CO Disrupts the Reduced H-Cluster of FeFe Hydrogenase. A Combined DFT and Protein Film Voltammetry Study

被引：56

作者：

Baffert, Carole ^{[2
]}

Bertini, Luca ^{[1
]}

Lautier, Thomas ^{[3
]}

Greco, Claudio ^{[1
]}

Sybirna, Kateryna

Ezanno, Pierre ^{[2
]}

Etienne, Emilien ^{[2
]}

Soucaille, Philippe ^{[3
]}

Bertrand, Patrick ^{[2
]}

Bottin, Herve ^{[4
]}

Meynial-Salles, Isabelle ^{[3
]}

De Gioia, Luca ^{[1
]}

Leger, Christophe ^{[2
]}

机构：

[1] Univ Milano Bicocca, Dept Biotechnol & Biosci, I-20126 Milan, Italy

[2] CNRS, UPR 9036, F-13402 Marseille 20, France

[3] Univ Toulouse, INSA, UPS,CNRS 135, INP,LISBP,INRA,UMR792,UMR 5504, F-31077 Toulouse, France

[4] CEA, iBiTec S, SB2SM, LPB,DSV,URA CNRS 2096, F-91191 Gif Sur Yvette, France

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2011年 / 133卷 / 07期

关键词：

CARBON-MONOXIDE BINDING; ACTIVE-SITE; ENZYMES; ANALOGS;

D O I：

10.1021/ja110627b

中图分类号：

O6 [化学];

学科分类号：

070301 [无机化学];

摘要：

Carbon monoxide is often described as a competitive inhibitor of FeFe hydrogenases, and it is used for probing H-2 binding to synthetic or in silico models of the active site H-cluster. Yet it does not always behave as a simple inhibitor. Using an original approach which combines accurate electrochemical measurements and theoretical calculations, we elucidate the mechanism by which, under certain conditions, CO binding can cause permanent damage to the H-cluster. Like in the case of oxygen inhibition, the reaction with CO engages the entire H-cluster, rather than only the Fe-2 subsite.

引用

页码：2096 / 2099

页数：4

共 28 条

[1]

ADAMS MWW, 1987, J BIOL CHEM, V262, P15054

[2]

A needle in a haystack:: The active site of the membrane-bound complex cytochrome c nitrite reductase [J].

Almeida, M. Gabriela ;

Silveira, Celia M. ;

Guigliarelli, Bruno ;

Bertrand, Patrick ;

Moura, Jose J. G. ;

Moura, Isabel ;

Leger, Christophe .

FEBS LETTERS, 2007, 581 (02) :284-288

[3]

Hydrogen-activating enzymes:: Activity does not correlate with oxygen sensitivity [J].

Baffert, Carole ;

Demuez, Marie ;

Cournac, Laurent ;

Burlat, Benedicte ;

Guigliarelli, Bruno ;

Bertrand, Patrick ;

Girbal, Laurence ;

Leger, Christophe .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2008, 47 (11) :2052-2054

[4]

Reversible carbon monoxide binding and inhibition at the active site of the Fe-only hydrogenase [J].

Bennett, B ;

Lemon, BJ ;

Peters, JW .

BIOCHEMISTRY, 2000, 39 (25) :7455-7460

[5]

CO Affinity and Bonding Properties of [FeFe] Hydrogenase Active Site Models. A DFT Study [J].

Bertini, Luca ;

Greco, Claudio ;

Bruschi, Maurizio ;

Fantucci, Piercarlo ;

De Gioia, Luca .

ORGANOMETALLICS, 2010, 29 (09) :2013-2025

[6]

Influence of the [2Fe]H Subcluster Environment on the Properties of Key Intermediates in the Catalytic Cycle of [FeFe] Hydrogenases: Hints for the Rational Design of Synthetic Catalysts [J].

Bruschi, Maurizio ;

Greco, Claudio ;

Kaukonen, Markus ;

Fantucci, Piercarlo ;

Ryde, Ulf ;

De Gioia, Luca .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2009, 48 (19) :3503-3506

[7]

Correcting for Electrocatalyst Desorption and Inactivation in Chronoamperometry Experiments [J].

Fourmond, Vincent ;

Lautier, Thomas ;

Baffert, Carole ;

Leroux, Fanny ;

Liebgott, Pierre-Pol ;

Dementin, Sebastien ;

Rousset, Marc ;

Arnoux, Pascal ;

Pignol, David ;

Meynial-Salles, Isabelle ;

Soucaille, Phillippe ;

Bertrand, Patrick ;

Leger, Christophe .

ANALYTICAL CHEMISTRY, 2009, 81 (08) :2962-2968

[8]

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

Gloaguen, Frederic ;

Rauchfuss, Thomas B. .

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

[9]

Goldet G, 2009, J AM CHEM SOC, V131, P14979, DOI [10.1021/ja905388j, 10.1021/ja905388i]

[10]

The quest for a functional substrate access tunnel in FeFe hydrogenase [J].

Lautier, Thomas ;

Ezanno, Pierre ;

Baffert, Carole ;

Fourmond, Vincent ;

Cournac, Laurent ;

Fontecilla-Camps, Juan C. ;

Soucaille, Philippe ;

Bertrand, Patrick ;

Meynial-Salles, Isabelle ;

Leger, Christophe .

FARADAY DISCUSSIONS, 2011, 148 :385-407

← 1 2 3 →