Self-assembly of the 2-His-1-carboxylate facial triad in mononuclear iron(II) and zinc(II) models of metalloenzyme active sites

被引:28
作者
Friese, Seth J.
Kucera, Benjamin E.
Que, Lawrence, Jr.
Tolman, William B.
机构
[1] Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA
[2] Univ Minnesota, Ctr Met Biocatalysis, Minneapolis, MN 55455 USA
关键词
D O I
10.1021/ic061564s
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
A synthetic strategy involving the use of sterically hindered N-donor and terphenylcarboxylate ligands has been used to prepare complexes of iron(II) and zinc(II) that feature N-2(carboxylate) donors. X-ray crystallographic and NMR data show that the 2-His-carboxylate facial triad found in metalloenzyme active sites is closely modeled by the mononuclear complexes. In addition, by virtue of the flexibility of the ligands used, the geometries and coordination environments of the complexes display carboxylate binding mode differences such as those seen in the enzymes.
引用
收藏
页码:8003 / 8005
页数:3
相关论文
共 22 条
[1]   Reaction mechanisms of mononuclear non-heme iron oxygenases [J].
Abu-Omar, MM ;
Loaiza, A ;
Hontzeas, N .
CHEMICAL REVIEWS, 2005, 105 (06) :2227-2252
[2]   Crystal structure of the ternary complex of the catalytic domain of human phenylalanine hydroxylase with tetrahydrobiopterin and 3-(2-thienyl)-L-alanine, and its implications for the mechanism of catalysis and substrate activation [J].
Andersen, OA ;
Flatmark, T ;
Hough, E .
JOURNAL OF MOLECULAR BIOLOGY, 2002, 320 (05) :1095-1108
[3]   High resolution crystal structures of the catalytic domain of human phenylalanine hydroxylase in its catalytically active Fe(II) form and binary complex with tetrahydrobiopterin [J].
Andersen, OA ;
Flatmark, T ;
Hough, E .
JOURNAL OF MOLECULAR BIOLOGY, 2001, 314 (02) :279-291
[4]   Bis(pyrazol-1-yl)acetates as tripodal heteroscorpionate Ligands in iron chemistry:: Syntheses and structures of Iron(II) and Iron(III) complexes with bpza, bdmpza, and bdtbpza ligands [J].
Beck, A ;
Barth, A ;
Hubner, E ;
Burzlaff, N .
INORGANIC CHEMISTRY, 2003, 42 (22) :7182-7188
[5]  
Beck A, 2001, EUR J INORG CHEM, P521
[6]   Di-, tri-, and tetranuclear zinc hydroxamate complexes as structural models for the inhibition of zinc hydrolases by hydroxamic acids [J].
Brown, David A. ;
Fitzpatrick, Noel J. ;
Muller-Bunz, Helge ;
Ryan, Aine T. .
INORGANIC CHEMISTRY, 2006, 45 (11) :4497-4507
[7]   Bis(1-methylimidazol-2-yl)propionates and bis(1-methylbenzimidazol-2-yl)-propionates:: A new family of biomimetic N,N,O Ligands -: Synthesis, structures and CuII coordination complexes [J].
Bruijnincx, PCA ;
Lutz, M ;
Spek, AL ;
van Faassen, EE ;
Weckhuysen, BM ;
van Koten, G ;
Gebbink, RJMK .
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, 2005, (04) :779-787
[8]   Dioxygen activation at mononuclear nonheme iron active sites: Enzymes, models, and intermediates [J].
Costas, M ;
Mehn, MP ;
Jensen, MP ;
Que, L .
CHEMICAL REVIEWS, 2004, 104 (02) :939-986
[9]  
DAVIES SC, 1997, DALTON T, P1981
[10]   Carboxypeptidase A: Native, zinc-removed and mercury-replaced forms [J].
Greenblatt, HM ;
Feinberg, H ;
Tucker, PA ;
Shoham, G .
ACTA CRYSTALLOGRAPHICA SECTION D-BIOLOGICAL CRYSTALLOGRAPHY, 1998, 54 :289-305