Green synthesis of Fe3O4@ZnO-supported Pd nanoparticles for oxidation and hydrogenation reactions in liquid systems

Detalhes bibliográficos
Autor(a) principal: Souto, Robson da Silva
Data de Publicação: 2022
Outros Autores: Razini, Samara da Silva, Kauffmann, Angélica Correa, Silva, Virgínia Claudia Paulino, Sousa Jr, Paulo Teixeira de, Bakuzis, Andris, Fontana, Luis Cesar, Jacinto, Marcos José
Tipo de documento: Artigo
Idioma: eng
Título da fonte: Research, Society and Development
Texto Completo: https://rsdjournal.org/index.php/rsd/article/view/36004
Resumo: In this work Pd nanoparticles immobilized on a hybrid solid support comprised of Fe3O4 coated by a ZnO layer were synthesized by a green method which makes use of water, a biological substrate from a local plant (Rhamnidium elaeocarpum) and inexpensive Fe3+ and Zn2+ salts. 1H-NMR and 13C-NM revealed β-sitosterol as the main component of the biological substrate. The catalytic support containing Pd nanoparticles was applied in three model solid-liquid catalytic systems, namely: alcohol oxidation, nitrocompound reduction and olefin hydrogenation. For the alcohol oxidation, benzyl alcohol was used as the substrate in a solvent-free condition with high selectivity towards benzaldehyde, and a single sample of the catalyst could be recycled up to 11 times before any loss of activity could be detected. TOF (turnover frequency) as high as 13,686 h-1 for the substrate oxidation was achieved with an average yield rate of 45.4% for formation of benzaldehyde and 81.6% of average substrate conversion after 6 catalytic cycles. For the hydrogenation experiments using cyclohexene and 4-nitrophenol as model substrates, conversion as high as 96% to 4-aminophenol and cyclohexane, respectively, was achieved after 30 minutes of reaction. Furthermore, a single sample of the catalyst could be recycled for up to 17 times for the reduction of 4-nitrophenol, and 21 times in the hydrogenation of cyclohexene. Catalytic recycling for all studied reactions was straightforward after due to the superparamagnetic property of the material, and catalyst isolation after each batch could be rapidly carried out using a Nd magnet. These results suggests that a highly active and stable catalytic system based on Pd nanoparticles supported on a multifunctional solid could be fabricated using green and inexpensive biomass under operationally simple synthesis conditions.
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spelling Green synthesis of Fe3O4@ZnO-supported Pd nanoparticles for oxidation and hydrogenation reactions in liquid systemsSíntesis verde de nanopartículas de Pd soportadas en Fe3O4@ZnO para reacciones de oxidación e hidrogenación en sistemas líquidosSíntese verde de nanopartículas de Pd suportadas em Fe3O4@ZnO para reações de oxidação e hidrogenação em sistemas líquidosNanomaterialsMagnetic separationBiosynthesis.NanomateriaisSeparação magnéticaBiossíntese.NanomaterialesSeparación magnéticaBiosíntesis.In this work Pd nanoparticles immobilized on a hybrid solid support comprised of Fe3O4 coated by a ZnO layer were synthesized by a green method which makes use of water, a biological substrate from a local plant (Rhamnidium elaeocarpum) and inexpensive Fe3+ and Zn2+ salts. 1H-NMR and 13C-NM revealed β-sitosterol as the main component of the biological substrate. The catalytic support containing Pd nanoparticles was applied in three model solid-liquid catalytic systems, namely: alcohol oxidation, nitrocompound reduction and olefin hydrogenation. For the alcohol oxidation, benzyl alcohol was used as the substrate in a solvent-free condition with high selectivity towards benzaldehyde, and a single sample of the catalyst could be recycled up to 11 times before any loss of activity could be detected. TOF (turnover frequency) as high as 13,686 h-1 for the substrate oxidation was achieved with an average yield rate of 45.4% for formation of benzaldehyde and 81.6% of average substrate conversion after 6 catalytic cycles. For the hydrogenation experiments using cyclohexene and 4-nitrophenol as model substrates, conversion as high as 96% to 4-aminophenol and cyclohexane, respectively, was achieved after 30 minutes of reaction. Furthermore, a single sample of the catalyst could be recycled for up to 17 times for the reduction of 4-nitrophenol, and 21 times in the hydrogenation of cyclohexene. Catalytic recycling for all studied reactions was straightforward after due to the superparamagnetic property of the material, and catalyst isolation after each batch could be rapidly carried out using a Nd magnet. These results suggests that a highly active and stable catalytic system based on Pd nanoparticles supported on a multifunctional solid could be fabricated using green and inexpensive biomass under operationally simple synthesis conditions.En este trabajo se sintetizaron nanopartículas de Pd inmovilizadas sobre un soporte sólido híbrido compuesto por Fe3O4 recubierto con una capa de ZnO mediante un método verde que utiliza agua, un sustrato biológico de una planta local (Rhamnidium elaeocarpum) y sales metálicas de Fe3+ y Zn2+. 1H-NMR y 13C-NM revelaron β-sitosterol como componente principal del sustrato biológico. El soporte catalítico que contiene nanopartículas de Pd se aplicó en tres modelos de sistemas catalíticos sólido-líquido, a saber: oxidación de alcoholes, reducción de nitrocompuestos e hidrogenación de olefinas. Para la oxidación del alcohol, se usó alcohol bencílico como sustrato en una condición libre de solventes, con alta selectividad hacia el benzaldehído, y una sola muestra del catalizador se pudo reciclar hasta 11 veces antes de que se pudiera detectar cualquier pérdida de actividad. Se logró un TOF (frecuencia de rotación) de 13 686 h-1 para la oxidación del sustrato con una tasa de rendimiento promedio del 45,4 % para la formación de benzaldehído y una conversión promedio del sustrato del 81,6 % después de 6 ciclos catalíticos. Para los experimentos de hidrogenación utilizando ciclohexeno y 4-nitrofenol como sustratos modelo, la conversión fue del 96 % para 4-aminofenol y ciclohexano, respectivamente, después de 30 minutos de reacción. Además, una sola muestra del catalizador podría reciclarse hasta 17 veces para la reducción de 4-nitrofenol y 21 veces para la hidrogenación de ciclohexeno. El reciclaje catalítico de todas las reacciones estudiadas se realizó de forma sencilla debido a la propiedad superparamagnética del material, y el aislamiento del catalizador después de cada lote se pudo realizar rápidamente utilizando un imán de Nd. Estos resultados sugieren que se puede fabricar un sistema catalítico altamente activo y estable basado en nanopartículas de Pd soportadas en un sólido multifuncional utilizando biomasa verde barata en condiciones de síntesis operativamente simples.Neste trabalho, nanopartículas de Pd imobilizadas em um suporte sólido híbrido composto de Fe3O4 revestido por uma camada de ZnO foram sintetizadas por um método verde que utiliza água, um substrato biológico de uma planta local (Rhamnidium elaeocarpum) e sais metálicos de Fe3+ e Zn2+. 1H-NMR e 13C-NM revelaram o β-sitosterol como o principal componente do substrato biológico. O suporte catalítico contendo nanopartículas de Pd foi aplicado em três modelos de sistemas catalíticos sólido-líquido, a saber: oxidação de álcool, redução de nitrocompostos e hidrogenação de olefinas. Para a oxidação do álcool, o álcool benzílico foi usado como substrato em uma condição livre de solvente, com alta seletividade em relação ao benzaldeído, e uma única amostra do catalisador pôde ser reciclada até 11 vezes antes que qualquer perda de atividade pudesse ser detectada. TOF (frequência de rotatividade) de 13.686 h-1 para a oxidação do substrato foi alcançado com uma taxa média de rendimento de 45,4% para a formação de benzaldeído e 81,6% de conversão média do substrato após 6 ciclos catalíticos. Para os experimentos de hidrogenação usando ciclohexeno e 4-nitrofenol como substratos modelo, a conversão foi de 96% para 4-aminofenol e ciclohexano, respectivamente, após 30 minutos de reação. Além disso, uma única amostra do catalisador pôde ser reciclada por até 17 vezes para a redução do 4-nitrofenol, e 21 vezes na hidrogenação do ciclohexeno. A reciclagem catalítica para todas as reações estudadas foi realizada de forma simples devido à propriedade superparamagnética do material, e o isolamento do catalisador após cada lote pôde ser realizado rapidamente usando um ímã de Nd. Esses resultados sugerem que um sistema catalítico altamente ativo e estável baseado em nanopartículas de Pd suportadas em um sólido multifuncional pode ser fabricado usando biomassa verde e barata em condições de síntese operacionalmente simples.Research, Society and Development2022-10-21info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionapplication/pdfhttps://rsdjournal.org/index.php/rsd/article/view/3600410.33448/rsd-v11i14.36004Research, Society and Development; Vol. 11 No. 14; e109111436004Research, Society and Development; Vol. 11 Núm. 14; e109111436004Research, Society and Development; v. 11 n. 14; e1091114360042525-3409reponame:Research, Society and Developmentinstname:Universidade Federal de Itajubá (UNIFEI)instacron:UNIFEIenghttps://rsdjournal.org/index.php/rsd/article/view/36004/30167Copyright (c) 2022 Robson da Silva Souto; Samara da Silva Razini; Angélica Correa Kauffmann; Virgínia Claudia Paulino Silva; Paulo Teixeira de Sousa Jr; Andris Bakuzis; Luis Cesar Fontana; Marcos José Jacintohttps://creativecommons.org/licenses/by/4.0info:eu-repo/semantics/openAccessSouto, Robson da Silva Razini, Samara da Silva Kauffmann, Angélica Correa Silva, Virgínia Claudia Paulino Sousa Jr, Paulo Teixeira de Bakuzis, AndrisFontana, Luis CesarJacinto, Marcos José 2022-11-08T13:36:27Zoai:ojs.pkp.sfu.ca:article/36004Revistahttps://rsdjournal.org/index.php/rsd/indexPUBhttps://rsdjournal.org/index.php/rsd/oairsd.articles@gmail.com2525-34092525-3409opendoar:2024-01-17T09:50:42.634507Research, Society and Development - Universidade Federal de Itajubá (UNIFEI)false
dc.title.none.fl_str_mv Green synthesis of Fe3O4@ZnO-supported Pd nanoparticles for oxidation and hydrogenation reactions in liquid systems
Síntesis verde de nanopartículas de Pd soportadas en Fe3O4@ZnO para reacciones de oxidación e hidrogenación en sistemas líquidos
Síntese verde de nanopartículas de Pd suportadas em Fe3O4@ZnO para reações de oxidação e hidrogenação em sistemas líquidos
title Green synthesis of Fe3O4@ZnO-supported Pd nanoparticles for oxidation and hydrogenation reactions in liquid systems
spellingShingle Green synthesis of Fe3O4@ZnO-supported Pd nanoparticles for oxidation and hydrogenation reactions in liquid systems
Souto, Robson da Silva
Nanomaterials
Magnetic separation
Biosynthesis.
Nanomateriais
Separação magnética
Biossíntese.
Nanomateriales
Separación magnética
Biosíntesis.
title_short Green synthesis of Fe3O4@ZnO-supported Pd nanoparticles for oxidation and hydrogenation reactions in liquid systems
title_full Green synthesis of Fe3O4@ZnO-supported Pd nanoparticles for oxidation and hydrogenation reactions in liquid systems
title_fullStr Green synthesis of Fe3O4@ZnO-supported Pd nanoparticles for oxidation and hydrogenation reactions in liquid systems
title_full_unstemmed Green synthesis of Fe3O4@ZnO-supported Pd nanoparticles for oxidation and hydrogenation reactions in liquid systems
title_sort Green synthesis of Fe3O4@ZnO-supported Pd nanoparticles for oxidation and hydrogenation reactions in liquid systems
author Souto, Robson da Silva
author_facet Souto, Robson da Silva
Razini, Samara da Silva
Kauffmann, Angélica Correa
Silva, Virgínia Claudia Paulino
Sousa Jr, Paulo Teixeira de
Bakuzis, Andris
Fontana, Luis Cesar
Jacinto, Marcos José
author_role author
author2 Razini, Samara da Silva
Kauffmann, Angélica Correa
Silva, Virgínia Claudia Paulino
Sousa Jr, Paulo Teixeira de
Bakuzis, Andris
Fontana, Luis Cesar
Jacinto, Marcos José
author2_role author
author
author
author
author
author
author
dc.contributor.author.fl_str_mv Souto, Robson da Silva
Razini, Samara da Silva
Kauffmann, Angélica Correa
Silva, Virgínia Claudia Paulino
Sousa Jr, Paulo Teixeira de
Bakuzis, Andris
Fontana, Luis Cesar
Jacinto, Marcos José
dc.subject.por.fl_str_mv Nanomaterials
Magnetic separation
Biosynthesis.
Nanomateriais
Separação magnética
Biossíntese.
Nanomateriales
Separación magnética
Biosíntesis.
topic Nanomaterials
Magnetic separation
Biosynthesis.
Nanomateriais
Separação magnética
Biossíntese.
Nanomateriales
Separación magnética
Biosíntesis.
description In this work Pd nanoparticles immobilized on a hybrid solid support comprised of Fe3O4 coated by a ZnO layer were synthesized by a green method which makes use of water, a biological substrate from a local plant (Rhamnidium elaeocarpum) and inexpensive Fe3+ and Zn2+ salts. 1H-NMR and 13C-NM revealed β-sitosterol as the main component of the biological substrate. The catalytic support containing Pd nanoparticles was applied in three model solid-liquid catalytic systems, namely: alcohol oxidation, nitrocompound reduction and olefin hydrogenation. For the alcohol oxidation, benzyl alcohol was used as the substrate in a solvent-free condition with high selectivity towards benzaldehyde, and a single sample of the catalyst could be recycled up to 11 times before any loss of activity could be detected. TOF (turnover frequency) as high as 13,686 h-1 for the substrate oxidation was achieved with an average yield rate of 45.4% for formation of benzaldehyde and 81.6% of average substrate conversion after 6 catalytic cycles. For the hydrogenation experiments using cyclohexene and 4-nitrophenol as model substrates, conversion as high as 96% to 4-aminophenol and cyclohexane, respectively, was achieved after 30 minutes of reaction. Furthermore, a single sample of the catalyst could be recycled for up to 17 times for the reduction of 4-nitrophenol, and 21 times in the hydrogenation of cyclohexene. Catalytic recycling for all studied reactions was straightforward after due to the superparamagnetic property of the material, and catalyst isolation after each batch could be rapidly carried out using a Nd magnet. These results suggests that a highly active and stable catalytic system based on Pd nanoparticles supported on a multifunctional solid could be fabricated using green and inexpensive biomass under operationally simple synthesis conditions.
publishDate 2022
dc.date.none.fl_str_mv 2022-10-21
dc.type.driver.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.uri.fl_str_mv https://rsdjournal.org/index.php/rsd/article/view/36004
10.33448/rsd-v11i14.36004
url https://rsdjournal.org/index.php/rsd/article/view/36004
identifier_str_mv 10.33448/rsd-v11i14.36004
dc.language.iso.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv https://rsdjournal.org/index.php/rsd/article/view/36004/30167
dc.rights.driver.fl_str_mv https://creativecommons.org/licenses/by/4.0
info:eu-repo/semantics/openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by/4.0
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Research, Society and Development
publisher.none.fl_str_mv Research, Society and Development
dc.source.none.fl_str_mv Research, Society and Development; Vol. 11 No. 14; e109111436004
Research, Society and Development; Vol. 11 Núm. 14; e109111436004
Research, Society and Development; v. 11 n. 14; e109111436004
2525-3409
reponame:Research, Society and Development
instname:Universidade Federal de Itajubá (UNIFEI)
instacron:UNIFEI
instname_str Universidade Federal de Itajubá (UNIFEI)
instacron_str UNIFEI
institution UNIFEI
reponame_str Research, Society and Development
collection Research, Society and Development
repository.name.fl_str_mv Research, Society and Development - Universidade Federal de Itajubá (UNIFEI)
repository.mail.fl_str_mv rsd.articles@gmail.com
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