Functional biomimetic models for the active site in the respiratory enzyme cytochrome c oxidase

被引:54
作者
Collman, James P. [1 ]
Decreau, Richard A. [1 ]
机构
[1] Stanford Univ, Dept Chem, Stanford, CA 94305 USA
关键词
D O I
10.1039/b808070b
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A functional analog of the active site in the respiratory enzyme, cytochrome c oxidase (CcO) reproduces every feature in CcO's active site: a myoglobin-like heme (heme a3), a distal tridentate imidazole copper complex (Cu-B), a phenol (Tyr244), and a proximal imidazole. When covalently attached to a liquid-crystalline SAM film on an Au electrode, this functional model continuously catalyzes the selective four-electron reduction of dioxygen at physiological potential and pH, under rate-limiting electron flux (as occurs in CcO).
引用
收藏
页码:5065 / 5076
页数:12
相关论文
共 103 条
[1]   STRUCTURE AT 2.8-ANGSTROM RESOLUTION OF F1-ATPASE FROM BOVINE HEART-MITOCHONDRIA [J].
ABRAHAMS, JP ;
LESLIE, AGW ;
LUTTER, R ;
WALKER, JE .
NATURE, 1994, 370 (6491) :621-628
[2]   OXYGEN ACTIVATION AND THE CONSERVATION OF ENERGY IN CELL RESPIRATION [J].
BABCOCK, GT ;
WIKSTROM, M .
NATURE, 1992, 356 (6367) :301-309
[3]   Covalently supported porphyrins as ligands for the preparation of heme a3/CuB binuclear active site analogues of heme-copper terminal oxidases and metallation under mild conditions [J].
Baeg, JO ;
Holm, RH .
CHEMICAL COMMUNICATIONS, 1998, (05) :571-572
[4]   Insights into the structure and function of redox-active tyrosines from model compounds [J].
Barry, BA ;
Einarsdóttir, O .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (15) :6972-6981
[5]   Exploring the proton pump mechanism of cytochrome c oxidase in real time [J].
Belevich, Ilya ;
Bloch, Dmitry A. ;
Belevich, Nikolai ;
Wikstrom, Marten ;
Verkhovsky, Michael I. .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2007, 104 (08) :2685-2690
[6]  
Blankenship R. E., 2002, MOL MECH PHOTOSYNTHE
[7]   Understanding the reaction that powers this world:: Biomimetic studies of respiratory O2 reduction by cytochrome oxidase [J].
Boulatov, R .
PURE AND APPLIED CHEMISTRY, 2004, 76 (02) :303-319
[8]   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
[9]   Supramolecular bioinorganic chemistry:: Model complexes of cytochrome c oxidase meet functional surfaces [J].
Broering, Martin .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2007, 46 (33) :6222-6224
[10]   CYTOCHROME-C-OXIDASE - SUBUNIT STRUCTURE AND PROTON PUMPING [J].
BRUNORI, M ;
ANTONINI, G ;
MALATESTA, F ;
SARTI, P ;
WILSON, MT .
EUROPEAN JOURNAL OF BIOCHEMISTRY, 1987, 169 (01) :1-8