Proton Transfer at a Dissymmetrically Disubstituted Diiron System Related to the [2Fe]H Subsite of [FeFe]H2ase [J].

Ezzaher, Salah ;

Capon, Jean-Francois ;

Gloaguen, Frederic ;

Petillon, Francois Y. ;

Schollhammer, Philippe ;

Talarmin, Jean ;

Kervarec, Nelly .

INORGANIC CHEMISTRY, 2009, 48 (01) :2-4

[8] Review of electrochemical studies of complexes containing the Fe2S2 core characteristic of [FeFe]-hydrogenases including catalysis by these complexes of the reduction of acids to form dihydrogen [J].

Felton, Greg A. N. ;

Mebi, Charles A. ;

Petro, Benjamin J. ;

Vannucci, Aaron K. ;

Evans, Dennis H. ;

Glass, Richard S. ;

Lichtenberger, Dennis L. .

JOURNAL OF ORGANOMETALLIC CHEMISTRY, 2009, 694 (17) :2681-2699

[9] Small molecule mimics of hydrogenases: hydrides and redox [J].

Gloaguen, Frederic ;

Rauchfuss, Thomas B. .

CHEMICAL SOCIETY REVIEWS, 2009, 38 (01) :100-108

[10] CORRELATION OF THE BASE STRENGTHS OF AMINES [J].

HALL, HK .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1957, 79 (20) :5441-5444

← 1 2 3 →