Kinetic study of phenol hydroxylation by H<inf>2</inf>O<inf>2</inf> in 3D Fe/SiC honeycomb monolithic reactors: Enabling the sustainable production of dihydroxybenzenes
The chemical kinetics of phenol hydroxylation by hydrogen peroxide (H2O2) to produce dihydroxybenzenes was studied using a 3D printed monolithic reactor. The monoliths were manufactured by the Robocasting technique. They consisted on honeycomb-structured Fe/SiC nanoparticles (13.5 mm in diameter and...
| Autores: | , , , |
|---|---|
| Tipo de recurso: | artículo |
| Fecha de publicación: | 2021 |
| País: | España |
| Institución: | Universidad Autónoma de Madrid |
| Repositorio: | Biblos-e Archivo. Repositorio Institucional de la UAM |
| Idioma: | inglés |
| OAI Identifier: | oai:repositorio.uam.es:10486/714797 |
| Acceso en línea: | http://hdl.handle.net/10486/714797 https://dx.doi.org/10.1016/j.cej.2021.131128 |
| Access Level: | acceso abierto |
| Palabra clave: | 3D printing Dihydroxybenzenes Heterogeneous kinetic model Monolithic reactor Phenol hydroxylation Robocasting Química |
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Kinetic study of phenol hydroxylation by H<inf>2</inf>O<inf>2</inf> in 3D Fe/SiC honeycomb monolithic reactors: Enabling the sustainable production of dihydroxybenzenesVega, GonzaloBelmonte, ManuelQuintanilla Gómez, María AsunciónCasas de Pedro, José Antonio3D printingDihydroxybenzenesHeterogeneous kinetic modelMonolithic reactorPhenol hydroxylationRobocastingQuímicaThe chemical kinetics of phenol hydroxylation by hydrogen peroxide (H2O2) to produce dihydroxybenzenes was studied using a 3D printed monolithic reactor. The monoliths were manufactured by the Robocasting technique. They consisted on honeycomb-structured Fe/SiC nanoparticles (13.5 mm in diameter and 14.8 mm in length) with triangle cell geometry and staggered interconnected channels (71 cells per cm2). The isothermal reactor was constituted by three stacked monoliths and was operated as an ideal plug flow reactor, according to the measured residence time distribution. The hydroxylation experiments were carried out at CPHENOL,0 = 0.33 M, phenol:H2O2 molar ratio 1:1, τ(space time) = 0–254 g h L-1, T = 80, 85 and 90 °C and water as unique solvent. Experimental results showed no mass transfer limitations. The best fits were obtained for H2O2 decomposition with a Langmuir-Hinshelwood-Hougen-Watson kinetic model and for phenol hydroxylation, as well as, catechol and hydroquinone production, with an Eley-Rideal kinetic model. The hydroxylation reaction mechanism underling to the developed model involved three elementary reactions: (1) adsorption of H2O2 molecules on the iron active sites, (2) chemical surface H2O2 decomposition into the hydroxyl radical species, and (3) reaction between adsorbed radical species and phenol in solution leading to the dihydroxybenzene formation and freeing the iron catalytic active sites (rds). This work contributes to the implementation of outstanding 3D Fe/SiC honeycomb monolithic reactors, with a dihydroxybenzene selectivity above 99% at 80 °C, for the sustainable production of hydroxylated aromaticsThe authors thank the financial support by the Community of Madrid through the project S2018/EMT-4341 and the Government of Spain through the projects: PID2019-105079RB-I00, PGC2018-095642-B-I00 and RTI2018-095052-B-I00 (MCIU/AEI/FEDER, UE). Also, G. Vega acknowledges the Universidad Autonoma de Madrid for the Predoctoral contract FPI/UAM2021ElsevierDepartamento de Ingeniería QuímicaFacultad de CienciasUAM. Departamento de Ingeniería Química20212021-07-06research articlehttp://purl.org/coar/resource_type/c_2df8fbb1AMhttp://purl.org/coar/version/c_ab4af688f83e57aainfo:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10486/714797https://dx.doi.org/10.1016/j.cej.2021.131128reponame:Biblos-e Archivo. Repositorio Institucional de la UAMinstname:Universidad Autónoma de MadridInglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution-NonCommercial-NoDerivatives 4.0 Internationalhttp://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessoai:repositorio.uam.es:10486/7147972026-06-23T12:46:27Z |
| dc.title.none.fl_str_mv |
Kinetic study of phenol hydroxylation by H<inf>2</inf>O<inf>2</inf> in 3D Fe/SiC honeycomb monolithic reactors: Enabling the sustainable production of dihydroxybenzenes |
| title |
Kinetic study of phenol hydroxylation by H<inf>2</inf>O<inf>2</inf> in 3D Fe/SiC honeycomb monolithic reactors: Enabling the sustainable production of dihydroxybenzenes |
| spellingShingle |
Kinetic study of phenol hydroxylation by H<inf>2</inf>O<inf>2</inf> in 3D Fe/SiC honeycomb monolithic reactors: Enabling the sustainable production of dihydroxybenzenes Vega, Gonzalo 3D printing Dihydroxybenzenes Heterogeneous kinetic model Monolithic reactor Phenol hydroxylation Robocasting Química |
| title_short |
Kinetic study of phenol hydroxylation by H<inf>2</inf>O<inf>2</inf> in 3D Fe/SiC honeycomb monolithic reactors: Enabling the sustainable production of dihydroxybenzenes |
| title_full |
Kinetic study of phenol hydroxylation by H<inf>2</inf>O<inf>2</inf> in 3D Fe/SiC honeycomb monolithic reactors: Enabling the sustainable production of dihydroxybenzenes |
| title_fullStr |
Kinetic study of phenol hydroxylation by H<inf>2</inf>O<inf>2</inf> in 3D Fe/SiC honeycomb monolithic reactors: Enabling the sustainable production of dihydroxybenzenes |
| title_full_unstemmed |
Kinetic study of phenol hydroxylation by H<inf>2</inf>O<inf>2</inf> in 3D Fe/SiC honeycomb monolithic reactors: Enabling the sustainable production of dihydroxybenzenes |
| title_sort |
Kinetic study of phenol hydroxylation by H<inf>2</inf>O<inf>2</inf> in 3D Fe/SiC honeycomb monolithic reactors: Enabling the sustainable production of dihydroxybenzenes |
| dc.creator.none.fl_str_mv |
Vega, Gonzalo Belmonte, Manuel Quintanilla Gómez, María Asunción Casas de Pedro, José Antonio |
| author |
Vega, Gonzalo |
| author_facet |
Vega, Gonzalo Belmonte, Manuel Quintanilla Gómez, María Asunción Casas de Pedro, José Antonio |
| author_role |
author |
| author2 |
Belmonte, Manuel Quintanilla Gómez, María Asunción Casas de Pedro, José Antonio |
| author2_role |
author author author |
| dc.contributor.none.fl_str_mv |
Departamento de Ingeniería Química Facultad de Ciencias UAM. Departamento de Ingeniería Química |
| dc.subject.none.fl_str_mv |
3D printing Dihydroxybenzenes Heterogeneous kinetic model Monolithic reactor Phenol hydroxylation Robocasting Química |
| topic |
3D printing Dihydroxybenzenes Heterogeneous kinetic model Monolithic reactor Phenol hydroxylation Robocasting Química |
| description |
The chemical kinetics of phenol hydroxylation by hydrogen peroxide (H2O2) to produce dihydroxybenzenes was studied using a 3D printed monolithic reactor. The monoliths were manufactured by the Robocasting technique. They consisted on honeycomb-structured Fe/SiC nanoparticles (13.5 mm in diameter and 14.8 mm in length) with triangle cell geometry and staggered interconnected channels (71 cells per cm2). The isothermal reactor was constituted by three stacked monoliths and was operated as an ideal plug flow reactor, according to the measured residence time distribution. The hydroxylation experiments were carried out at CPHENOL,0 = 0.33 M, phenol:H2O2 molar ratio 1:1, τ(space time) = 0–254 g h L-1, T = 80, 85 and 90 °C and water as unique solvent. Experimental results showed no mass transfer limitations. The best fits were obtained for H2O2 decomposition with a Langmuir-Hinshelwood-Hougen-Watson kinetic model and for phenol hydroxylation, as well as, catechol and hydroquinone production, with an Eley-Rideal kinetic model. The hydroxylation reaction mechanism underling to the developed model involved three elementary reactions: (1) adsorption of H2O2 molecules on the iron active sites, (2) chemical surface H2O2 decomposition into the hydroxyl radical species, and (3) reaction between adsorbed radical species and phenol in solution leading to the dihydroxybenzene formation and freeing the iron catalytic active sites (rds). This work contributes to the implementation of outstanding 3D Fe/SiC honeycomb monolithic reactors, with a dihydroxybenzene selectivity above 99% at 80 °C, for the sustainable production of hydroxylated aromatics |
| publishDate |
2021 |
| dc.date.none.fl_str_mv |
2021 2021-07-06 |
| dc.type.none.fl_str_mv |
research article http://purl.org/coar/resource_type/c_2df8fbb1 AM http://purl.org/coar/version/c_ab4af688f83e57aa |
| dc.type.openaire.fl_str_mv |
info:eu-repo/semantics/article |
| format |
article |
| dc.identifier.none.fl_str_mv |
http://hdl.handle.net/10486/714797 https://dx.doi.org/10.1016/j.cej.2021.131128 |
| url |
http://hdl.handle.net/10486/714797 https://dx.doi.org/10.1016/j.cej.2021.131128 |
| dc.language.none.fl_str_mv |
Inglés eng |
| language_invalid_str_mv |
Inglés |
| language |
eng |
| dc.rights.none.fl_str_mv |
open access http://purl.org/coar/access_right/c_abf2 Attribution-NonCommercial-NoDerivatives 4.0 International http://creativecommons.org/licenses/by-nc-nd/4.0/ |
| dc.rights.openaire.fl_str_mv |
info:eu-repo/semantics/openAccess |
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open access http://purl.org/coar/access_right/c_abf2 Attribution-NonCommercial-NoDerivatives 4.0 International http://creativecommons.org/licenses/by-nc-nd/4.0/ |
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openAccess |
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application/pdf |
| dc.publisher.none.fl_str_mv |
Elsevier |
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Elsevier |
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reponame:Biblos-e Archivo. Repositorio Institucional de la UAM instname:Universidad Autónoma de Madrid |
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Universidad Autónoma de Madrid |
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Biblos-e Archivo. Repositorio Institucional de la UAM |
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Biblos-e Archivo. Repositorio Institucional de la UAM |
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