Enzymatic Nanoreactors for Environmentally Benign Biotransformations. 1. Formation and Catalytic Activity of Supramolecular Complexes of Laccase and Linear−Dendritic Block Copolymers
We describe the construction of enzymatic nanoreactors through noncovalent envelopment of a glycoprotein by amphiphilic linear−dendritic AB or ABA copolymers. The synthetic procedure is based on the regioselective adsorption of dendritic poly(benzyl ether)-block-linear poly(ethylene glycol)-block-de...
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| Veröffentlicht in: | Biomacromolecules 2008-03, Vol.9 (3), p.804-811 |
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| container_title | Biomacromolecules |
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| creator | Gitsov, Ivan Hamzik, James Ryan, Joseph Simonyan, Arsen Nakas, James P Omori, Shigetoshi Krastanov, Albert Cohen, Tomer Tanenbaum, Stuart W |
| description | We describe the construction of enzymatic nanoreactors through noncovalent envelopment of a glycoprotein by amphiphilic linear−dendritic AB or ABA copolymers. The synthetic procedure is based on the regioselective adsorption of dendritic poly(benzyl ether)-block-linear poly(ethylene glycol)-block-dendritic poly(benzyl ether) or linear poly(ethylene oxide)-block-dendritic poly(benzyl ether) copolymers onto the oxidative enzyme laccase from Trametes versicolor in aqueous medium. The complexes formed have improved catalytic activity compared with the native enzyme (77–85 nkat/mL vs 60 nkat/mL, respectively) and are more stable at elevated temperatures up to 70 °C. Experiments with deglycosylated laccase confirm that the glycoside fragments in the native enzyme serve as the anchor sites for the linear−dendritic copolymers. The enzymatic nanoreactors are able to effectively oxidize series of substrates: phenolic compounds (syringaldazine) and hydrophobic polyaromatic hydrocarbons (anthracene and benzo[a]pyrene) under “green” chemistry conditions. |
| doi_str_mv | 10.1021/bm701081m |
| format | Article |
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Formation and Catalytic Activity of Supramolecular Complexes of Laccase and Linear−Dendritic Block Copolymers</title><source>MEDLINE</source><source>ACS Publications</source><creator>Gitsov, Ivan ; Hamzik, James ; Ryan, Joseph ; Simonyan, Arsen ; Nakas, James P ; Omori, Shigetoshi ; Krastanov, Albert ; Cohen, Tomer ; Tanenbaum, Stuart W</creator><creatorcontrib>Gitsov, Ivan ; Hamzik, James ; Ryan, Joseph ; Simonyan, Arsen ; Nakas, James P ; Omori, Shigetoshi ; Krastanov, Albert ; Cohen, Tomer ; Tanenbaum, Stuart W</creatorcontrib><description>We describe the construction of enzymatic nanoreactors through noncovalent envelopment of a glycoprotein by amphiphilic linear−dendritic AB or ABA copolymers. The synthetic procedure is based on the regioselective adsorption of dendritic poly(benzyl ether)-block-linear poly(ethylene glycol)-block-dendritic poly(benzyl ether) or linear poly(ethylene oxide)-block-dendritic poly(benzyl ether) copolymers onto the oxidative enzyme laccase from Trametes versicolor in aqueous medium. The complexes formed have improved catalytic activity compared with the native enzyme (77–85 nkat/mL vs 60 nkat/mL, respectively) and are more stable at elevated temperatures up to 70 °C. Experiments with deglycosylated laccase confirm that the glycoside fragments in the native enzyme serve as the anchor sites for the linear−dendritic copolymers. The enzymatic nanoreactors are able to effectively oxidize series of substrates: phenolic compounds (syringaldazine) and hydrophobic polyaromatic hydrocarbons (anthracene and benzo[a]pyrene) under “green” chemistry conditions.</description><identifier>ISSN: 1525-7797</identifier><identifier>EISSN: 1526-4602</identifier><identifier>DOI: 10.1021/bm701081m</identifier><identifier>PMID: 18257555</identifier><language>eng</language><publisher>Washington, DC: American Chemical Society</publisher><subject>Applied sciences ; Biodegradation, Environmental ; Bioreactors ; Catalysis ; Dendrimers - chemical synthesis ; Dendrimers - chemistry ; Exact sciences and technology ; Glycoproteins - chemistry ; Laccase - chemistry ; Nanotechnology - methods ; Organic polymers ; Oxidation-Reduction ; Phenols - metabolism ; Physicochemistry of polymers ; Polycyclic Aromatic Hydrocarbons - metabolism ; Polyethylene Glycols - chemistry ; Polyporales - enzymology ; Properties and characterization ; Special properties (catalyst, reagent or carrier) ; Trametes versicolor</subject><ispartof>Biomacromolecules, 2008-03, Vol.9 (3), p.804-811</ispartof><rights>Copyright © 2008 American Chemical Society</rights><rights>2008 INIST-CNRS</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a375t-e13dba41052eba47a25a3b953bb39b0ccadaf5d00ac69c7c1ff17760aa373dd73</citedby><cites>FETCH-LOGICAL-a375t-e13dba41052eba47a25a3b953bb39b0ccadaf5d00ac69c7c1ff17760aa373dd73</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/bm701081m$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/bm701081m$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,780,784,2765,27076,27924,27925,56738,56788</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=20190040$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/18257555$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Gitsov, Ivan</creatorcontrib><creatorcontrib>Hamzik, James</creatorcontrib><creatorcontrib>Ryan, Joseph</creatorcontrib><creatorcontrib>Simonyan, Arsen</creatorcontrib><creatorcontrib>Nakas, James P</creatorcontrib><creatorcontrib>Omori, Shigetoshi</creatorcontrib><creatorcontrib>Krastanov, Albert</creatorcontrib><creatorcontrib>Cohen, Tomer</creatorcontrib><creatorcontrib>Tanenbaum, Stuart W</creatorcontrib><title>Enzymatic Nanoreactors for Environmentally Benign Biotransformations. 1. Formation and Catalytic Activity of Supramolecular Complexes of Laccase and Linear−Dendritic Block Copolymers</title><title>Biomacromolecules</title><addtitle>Biomacromolecules</addtitle><description>We describe the construction of enzymatic nanoreactors through noncovalent envelopment of a glycoprotein by amphiphilic linear−dendritic AB or ABA copolymers. The synthetic procedure is based on the regioselective adsorption of dendritic poly(benzyl ether)-block-linear poly(ethylene glycol)-block-dendritic poly(benzyl ether) or linear poly(ethylene oxide)-block-dendritic poly(benzyl ether) copolymers onto the oxidative enzyme laccase from Trametes versicolor in aqueous medium. The complexes formed have improved catalytic activity compared with the native enzyme (77–85 nkat/mL vs 60 nkat/mL, respectively) and are more stable at elevated temperatures up to 70 °C. Experiments with deglycosylated laccase confirm that the glycoside fragments in the native enzyme serve as the anchor sites for the linear−dendritic copolymers. The enzymatic nanoreactors are able to effectively oxidize series of substrates: phenolic compounds (syringaldazine) and hydrophobic polyaromatic hydrocarbons (anthracene and benzo[a]pyrene) under “green” chemistry conditions.</description><subject>Applied sciences</subject><subject>Biodegradation, Environmental</subject><subject>Bioreactors</subject><subject>Catalysis</subject><subject>Dendrimers - chemical synthesis</subject><subject>Dendrimers - chemistry</subject><subject>Exact sciences and technology</subject><subject>Glycoproteins - chemistry</subject><subject>Laccase - chemistry</subject><subject>Nanotechnology - methods</subject><subject>Organic polymers</subject><subject>Oxidation-Reduction</subject><subject>Phenols - metabolism</subject><subject>Physicochemistry of polymers</subject><subject>Polycyclic Aromatic Hydrocarbons - metabolism</subject><subject>Polyethylene Glycols - chemistry</subject><subject>Polyporales - enzymology</subject><subject>Properties and characterization</subject><subject>Special properties (catalyst, reagent or carrier)</subject><subject>Trametes versicolor</subject><issn>1525-7797</issn><issn>1526-4602</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2008</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNptkc9u1DAQxi0EoqVw4AWQLwhxyDKO4_Xm2F22gLSCA3COJo6DXPwn2ElFeALOPA3Pw5PgtEt74TQzmt_3jTQfIU8ZrBiU7FXrJDDYMHePnDJRrotqDeX9614UUtbyhDxK6RIAal6Jh-SEbUohhRCn5Pfe_5gdjkbR9-hD1KjGEBPtQ6R7f2Vi8E77Ea2d6VZ788XTrQljRJ8ysgiDTyvKVvTi30jRd3SHWTMvtudqNFdmnGno6cdpiOiC1WqyGOkuuMHq7zotuwMqhUlfqw_Ga4x_fv56rX0XzWKztUF9zYoh2NnpmB6TBz3apJ8c6xn5fLH_tHtbHD68ebc7PxTIpRgLzXjXYsVAlDpXiaVA3taCty2vW8gnO-xFB4BqXSupWN8zKdeAWc67TvIz8uLGd4jh26TT2DiTlLYWvQ5TaqSoRLUB4Jl8eUOqGFKKum-GaBzGuWHQLDk1tzll9tnRdWqd7u7IYzAZeH4EMCm0fX64MumWK4HVABXccahScxmm6PMz_nPwL2U5rJI</recordid><startdate>20080301</startdate><enddate>20080301</enddate><creator>Gitsov, Ivan</creator><creator>Hamzik, James</creator><creator>Ryan, Joseph</creator><creator>Simonyan, Arsen</creator><creator>Nakas, James P</creator><creator>Omori, Shigetoshi</creator><creator>Krastanov, Albert</creator><creator>Cohen, Tomer</creator><creator>Tanenbaum, Stuart W</creator><general>American Chemical Society</general><scope>IQODW</scope><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>7QO</scope><scope>8FD</scope><scope>FR3</scope><scope>P64</scope></search><sort><creationdate>20080301</creationdate><title>Enzymatic Nanoreactors for Environmentally Benign Biotransformations. 1. Formation and Catalytic Activity of Supramolecular Complexes of Laccase and Linear−Dendritic Block Copolymers</title><author>Gitsov, Ivan ; Hamzik, James ; Ryan, Joseph ; Simonyan, Arsen ; Nakas, James P ; Omori, Shigetoshi ; Krastanov, Albert ; Cohen, Tomer ; Tanenbaum, Stuart W</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a375t-e13dba41052eba47a25a3b953bb39b0ccadaf5d00ac69c7c1ff17760aa373dd73</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2008</creationdate><topic>Applied sciences</topic><topic>Biodegradation, Environmental</topic><topic>Bioreactors</topic><topic>Catalysis</topic><topic>Dendrimers - chemical synthesis</topic><topic>Dendrimers - chemistry</topic><topic>Exact sciences and technology</topic><topic>Glycoproteins - chemistry</topic><topic>Laccase - chemistry</topic><topic>Nanotechnology - methods</topic><topic>Organic polymers</topic><topic>Oxidation-Reduction</topic><topic>Phenols - metabolism</topic><topic>Physicochemistry of polymers</topic><topic>Polycyclic Aromatic Hydrocarbons - metabolism</topic><topic>Polyethylene Glycols - chemistry</topic><topic>Polyporales - enzymology</topic><topic>Properties and characterization</topic><topic>Special properties (catalyst, reagent or carrier)</topic><topic>Trametes versicolor</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Gitsov, Ivan</creatorcontrib><creatorcontrib>Hamzik, James</creatorcontrib><creatorcontrib>Ryan, Joseph</creatorcontrib><creatorcontrib>Simonyan, Arsen</creatorcontrib><creatorcontrib>Nakas, James P</creatorcontrib><creatorcontrib>Omori, Shigetoshi</creatorcontrib><creatorcontrib>Krastanov, Albert</creatorcontrib><creatorcontrib>Cohen, Tomer</creatorcontrib><creatorcontrib>Tanenbaum, Stuart W</creatorcontrib><collection>Pascal-Francis</collection><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>Biotechnology Research Abstracts</collection><collection>Technology Research Database</collection><collection>Engineering Research Database</collection><collection>Biotechnology and BioEngineering Abstracts</collection><jtitle>Biomacromolecules</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Gitsov, Ivan</au><au>Hamzik, James</au><au>Ryan, Joseph</au><au>Simonyan, Arsen</au><au>Nakas, James P</au><au>Omori, Shigetoshi</au><au>Krastanov, Albert</au><au>Cohen, Tomer</au><au>Tanenbaum, Stuart W</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Enzymatic Nanoreactors for Environmentally Benign Biotransformations. 1. Formation and Catalytic Activity of Supramolecular Complexes of Laccase and Linear−Dendritic Block Copolymers</atitle><jtitle>Biomacromolecules</jtitle><addtitle>Biomacromolecules</addtitle><date>2008-03-01</date><risdate>2008</risdate><volume>9</volume><issue>3</issue><spage>804</spage><epage>811</epage><pages>804-811</pages><issn>1525-7797</issn><eissn>1526-4602</eissn><abstract>We describe the construction of enzymatic nanoreactors through noncovalent envelopment of a glycoprotein by amphiphilic linear−dendritic AB or ABA copolymers. The synthetic procedure is based on the regioselective adsorption of dendritic poly(benzyl ether)-block-linear poly(ethylene glycol)-block-dendritic poly(benzyl ether) or linear poly(ethylene oxide)-block-dendritic poly(benzyl ether) copolymers onto the oxidative enzyme laccase from Trametes versicolor in aqueous medium. The complexes formed have improved catalytic activity compared with the native enzyme (77–85 nkat/mL vs 60 nkat/mL, respectively) and are more stable at elevated temperatures up to 70 °C. Experiments with deglycosylated laccase confirm that the glycoside fragments in the native enzyme serve as the anchor sites for the linear−dendritic copolymers. The enzymatic nanoreactors are able to effectively oxidize series of substrates: phenolic compounds (syringaldazine) and hydrophobic polyaromatic hydrocarbons (anthracene and benzo[a]pyrene) under “green” chemistry conditions.</abstract><cop>Washington, DC</cop><pub>American Chemical Society</pub><pmid>18257555</pmid><doi>10.1021/bm701081m</doi><tpages>8</tpages></addata></record> |
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| ispartof | Biomacromolecules, 2008-03, Vol.9 (3), p.804-811 |
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| subjects | Applied sciences Biodegradation, Environmental Bioreactors Catalysis Dendrimers - chemical synthesis Dendrimers - chemistry Exact sciences and technology Glycoproteins - chemistry Laccase - chemistry Nanotechnology - methods Organic polymers Oxidation-Reduction Phenols - metabolism Physicochemistry of polymers Polycyclic Aromatic Hydrocarbons - metabolism Polyethylene Glycols - chemistry Polyporales - enzymology Properties and characterization Special properties (catalyst, reagent or carrier) Trametes versicolor |
| title | Enzymatic Nanoreactors for Environmentally Benign Biotransformations. 1. Formation and Catalytic Activity of Supramolecular Complexes of Laccase and Linear−Dendritic Block Copolymers |
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