Enhancing the Photocatalytic Conversion of Pt(IV) Substrates by Flavoprotein Engineering
Our recent work demonstrates that certain flavoproteins can catalyze the redox activation of Pt(IV) prodrug complexes under light irradiation. Herein, we used site-directed mutagenesis on the mini singlet oxygen generator (mSOG) to modulate the photocatalytic activity of this flavoprotein toward tw...
Gespeichert in:
Veröffentlicht in: | The journal of physical chemistry letters 2021-05, Vol.12 (19), p.4504-4508 |
---|---|
Hauptverfasser: | , , , , , , , |
Format: | Artikel |
Sprache: | eng |
Schlagworte: | |
Online-Zugang: | Volltext |
Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
container_end_page | 4508 |
---|---|
container_issue | 19 |
container_start_page | 4504 |
container_title | The journal of physical chemistry letters |
container_volume | 12 |
creator | Gurruchaga-Pereda, Juan Martínez-Martínez, Virginia Formoso, Elena Azpitarte, Oksana Rezabal, Elixabete Lopez, Xabier Cortajarena, Aitziber L Salassa, Luca |
description | Our recent work demonstrates that certain flavoproteins can catalyze the redox activation of Pt(IV) prodrug complexes under light irradiation. Herein, we used site-directed mutagenesis on the mini singlet oxygen generator (mSOG) to modulate the photocatalytic activity of this flavoprotein toward two model Pt(IV) substrates. Among the prepared mutants, Q103V mSOG displayed enhanced catalytic efficiency as a result of its longer triplet excited-state lifetime. This study shows, for the first time, that protein engineering can improve the catalytic capacity of a protein toward metal-containing substrates. |
doi_str_mv | 10.1021/acs.jpclett.1c00802 |
format | Article |
fullrecord | <record><control><sourceid>acs_cross</sourceid><recordid>TN_cdi_crossref_primary_10_1021_acs_jpclett_1c00802</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>h00874863</sourcerecordid><originalsourceid>FETCH-LOGICAL-a390t-afe06faeb33884d2a034e79d0d125e3edd29ccf4d0ba7e8f8f97060a6e32c1c13</originalsourceid><addsrcrecordid>eNp9kF1LwzAUhoMobk5_gSC51IvOk6Zr00sZmw4GDvzAu5KmJ1tHl5QkG-zfW90Ur7w678X7vHAeQq4ZDBnE7F4qP1y3qsEQhkwBCIhPSJ_liYgyJkanf3KPXHi_BkhzENk56XGep5DlWZ98TMxKGlWbJQ0rpIuVDVbJIJt9qBUdW7ND52trqNV0EW5n73f0ZVv64GRAT8s9nTZyZ1tnA9aGTsyyNoium7skZ1o2Hq-Od0DeppPX8VM0f36cjR_mkeQ5hEhqhFRLLDkXIqliCTzBLK-gYvEIOVZVnCulkwpKmaHQQucZpCBT5LFiivEB4Ydd5az3DnXRunoj3b5gUHx5KjpPxdFTcfTUUTcHqt2WG6x-mR8xXeH-UPim7daZ7ol_Jz8BLVF4_Q</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype></control><display><type>article</type><title>Enhancing the Photocatalytic Conversion of Pt(IV) Substrates by Flavoprotein Engineering</title><source>ACS Publications</source><creator>Gurruchaga-Pereda, Juan ; Martínez-Martínez, Virginia ; Formoso, Elena ; Azpitarte, Oksana ; Rezabal, Elixabete ; Lopez, Xabier ; Cortajarena, Aitziber L ; Salassa, Luca</creator><creatorcontrib>Gurruchaga-Pereda, Juan ; Martínez-Martínez, Virginia ; Formoso, Elena ; Azpitarte, Oksana ; Rezabal, Elixabete ; Lopez, Xabier ; Cortajarena, Aitziber L ; Salassa, Luca</creatorcontrib><description>Our recent work demonstrates that certain flavoproteins can catalyze the redox activation of Pt(IV) prodrug complexes under light irradiation. Herein, we used site-directed mutagenesis on the mini singlet oxygen generator (mSOG) to modulate the photocatalytic activity of this flavoprotein toward two model Pt(IV) substrates. Among the prepared mutants, Q103V mSOG displayed enhanced catalytic efficiency as a result of its longer triplet excited-state lifetime. This study shows, for the first time, that protein engineering can improve the catalytic capacity of a protein toward metal-containing substrates.</description><identifier>ISSN: 1948-7185</identifier><identifier>EISSN: 1948-7185</identifier><identifier>DOI: 10.1021/acs.jpclett.1c00802</identifier><identifier>PMID: 33960797</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>Physical Insights into Chemistry, Catalysis, and Interfaces</subject><ispartof>The journal of physical chemistry letters, 2021-05, Vol.12 (19), p.4504-4508</ispartof><rights>2021 American Chemical Society</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a390t-afe06faeb33884d2a034e79d0d125e3edd29ccf4d0ba7e8f8f97060a6e32c1c13</citedby><cites>FETCH-LOGICAL-a390t-afe06faeb33884d2a034e79d0d125e3edd29ccf4d0ba7e8f8f97060a6e32c1c13</cites><orcidid>0000-0003-0397-6140 ; 0000-0002-5331-114X ; 0000-0002-2112-9095 ; 0000-0002-7106-3717</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.1c00802$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.jpclett.1c00802$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,778,782,2754,27063,27911,27912,56725,56775</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/33960797$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Gurruchaga-Pereda, Juan</creatorcontrib><creatorcontrib>Martínez-Martínez, Virginia</creatorcontrib><creatorcontrib>Formoso, Elena</creatorcontrib><creatorcontrib>Azpitarte, Oksana</creatorcontrib><creatorcontrib>Rezabal, Elixabete</creatorcontrib><creatorcontrib>Lopez, Xabier</creatorcontrib><creatorcontrib>Cortajarena, Aitziber L</creatorcontrib><creatorcontrib>Salassa, Luca</creatorcontrib><title>Enhancing the Photocatalytic Conversion of Pt(IV) Substrates by Flavoprotein Engineering</title><title>The journal of physical chemistry letters</title><addtitle>J. Phys. Chem. Lett</addtitle><description>Our recent work demonstrates that certain flavoproteins can catalyze the redox activation of Pt(IV) prodrug complexes under light irradiation. Herein, we used site-directed mutagenesis on the mini singlet oxygen generator (mSOG) to modulate the photocatalytic activity of this flavoprotein toward two model Pt(IV) substrates. Among the prepared mutants, Q103V mSOG displayed enhanced catalytic efficiency as a result of its longer triplet excited-state lifetime. This study shows, for the first time, that protein engineering can improve the catalytic capacity of a protein toward metal-containing substrates.</description><subject>Physical Insights into Chemistry, Catalysis, and Interfaces</subject><issn>1948-7185</issn><issn>1948-7185</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNp9kF1LwzAUhoMobk5_gSC51IvOk6Zr00sZmw4GDvzAu5KmJ1tHl5QkG-zfW90Ur7w678X7vHAeQq4ZDBnE7F4qP1y3qsEQhkwBCIhPSJ_liYgyJkanf3KPXHi_BkhzENk56XGep5DlWZ98TMxKGlWbJQ0rpIuVDVbJIJt9qBUdW7ND52trqNV0EW5n73f0ZVv64GRAT8s9nTZyZ1tnA9aGTsyyNoium7skZ1o2Hq-Od0DeppPX8VM0f36cjR_mkeQ5hEhqhFRLLDkXIqliCTzBLK-gYvEIOVZVnCulkwpKmaHQQucZpCBT5LFiivEB4Ydd5az3DnXRunoj3b5gUHx5KjpPxdFTcfTUUTcHqt2WG6x-mR8xXeH-UPim7daZ7ol_Jz8BLVF4_Q</recordid><startdate>20210520</startdate><enddate>20210520</enddate><creator>Gurruchaga-Pereda, Juan</creator><creator>Martínez-Martínez, Virginia</creator><creator>Formoso, Elena</creator><creator>Azpitarte, Oksana</creator><creator>Rezabal, Elixabete</creator><creator>Lopez, Xabier</creator><creator>Cortajarena, Aitziber L</creator><creator>Salassa, Luca</creator><general>American Chemical Society</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><orcidid>https://orcid.org/0000-0003-0397-6140</orcidid><orcidid>https://orcid.org/0000-0002-5331-114X</orcidid><orcidid>https://orcid.org/0000-0002-2112-9095</orcidid><orcidid>https://orcid.org/0000-0002-7106-3717</orcidid></search><sort><creationdate>20210520</creationdate><title>Enhancing the Photocatalytic Conversion of Pt(IV) Substrates by Flavoprotein Engineering</title><author>Gurruchaga-Pereda, Juan ; Martínez-Martínez, Virginia ; Formoso, Elena ; Azpitarte, Oksana ; Rezabal, Elixabete ; Lopez, Xabier ; Cortajarena, Aitziber L ; Salassa, Luca</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a390t-afe06faeb33884d2a034e79d0d125e3edd29ccf4d0ba7e8f8f97060a6e32c1c13</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Physical Insights into Chemistry, Catalysis, and Interfaces</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Gurruchaga-Pereda, Juan</creatorcontrib><creatorcontrib>Martínez-Martínez, Virginia</creatorcontrib><creatorcontrib>Formoso, Elena</creatorcontrib><creatorcontrib>Azpitarte, Oksana</creatorcontrib><creatorcontrib>Rezabal, Elixabete</creatorcontrib><creatorcontrib>Lopez, Xabier</creatorcontrib><creatorcontrib>Cortajarena, Aitziber L</creatorcontrib><creatorcontrib>Salassa, Luca</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><jtitle>The journal of physical chemistry letters</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Gurruchaga-Pereda, Juan</au><au>Martínez-Martínez, Virginia</au><au>Formoso, Elena</au><au>Azpitarte, Oksana</au><au>Rezabal, Elixabete</au><au>Lopez, Xabier</au><au>Cortajarena, Aitziber L</au><au>Salassa, Luca</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Enhancing the Photocatalytic Conversion of Pt(IV) Substrates by Flavoprotein Engineering</atitle><jtitle>The journal of physical chemistry letters</jtitle><addtitle>J. Phys. Chem. Lett</addtitle><date>2021-05-20</date><risdate>2021</risdate><volume>12</volume><issue>19</issue><spage>4504</spage><epage>4508</epage><pages>4504-4508</pages><issn>1948-7185</issn><eissn>1948-7185</eissn><abstract>Our recent work demonstrates that certain flavoproteins can catalyze the redox activation of Pt(IV) prodrug complexes under light irradiation. Herein, we used site-directed mutagenesis on the mini singlet oxygen generator (mSOG) to modulate the photocatalytic activity of this flavoprotein toward two model Pt(IV) substrates. Among the prepared mutants, Q103V mSOG displayed enhanced catalytic efficiency as a result of its longer triplet excited-state lifetime. This study shows, for the first time, that protein engineering can improve the catalytic capacity of a protein toward metal-containing substrates.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>33960797</pmid><doi>10.1021/acs.jpclett.1c00802</doi><tpages>5</tpages><orcidid>https://orcid.org/0000-0003-0397-6140</orcidid><orcidid>https://orcid.org/0000-0002-5331-114X</orcidid><orcidid>https://orcid.org/0000-0002-2112-9095</orcidid><orcidid>https://orcid.org/0000-0002-7106-3717</orcidid><oa>free_for_read</oa></addata></record> |
fulltext | fulltext |
identifier | ISSN: 1948-7185 |
ispartof | The journal of physical chemistry letters, 2021-05, Vol.12 (19), p.4504-4508 |
issn | 1948-7185 1948-7185 |
language | eng |
recordid | cdi_crossref_primary_10_1021_acs_jpclett_1c00802 |
source | ACS Publications |
subjects | Physical Insights into Chemistry, Catalysis, and Interfaces |
title | Enhancing the Photocatalytic Conversion of Pt(IV) Substrates by Flavoprotein Engineering |
url | https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2025-01-16T03%3A08%3A21IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-acs_cross&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Enhancing%20the%20Photocatalytic%20Conversion%20of%20Pt(IV)%20Substrates%20by%20Flavoprotein%20Engineering&rft.jtitle=The%20journal%20of%20physical%20chemistry%20letters&rft.au=Gurruchaga-Pereda,%20Juan&rft.date=2021-05-20&rft.volume=12&rft.issue=19&rft.spage=4504&rft.epage=4508&rft.pages=4504-4508&rft.issn=1948-7185&rft.eissn=1948-7185&rft_id=info:doi/10.1021/acs.jpclett.1c00802&rft_dat=%3Cacs_cross%3Eh00874863%3C/acs_cross%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_id=info:pmid/33960797&rfr_iscdi=true |