Open Access
Open access
volume 383 issue 6681 pages 438-443

Directed evolution of enzymatic silicon-carbon bond cleavage in siloxanes

Nicholas S Sarai 1
Tyler J Fulton 1
Ryen L. O’Meara 1
Kadina E Johnston 2
Sabine Brinkmann Chen 1
Ryan R. Maar 3
Ron E. Tecklenburg 3
John M Roberts 3
Jordan C. T. Reddel 3
D.E Katsoulis 4
Frances Arnold 1
Publication typeJournal Article
Publication date2024-01-26
scimago Q1
wos Q1
SJR10.416
CiteScore48.4
Impact factor45.8
ISSN00368075, 10959203
Multidisciplinary
Abstract

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 BM3 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.

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GOST |
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GOST Copy
Sarai N. S. et al. Directed evolution of enzymatic silicon-carbon bond cleavage in siloxanes // Science. 2024. Vol. 383. No. 6681. pp. 438-443.
GOST all authors (up to 50) Copy
Sarai N. S., Fulton T. J., O’Meara R. L., Johnston K. E., Brinkmann Chen S., Maar R. R., Tecklenburg R. E., Roberts J. M., Reddel J. C. T., Katsoulis D., Arnold F. Directed evolution of enzymatic silicon-carbon bond cleavage in siloxanes // Science. 2024. Vol. 383. No. 6681. pp. 438-443.
RIS |
Cite this
RIS Copy
TY - JOUR
DO - 10.1126/science.adi5554
UR - https://doi.org/10.1126/science.adi5554
TI - Directed evolution of enzymatic silicon-carbon bond cleavage in siloxanes
T2 - Science
AU - Sarai, Nicholas S
AU - Fulton, Tyler J
AU - O’Meara, Ryen L.
AU - Johnston, Kadina E
AU - Brinkmann Chen, Sabine
AU - Maar, Ryan R.
AU - Tecklenburg, Ron E.
AU - Roberts, John M
AU - Reddel, Jordan C. T.
AU - Katsoulis, D.E
AU - Arnold, Frances
PY - 2024
DA - 2024/01/26
PB - American Association for the Advancement of Science (AAAS)
SP - 438-443
IS - 6681
VL - 383
PMID - 38271505
SN - 0036-8075
SN - 1095-9203
ER -
BibTex |
Cite this
BibTex (up to 50 authors) Copy
@article{2024_Sarai,
author = {Nicholas S Sarai and Tyler J Fulton and Ryen L. O’Meara and Kadina E Johnston and Sabine Brinkmann Chen and Ryan R. Maar and Ron E. Tecklenburg and John M Roberts and Jordan C. T. Reddel and D.E Katsoulis and Frances Arnold},
title = {Directed evolution of enzymatic silicon-carbon bond cleavage in siloxanes},
journal = {Science},
year = {2024},
volume = {383},
publisher = {American Association for the Advancement of Science (AAAS)},
month = {jan},
url = {https://doi.org/10.1126/science.adi5554},
number = {6681},
pages = {438--443},
doi = {10.1126/science.adi5554}
}
MLA
Cite this
MLA Copy
Sarai, Nicholas S., et al. “Directed evolution of enzymatic silicon-carbon bond cleavage in siloxanes.” Science, vol. 383, no. 6681, Jan. 2024, pp. 438-443. https://doi.org/10.1126/science.adi5554.