Syntheses and characterization of aqua-bridged dimetallic complexes, M2(mu-H2O)(mu-OAc)2(Im)4(OAc)2(M=Mg2+, Mn2+, and Ni2+). Structural models for the active sites of dimetallic hydrolases

J Inorg Biochem. 2002 Nov 11;92(2):128-36. doi: 10.1016/s0162-0134(02)00496-8.

Abstract

Four novel aqua-bridged dinuclear complexes with a formula M2(mu-H2O)(mu-OAc)2(Im)4(OAc)2(Im)4(OAc)2 (where Im=imidazole, M=Mg2+ 1, Mn2+ 2, Ni2+ 3 and Co2+ 4) have been synthesized and characterized. Complexes 1, 2 and 3 have been characterized by X-ray crystallography. Two M2+ ions are bridged by an aqua molecule and two carboxylate anion with M...M=3.635-3.777 A, M-OH(2)=2.109-2.246 A and M-OH(2)-M=114.4-119.0 degrees, respectively. Each complex is further stabilized by two intramolecular hydrogen bonds between the hydrogens of the bridging aqua and the oxygens of the terminal monodentate acetates with a distance of O...O=2.6 A. The terminal monodentate acetates display "reversed" C-O distances, namely the C-O(free) distances are actually longer than the C-O(coordinating) distances. This abnormal geometry of a monodentate carboxylate would be caused by the strong "pulling effect" on the terminal carboxylates by intra- and intermolecular hydrogen bonds. The O-H stretching vibration of the bridging water was identified at ca. 2328 cm(-1) in IR spectra based on the deuterium isotope shift. The solid state 13C and 15N NMR spectra of 1 displayed two sets of peaks for acetate and Im ligands, respectively, consistent with the presence of two types of coordination modes of acetate and the two symmetrically non-equivalent Im as revealed by X-ray structure. 15N chemical shift of NH in Im ligands underwent about 6 ppm downfield shift due to its involvement in an intermolecular hydrogen bond.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Bridged-Ring Compounds / chemical synthesis*
  • Bridged-Ring Compounds / chemistry*
  • Catalytic Domain
  • Crystallography, X-Ray
  • Hydrogen Bonding
  • Hydrolases / chemistry*
  • Imidazoles / chemical synthesis
  • Imidazoles / chemistry
  • Ligands
  • Models, Molecular
  • Molecular Structure
  • Nuclear Magnetic Resonance, Biomolecular
  • Organometallic Compounds / chemical synthesis*
  • Organometallic Compounds / chemistry*
  • Spectroscopy, Fourier Transform Infrared
  • Water / chemistry

Substances

  • Bridged-Ring Compounds
  • Imidazoles
  • Ligands
  • Organometallic Compounds
  • Water
  • Hydrolases