Quantum Refinement Does Not Support Dinuclear Copper Sites in Crystal Structures of Particulate Methane Monooxygenase

Lili Cao, Octav Caldararu, Amy C. Rosenzweig, Ulf Ryde*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

61 Scopus citations

Abstract

Particulate methane monooxygenase (pMMO) is one of the few enzymes that can activate methane. The metal content of this enzyme has been highly controversial, with suggestions of a dinuclear Fe site or mono-, di-, or trinuclear Cu sites. Crystal structures have shown a mono- or dinuclear Cu site, but the resolution was low and the geometry of the dinuclear site unusual. We have employed quantum refinement (crystallographic refinement enhanced with quantum-mechanical calculations) to improve the structure of the active site. We compared a number of different mono- and dinuclear geometries, in some cases enhanced with more protein ligands or one or two water molecules, to determine which structure fits two sets of crystallographic raw data best. In all cases, the best results were obtained with mononuclear Cu sites, occasionally with an extra water molecule. Thus, we conclude that there is no crystallographic support for a dinuclear Cu site in pMMO.

Original languageEnglish (US)
Pages (from-to)162-166
Number of pages5
JournalAngewandte Chemie - International Edition
Volume57
Issue number1
DOIs
StatePublished - Jan 2 2018

Keywords

  • copper
  • density functional theory
  • particulate methane monooxygenase
  • quantum refinement

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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