Geometric control of reduction potential in oxomolybdenum centers: Implications to the serine coordination in DMSO reductase

被引：25

作者：

Davie, SR

Rubie, ND

Hammes, BS

Carrano, CJ ^{[1
]}

Kirk, ML

Basu, P

机构：

[1] Duquesne Univ, Dept Chem & Biochem, Pittsburgh, PA 15282 USA

[2] SW Texas State Univ, Dept Chem, San Marcos, TX 78666 USA

[3] Univ New Mexico, Dept Chem, Albuquerque, NM 87131 USA

来源：

INORGANIC CHEMISTRY | 2001年 / 40卷 / 12期

关键词：

D O I：

10.1021/ic0012017

中图分类号：

O61 [无机化学];

学科分类号：

070301 ; 081704 ;

摘要：

Two isomers (cis and trans) of (L1O)MoOCl2 have been synthesized and separated using the heteroscorpinate ligand L1OH, which possesses an N2O donor set. These geometric isomers differ in the orientation of the phenolate oxygen with respect to the terminal oxo group. The cis isomer spontaneously converts to the thermodynamically more stable trans isomer. Since the reduction potentials of the two isomers differ by similar to 220 mV and crystal structures of DMSOR and TMAOR exhibit a wide range of O-t-Mo-O-ser angles, we suggest that this angular variation may play a crucial role in gating the electron transfer process in the regeneration step.

引用

收藏

页码：2632 / 2633

页数：2

相关论文

共 26 条

[1] MICROBIAL-DEGRADATION OF METHANESULFONIC-ACID - A MISSING LINK IN THE BIOGEOCHEMICAL SULFUR CYCLE [J].

BAKER, SC ;

KELLY, DP ;

MURRELL, JC .

NATURE, 1991, 350 (6319) :627-628

[2] Mononuclear and binuclear molybdenum(V) complexes of the ligand N,N'-dimethyl-N,N'-bis(2-mercaptophenyl)ethylenediamine: Geometric isomers [J].

Barnard, KR ;

Bruck, M ;

Huber, S ;

Grittini, C ;

Enemark, JH ;

Gable, RW ;

Wedd, AG .

INORGANIC CHEMISTRY, 1997, 36 (04) :637-649

[3] X-ray absorption spectroscopy of dimethylsulfoxide reductase from Rhodobacter capsulatus [J].

Baugh, PE ;

Garner, CD ;

Charnock, JM ;

Collison, D ;

Davies, ES ;

McAlpine, AS ;

Bailey, S ;

Lane, I ;

Hanson, GR ;

McEwan, AG .

JOURNAL OF BIOLOGICAL INORGANIC CHEMISTRY, 1997, 2 (05) :634-643

[4] Reversible dissociation of thiolate ligands from molybdenum in an enzyme of the dimethyl sulfoxide reductase family [J].

Bray, RC ;

Adams, B ;

Smith, AT ;

Bennett, B ;

Bailey, S .

BIOCHEMISTRY, 2000, 39 (37) :11258-11269

[5] HE-I VALENCE PHOTOELECTRON-SPECTRA OF OXOMOLYBDENUM(V) COMPLEXES CONTAINING DIOLATO OR ALKOXIDE LIGANDS [J].

CHANG, CSJ ;

RAICHAUDHURI, A ;

LICHTENBERGER, DL ;

ENEMARK, JH .

POLYHEDRON, 1990, 9 (15-16) :1965-1973

[6] OCEANIC PHYTOPLANKTON, ATMOSPHERIC SULFUR, CLOUD ALBEDO AND CLIMATE [J].

CHARLSON, RJ ;

LOVELOCK, JE ;

ANDREAE, MO ;

WARREN, SG .

NATURE, 1987, 326 (6114) :655-661

[7] SYNTHESES, STRUCTURES, AND SPECTROSCOPIC PROPERTIES OF 6-COORDINATE MONONUCLEAR OXO-MOLYBDENUM(V) COMPLEXES STABILIZED BY THE HYDROTRIS(3,5-DIMETHYL-1-PYRAZOLYL)BORATE LIGAND [J].

CLELAND, WE ;

BARNHART, KM ;

YAMANOUCHI, K ;

COLLISON, D ;

MABBS, FE ;

ORTEGA, RB ;

ENEMARK, JH .

INORGANIC CHEMISTRY, 1987, 26 (07) :1017-1025

[8] Crystal structure of oxidized trimethylamine N-oxide reductase from Shewanella massilia at 2.5 Å resolution [J].

Czjzek, M ;

Dos Santos, JP ;

Pommier, J ;

Giordano, G ;

Méjean, V ;

Haser, R .

JOURNAL OF MOLECULAR BIOLOGY, 1998, 284 (02) :435-447

[9]

Enemark J. H., 1993, ADV INORG CHEM, V40, P1, DOI DOI 10.1016/S0898-8838(08)60181-6

[10] The coordination chemistry and function of the molybdenum centres of the oxomolybdoenzymes [J].

Enemark, JH ;

Garner, CD .

JOURNAL OF BIOLOGICAL INORGANIC CHEMISTRY, 1997, 2 (06) :817-822