Phenoxyl radicals hydrogen-bonded to imidazolium: Analogues of tyrosyl D of photosystem II: High-field EPR and DFT studies

被引：67

作者：

Benisvy, L

Bittl, R

Bothe, E

Garner, CD

McMaster, J

Ross, S

Teutloff, C

Neese, F

机构：

[1] Max Planck Inst Bioanorgan Chem, D-45470 Mulheim, Germany

[2] Univ Nottingham, Sch Chem, Nottingham NG7 2RD, England

[3] Free Univ Berlin, Inst Phys Expt, D-14195 Berlin, Germany

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2005年 / 44卷 / 33期

关键词：

density functional calculations; electronic structure; EPR spectroscopy; hydrogen bonds; radical ions;

D O I：

10.1002/anie.200501132

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

(Chemical Equation Presented) The one-electron oxidation of compounds 1H-3H occurs by a proton-coupled electron-transfer mechanism to produce a phenoxyl radical hydrogen-bonded to an imidazolium carbon atom. Thus, these compounds serve as analogues for tyrosyl D. in photosystem II. This insight was obtained from a combination of W-band EPR spectroscopy and DFT calculations. © 2005 Wiley-VCH Verlag GmbH & Co. KGaA.

引用

页码：5314 / 5317

页数：4

共 40 条

[1] Characterization of a new tyrosyl free radical in Salmonella typhimurium ribonucleotide reductase with EPR at 9.45 and 245 GHz
Allard, P
Barra, AL
Andersson, KK
Schmidt, PP
Atta, M
Graslund, A
[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1996, 118 (04) : 895 - 896
[2] A functional role for tyrosine-D in assembly of the inorganic core of the water oxidase complex of photosystem II and the kinetics of water oxidation
Ananyev, GA
Sakiyan, I
Diner, BA
Dismukes, GC
[J]. BIOCHEMISTRY, 2002, 41 (03) : 974 - 980
[3] Ab initio molecular dynamics simulations and g-tensor calculations of aqueous benzosemiquinone radical anion: Effects of regular and "T-stacked" hydrogen bonds
Asher, JR
Doltsinis, NL
Kaupp, M
[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (31) : 9854 - 9861
[4] Tyrosyl radicals in enzyme catalysis: Some properties and a focus on photosynthetic water oxidation
Babcock, GT
Espe, M
Hoganson, C
LydakisSimantiris, N
McCracken, J
Shi, WJ
Styring, S
Tommos, C
Warncke, K
[J]. ACTA CHEMICA SCANDINAVICA, 1997, 51 (05): : 533 - 540
[5] Barone V., 1996, RECENT ADV DENSITY F
[6] DENSITY-FUNCTIONAL THERMOCHEMISTRY .3. THE ROLE OF EXACT EXCHANGE
BECKE, AD
[J]. JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (07) : 5648 - 5652
[7] DENSITY-FUNCTIONAL EXCHANGE-ENERGY APPROXIMATION WITH CORRECT ASYMPTOTIC-BEHAVIOR
BECKE, AD
[J]. PHYSICAL REVIEW A, 1988, 38 (06): : 3098 - 3100
[8] Phenolate and phenoxyl radical complexes of Co(II) and Co(III)
Benisvy, L
Bill, E
Blake, AJ
Collison, D
Davies, ES
Garner, CD
Guindy, CI
McInnes, EJL
McArdle, G
McMaster, J
Wilson, C
Wolowska, J
[J]. DALTON TRANSACTIONS, 2004, (21) : 3647 - 3653
[9] A phenol-imidazole pro-ligand that can exist as a phenoxyl radical, alone and when complexed to copper(II) and zinc(II)
Benisvy, L
Blake, AJ
Collison, D
Davies, ES
Garner, CD
McInnes, EJL
McMaster, J
Whittaker, G
Wilson, C
[J]. DALTON TRANSACTIONS, 2003, (10) : 1975 - 1985
[10] A phenoxyl radical complex of copper(II)
Benisvy, L
Blake, AJ
Collison, D
Davies, ES
Garner, CD
McInnes, EJL
McMaster, J
Whittaker, G
Wilson, C
[J]. CHEMICAL COMMUNICATIONS, 2001, (18) : 1824 - 1825

← 1 2 3 4 →