Indication of a hydrogen-atom abstraction reaction relevant to a mechanistic proposal for the oxygen-evolving complex of photosystem II

被引:7
作者
Jensen, KB [1 ]
McKenzie, CJ [1 ]
Pedersen, JZ [1 ]
机构
[1] Univ So Denmark, Inst Chem, DK-5230 Odense M, Denmark
关键词
D O I
10.1021/ic0155380
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
The hydroxide-bridged Cr(III)-Mn(II) complex [(Me(3)tacn)Cr(mu -OH)(mu -CH3CO2)(2)Mn(MeDPA)](2+) (Me(3)tacn = tri-N,N ' ,N " -methyltriazacyclononane, MeDPA = N-methyl-N-bis(2-pyridylmethylamine) is oxidized by the 2,4,6-triphenylphenoxide radical to give the oxo-bridged Cr(III)-Mn(III) complex [(Me(3)tacn)Cr(mu -O)(mu -CH3CO2)(2)Mn(MeDPA)](2+). This reaction is a potential model for H-atom abstraction steps in mechanistic proposals for water oxidation in photosynthesis. [GRAPHICS]
引用
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页码:5066 / +
页数:3
相关论文
共 13 条
[1]   Energetics of proton-coupled electron transfer in high-valent Mn-2(mu-O)(2) systems: Models for water oxidation by the oxygen-evolving complex of photosystem II [J].
Baldwin, MJ ;
Pecoraro, VL .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1996, 118 (45) :11325-11326
[2]   Thermodynamic viability of hydrogen atom transfer from water coordinated to the oxygen-evolving complex of photosystem II [J].
Caudle, MT ;
Pecoraro, VL .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1997, 119 (14) :3415-3416
[3]   GENERAL-ROUTE TO MU-HYDROXO-BIS(MU-ACETATO)-BRIDGED HETEROMETAL DINUCLEAR COMPLEXES - SYNTHESES, MAGNETIC AND REDOX PROPERTIES, ELECTRONIC-SPECTRA, AND MOLECULAR-STRUCTURES OF THE CR(III)-CO(II) AND CR(III)-FE(II) SPECIES [J].
CHAUDHURI, P ;
WINTER, M ;
KUPPERS, HJ ;
WIEGHARDT, K ;
NUBER, B ;
WEISS, J .
INORGANIC CHEMISTRY, 1987, 26 (20) :3302-3310
[4]  
DIMROTH K, 1959, LIEBIGS ANN CHEM, V624, P51
[5]   UNDERSTANDING C-H BOND OXIDATIONS - H-CENTER-DOT AND H- TRANSFER IN THE OXIDATION OF TOLUENE BY PERMANGANATE [J].
GARDNER, KA ;
MAYER, JM .
SCIENCE, 1995, 269 (5232) :1849-1851
[6]   A metalloradical mechanism for the generation of oxygen from water in photosynthesis [J].
Hoganson, CW ;
Babcock, GT .
SCIENCE, 1997, 277 (5334) :1953-1956
[7]   SPIN EXCHANGE COUPLING IN ASYMMETRIC HETERODINUCLEAR COMPLEXES CONTAINING THE MU-OXO-BIS(MU-ACETATO)DIMETAL CORE [J].
HOTZELMANN, R ;
WIEGHARDT, K ;
FLORKE, U ;
HAUPT, HJ ;
WEATHERBURN, DC ;
BONVOISIN, J ;
BLONDIN, G ;
GIRERD, JJ .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1992, 114 (05) :1681-1696
[8]   Hydrogen atom abstraction by metal-oxo complexes: Understanding the analogy with organic radical reactions [J].
Mayer, JM .
ACCOUNTS OF CHEMICAL RESEARCH, 1998, 31 (08) :441-450
[9]   Peroxo-, oxo-, and hydroxo-bridged dicopper complexes:: Observation of exogenous hydrocarbon substrate oxidation [J].
Obias, HV ;
Lin, Y ;
Murthy, NN ;
Pidcock, E ;
Solomon, EI ;
Ralle, M ;
Blackburn, NJ ;
Neuhold, YM ;
Zuberbühler, AD ;
Karlin, KD .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1998, 120 (49) :12960-12961
[10]   A proposal for water oxidation in photosystem II [J].
Pecoraro, VL ;
Baldwin, MJ ;
Caudle, MT ;
Hsieh, WY ;
Law, NA .
PURE AND APPLIED CHEMISTRY, 1998, 70 (04) :925-929