Carbon Monoxide Dehydrogenase Reduces Cyanate to Cyanide
| Autor: | Alexandre Ciaccafava, Daria Tombolelli, Ingo Zebger, Jae-Hun Jeoung, Maria Andrea Mroginski, Holger Dobbek, Lilith Domnik, Peter Hildebrandt |
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| Přispěvatelé: | Institut für Chemie [TUB Berlin], Technische Universität Berlin (TU) |
| Rok vydání: | 2017 |
| Předmět: |
Spectrophotometry
Infrared Stereochemistry Protein Conformation Cyanide Carboxydothermus hydrogenoformans Electrons Thermoanaerobacter 010402 general chemistry 01 natural sciences Catalysis Adduct Substrate Specificity chemistry.chemical_compound Multienzyme Complexes Organic chemistry ComputingMilieux_MISCELLANEOUS Cyanates chemistry.chemical_classification Crystallography Cyanides biology 010405 organic chemistry General Chemistry Carbon Dioxide Models Theoretical Cyanate biology.organism_classification Aldehyde Oxidoreductases 0104 chemical sciences [SDV.BBM.BP]Life Sciences [q-bio]/Biochemistry Molecular Biology/Biophysics Enzyme chemistry biology.protein Biocatalysis Oxidation-Reduction Carbon monoxide dehydrogenase |
| Zdroj: | Angewandte Chemie International Edition Angewandte Chemie International Edition, Wiley-VCH Verlag, 2017, 56 (26), pp.7398-7401. ⟨10.1002/anie.201703225⟩ |
| ISSN: | 1521-3773 1433-7851 |
| DOI: | 10.1002/anie.201703225⟩ |
| Popis: | The biocatalytic function of carbon monoxide dehydrogenase (CODH) has a high environmental relevance owing to its ability to reduce CO2 . Despite numerous studies on CODH over the past decades, its catalytic mechanism is not yet fully understood. In the present combined spectroscopic and theoretical study, we report first evidences for a cyanate (NCO- ) to cyanide (CN- ) reduction at the C-cluster. The adduct remains bound to the catalytic center to form the so-called CN- -inhibited state. Notably, this conversion does not occur in crystals of the Carboxydothermus hydrogenoformans CODH enzyme (CODHIICh ), as indicated by the lack of the corresponding CN- stretching mode. The transformation of NCO- , which also acts as an inhibitor of the two-electron-reduced Cred2 state of CODH, could thus mimic CO2 turnover and open new perspectives for elucidation of the detailed catalytic mechanism of CODH. |
| Databáze: | OpenAIRE |
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