Unravelling novel synergies between organometallic and biological partners: A quantum mechanics/molecular mechanics study of an artificial metalloenzyme

Elisabeth Ortega-Carrasco, Agustí Lledós, Jean Didier Maréchal

Research output: Contribution to journalArticleResearchpeer-review

8 Citations (Scopus)

Abstract

In recent years, the design of artificialmetalloenzymes obtained by the insertion of homogeneous catalysts into biological macromolecules has become a major field of research. These hybrids, and the corresponding X-ray structures of several of them, are offering opportunities to better understand the synergy between organometallic and biological subsystems. In this work, we investigate the resting state and activation process of a hybrid inspired by an oxidative haemoenzyme but presenting an unexpected reactivity and structural features. An extensive series of quantum mechanics/molecular mechanics calculations show that the resting state and the activation processes of the novel enzyme differ from naturally occurring haemoenzymes in terms of the electronic state of the metal, participation of the first coordination sphere of the metal and the dynamic process. This study presents novel insights into the sensitivity of the association between organometallic and biological partners and illustrates the molecular challenge that represents the design of efficient enzymes based on this strategy. © 2014 The Author(s) Published by the Royal Society. All rights reserved.
Original languageEnglish
Article number20140090
JournalJournal of the Royal Society Interface
Volume11
Issue number96
DOIs
Publication statusPublished - 6 Jul 2014

Keywords

  • Activation process
  • Artificial metalloenzymes
  • Computational bioinorganics
  • Resting state

Fingerprint Dive into the research topics of 'Unravelling novel synergies between organometallic and biological partners: A quantum mechanics/molecular mechanics study of an artificial metalloenzyme'. Together they form a unique fingerprint.

  • Cite this