Encapsulation of Microperoxidase‑8 in MIL-101(Cr)‑X Nanoparticles: Influence of Metal–Organic Framework Functionalization on Enzymatic Immobilization and Catalytic Activity
Microperoxidase 8 (MP8) was immobilized within MIL-101(Cr) bearing terephthalate linkers with functionalized groups (-NH2 and -SO3H). A synthesis protocol for MIL-101(Cr)-SO3H that avoids the use of toxic Cr(VI) and HF was developed. The electrostatic interactions between the MP8 molecules and th...
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| Veröffentlicht in: | ACS applied nano materials 2020-04, Vol.3 (4), p.3233-3243 |
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| creator | Gkaniatsou, Effrosyni Ricoux, Rémy Kariyawasam, Kalani Stenger, Ingrid Fan, Benhui Ayoub, Narjès Salas, Samanta Patriarche, Gilles Serre, Christian Mahy, Jean-Pierre Steunou, Nathalie Sicard, Clémence |
| description | Microperoxidase 8 (MP8) was immobilized within MIL-101(Cr) bearing terephthalate linkers with functionalized groups (-NH2 and -SO3H). A synthesis protocol for MIL-101(Cr)-SO3H that avoids the use of toxic Cr(VI) and HF was developed. The electrostatic interactions between the MP8 molecules and the MOF matrices were found to be crucial for a successful immobilization. Raman spectroscopy revealed the dispersion of the immobilized MP8 molecules in MIL-101(Cr)-X matrices as monomers without aggregation. The presence of functional groups resulted in higher amounts of immobilized MP8 in comparison to the bare MIL-101(Cr). The catalytic activity of MP8@MIL-101(Cr)-NH2 per material mass was higher than that for MP8@MIL-101(Cr). The presence of free amino groups can thus improve the immobilization efficiency, leading to a higher amount of catalytically active species and improving the subsequent catalytic activity of the heterogeneous biocatalysts. MP8@MIL(Cr)-X also successfully catalyzed the selective oxidation of thioanisole derivatives into sulfoxides. |
| doi_str_mv | 10.1021/acsanm.9b02464 |
| format | Article |
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A synthesis protocol for MIL-101(Cr)-SO3H that avoids the use of toxic Cr(VI) and HF was developed. The electrostatic interactions between the MP8 molecules and the MOF matrices were found to be crucial for a successful immobilization. Raman spectroscopy revealed the dispersion of the immobilized MP8 molecules in MIL-101(Cr)-X matrices as monomers without aggregation. The presence of functional groups resulted in higher amounts of immobilized MP8 in comparison to the bare MIL-101(Cr). The catalytic activity of MP8@MIL-101(Cr)-NH2 per material mass was higher than that for MP8@MIL-101(Cr). The presence of free amino groups can thus improve the immobilization efficiency, leading to a higher amount of catalytically active species and improving the subsequent catalytic activity of the heterogeneous biocatalysts. MP8@MIL(Cr)-X also successfully catalyzed the selective oxidation of thioanisole derivatives into sulfoxides.</description><identifier>ISSN: 2574-0970</identifier><identifier>EISSN: 2574-0970</identifier><identifier>DOI: 10.1021/acsanm.9b02464</identifier><language>eng</language><publisher>American Chemical Society</publisher><subject>Catalysis ; Chemical Sciences ; Material chemistry</subject><ispartof>ACS applied nano materials, 2020-04, Vol.3 (4), p.3233-3243</ispartof><rights>Distributed under a Creative Commons Attribution 4.0 International License</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a348t-34fbb0dceb8b9f526f223666c24f402bea86035cb1aeeaedc38b1d868c27b7d63</citedby><cites>FETCH-LOGICAL-a348t-34fbb0dceb8b9f526f223666c24f402bea86035cb1aeeaedc38b1d868c27b7d63</cites><orcidid>0000-0002-7049-7388 ; 0000-0002-3464-7895 ; 0000-0003-3040-2564 ; 0000-0001-6502-7923 ; 0000-0002-3312-9025 ; 0000-0002-3917-2470</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/acsanm.9b02464$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acsanm.9b02464$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>230,314,776,780,881,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttps://hal.science/hal-02677097$$DView record in HAL$$Hfree_for_read</backlink></links><search><creatorcontrib>Gkaniatsou, Effrosyni</creatorcontrib><creatorcontrib>Ricoux, Rémy</creatorcontrib><creatorcontrib>Kariyawasam, Kalani</creatorcontrib><creatorcontrib>Stenger, Ingrid</creatorcontrib><creatorcontrib>Fan, Benhui</creatorcontrib><creatorcontrib>Ayoub, Narjès</creatorcontrib><creatorcontrib>Salas, Samanta</creatorcontrib><creatorcontrib>Patriarche, Gilles</creatorcontrib><creatorcontrib>Serre, Christian</creatorcontrib><creatorcontrib>Mahy, Jean-Pierre</creatorcontrib><creatorcontrib>Steunou, Nathalie</creatorcontrib><creatorcontrib>Sicard, Clémence</creatorcontrib><title>Encapsulation of Microperoxidase‑8 in MIL-101(Cr)‑X Nanoparticles: Influence of Metal–Organic Framework Functionalization on Enzymatic Immobilization and Catalytic Activity</title><title>ACS applied nano materials</title><addtitle>ACS Appl. Nano Mater</addtitle><description>Microperoxidase 8 (MP8) was immobilized within MIL-101(Cr) bearing terephthalate linkers with functionalized groups (-NH2 and -SO3H). A synthesis protocol for MIL-101(Cr)-SO3H that avoids the use of toxic Cr(VI) and HF was developed. The electrostatic interactions between the MP8 molecules and the MOF matrices were found to be crucial for a successful immobilization. Raman spectroscopy revealed the dispersion of the immobilized MP8 molecules in MIL-101(Cr)-X matrices as monomers without aggregation. The presence of functional groups resulted in higher amounts of immobilized MP8 in comparison to the bare MIL-101(Cr). The catalytic activity of MP8@MIL-101(Cr)-NH2 per material mass was higher than that for MP8@MIL-101(Cr). The presence of free amino groups can thus improve the immobilization efficiency, leading to a higher amount of catalytically active species and improving the subsequent catalytic activity of the heterogeneous biocatalysts. MP8@MIL(Cr)-X also successfully catalyzed the selective oxidation of thioanisole derivatives into sulfoxides.</description><subject>Catalysis</subject><subject>Chemical Sciences</subject><subject>Material chemistry</subject><issn>2574-0970</issn><issn>2574-0970</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNp1UbFOwzAUjBBIVNCV2SNFSrGd1EnYqqqFSIUuILFFz44DhsSu7BQoE7-A-BM-iS_BoRViYfLzvbt70l0QHBE8JJiSUxAOdDPMOKYxi3eCHh0lcYizBO_-mfeDvnMPGGOSERZh3As-p1rA0q1qaJXRyFToUglrltKaF1WCk19v7ylSGl3m85BgcjyxAw_doivQZgm2VaKW7gzluqpXUgv5YyFbqL_ePhb2DrQSaGahkc_GPqLZSovuENTqdXtRo6l-XTf-J1DeNIar3x3oEk3Ae6275dgrn1S7Pgz2Kqid7G_fg-BmNr2eXITzxXk-Gc9DiOK0DaO44hyXQvKUZ9WIsorSiDEmaFzFmHIJKcPRSHACUoIsRZRyUqYsFTThScmig2Cw8b2Hulha1YBdFwZUcTGeFx2GKUsSH-sT8dzhhuuzc87K6ldAcNEVVGwKKrYFecHJRuDx4sGsrI_E_Uf-BipOmS8</recordid><startdate>20200424</startdate><enddate>20200424</enddate><creator>Gkaniatsou, Effrosyni</creator><creator>Ricoux, Rémy</creator><creator>Kariyawasam, Kalani</creator><creator>Stenger, Ingrid</creator><creator>Fan, Benhui</creator><creator>Ayoub, Narjès</creator><creator>Salas, Samanta</creator><creator>Patriarche, Gilles</creator><creator>Serre, Christian</creator><creator>Mahy, Jean-Pierre</creator><creator>Steunou, Nathalie</creator><creator>Sicard, Clémence</creator><general>American Chemical Society</general><scope>AAYXX</scope><scope>CITATION</scope><scope>1XC</scope><scope>VOOES</scope><orcidid>https://orcid.org/0000-0002-7049-7388</orcidid><orcidid>https://orcid.org/0000-0002-3464-7895</orcidid><orcidid>https://orcid.org/0000-0003-3040-2564</orcidid><orcidid>https://orcid.org/0000-0001-6502-7923</orcidid><orcidid>https://orcid.org/0000-0002-3312-9025</orcidid><orcidid>https://orcid.org/0000-0002-3917-2470</orcidid></search><sort><creationdate>20200424</creationdate><title>Encapsulation of Microperoxidase‑8 in MIL-101(Cr)‑X Nanoparticles: Influence of Metal–Organic Framework Functionalization on Enzymatic Immobilization and Catalytic Activity</title><author>Gkaniatsou, Effrosyni ; Ricoux, Rémy ; Kariyawasam, Kalani ; Stenger, Ingrid ; Fan, Benhui ; Ayoub, Narjès ; Salas, Samanta ; Patriarche, Gilles ; Serre, Christian ; Mahy, Jean-Pierre ; Steunou, Nathalie ; Sicard, Clémence</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a348t-34fbb0dceb8b9f526f223666c24f402bea86035cb1aeeaedc38b1d868c27b7d63</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>Catalysis</topic><topic>Chemical Sciences</topic><topic>Material chemistry</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Gkaniatsou, Effrosyni</creatorcontrib><creatorcontrib>Ricoux, Rémy</creatorcontrib><creatorcontrib>Kariyawasam, Kalani</creatorcontrib><creatorcontrib>Stenger, Ingrid</creatorcontrib><creatorcontrib>Fan, Benhui</creatorcontrib><creatorcontrib>Ayoub, Narjès</creatorcontrib><creatorcontrib>Salas, Samanta</creatorcontrib><creatorcontrib>Patriarche, Gilles</creatorcontrib><creatorcontrib>Serre, Christian</creatorcontrib><creatorcontrib>Mahy, Jean-Pierre</creatorcontrib><creatorcontrib>Steunou, Nathalie</creatorcontrib><creatorcontrib>Sicard, Clémence</creatorcontrib><collection>CrossRef</collection><collection>Hyper Article en Ligne (HAL)</collection><collection>Hyper Article en Ligne (HAL) (Open Access)</collection><jtitle>ACS applied nano materials</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Gkaniatsou, Effrosyni</au><au>Ricoux, Rémy</au><au>Kariyawasam, Kalani</au><au>Stenger, Ingrid</au><au>Fan, Benhui</au><au>Ayoub, Narjès</au><au>Salas, Samanta</au><au>Patriarche, Gilles</au><au>Serre, Christian</au><au>Mahy, Jean-Pierre</au><au>Steunou, Nathalie</au><au>Sicard, Clémence</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Encapsulation of Microperoxidase‑8 in MIL-101(Cr)‑X Nanoparticles: Influence of Metal–Organic Framework Functionalization on Enzymatic Immobilization and Catalytic Activity</atitle><jtitle>ACS applied nano materials</jtitle><addtitle>ACS Appl. Nano Mater</addtitle><date>2020-04-24</date><risdate>2020</risdate><volume>3</volume><issue>4</issue><spage>3233</spage><epage>3243</epage><pages>3233-3243</pages><issn>2574-0970</issn><eissn>2574-0970</eissn><abstract>Microperoxidase 8 (MP8) was immobilized within MIL-101(Cr) bearing terephthalate linkers with functionalized groups (-NH2 and -SO3H). A synthesis protocol for MIL-101(Cr)-SO3H that avoids the use of toxic Cr(VI) and HF was developed. The electrostatic interactions between the MP8 molecules and the MOF matrices were found to be crucial for a successful immobilization. Raman spectroscopy revealed the dispersion of the immobilized MP8 molecules in MIL-101(Cr)-X matrices as monomers without aggregation. The presence of functional groups resulted in higher amounts of immobilized MP8 in comparison to the bare MIL-101(Cr). The catalytic activity of MP8@MIL-101(Cr)-NH2 per material mass was higher than that for MP8@MIL-101(Cr). The presence of free amino groups can thus improve the immobilization efficiency, leading to a higher amount of catalytically active species and improving the subsequent catalytic activity of the heterogeneous biocatalysts. MP8@MIL(Cr)-X also successfully catalyzed the selective oxidation of thioanisole derivatives into sulfoxides.</abstract><pub>American Chemical Society</pub><doi>10.1021/acsanm.9b02464</doi><tpages>11</tpages><orcidid>https://orcid.org/0000-0002-7049-7388</orcidid><orcidid>https://orcid.org/0000-0002-3464-7895</orcidid><orcidid>https://orcid.org/0000-0003-3040-2564</orcidid><orcidid>https://orcid.org/0000-0001-6502-7923</orcidid><orcidid>https://orcid.org/0000-0002-3312-9025</orcidid><orcidid>https://orcid.org/0000-0002-3917-2470</orcidid><oa>free_for_read</oa></addata></record> |
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| title | Encapsulation of Microperoxidase‑8 in MIL-101(Cr)‑X Nanoparticles: Influence of Metal–Organic Framework Functionalization on Enzymatic Immobilization and Catalytic Activity |
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