Nanozeolites as support for laccase immobilization: Application to mediated glycerol oxidation
Autor(a) principal: | |
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Data de Publicação: | 2021 |
Outros Autores: | , , |
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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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 |
|
_version_ |
1808128809981968384 |