O2 reduction by a functional heme/nonheme bis-iron NOR model complex

被引：27

作者：

Collman, James P. ^{[1
]}

Dey, Abhishek ^{[1
]}

Yang, Ying ^{[1
]}

Ghosh, Somdatta ^{[1
]}

Decreau, Richard A. ^{[1
]}

机构：

[1] Stanford Univ, Dept Chem, Stanford, CA 94305 USA

来源：

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA | 2009年 / 106卷 / 26期

基金：

美国国家卫生研究院;

关键词：

electrochemistry; ferryl; NOR functional model; O-2; reductase; PROS; NITRIC-OXIDE REDUCTASE; CYTOCHROME-C-OXIDASE; INTERDIGITATED ARRAY ELECTRODE; RING-DISK ELECTRODE; HEME-PROTEINS; FE-IV=O; OXYGEN; DIOXYGEN; PROTON; MONOLAYERS;

D O I：

10.1073/pnas.0904634106

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

O-2 reactivity of a functional NOR model is investigated by using electrochemistry and spectroscopy. The electrochemical measurements using interdigitated electrodes show very high selectivity for 4e O-2 reduction with minimal production of partially reduced oxygen species (PROS) under both fast and slow electron flux. Intermediates trapped at cryogenic temperatures and characterized by using resonance Raman spectroscopy under single-turnover conditions indicate that an initial bridging peroxide intermediate undergoes homolytic O-O bond cleavage generating a trans heme/nonheme bis-ferryl intermediate. This bis ferryl species can oxygenate 2 equivalents of a reactive substrate.

引用

收藏

页码：10528 / 10533

页数：6

相关论文

共 62 条

[1] Functional analogues of the dioxygen reduction site in cytochrome oxidase:: Mechanistic aspects and possible effects of CuB [J].

Boulatov, R ;

Collman, JP ;

Shiryaeva, IM ;

Sunderland, CJ .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2002, 124 (40) :11923-11935

[2] REACTIONS OF NITRIC-OXIDE WITH CYTOCHROME-C OXIDASE [J].

BRUDVIG, GW ;

STEVENS, TH ;

CHAN, SI .

BIOCHEMISTRY, 1980, 19 (23) :5275-5285

[3] Nitric oxide and the respiratory enzyme [J].

Brunori, Maurizio ;

Forte, Elena ;

Arese, Marzia ;

Mastronicola, Daniela ;

Giuffre, Alessandro ;

Sarti, Paolo .

BIOCHIMICA ET BIOPHYSICA ACTA-BIOENERGETICS, 2006, 1757 (9-10) :1144-1154

[4] STRUCTURE-SENSITIVE RESONANCE RAMAN BANDS OF TETRAPHENYL AND PICKET FENCE PORPHYRIN-IRON COMPLEXES, INCLUDING AN OXYHEMOGLOBIN ANALOG [J].

BURKE, JM ;

KINCAID, JR ;

PETERS, S ;

GAGNE, RR ;

COLLMAN, JP ;

SPIRO, TG .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1978, 100 (19) :6083-6088

[5] Two conserved glutamates in the bacterial nitric oxide reductase are essential for activity but not assembly of the enzyme [J].

Butland, G ;

Spiro, S ;

Watmough, NJ ;

Richardson, DJ .

JOURNAL OF BACTERIOLOGY, 2001, 183 (01) :189-199

[6] MICROMETER-SPACED PLATINUM INTERDIGITATED ARRAY ELECTRODE - FABRICATION, THEORY, AND INITIAL USE [J].

CHIDSEY, CE ;

FELDMAN, BJ ;

LUNDGREN, C ;

MURRAY, RW .

ANALYTICAL CHEMISTRY, 1986, 58 (03) :601-607

[7] Isolation and crystal structure of a peroxo-bridged heme-copper complex [J].

Chishiro, T ;

Shimazaki, Y ;

Tani, F ;

Tachi, Y ;

Naruta, Y ;

Karasawa, S ;

Hayami, S ;

Maeda, Y .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2003, 42 (24) :2788-2791

[8] A functional nitric oxide reductase model [J].

Collman, James P. ;

Yang, Ying ;

Dey, Abhishek ;

Decreau, Richard A. ;

Ghosh, Somdatta ;

Ohta, Takehiro ;

Solomon, Edward I. .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2008, 105 (41) :15660-15665

[9] Interaction of nitric oxide with a functional model of cytochrome c oxidase [J].

Collman, James P. ;

Dey, Abhishek ;

Decreau, Richard A. ;

Yang, Ying ;

Hosseini, Ali ;

Solomon, Edward I. ;

Eberspacher, Todd A. .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2008, 105 (29) :9892-9896

[10] Intramolecular single-turnover reaction in a cytochrome c oxidase model bearing a Tyr244 mimic [J].

Collman, James P. ;

Decreau, Richard A. ;

Yan, Yilong ;

Yoon, Jungjoo ;

Solomon, Edward I. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (18) :5794-+

← 1 2 3 4 5 6 7 →