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HIGH-GEAR SIGNED

High-valent protein-coordinated catalytic metal sites: Geometric and Electronic ARchitecture

Total Cost €

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EC-Contrib. €

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Partnership

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Project "HIGH-GEAR" data sheet

The following table provides information about the project.

Coordinator
STOCKHOLMS UNIVERSITET 

Organization address
address: UNIVERSITETSVAGEN 10
city: STOCKHOLM
postcode: 10691
website: www.su.se

contact info
title: n.a.
name: n.a.
surname: n.a.
function: n.a.
email: n.a.
telephone: n.a.
fax: n.a.

 Coordinator Country Sweden [SE]
 Total cost 1˙968˙375 €
 EC max contribution 1˙968˙375 € (100%)
 Programme 1. H2020-EU.1.1. (EXCELLENT SCIENCE - European Research Council (ERC))
 Code Call ERC-2016-COG
 Funding Scheme ERC-COG
 Starting year 2017
 Duration (year-month-day) from 2017-06-01   to  2022-05-31

 Partnership

Take a look of project's partnership.

# participants  country  role  EC contrib. [€] 
1    STOCKHOLMS UNIVERSITET SE (STOCKHOLM) coordinator 1˙968˙375.00

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 Project objective

It is estimated that almost half of all enzymes utilize metal cofactors for their function, for example the respiratory complexes and the oxygen-evolving photosystem II, the most fundamental requirements for aerobic life as we know it. If we could mimic nature’s use of metals for harvesting sunlight, energy conversion and chemical synthesis it would eliminate the need for fossil fuels and greatly increase the possibilities of chemical industry while reducing the environmental impact. Achieving this type of chemistry is an outstanding testament to evolution and understanding it is a glaring challenge to mankind.

These types of reactions are based on very challenging redox chemistry (involving one or several electrons). The key catalytic species are generally high-valent metal clusters with a varying ligand environment, provided by the protein and other bound molecules, that directly controls the reactivity of the inorganic core. To be able to understand and mimic this chemistry it is of central importance to know the geometric and electronic structures of the metal core as well as the entire ligand environment for these usually short-lived and very reactive intermediates. It has, for a number of reasons, proven extremely challenging to obtain these for protein-coordinated catalysts.

The central goal of this project is to determine true and accurate geometric and electronic structures of high-valent di-nuclear Fe/Fe and Mn/Fe metal sites coordinated in protein matrices known to direct these for varied and important chemistry. By combining new X-ray diffraction based techniques with advanced spectroscopy we aim to define how the protein controls the entatic state as well as reactivity and mechanism for some of the most potent catalysts in nature. The results will serve as a basis for design of oxygen-activating catalysts with novel properties.

 Publications

year authors and title journal last update
List of publications.
2019 Yury Kutin, Ramona Kositzki, Rui M. M. Branca, Vivek Srinivas, Daniel Lundin, Michael Haumann, Martin Högbom, Nicholas Cox, Julia J. Griese
Chemical flexibility of heterobimetallic Mn/Fe cofactors: R2lox and R2c proteins
published pages: 18372-18386, ISSN: 0021-9258, DOI: 10.1074/jbc.ra119.010570
Journal of Biological Chemistry 294/48 2020-01-28
2019 Stefan Mebs, Vivek Srinivas, Ramona Kositzki, Julia J. Griese, Martin Högbom, Michael Haumann
Fate of oxygen species from O2 activation at dimetal cofactors in an oxidase enzyme revealed by 57Fe nuclear resonance X-ray scattering and quantum chemistry
published pages: 148060, ISSN: 0005-2728, DOI: 10.1016/j.bbabio.2019.148060
Biochimica et Biophysica Acta (BBA) - Bioenergetics 1860/12 2020-01-28
2019 Julia J. Griese, Ramona Kositzki, Michael Haumann, Martin Högbom
Assembly of a heterodinuclear Mn/Fe cofactor is coupled to tyrosine–valine ether cross-link formation in the R2-like ligand-binding oxidase
published pages: 211-221, ISSN: 0949-8257, DOI: 10.1007/s00775-019-01639-4
JBIC Journal of Biological Inorganic Chemistry 24/2 2020-01-28
2019 Julia J. Griese, Martin Högbom
Location-specific quantification of protein-bound metal ions by X-ray anomalous dispersion: Q-XAD
published pages: 764-771, ISSN: 2059-7983, DOI: 10.1107/s2059798319009926
Acta Crystallographica Section D Structural Biology 75/8 2020-01-28
2019 Hongyi Xu, Hugo Lebrette, Max T. B. Clabbers, Jingjing Zhao, Julia J. Griese, Xiaodong Zou, Martin Högbom
Solving a new R2lox protein structure by microcrystal electron diffraction
published pages: eaax4621, ISSN: 2375-2548, DOI: 10.1126/sciadv.aax4621
Science Advances 5/8 2020-01-28
2019 Kristīne Grāve, Wietske Lambert, Gustav Berggren, Julia J. Griese, Matthew D. Bennett, Derek T. Logan, Martin Högbom
Redox-induced structural changes in the di-iron and di-manganese forms of Bacillus anthracis ribonucleotide reductase subunit NrdF suggest a mechanism for gating of radical access
published pages: 849-861, ISSN: 0949-8257, DOI: 10.1007/s00775-019-01703-z
JBIC Journal of Biological Inorganic Chemistry 24/6 2020-01-28
2018 Vivek Srinivas, Hugo Lebrette, Daniel Lundin, Yuri Kutin, Margareta Sahlin, Michael Lerche, Jürgen Eirich, Rui M. M. Branca, Nicholas Cox, Britt-Marie Sjöberg, Martin Högbom
Metal-free ribonucleotide reduction powered by a DOPA radical in Mycoplasma pathogens
published pages: 416-420, ISSN: 0028-0836, DOI: 10.1038/s41586-018-0653-6
Nature 563/7731 2019-05-14
2018 Pearson T. Maugeri, Julia J. Griese, Rui M. Branca, Effie K. Miller, Zachary R. Smith, Jürgen Eirich, Martin Högbom, Hannah S. Shafaat
Driving Protein Conformational Changes with Light: Photoinduced Structural Rearrangement in a Heterobimetallic Oxidase
published pages: 1471-1480, ISSN: 0002-7863, DOI: 10.1021/jacs.7b11966
Journal of the American Chemical Society 140/4 2019-05-14
2018 Julia J. Griese, Rui M. M. Branca, Vivek Srinivas, Martin Högbom
Ether cross-link formation in the R2-like ligand-binding oxidase
published pages: 879-886, ISSN: 0949-8257, DOI: 10.1007/s00775-018-1583-3
JBIC Journal of Biological Inorganic Chemistry 23/6 2019-05-14

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