Green synthesis of Fe3O4@ZnO-supported Pd nanoparticles for oxidation and hydrogenation reactions in liquid systems
Autor(a) principal: | |
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Data de Publicação: | 2022 |
Outros Autores: | , , , , , , |
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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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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1797052725958017024 |