A Serine-Substituted P450 Catalyzes Highly Efficient Carbene Transfer to Olefins In Vivo
Pedro S. Coelho,Z. Jane Wang,Maraia E. Ener,Stefanie A. Baril,Arvind Kannan,Frances H. Arnold,Eric M. Brustad +6 more
TLDR
A unique serine-heme ligated cytochrome “P411” that catalyzes efficient and selective carbene transfers from diazoesters to olefins in intact Escherichia coli cells is designed.Abstract:
Whole-cell catalysts for non-natural chemical reactions will open new routes to sustainable production of chemicals. We designed a cytochrome 'P411' with unique serine-heme ligation that catalyzes efficient and selective olefin cyclopropanation in intact Escherichia coli cells. The mutation C400S in cytochrome P450(BM3) gives a signature ferrous CO Soret peak at 411 nm, abolishes monooxygenation activity, raises the resting-state Fe(III)-to-Fe(II) reduction potential and substantially improves NAD(P)H-driven activity.read more
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Directed evolution of cytochrome c for carbon–silicon bond formation: Bringing silicon to life
TL;DR: It is discovered that heme proteins catalyze the formation of organosilicon compounds under physiological conditions via carbene insertion into silicon–hydrogen bonds, offering an environmentally friendly and highly efficient route to producing enantiopure organosILicon molecules.
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Expanding the Enzyme Universe: Accessing Non‐Natural Reactions by Mechanism‐Guided Directed Evolution
TL;DR: An evolutionary approach to engineering enzymes to catalyze reactions not found in nature to create new catalysts is outlined, with an emphasis on reactions that do not have natural counterparts.
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Engineering new catalytic activities in enzymes
Kai Chen,Frances H. Arnold +1 more
TL;DR: This Review outlines the ways that enzymes have been engineered to achieve reactivities well beyond their original functions and identifies genetically encoded catalysts that can be tuned and diversified by engineering the protein sequence.
Journal ArticleDOI
Protein design: toward functional metalloenzymes.
Fangting Yu,Virginia M. Cangelosi,Melissa L. Zastrow,Matteo Tegoni,Jefferson S. Plegaria,Alison G. Tebo,Catherine S. Mocny,Leela Ruckthong,Hira Qayyum,Vincent L. Pecoraro +9 more
TL;DR: De Novo Designed Functional Metalloproteins: The Grail Quest of Protein Design AX 3.2.1.
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Cytochromes P450 as promising catalysts for biotechnological application: chances and limitations.
Rita Bernhardt,Vlada B. Urlacher +1 more
TL;DR: A critical overview about possibilities and chances for application of these interesting catalysts as well as to discuss drawbacks and problems related to their use are given.
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