2011 Annual Science Report

Montana State University Reporting  |  SEP 2010 – AUG 2011

Minerals to Enzymes: The Path to CO Dehydrogenase/Acetyl – CoA Synthase

Project Summary

We have through NAI Director’s discretionary initiated a project to probing the structural determinants for nickel-iron-sulfur based reversible carbon monoxide oxidation. We are probing whether we can mimic the reactivity of carbon monoxide dehydrogenase to some extent by simple organic nesting and synthesis of nickel-iron-sulfur clusters using a model system we have developed.

4 Institutions
3 Teams
0 Publications
0 Field Sites
Field Sites

Project Progress

The major emphasis of the research in the ABRC is relating the structure and reactivity of iron-sulfur minerals and iron-sulfur enzymes to better understand the origin of biological processes. Specifically we are using iron-sulfur motifs as a model system to understand the transition between the abiotic early Earth and biology. We have been able to provide growing support for our overarching hypothesis that there is a distinct connection between iron-sulfur minerals and iron-sulfur enzymes worthy of this line of inquiry in work on the complex iron sulfur containing nitrogenases (nitrogen fixation) and hydrogenases (hydrogen metabolism). The enzymes responsible for reversible carbon dioxide oxidation (carbon monoxide dehydrogenases) are also complex iron-sulfur enzymes. In this project we are testing the hypothesis that the path from minerals to enzymes occur through the organic nesting of clusters and that the evolutionary ancestors of modern iron sulfur enzymes were simply peptides or polypeptides capable of binding metal clusters. In this work we have used a model enzyme which we have structurally characterized and found to have an open cavity with metal binding ligands and the capacity to bind metal clusters. When we incubate this protein with the various concentrations of nickel, iron, and sulfur we are able to generate different metal clusters some of which have detectable levels of carbon monoxide oxidation catalytic activity. We are in the process now of designing minimal cluster forming peptide motifs to indentify the minimum structural determinants of catalysis.

  • PROJECT INVESTIGATORS:
    John Peters John Peters
    Co-Investigator
  • PROJECT MEMBERS:
    Robert Szilagyi
    Project Investigator

    Joan Broderick
    Co-Investigator

    James Ferry
    Co-Investigator

    Michael Russell
    Co-Investigator

    Martin Schoonen
    Co-Investigator

    Guana Siluvai Pitchai
    Postdoc

    Logan Giles
    Doctoral Student

    Travis Harris
    Doctoral Student

    Kevin Swanson
    Doctoral Student

    Mingyu Wang
    Doctoral Student

  • RELATED OBJECTIVES:
    Objective 3.1
    Sources of prebiotic materials and catalysts

    Objective 3.2
    Origins and evolution of functional biomolecules

    Objective 3.3
    Origins of energy transduction

    Objective 3.4
    Origins of cellularity and protobiological systems

    Objective 7.1
    Biosignatures to be sought in Solar System materials

    Objective 7.2
    Biosignatures to be sought in nearby planetary systems