A designed heme-[4Fe-4S] metalloenzyme catalyzes sulfite reduction like the native enzyme

التفاصيل البيبلوغرافية
العنوان: A designed heme-[4Fe-4S] metalloenzyme catalyzes sulfite reduction like the native enzyme
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