Spectroscopic Elucidation of a New Heme/Copper Dioxygen Structure Type: Implications for O•••O Bond Rupture in Cytochrome c Oxidase

被引：37
作者：
Kieber-Emmons, Matthew T. [2 ]
Qayyum, Munzarin F. [2 ]
Li, Yuqi [1 ]
Halime, Zakaria [1 ]
Hodgson, Keith O. [2 ,3 ]
Hedman, Britt [3 ]
Karlin, Kenneth D. [1 ]
Solomon, Edward I. [2 ,3 ]
机构：
[1] Johns Hopkins Univ, Dept Chem, Baltimore, MD 21218 USA
[2] Stanford Univ, Dept Chem, Stanford, CA 94305 USA
[3] Stanford Univ, SLAC Natl Accelerator Lab, Stanford, CA 94309 USA
来源：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2012年 / 51卷 / 01期
关键词：
copper; cytochromes; dioxygen ligands; heme proteins; Raman spectroscopy; PARACOCCUS-DENITRIFICANS; ESCHERICHIA-COLI; ACTIVE-SITE; OXYGEN; INTERMEDIATE; MODEL; REACTIVITY; REDUCTION; RESONANCE; PEROXIDE;
D O I：
10.1002/anie.201104080
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
All's well that ends well: The geometric and electronic structure of the first end-on heme-peroxo-copper adduct (see picture) was elucidated using UV/Vis, resonance Raman, and X-ray absorption spectroscopy and is supported by DFT calculations. Coordination of the axial base is correlated to a spin-state change, leading to enhanced biomimetic reactivity, and gives insight into O-O bond cleavage by cytochrome c oxidase. © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
引用
收藏
页码：168 / 172
页数：5
相关论文
共 35 条
  • [1] A peroxide bridge between Fe and Cu ions in the O2 reduction site of fully oxidized cytochrome c oxidase could suppress the proton pump
    Aoyama, Hiroshi
    Muramoto, Kazumasa
    Shinzawa-Itoh, Kyoko
    Hirata, Kunio
    Yamashita, Eiki
    Tsukihara, Tomitake
    Ogura, Takashi
    Yoshikawa, Shinya
    [J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2009, 106 (07) : 2165 - 2169
  • [2] SPECTROSCOPIC AND THEORETICAL-STUDIES OF AN END-ON PEROXIDE-BRIDGED COUPLED BINUCLEAR COPPER(II) MODEL COMPLEX OF RELEVANCE TO THE ACTIVE-SITES IN HEMOCYANIN AND TYROSINASE
    BALDWIN, MJ
    ROSS, PK
    PATE, JE
    TYEKLAR, Z
    KARLIN, KD
    SOLOMON, EI
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1991, 113 (23) : 8671 - 8679
  • [3] Metal-bridging mechanism for O-O bond cleavage in cytochrome c oxidase
    Blomberg, MRA
    Siegbahn, PEM
    Wikström, M
    [J]. INORGANIC CHEMISTRY, 2003, 42 (17) : 5231 - 5243
  • [4] Reactivity studies on FeIII-(O22-)-CuII compounds:: Influence of the ligand architecture and copper ligand denticity
    Chufan, Eduardo E.
    Mondal, Biplab
    Gandhi, Thirumanavelan
    Kim, Eunsuk
    Rubie, Nick D.
    Moeenne-Loccoz, Pierre
    Karlin, Kenneth D.
    [J]. INORGANIC CHEMISTRY, 2007, 46 (16) : 6382 - 6394
  • [5] Heme-copper/dioxygen adduct formation, properties, and reactivity
    Chufan, Eduardo E.
    Puiu, Simona C.
    Karlin, Kenneth D.
    [J]. ACCOUNTS OF CHEMICAL RESEARCH, 2007, 40 (07) : 563 - 572
  • [6] CHARACTERIZATION OF THE LOW-TEMPERATURE INTERMEDIATES OF THE REACTION OF FULLY REDUCED SOLUBLE CYTOCHROME-OXIDASE WITH OXYGEN BY ELECTRON-PARAMAGNETIC-RESONANCE AND OPTICAL SPECTROSCOPY
    CLORE, GM
    ANDREASSON, LE
    KARLSSON, B
    AASA, R
    MALMSTROM, BG
    [J]. BIOCHEMICAL JOURNAL, 1980, 185 (01) : 139 - 154
  • [7] A cytochrome c oxidase model catalyzes oxygen to water reduction under rate-limiting electron flux
    Collman, James P.
    Devaraj, Neal K.
    Decreau, Richard A.
    Yang, Ying
    Yan, Yi-Long
    Ebina, Wataru
    Eberspacher, Todd A.
    Chidsey, Christopher E. D.
    [J]. SCIENCE, 2007, 315 (5818) : 1565 - 1568
  • [8] Single-turnover intermolecular reaction between a FeIII-superoxide-CuI cytochrome c oxidase model and exogeneous Tyr244 mimics
    Collman, James P.
    Decreau, Richard A.
    Sunderland, Christopher J.
    [J]. CHEMICAL COMMUNICATIONS, 2006, (37) : 3894 - 3896
  • [9] A SYNTHETIC ANALOG FOR THE OXYGEN-BINDING SITE IN CYTOCHROME-C-OXIDASE
    COLLMAN, JP
    HERRMANN, PC
    BOITREL, B
    ZHANG, XM
    EBERSPACHER, TA
    FU, L
    WANG, JL
    ROUSSEAU, DL
    WILLIAMS, ER
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1994, 116 (21) : 9783 - 9784
  • [10] The post-translational modification cytochrome c oxidase is required to establish a functional environment of the catalytic site
    Das, TK
    Pecoraro, C
    Tomson, FL
    Gennis, RB
    Rousseau, DL
    [J]. BIOCHEMISTRY, 1998, 37 (41) : 14471 - 14476
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