Directed evolution of enzymatic silicon-carbon bond cleavage in siloxanes

Volatile methylsiloxanes (VMS) are man-made, nonbiodegradable chemicals produced at a megaton-per-year scale, which leads to concern over their potential for environmental persistence, long-range transport, and bioaccumulation. We used directed evolution to engineer a variant of bacterial cytochrome...

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Veröffentlicht in:Science (American Association for the Advancement of Science) 2024-01, Vol.383 (6681), p.438-443
Hauptverfasser: Sarai, Nicholas S, Fulton, Tyler J, O'Meara, Ryen L, Johnston, Kadina E, Brinkmann-Chen, Sabine, Maar, Ryan R, Tecklenburg, Ron E, Roberts, John M, Reddel, Jordan C T, Katsoulis, Dimitris E, Arnold, Frances H
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Sprache:eng
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Zusammenfassung:Volatile methylsiloxanes (VMS) are man-made, nonbiodegradable chemicals produced at a megaton-per-year scale, which leads to concern over their potential for environmental persistence, long-range transport, and bioaccumulation. We used directed evolution to engineer a variant of bacterial cytochrome P450 to break silicon-carbon bonds in linear and cyclic VMS. To accomplish silicon-carbon bond cleavage, the enzyme catalyzes two tandem oxidations of a siloxane methyl group, which is followed by putative [1,2]-Brook rearrangement and hydrolysis. Discovery of this so-called siloxane oxidase opens possibilities for the eventual biodegradation of VMS.
ISSN:0036-8075
1095-9203
DOI:10.1126/science.adi5554