Protonation and dehydration reactions of the Mn4O4L6 cubane and synthesis and crystal structure of the oxidized cubane [Mn4O4L6]+:: A model for the photosynthetic water oxidizing complex

被引:83
作者
Ruettinger, WF [1 ]
Ho, DM [1 ]
Dismukes, GC [1 ]
机构
[1] Princeton Univ, Dept Chem, Hoyt Lab, Princeton, NJ 08544 USA
关键词
D O I
10.1021/ic981145y
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
The synthesis and! atomic structure of [Mn4O4L6](+)(CF3SO3-). 1(+)OTf(-) (L = diphenylphosphinate), is reported. This new model for the photosynthetic water oxidizing complex extends the known [Mn4O4](n+) cubane core type to the Mn-4(III,3IV) oxidation state. Synthesis of this cluster is achieved by one-electron oxidation of Mn4O4L6 (1) by molecular oxygen in a series of steps initiated by the protonation or silylation of one oxide bridge in 1.
引用
收藏
页码:1036 / +
页数:3
相关论文
共 28 条
[1]   Calcium induces binding and formation of a spin-coupled dimanganese(II,II) center in the apo-water oxidation complex of photosystem II as precursor to the functional tetra-Mn/Ca cluster [J].
Ananyev, GM ;
Dismukes, GC .
BIOCHEMISTRY, 1997, 36 (38) :11342-11350
[2]  
ARMSTRONG WH, 1992, MANGANESE REDOX ENZY, P261
[3]   Modeling the photosynthetic water oxidation complex:: Activation of water by controlled deprotonation and incorporation into a tetranuclear manganese complex [J].
Aromí, G ;
Wemple, MW ;
Aubin, SJ ;
Folting, K ;
Hendrickson, DN ;
Christou, G .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1998, 120 (23) :5850-5851
[4]   Resonant magnetization tunneling in the trigonal pyramidal Mn(IV)Mn-3(III) complex [Mn4O3Cl(O2CCH3)3(dbm)3] [J].
Aubin, SMJ ;
Dilley, NR ;
Pardi, L ;
Krzystek, J ;
Wemple, MW ;
Brunel, LC ;
Maple, MB ;
Christou, G ;
Hendrickson, DN .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1998, 120 (20) :4991-5004
[5]   Distorted MnIVMn3III cubane complexes as single-molecule magnets [J].
Aubin, SMJ ;
Wemple, MW ;
Adams, DM ;
Tsai, HL ;
Christou, G ;
Hendrickson, DN .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1996, 118 (33) :7746-7754
[6]   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
[7]   MECHANISM FOR PHOTOSYNTHETIC O-2 EVOLUTION [J].
BRUDVIG, GW ;
CRABTREE, RH .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 1986, 83 (13) :4586-4588
[8]   MANGANESE CARBOXYLATE CHEMISTRY AND ITS BIOLOGICAL RELEVANCE [J].
CHRISTOU, G .
ACCOUNTS OF CHEMICAL RESEARCH, 1989, 22 (09) :328-335
[9]   MIXED-VALENCE INTERACTIONS IN DI-MU-OXO BRIDGED MANGANESE COMPLEXES [J].
COOPER, SR ;
CALVIN, M .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1977, 99 (20) :6623-6630
[10]   THE MANGANESE AND CALCIUM-IONS OF PHOTOSYNTHETIC OXYGEN EVOLUTION [J].
DEBUS, RJ .
BIOCHIMICA ET BIOPHYSICA ACTA, 1992, 1102 (03) :269-352