Resonance Raman evidence for the interconversion between an [FeIII-η1-OOH] 2+ and [FeIII-η2-O2]+ species and mechanistic implications thereof

被引:82
作者
Ho, RYN
Roelfes, G
Hermant, R
Hage, R
Feringa, BL [1 ]
Que, L
机构
[1] Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA
[2] Univ Minnesota, Ctr Met Biocatalysis, Minneapolis, MN 55455 USA
[3] Univ Groningen, Dept Organ & Mol Inorgan Chem, NL-9747 AG Groningen, Netherlands
[4] Unilever Res Labs Vlaardingen, NL-3133 AT Vlaardingen, Netherlands
关键词
D O I
10.1039/a905535e
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The deprotonation of [Fe-III(N4Py)(eta(1)-OOH)](2+) 1 gives [Fe-III(N4Py)(eta(2)-OO)](+) 2, as unequivocally demonstrated by resonance Raman spectroscopy, and leads to the loss of alkane hydroxylation activity by 1.
引用
收藏
页码:2161 / 2162
页数:2
相关论文
共 22 条
[11]   NONHEME IRON CENTERS IN OXYGEN ACTIVATION - CHARACTERIZATION OF AN IRON(III) HYDROPEROXIDE INTERMEDIATE [J].
LUBBEN, M ;
MEETSMA, A ;
WILKINSON, EC ;
FERINGA, B ;
QUE, L .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION IN ENGLISH, 1995, 34 (13-14) :1512-1514
[12]   REACTIONS OF SUPEROXIDE WITH IRON PORPHYRINS IN APROTIC-SOLVENTS - A HIGH-SPIN FERRIC PORPHYRIN PEROXO COMPLEX [J].
MCCANDLISH, E ;
MIKSZTAL, AR ;
NAPPA, M ;
SPRENGER, AQ ;
VALENTINE, JS ;
STONG, JD ;
SPIRO, TG .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1980, 102 (12) :4268-4271
[13]   Detailed spectroscopic and theoretical studies on [Fe(EDTA)(O2)]3-:: Electronic structure of the side-on ferric-peroxide bond and its relevance to reactivity [J].
Neese, F ;
Solomon, EI .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1998, 120 (49) :12829-12848
[14]   Dioxygen activation by enzymes with mononuclear non-heme iron active sites [J].
Que, L ;
Ho, RYN .
CHEMICAL REVIEWS, 1996, 96 (07) :2607-2624
[15]   Iron chemistry of a pentadentate ligand that generates a metastable FeIII-OOH intermediate [J].
Roelfes, G ;
Lubben, M ;
Chen, K ;
Ho, RYN ;
Meetsma, A ;
Genseberger, S ;
Hermant, RM ;
Hage, R ;
Mandal, SK ;
Young, VG ;
Zang, Y ;
Kooijman, H ;
Spek, AL ;
Que, L ;
Feringa, BL .
INORGANIC CHEMISTRY, 1999, 38 (08) :1929-1936
[16]   ELECTROSPRAY MASS-SPECTROMETRY OF IRON BLEOMYCIN - DEMONSTRATION THAT ACTIVATED BLEOMYCIN IS A FERRIC PEROXIDE COMPLEX [J].
SAM, JW ;
TANG, XJ ;
PEISACH, J .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1994, 116 (12) :5250-5256
[17]   Switching on the nucleophilic reactivity of a ferric porphyrin peroxo complex [J].
Selke, M ;
Valentine, JS .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1998, 120 (11) :2652-2653
[18]  
Simaan AJ, 1999, EUR J INORG CHEM, P993
[19]   Heme-containing oxygenases [J].
Sono, M ;
Roach, MP ;
Coulter, ED ;
Dawson, JH .
CHEMICAL REVIEWS, 1996, 96 (07) :2841-2887
[20]   MECHANISMS OF BLEOMYCIN-INDUCED DNA-DEGRADATION [J].
STUBBE, J ;
KOZARICH, JW .
CHEMICAL REVIEWS, 1987, 87 (05) :1107-1136