A designed heme-[4Fe-4S] metalloenzyme catalyzes sulfite reduction like the native enzyme
العنوان: | A designed heme-[4Fe-4S] metalloenzyme catalyzes sulfite reduction like the native enzyme |
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المؤلفون: | Mirts, Evan N., Petrik, Igor D., Hosseinzadeh, Parisa, Nilges, Mark J., Lu, Yi |
سنة النشر: | 2023 |
المجموعة: | SciTec Connect (Office of Scientific and Technical Information - OSTI, U.S. Department of Energy) |
مصطلحات موضوعية: | 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY, 59 BASIC BIOLOGICAL SCIENCES |
الوصف: | Multielectron redox reactions often require multicofactor metalloenzymes to facilitate coupled electron and proton movement, but it is challenging to design artificial enzymes to catalyze these important reactions, owing to their structural and functional complexity. Here, we report a designed heteronuclear heme-[4Fe-4S] cofactor in cytochrome c peroxidase as a structural and functional model of the enzyme sulfite reductase. The initial model exhibits spectroscopic and ligand-binding properties of the native enzyme, and sulfite reduction activity was improved—through rational tuning of the secondary sphere interactions around the [4Fe-4S] and the substrate-binding sites—to be close to that of the native enzyme. By offering insight into the requirements for a demanding six-electron, seven-proton reaction that has so far eluded synthetic catalysts, this study provides strategies for designing highly functional multicofactor artificial enzymes. |
نوع الوثيقة: | other/unknown material |
وصف الملف: | application/pdf |
اللغة: | unknown |
Relation: | http://www.osti.gov/servlets/purl/1470758; https://www.osti.gov/biblio/1470758; https://doi.org/10.1126/science.aat8474 |
DOI: | 10.1126/science.aat8474 |
الاتاحة: | http://www.osti.gov/servlets/purl/1470758 https://www.osti.gov/biblio/1470758 https://doi.org/10.1126/science.aat8474 |
رقم الانضمام: | edsbas.559F2935 |
قاعدة البيانات: | BASE |
DOI: | 10.1126/science.aat8474 |
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