Reversible Protonation of a Thiolate Ligand in an [Fe]-Hydrogenase Model Complex

被引：47

作者：

Chen, Dafa ^{[1
]}

Scopelliti, Rosario ^{[1
]}

Hu, Xile ^{[1
]}

机构：

[1] Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Inorgan Synth & Catalysis, ISIC LSCI, CH-1015 Lausanne, Switzerland

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2012年 / 51卷 / 08期

基金：

瑞士国家科学基金会;

关键词：

enzyme models; hydrogenases; iron; protonation; sulfur; CLUSTER-FREE HYDROGENASE; ACTIVE-SITE; CRYSTAL-STRUCTURE; METHANOGENIC ARCHAEA; 3RD HYDROGENASE; H-2; ACTIVATION; LIGHT-INACTIVATION; OXIDATIVE ADDITION; FE HYDROGENASE; IRON CENTER;

D O I：

10.1002/anie.201107634

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

What is the channel? The thiolate ligand in the five-coordinate model complex 1 of [Fe]-hydrogenase is preferentially and reversibly protonated, even in the presence of an acyl ligand. The results suggest that the Cys176 thiolate ligand in [Fe]-hydrogenase can serve as the internal base to accept the proton after heterolytic splitting of H 2. © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

引用

页码：1919 / 1921

页数：3

共 41 条

[1]

Chen D., 2010, Angew. Chem, V122, P7674

[2]

Chen D. F., 2011, ANGEW CHEM, V123, P5789

[3] A Five-Coordinate Iron Center in the Active Site of [Fe]-Hydrogenase: Hints from a Model Study [J].

Chen, Dafa ;

Scopelliti, Rosario ;

Hu, Xile .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2011, 50 (25) :5670-5672

[4] Synthesis and Characterization of a Series of Model Complexes of the Active Site of [Fe]-Hydrogenase (Hmd) [J].

Chen, Dafa ;

Ahrens-Botzong, Annegret ;

Schuemann, Volker ;

Scopelliti, Rosario ;

Hu, Xile .

INORGANIC CHEMISTRY, 2011, 50 (11) :5249-5257

[5] [Fe]-Hydrogenase Models Featuring Acylmethylpyridinyl Ligands [J].

Chen, Dafa ;

Scopelliti, Rosario ;

Hu, Xile .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2010, 49 (41) :7512-7515

[6] Synthesis and Reactivity of Iron Acyl Complexes Modeling the Active Site of [Fe]-Hydrogenase [J].

Chen, Dafa ;

Scopelliti, Rosario ;

Hu, Xile .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (03) :928-+

[7] Evolution in the understanding of [Fe]-hydrogenase [J].

Corr, Michael J. ;

Murphy, John A. .

CHEMICAL SOCIETY REVIEWS, 2011, 40 (05) :2279-2292

[8] PROTONATION SITES IN THIOLATO IRON CARBONYLATES - EVIDENCE FOR AN ARRESTED FE(RS-H) OXIDATIVE ADDITION [J].

DARENSBOURG, MY ;

LIAW, WF ;

RIORDAN, CG .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1989, 111 (20) :8051-8052

[9] Characterization of the Fe site in iron-sulfur cluster-free hydrogenase (Hmd) and of a model compound via nuclear resonance vibrational spectroscopy (NRVS) [J].

Guo, Yisong ;

Wang, Hongxin ;

Xiao, Yuming ;

Vogt, Sonja ;

Thauer, Rudolf K. ;

Shima, Seigo ;

Volkers, Phillip I. ;

Rauchfuss, Thomas B. ;

Pelmenschikov, Vladimir ;

Case, David A. ;

Alp, Ercan E. ;

Sturhahn, Wolfgang ;

Yoda, Yoshitaka ;

Cramer, Stephen P. .

INORGANIC CHEMISTRY, 2008, 47 (10) :3969-3977

[10]

Hiromoto T., 2009, ANGEW CHEM, V121, P6579

← 1 2 3 4 5 →