Nanozeolites as support for laccase immobilization: Application to mediated glycerol oxidation

Detalhes bibliográficos
Autor(a) principal: Miller, Alex Henrique [UNESP]
Data de Publicação: 2021
Outros Autores: de Vasconcellos, Adriano [UNESP], Fielding, Alistair John, Nery, José Geraldo [UNESP]
Tipo de documento: Artigo
Idioma: eng
Título da fonte: Repositório Institucional da UNESP
Texto Completo: http://dx.doi.org/10.1016/j.apcata.2021.118361
http://hdl.handle.net/11449/229609
Resumo: This study investigated the use of nanozeolites as support for laccases from P. ostreatus (LPO), Aspergillus sp (LAsp) and A. bisporus (LAB) immobilization applied to 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO) mediated glycerol oxidation. Selected complexes led to up to 5% glycerol conversion, and interestingly, up to 100% selectivity to glyceraldehyde after 48 h. Free enzymes led to significantly higher yields (up to 82%) but lacked selectivity when tested under the same conditions. These findings suggest that laccases immobilized into nanozeolites are promising catalysts for the selective oxidation of glycerol. With the aim to understand the different behavior of free or immobilized enzymes, electron paramagnetic resonance (EPR) spectroscopy was applied. A significant shift of the T2 parallel copper hyperfine coupling constant was observed. This suggested a perturbation on the catalytic site after immobilization due to pH variation of the enzymatic microenvironments, thus influencing performance of laccase immobilized on nanozeolites.
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spelling Nanozeolites as support for laccase immobilization: Application to mediated glycerol oxidationEPRGlycerolImmobilizationLaccaseNanozeolitesOxidationThis study investigated the use of nanozeolites as support for laccases from P. ostreatus (LPO), Aspergillus sp (LAsp) and A. bisporus (LAB) immobilization applied to 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO) mediated glycerol oxidation. Selected complexes led to up to 5% glycerol conversion, and interestingly, up to 100% selectivity to glyceraldehyde after 48 h. Free enzymes led to significantly higher yields (up to 82%) but lacked selectivity when tested under the same conditions. These findings suggest that laccases immobilized into nanozeolites are promising catalysts for the selective oxidation of glycerol. With the aim to understand the different behavior of free or immobilized enzymes, electron paramagnetic resonance (EPR) spectroscopy was applied. A significant shift of the T2 parallel copper hyperfine coupling constant was observed. This suggested a perturbation on the catalytic site after immobilization due to pH variation of the enzymatic microenvironments, thus influencing performance of laccase immobilized on nanozeolites.Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)Physics Department Institute of Biosciences Letters and Exact Sciences – IBILCE/São Paulo State University – UNESP, São José do Rio PretoCentre for Natural Products Discovery School of Pharmacy and Biomolecular Science Liverpool John Moores University James Parsons Building, Byrom StreetPhysics Department Institute of Biosciences Letters and Exact Sciences – IBILCE/São Paulo State University – UNESP, São José do Rio PretoFAPESP: 2016/24303-0FAPESP: 2018/21483-3CNPq: 406761/2013-2CNPq: 465594/2014-0CNPq: RF-2019-474\4Universidade Estadual Paulista (UNESP)James Parsons BuildingMiller, Alex Henrique [UNESP]de Vasconcellos, Adriano [UNESP]Fielding, Alistair JohnNery, José Geraldo [UNESP]2022-04-29T08:33:34Z2022-04-29T08:33:34Z2021-09-25info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articlehttp://dx.doi.org/10.1016/j.apcata.2021.118361Applied Catalysis A: General, v. 626.0926-860Xhttp://hdl.handle.net/11449/22960910.1016/j.apcata.2021.1183612-s2.0-85115936386Scopusreponame:Repositório Institucional da UNESPinstname:Universidade Estadual Paulista (UNESP)instacron:UNESPengApplied Catalysis A: Generalinfo:eu-repo/semantics/openAccess2022-04-29T08:33:34Zoai:repositorio.unesp.br:11449/229609Repositório InstitucionalPUBhttp://repositorio.unesp.br/oai/requestopendoar:29462024-08-05T17:25:52.949754Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)false
dc.title.none.fl_str_mv Nanozeolites as support for laccase immobilization: Application to mediated glycerol oxidation
title Nanozeolites as support for laccase immobilization: Application to mediated glycerol oxidation
spellingShingle Nanozeolites as support for laccase immobilization: Application to mediated glycerol oxidation
Miller, Alex Henrique [UNESP]
EPR
Glycerol
Immobilization
Laccase
Nanozeolites
Oxidation
title_short Nanozeolites as support for laccase immobilization: Application to mediated glycerol oxidation
title_full Nanozeolites as support for laccase immobilization: Application to mediated glycerol oxidation
title_fullStr Nanozeolites as support for laccase immobilization: Application to mediated glycerol oxidation
title_full_unstemmed Nanozeolites as support for laccase immobilization: Application to mediated glycerol oxidation
title_sort Nanozeolites as support for laccase immobilization: Application to mediated glycerol oxidation
author Miller, Alex Henrique [UNESP]
author_facet Miller, Alex Henrique [UNESP]
de Vasconcellos, Adriano [UNESP]
Fielding, Alistair John
Nery, José Geraldo [UNESP]
author_role author
author2 de Vasconcellos, Adriano [UNESP]
Fielding, Alistair John
Nery, José Geraldo [UNESP]
author2_role author
author
author
dc.contributor.none.fl_str_mv Universidade Estadual Paulista (UNESP)
James Parsons Building
dc.contributor.author.fl_str_mv Miller, Alex Henrique [UNESP]
de Vasconcellos, Adriano [UNESP]
Fielding, Alistair John
Nery, José Geraldo [UNESP]
dc.subject.por.fl_str_mv EPR
Glycerol
Immobilization
Laccase
Nanozeolites
Oxidation
topic EPR
Glycerol
Immobilization
Laccase
Nanozeolites
Oxidation
description This study investigated the use of nanozeolites as support for laccases from P. ostreatus (LPO), Aspergillus sp (LAsp) and A. bisporus (LAB) immobilization applied to 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO) mediated glycerol oxidation. Selected complexes led to up to 5% glycerol conversion, and interestingly, up to 100% selectivity to glyceraldehyde after 48 h. Free enzymes led to significantly higher yields (up to 82%) but lacked selectivity when tested under the same conditions. These findings suggest that laccases immobilized into nanozeolites are promising catalysts for the selective oxidation of glycerol. With the aim to understand the different behavior of free or immobilized enzymes, electron paramagnetic resonance (EPR) spectroscopy was applied. A significant shift of the T2 parallel copper hyperfine coupling constant was observed. This suggested a perturbation on the catalytic site after immobilization due to pH variation of the enzymatic microenvironments, thus influencing performance of laccase immobilized on nanozeolites.
publishDate 2021
dc.date.none.fl_str_mv 2021-09-25
2022-04-29T08:33:34Z
2022-04-29T08:33:34Z
dc.type.status.fl_str_mv info:eu-repo/semantics/publishedVersion
dc.type.driver.fl_str_mv info:eu-repo/semantics/article
format article
status_str publishedVersion
dc.identifier.uri.fl_str_mv http://dx.doi.org/10.1016/j.apcata.2021.118361
Applied Catalysis A: General, v. 626.
0926-860X
http://hdl.handle.net/11449/229609
10.1016/j.apcata.2021.118361
2-s2.0-85115936386
url http://dx.doi.org/10.1016/j.apcata.2021.118361
http://hdl.handle.net/11449/229609
identifier_str_mv Applied Catalysis A: General, v. 626.
0926-860X
10.1016/j.apcata.2021.118361
2-s2.0-85115936386
dc.language.iso.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv Applied Catalysis A: General
dc.rights.driver.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.source.none.fl_str_mv Scopus
reponame:Repositório Institucional da UNESP
instname:Universidade Estadual Paulista (UNESP)
instacron:UNESP
instname_str Universidade Estadual Paulista (UNESP)
instacron_str UNESP
institution UNESP
reponame_str Repositório Institucional da UNESP
collection Repositório Institucional da UNESP
repository.name.fl_str_mv Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)
repository.mail.fl_str_mv
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