Abstract

Upgraded X-ray Detector for Characterization of Hydrogenase Enzyme Models X-ray crystallography is the principal tool in the characterization of models of the active sites of hydrogenases. Our NIH-supported work focuses on both broad classes of hydrogenases ([FeFe]- and [NiFe]) which are relevant to the metabolism of pathogens and significant in energy technology relative to hydrogen production. The goal of the research is to elucidate mechanisms by which these enzymes operate as well as the pathways by which they are biosynthesized. The utility of crystallography hinges on our ability to obtain suitable single crystals and the capability of the diffractometer to extract reflection data. The suitability of crystals depends both on their quality and size. The requested instrumentation will allow characterization of single crystals of far smaller dimensions than currently possible. Growing single crystals is the single greatest time sink in this project. The requested instrumentation will be maintained by two state-supported PhD-level permanent staff and made available to other researchers, many of whom pursue NIH-supported projects.

Public Health Relevance

We seek to upgrade the Photon 100 detector to a Photon II detector for our X-ray diffractometer. Owing to it improved sensitivity and tolerance of small crystals, the new capability will accelerate discovery and research on the biosynthesis of models for the [FeFe]-hydrogenases.

  Funding Agency

Agency
National Institute of Health (NIH)
Institute
National Institute of General Medical Sciences (NIGMS)
Type
Research Project (R01)
Project #
3R01GM061153-17S1
Application #
9708059
Study Section
Program Officer
Anderson, Vernon
Project Start
2000-07-01
Project End
2022-04-30
Budget Start
2018-05-01
Budget End
2019-04-30
Support Year
17
Fiscal Year
2018
Total Cost
Indirect Cost

  Institution

Name
University of Illinois Urbana-Champaign
Department
Chemistry
Type
Schools of Arts and Sciences
DUNS #
041544081
City
Champaign
State
IL
Country
United States
Zip Code
61820

  Publications

Li, Qianli; Lalaoui, Noémie; Woods, Toby J et al. (2018) Electron-Rich, Diiron Bis(monothiolato) Carbonyls: C-S Bond Homolysis in a Mixed Valence Diiron Dithiolate. Inorg Chem 57:4409-4418
Sommer, Constanze; Richers, Casseday P; Lubitz, Wolfgang et al. (2018) A [RuRu] Analogue of an [FeFe]-Hydrogenase Traps the Key Hydride Intermediate of the Catalytic Cycle. Angew Chem Int Ed Engl 57:5429-5432
Carlson, Michaela R; Gray, Danielle L; Richers, Casseday P et al. (2018) Sterically Stabilized Terminal Hydride of a Diiron Dithiolate. Inorg Chem 57:1988-2001
Pelmenschikov, Vladimir; Birrell, James A; Pham, Cindy C et al. (2017) Reaction Coordinate Leading to H2 Production in [FeFe]-Hydrogenase Identified by Nuclear Resonance Vibrational Spectroscopy and Density Functional Theory. J Am Chem Soc 139:16894-16902
Lalaoui, Noémie; Woods, Toby; Rauchfuss, Thomas B et al. (2017) Characterization of a Borane ? Complex of a Diiron Dithiolate: Model for an Elusive Dihydrogen Adduct. Organometallics 36:2054-2057
Yu, Xin; Tung, Chen-Ho; Wang, Wenguang et al. (2017) Interplay between Terminal and Bridging Diiron Hydrides in Neutral and Oxidized States. Organometallics 36:2245-2253
Schilter, David; Gray, Danielle L; Fuller, Amy L et al. (2017) Synthetic Models for Nickel-Iron Hydrogenase Featuring Redox-Active Ligands. Aust J Chem 70:505-515
Reijerse, Edward J; Pham, Cindy C; Pelmenschikov, Vladimir et al. (2017) Direct Observation of an Iron-Bound Terminal Hydride in [FeFe]-Hydrogenase by Nuclear Resonance Vibrational Spectroscopy. J Am Chem Soc 139:4306-4309
Carlson, Michaela R; Gilbert-Wilson, Ryan; Gray, Danielle R et al. (2017) Diiron Dithiolate Hydrides Complemented with Proton-Responsive Phosphine-Amine Ligands. Eur J Inorg Chem 2017:3169-3173
Zhao, Peihua; Gray, Danielle L; Rauchfuss, Thomas B (2016) Rational Synthesis of the Carbonyl(perthiolato)diiron [Fe2(S3CPh2)(CO)6] and Related Complexes. Eur J Inorg Chem 2016:2681-2683

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