Autocatalytic effect boosts the production of medium-chain hydrocarbons by fatty acid photodecarboxylase
Ongoing climate change is driving the search for renewable and carbon-neutral alternatives to fossil fuels. Photocatalytic conversion of fatty acids to hydrocarbons by fatty acid photodecarboxylase (FAP) represents a promising route to green fuels. However, the alleged low activity of FAP on C2 to C...
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| Veröffentlicht in: | Science advances 2023-03, Vol.9 (13), p.eadg3881 |
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| creator | Samire, Poutoum P Zhuang, Bo Légeret, Bertrand Baca-Porcel, Ángel Peltier, Gilles Sorigué, Damien Aleksandrov, Alexey Beisson, Frédéric Müller, Pavel |
| description | Ongoing climate change is driving the search for renewable and carbon-neutral alternatives to fossil fuels. Photocatalytic conversion of fatty acids to hydrocarbons by fatty acid photodecarboxylase (FAP) represents a promising route to green fuels. However, the alleged low activity of FAP on C2 to C12 fatty acids seemed to preclude the use for synthesis of gasoline-range hydrocarbons. Here, we reveal that
FAP (
FAP) can convert
-octanoic acid in vitro four times faster than
-hexadecanoic acid, its best substrate reported to date. In vivo, this translates into a
FAP-based production rate over 10-fold higher for
-heptane than for
-pentadecane. Time-resolved spectroscopy and molecular modeling demonstrate that
FAP's high catalytic activity on
-octanoic acid is, in part, due to an autocatalytic effect of its
-heptane product, which fills the rest of the binding pocket. These results represent an important step toward a bio-based and light-driven production of gasoline-like hydrocarbons. |
| doi_str_mv | 10.1126/sciadv.adg3881 |
| format | Article |
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FAP (
FAP) can convert
-octanoic acid in vitro four times faster than
-hexadecanoic acid, its best substrate reported to date. In vivo, this translates into a
FAP-based production rate over 10-fold higher for
-heptane than for
-pentadecane. Time-resolved spectroscopy and molecular modeling demonstrate that
FAP's high catalytic activity on
-octanoic acid is, in part, due to an autocatalytic effect of its
-heptane product, which fills the rest of the binding pocket. These results represent an important step toward a bio-based and light-driven production of gasoline-like hydrocarbons.</description><identifier>ISSN: 2375-2548</identifier><identifier>EISSN: 2375-2548</identifier><identifier>DOI: 10.1126/sciadv.adg3881</identifier><identifier>PMID: 37000872</identifier><language>eng</language><publisher>United States: American Association for the Advancement of Science (AAAS)</publisher><subject>Biochemistry ; Biochemistry, Molecular Biology ; Biophysics ; Caprylates - metabolism ; Catalysis ; Chemical Sciences ; Chlorella - metabolism ; Fatty Acids - metabolism ; Gasoline ; Hydrocarbons ; Life Sciences ; Physical and Materials Sciences ; SciAdv r-articles</subject><ispartof>Science advances, 2023-03, Vol.9 (13), p.eadg3881</ispartof><rights>Distributed under a Creative Commons Attribution 4.0 International License</rights><rights>Copyright © 2023 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution License 4.0 (CC BY). 2023 The Authors</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c425t-a0543f8473730cdc9aa98d995dfbc0f0bbb194cf355e38cd335766d58075a8e73</citedby><cites>FETCH-LOGICAL-c425t-a0543f8473730cdc9aa98d995dfbc0f0bbb194cf355e38cd335766d58075a8e73</cites><orcidid>0000-0002-2226-3931 ; 0000-0001-9995-7387 ; 0000-0003-1555-6266 ; 0000-0002-3245-0810 ; 0000-0002-0957-4700 ; 0000-0002-9906-1190 ; 0000-0002-8150-3931 ; 0000-0003-4572-9666</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC10065435/pdf/$$EPDF$$P50$$Gpubmedcentral$$Hfree_for_read</linktopdf><linktohtml>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC10065435/$$EHTML$$P50$$Gpubmedcentral$$Hfree_for_read</linktohtml><link.rule.ids>230,314,723,776,780,860,881,27901,27902,53766,53768</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/37000872$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://hal.science/hal-04055084$$DView record in HAL$$Hfree_for_read</backlink></links><search><creatorcontrib>Samire, Poutoum P</creatorcontrib><creatorcontrib>Zhuang, Bo</creatorcontrib><creatorcontrib>Légeret, Bertrand</creatorcontrib><creatorcontrib>Baca-Porcel, Ángel</creatorcontrib><creatorcontrib>Peltier, Gilles</creatorcontrib><creatorcontrib>Sorigué, Damien</creatorcontrib><creatorcontrib>Aleksandrov, Alexey</creatorcontrib><creatorcontrib>Beisson, Frédéric</creatorcontrib><creatorcontrib>Müller, Pavel</creatorcontrib><title>Autocatalytic effect boosts the production of medium-chain hydrocarbons by fatty acid photodecarboxylase</title><title>Science advances</title><addtitle>Sci Adv</addtitle><description>Ongoing climate change is driving the search for renewable and carbon-neutral alternatives to fossil fuels. Photocatalytic conversion of fatty acids to hydrocarbons by fatty acid photodecarboxylase (FAP) represents a promising route to green fuels. However, the alleged low activity of FAP on C2 to C12 fatty acids seemed to preclude the use for synthesis of gasoline-range hydrocarbons. Here, we reveal that
FAP (
FAP) can convert
-octanoic acid in vitro four times faster than
-hexadecanoic acid, its best substrate reported to date. In vivo, this translates into a
FAP-based production rate over 10-fold higher for
-heptane than for
-pentadecane. Time-resolved spectroscopy and molecular modeling demonstrate that
FAP's high catalytic activity on
-octanoic acid is, in part, due to an autocatalytic effect of its
-heptane product, which fills the rest of the binding pocket. These results represent an important step toward a bio-based and light-driven production of gasoline-like hydrocarbons.</description><subject>Biochemistry</subject><subject>Biochemistry, Molecular Biology</subject><subject>Biophysics</subject><subject>Caprylates - metabolism</subject><subject>Catalysis</subject><subject>Chemical Sciences</subject><subject>Chlorella - metabolism</subject><subject>Fatty Acids - metabolism</subject><subject>Gasoline</subject><subject>Hydrocarbons</subject><subject>Life Sciences</subject><subject>Physical and Materials Sciences</subject><subject>SciAdv r-articles</subject><issn>2375-2548</issn><issn>2375-2548</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNpdUU1v1DAQtRCIVqVXjpWPcMhix3bsnNCqgrbSSlzgbE380Rhl463trJp_T5bdVm1P8_Xemxk9hD5TsqK0br5lE8DuV2DvmVL0HTqvmRRVLbh6_yI_Q5c5_yWEUN40grYf0RmTS6lkfY769VSigQLDXILBzntnCu5izCXj0ju8S9FOpoQ44ujx1tkwbSvTQxhxP9u0cFMXx4y7GXsoZcZggsW7PpZo3f_h4zxAdp_QBw9DdpeneIH-_Pzx-_q22vy6ubtebyrDa1EqIIIzr7hkkhFjTQvQKtu2wvrOEE-6rqMtN54J4ZgyljEhm8YKRaQA5SS7QN-PurupW641biwJBr1LYQtp1hGCfj0ZQ6_v415TQpplt1gUvh4V-je82_VGH3qEEyGI4nu6YL-ctqX4MLlc9DZk44YBRhenrGvZslZxxg6HrY5Qk2LOyflnbUr0wU59tFOf7FwIVy8_eYY_mcf-AdvRn9c</recordid><startdate>20230331</startdate><enddate>20230331</enddate><creator>Samire, Poutoum P</creator><creator>Zhuang, Bo</creator><creator>Légeret, Bertrand</creator><creator>Baca-Porcel, Ángel</creator><creator>Peltier, Gilles</creator><creator>Sorigué, Damien</creator><creator>Aleksandrov, Alexey</creator><creator>Beisson, Frédéric</creator><creator>Müller, Pavel</creator><general>American Association for the Advancement of Science (AAAS)</general><general>American Association for the Advancement of Science</general><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><scope>1XC</scope><scope>VOOES</scope><scope>5PM</scope><orcidid>https://orcid.org/0000-0002-2226-3931</orcidid><orcidid>https://orcid.org/0000-0001-9995-7387</orcidid><orcidid>https://orcid.org/0000-0003-1555-6266</orcidid><orcidid>https://orcid.org/0000-0002-3245-0810</orcidid><orcidid>https://orcid.org/0000-0002-0957-4700</orcidid><orcidid>https://orcid.org/0000-0002-9906-1190</orcidid><orcidid>https://orcid.org/0000-0002-8150-3931</orcidid><orcidid>https://orcid.org/0000-0003-4572-9666</orcidid></search><sort><creationdate>20230331</creationdate><title>Autocatalytic effect boosts the production of medium-chain hydrocarbons by fatty acid photodecarboxylase</title><author>Samire, Poutoum P ; 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FAP (
FAP) can convert
-octanoic acid in vitro four times faster than
-hexadecanoic acid, its best substrate reported to date. In vivo, this translates into a
FAP-based production rate over 10-fold higher for
-heptane than for
-pentadecane. Time-resolved spectroscopy and molecular modeling demonstrate that
FAP's high catalytic activity on
-octanoic acid is, in part, due to an autocatalytic effect of its
-heptane product, which fills the rest of the binding pocket. These results represent an important step toward a bio-based and light-driven production of gasoline-like hydrocarbons.</abstract><cop>United States</cop><pub>American Association for the Advancement of Science (AAAS)</pub><pmid>37000872</pmid><doi>10.1126/sciadv.adg3881</doi><orcidid>https://orcid.org/0000-0002-2226-3931</orcidid><orcidid>https://orcid.org/0000-0001-9995-7387</orcidid><orcidid>https://orcid.org/0000-0003-1555-6266</orcidid><orcidid>https://orcid.org/0000-0002-3245-0810</orcidid><orcidid>https://orcid.org/0000-0002-0957-4700</orcidid><orcidid>https://orcid.org/0000-0002-9906-1190</orcidid><orcidid>https://orcid.org/0000-0002-8150-3931</orcidid><orcidid>https://orcid.org/0000-0003-4572-9666</orcidid><oa>free_for_read</oa></addata></record> |
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| source | MEDLINE; DOAJ Directory of Open Access Journals; Elektronische Zeitschriftenbibliothek - Frei zugängliche E-Journals; PubMed Central |
| subjects | Biochemistry Biochemistry, Molecular Biology Biophysics Caprylates - metabolism Catalysis Chemical Sciences Chlorella - metabolism Fatty Acids - metabolism Gasoline Hydrocarbons Life Sciences Physical and Materials Sciences SciAdv r-articles |
| title | Autocatalytic effect boosts the production of medium-chain hydrocarbons by fatty acid photodecarboxylase |
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