Proton coupling to [4Fe-4S]2+/+ and [4Fe-4Se]2+/+ oxidation and reduction in a designed protein

被引：45

作者：

Kennedy, ML ^{[1
]}

Gibney, BR ^{[1
]}

机构：

[1] Columbia Univ, Dept Chem, New York, NY 10027 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2002年 / 124卷 / 24期

关键词：

D O I：

10.1021/ja0171613

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The coupling of a single proton to [4Fe-4S]2+/+ oxidation/reduction in a de novo designed iron-sulfur protein maquette is presented. The reduced state pKared is 9.3, and the oxidized state pKaox is <6.5. The reduced state pKared shifts to 8.3 upon incorporation of a [4Fe-4Se]2+/+ cluster, implicating the cluster itself or its primary coordination sphere as the proton-coupling site. Copyright © 2002 American Chemical Society.

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页码：6826 / 6827

页数：2

相关论文

共 26 条

[1] Iron-sulfur clusters: Nature's modular, multipurpose structures [J].

Beinert, H ;

Holm, RH ;

Munck, E .

SCIENCE, 1997, 277 (5326) :653-659

[2]

Beinert H, 1978, Methods Enzymol, V54, P435

[3] Proton-translocation by membrane-bound NADH:ubiquinone-oxidoreductase (complex I) through redox-gated ligand conduction [J].

Brandt, U .

BIOCHIMICA ET BIOPHYSICA ACTA-BIOENERGETICS, 1997, 1318 (1-2) :79-91

[4] ALTERNATIVE SPIN STATES IN SYNTHETIC ANALOGS OF BIOLOGICAL CLUSTERS - SPIN-QUARTET GROUND-STATES AND STRUCTURES OF [FE4S4(SPH)4]3- AND [FE4SE4(SPH)4]3- AS THEIR TETRAMETHYLAMMONIUM SALTS [J].

CARNEY, MJ ;

PAPAEFTHYMIOU, GC ;

WHITENER, MA ;

SPARTALIAN, K ;

FRANKEL, RB ;

HOLM, RH .

INORGANIC CHEMISTRY, 1988, 27 (02) :346-352

[5] Atomically defined mechanism for proton transfer to a buried redox centre in a protein [J].

Chen, KS ;

Hirst, J ;

Camba, R ;

Bonagura, CA ;

Stout, CD ;

Burgess, BK ;

Armstrong, FA .

NATURE, 2000, 405 (6788) :814-817

[6] The rational design and construction of a cuboidal iron-sulfur protein [J].

Coldren, CD ;

Hellinga, HW ;

Caradonna, JP .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 1997, 94 (13) :6635-6640

[7] RAPID COLORIMETRIC MICROMETHOD FOR THE QUANTITATION OF COMPLEXED IRON IN BIOLOGICAL SAMPLES [J].

FISH, WW .

METHODS IN ENZYMOLOGY, 1988, 158 :357-364

[8] Ferredoxin and ferredoxin-heme maquettes [J].

Gibney, BR ;

Mulholland, SE ;

Rabanal, F ;

Dutton, PL .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 1996, 93 (26) :15041-15046

[9]

HONG JS, 1970, J BIOL CHEM, V245, P4982

[10]

JOHNSON MK, 1994, ENCY INORGANIC CHEM, V4, P1896