Spectroscopic characterization of reaction intermediates in a model for copper nitrite reductase

被引：39

作者：

Kujime, M ^{[1
]}

Fujii, H

机构：

[1] Natl Inst Nat Sci, Inst Mol Sci, Okazaki, Aichi 4448787, Japan

[2] Natl Inst Nat Sci, Okazaki Inst Integrat Biosci, Okazaki, Aichi 4448787, Japan

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2006年 / 45卷 / 07期

关键词：

bioinorganic chemistry; copper; enzyme models; reaction mechanisms; reactive intermediates;

D O I：

10.1002/anie.200503555

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

(Chemical Equation Presented) A nitrous acid complex was identified by spectroscopic and kinetic analyses under stopped-flow conditions as an intermediate in the reaction of copper(I) nitrite complex 1 with trifluoroacetic acid (see scheme). A reaction mechanism was proposed in which two protons are transferred in a stepwise manner to the nitrite anion. Intramolecular electron transfer from copper to the nitrite ligand occurs in the second protonation step. © 2006 Wiley-VCH Verlag GmbH & Co. KGaA.

引用

页码：1089 / 1092

页数：4

共 25 条

[1]

ADMAN ET, 1993, BIOINORGANIC CHEM CO, P397

[2] Atomic resolution structures of resting-state, substrate- and product-complexed Cu-nitrite reductase provide insight into catalytic mechanism [J].

Antonyuk, SV ;

Strange, RW ;

Sawers, G ;

Eady, RR ;

Hasnain, SS .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2005, 102 (34) :12041-12046

[3] Dissimilatory nitrite and nitric oxide reductases [J].

Averill, BA .

CHEMICAL REVIEWS, 1996, 96 (07) :2951-2964

[4] Catalytic roles for two water bridged residues (Asp-98 and His-255) in the active site of copper-containing nitrite reductase [J].

Boulanger, MJ ;

Kukimoto, M ;

Nishiyama, M ;

Horinouchi, S ;

Murphy, MEP .

JOURNAL OF BIOLOGICAL CHEMISTRY, 2000, 275 (31) :23957-23964

[5] Nitrogen cycle enzymology [J].

Ferguson, SJ .

CURRENT OPINION IN CHEMICAL BIOLOGY, 1998, 2 (02) :182-193

[6] Synthetic modeling of nitrite binding and activation by reduced copper proteins. Characterization of copper(I)-nitrite complexes that evolve nitric oxide [J].

Halfen, JA ;

Mahapatra, S ;

Wilkinson, EC ;

Gengenbach, AJ ;

Young, VG ;

Que, L ;

Tolman, WB .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1996, 118 (04) :763-776

[7] SYNTHETIC MODEL OF THE SUBSTRATE ADDUCT TO THE REDUCED ACTIVE-SITE OF COPPER NITRITE REDUCTASE [J].

HALFEN, JA ;

TOLMAN, WB .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1994, 116 (12) :5475-5476

[8] EVIDENCE FOR A COPPER NITROSYL INTERMEDIATE IN DENITRIFICATION BY THE COPPER-CONTAINING NITRITE REDUCTASE OF ACHROMOBACTER-CYCLOCLASTES [J].

HULSE, CL ;

AVERILL, BA ;

TIEDJE, JM .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1989, 111 (06) :2322-2323

[9] EVIDENCE FOR AN NO-REBOUND MECHANISM FOR PRODUCTION OF N2O FROM NITRITE BY THE COPPER-CONTAINING NITRITE REDUCTASE FROM ACHROMOBACTER-CYCLOCLASTES [J].

JACKSON, MA ;

TIEDJE, JM ;

AVERILL, BA .

FEBS LETTERS, 1991, 291 (01) :41-44

[10] CRYSTAL-STRUCTURE AND ELECTRON-SPIN ECHO ENVELOPE MODULATION STUDY OF [CU(II)(TEPA)(NO2)]PF6 (TEPA = TRIS[2-(2-PYRIDYL)ETHYL]AMINE) - A MODEL FOR THE PURPORTED STRUCTURE OF THE NITRITE DERIVATIVE OF HEMOCYANIN [J].

JIANG, F ;

CONRY, RR ;

BUBACCO, L ;

TYEKLAR, Z ;

JACOBSON, RR ;

KARLIN, KD ;

PEISACH, J .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1993, 115 (06) :2093-2102

← 1 2 3 →