Esterification of Levulinic Acid to Methyl Levulinate over Zr-MOFs Catalysts
- Autores
- Bravo Fuchineco, Daiana Antonella; Heredia, Angelica Constanza; Mendoza, Sandra Marina; Rodríguez Castellón, Enrique; Crivello, Mónica Elsie
- Año de publicación
- 2022
- Idioma
- inglés
- Tipo de recurso
- artículo
- Estado
- versión publicada
- Descripción
- At present, the trend towards partial replacement of petroleum‐derived fuels by those from the revaluation of biomass has become of great importance. An effective strategy for pro-cessing complex biomass feedstocks involves prior conversion to simpler compounds (platform molecules) that are more easily transformed in subsequent reactions. This study analyzes the met-al–organic frameworks (MOFs) that contain Zr metal clusters formed by ligands of terephthalic acid (UiO‐66) and aminoterephthalic acid (UiO‐66‐NH2), as active and stable catalysts for the esterification of levulinic acid with methanol. An alternative synthesis is presented by means of ultrasonic stirring at room temperature and 60 °C, in order to improve the structural properties of the catalysts. They were analyzed by X‐ray diffraction, scanning electron microscopy, infrared spectroscopy, X‐ray photoelectron spectroscopy, microwave plasma atomic emission spectroscopy, acidity measurement, and N2 adsorption. The catalytic reaction was carried out in a batch system and under pressure in an autoclave. Its progress was followed by gas chromatography and mass spectrometry. Parameters such as temperature, catalyst mass, and molar ratio of reactants were optimized to improve the catalytic performance. The MOF that presented the highest activity and selectivity to the desired product was obtained by synthesis with ultrasound and 60 °C with ami-noterephthalic acid. The methyl levulinate yield was 67.77% in batch at 5 h and 85.89% in an auto-clave at 1 h. An analysis of the kinetic parameters of the reaction is presented. The spent material can be activated by ethanol washing allowing the catalytic activity to be maintained in the recycles.
Fil: Bravo Fuchineco, Daiana Antonella. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina
Fil: Heredia, Angelica Constanza. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina
Fil: Mendoza, Sandra Marina. Universidad Tecnológica Nacional. Facultad Regional Reconquista; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba; Argentina
Fil: Rodríguez Castellón, Enrique. Dpto. Química Inorgánica, Cristalografía y Mineralogía; España
Fil: Crivello, Mónica Elsie. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina - Materia
-
BATCH AND PRESSURE REACTIONS
ESTERIFICATION KINETICS
LEVULINIC ACID
METHYL LEVULINATE
UIO‐66
UIO‐66‐NH2 - Nivel de accesibilidad
- acceso abierto
- Condiciones de uso
- https://creativecommons.org/licenses/by/2.5/ar/
- Repositorio
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/163282
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Esterification of Levulinic Acid to Methyl Levulinate over Zr-MOFs CatalystsBravo Fuchineco, Daiana AntonellaHeredia, Angelica ConstanzaMendoza, Sandra MarinaRodríguez Castellón, EnriqueCrivello, Mónica ElsieBATCH AND PRESSURE REACTIONSESTERIFICATION KINETICSLEVULINIC ACIDMETHYL LEVULINATEUIO‐66UIO‐66‐NH2https://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2At present, the trend towards partial replacement of petroleum‐derived fuels by those from the revaluation of biomass has become of great importance. An effective strategy for pro-cessing complex biomass feedstocks involves prior conversion to simpler compounds (platform molecules) that are more easily transformed in subsequent reactions. This study analyzes the met-al–organic frameworks (MOFs) that contain Zr metal clusters formed by ligands of terephthalic acid (UiO‐66) and aminoterephthalic acid (UiO‐66‐NH2), as active and stable catalysts for the esterification of levulinic acid with methanol. An alternative synthesis is presented by means of ultrasonic stirring at room temperature and 60 °C, in order to improve the structural properties of the catalysts. They were analyzed by X‐ray diffraction, scanning electron microscopy, infrared spectroscopy, X‐ray photoelectron spectroscopy, microwave plasma atomic emission spectroscopy, acidity measurement, and N2 adsorption. The catalytic reaction was carried out in a batch system and under pressure in an autoclave. Its progress was followed by gas chromatography and mass spectrometry. Parameters such as temperature, catalyst mass, and molar ratio of reactants were optimized to improve the catalytic performance. The MOF that presented the highest activity and selectivity to the desired product was obtained by synthesis with ultrasound and 60 °C with ami-noterephthalic acid. The methyl levulinate yield was 67.77% in batch at 5 h and 85.89% in an auto-clave at 1 h. An analysis of the kinetic parameters of the reaction is presented. The spent material can be activated by ethanol washing allowing the catalytic activity to be maintained in the recycles.Fil: Bravo Fuchineco, Daiana Antonella. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; ArgentinaFil: Heredia, Angelica Constanza. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; ArgentinaFil: Mendoza, Sandra Marina. Universidad Tecnológica Nacional. Facultad Regional Reconquista; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba; ArgentinaFil: Rodríguez Castellón, Enrique. Dpto. Química Inorgánica, Cristalografía y Mineralogía; EspañaFil: Crivello, Mónica Elsie. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; ArgentinaMDPI2022-03-25info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/163282Bravo Fuchineco, Daiana Antonella; Heredia, Angelica Constanza; Mendoza, Sandra Marina; Rodríguez Castellón, Enrique; Crivello, Mónica Elsie; Esterification of Levulinic Acid to Methyl Levulinate over Zr-MOFs Catalysts; MDPI; ChemEngineering; 25-3-20222305-7084CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.3390/chemengineering6020026info:eu-repo/semantics/altIdentifier/url/https://www.mdpi.com/2305-7084/6/2/26info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T10:03:25Zoai:ri.conicet.gov.ar:11336/163282instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-03 10:03:26.794CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse |
dc.title.none.fl_str_mv |
Esterification of Levulinic Acid to Methyl Levulinate over Zr-MOFs Catalysts |
title |
Esterification of Levulinic Acid to Methyl Levulinate over Zr-MOFs Catalysts |
spellingShingle |
Esterification of Levulinic Acid to Methyl Levulinate over Zr-MOFs Catalysts Bravo Fuchineco, Daiana Antonella BATCH AND PRESSURE REACTIONS ESTERIFICATION KINETICS LEVULINIC ACID METHYL LEVULINATE UIO‐66 UIO‐66‐NH2 |
title_short |
Esterification of Levulinic Acid to Methyl Levulinate over Zr-MOFs Catalysts |
title_full |
Esterification of Levulinic Acid to Methyl Levulinate over Zr-MOFs Catalysts |
title_fullStr |
Esterification of Levulinic Acid to Methyl Levulinate over Zr-MOFs Catalysts |
title_full_unstemmed |
Esterification of Levulinic Acid to Methyl Levulinate over Zr-MOFs Catalysts |
title_sort |
Esterification of Levulinic Acid to Methyl Levulinate over Zr-MOFs Catalysts |
dc.creator.none.fl_str_mv |
Bravo Fuchineco, Daiana Antonella Heredia, Angelica Constanza Mendoza, Sandra Marina Rodríguez Castellón, Enrique Crivello, Mónica Elsie |
author |
Bravo Fuchineco, Daiana Antonella |
author_facet |
Bravo Fuchineco, Daiana Antonella Heredia, Angelica Constanza Mendoza, Sandra Marina Rodríguez Castellón, Enrique Crivello, Mónica Elsie |
author_role |
author |
author2 |
Heredia, Angelica Constanza Mendoza, Sandra Marina Rodríguez Castellón, Enrique Crivello, Mónica Elsie |
author2_role |
author author author author |
dc.subject.none.fl_str_mv |
BATCH AND PRESSURE REACTIONS ESTERIFICATION KINETICS LEVULINIC ACID METHYL LEVULINATE UIO‐66 UIO‐66‐NH2 |
topic |
BATCH AND PRESSURE REACTIONS ESTERIFICATION KINETICS LEVULINIC ACID METHYL LEVULINATE UIO‐66 UIO‐66‐NH2 |
purl_subject.fl_str_mv |
https://purl.org/becyt/ford/2.4 https://purl.org/becyt/ford/2 |
dc.description.none.fl_txt_mv |
At present, the trend towards partial replacement of petroleum‐derived fuels by those from the revaluation of biomass has become of great importance. An effective strategy for pro-cessing complex biomass feedstocks involves prior conversion to simpler compounds (platform molecules) that are more easily transformed in subsequent reactions. This study analyzes the met-al–organic frameworks (MOFs) that contain Zr metal clusters formed by ligands of terephthalic acid (UiO‐66) and aminoterephthalic acid (UiO‐66‐NH2), as active and stable catalysts for the esterification of levulinic acid with methanol. An alternative synthesis is presented by means of ultrasonic stirring at room temperature and 60 °C, in order to improve the structural properties of the catalysts. They were analyzed by X‐ray diffraction, scanning electron microscopy, infrared spectroscopy, X‐ray photoelectron spectroscopy, microwave plasma atomic emission spectroscopy, acidity measurement, and N2 adsorption. The catalytic reaction was carried out in a batch system and under pressure in an autoclave. Its progress was followed by gas chromatography and mass spectrometry. Parameters such as temperature, catalyst mass, and molar ratio of reactants were optimized to improve the catalytic performance. The MOF that presented the highest activity and selectivity to the desired product was obtained by synthesis with ultrasound and 60 °C with ami-noterephthalic acid. The methyl levulinate yield was 67.77% in batch at 5 h and 85.89% in an auto-clave at 1 h. An analysis of the kinetic parameters of the reaction is presented. The spent material can be activated by ethanol washing allowing the catalytic activity to be maintained in the recycles. Fil: Bravo Fuchineco, Daiana Antonella. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina Fil: Heredia, Angelica Constanza. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina Fil: Mendoza, Sandra Marina. Universidad Tecnológica Nacional. Facultad Regional Reconquista; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba; Argentina Fil: Rodríguez Castellón, Enrique. Dpto. Química Inorgánica, Cristalografía y Mineralogía; España Fil: Crivello, Mónica Elsie. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina |
description |
At present, the trend towards partial replacement of petroleum‐derived fuels by those from the revaluation of biomass has become of great importance. An effective strategy for pro-cessing complex biomass feedstocks involves prior conversion to simpler compounds (platform molecules) that are more easily transformed in subsequent reactions. This study analyzes the met-al–organic frameworks (MOFs) that contain Zr metal clusters formed by ligands of terephthalic acid (UiO‐66) and aminoterephthalic acid (UiO‐66‐NH2), as active and stable catalysts for the esterification of levulinic acid with methanol. An alternative synthesis is presented by means of ultrasonic stirring at room temperature and 60 °C, in order to improve the structural properties of the catalysts. They were analyzed by X‐ray diffraction, scanning electron microscopy, infrared spectroscopy, X‐ray photoelectron spectroscopy, microwave plasma atomic emission spectroscopy, acidity measurement, and N2 adsorption. The catalytic reaction was carried out in a batch system and under pressure in an autoclave. Its progress was followed by gas chromatography and mass spectrometry. Parameters such as temperature, catalyst mass, and molar ratio of reactants were optimized to improve the catalytic performance. The MOF that presented the highest activity and selectivity to the desired product was obtained by synthesis with ultrasound and 60 °C with ami-noterephthalic acid. The methyl levulinate yield was 67.77% in batch at 5 h and 85.89% in an auto-clave at 1 h. An analysis of the kinetic parameters of the reaction is presented. The spent material can be activated by ethanol washing allowing the catalytic activity to be maintained in the recycles. |
publishDate |
2022 |
dc.date.none.fl_str_mv |
2022-03-25 |
dc.type.none.fl_str_mv |
info:eu-repo/semantics/article info:eu-repo/semantics/publishedVersion http://purl.org/coar/resource_type/c_6501 info:ar-repo/semantics/articulo |
format |
article |
status_str |
publishedVersion |
dc.identifier.none.fl_str_mv |
http://hdl.handle.net/11336/163282 Bravo Fuchineco, Daiana Antonella; Heredia, Angelica Constanza; Mendoza, Sandra Marina; Rodríguez Castellón, Enrique; Crivello, Mónica Elsie; Esterification of Levulinic Acid to Methyl Levulinate over Zr-MOFs Catalysts; MDPI; ChemEngineering; 25-3-2022 2305-7084 CONICET Digital CONICET |
url |
http://hdl.handle.net/11336/163282 |
identifier_str_mv |
Bravo Fuchineco, Daiana Antonella; Heredia, Angelica Constanza; Mendoza, Sandra Marina; Rodríguez Castellón, Enrique; Crivello, Mónica Elsie; Esterification of Levulinic Acid to Methyl Levulinate over Zr-MOFs Catalysts; MDPI; ChemEngineering; 25-3-2022 2305-7084 CONICET Digital CONICET |
dc.language.none.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
info:eu-repo/semantics/altIdentifier/doi/10.3390/chemengineering6020026 info:eu-repo/semantics/altIdentifier/url/https://www.mdpi.com/2305-7084/6/2/26 |
dc.rights.none.fl_str_mv |
info:eu-repo/semantics/openAccess https://creativecommons.org/licenses/by/2.5/ar/ |
eu_rights_str_mv |
openAccess |
rights_invalid_str_mv |
https://creativecommons.org/licenses/by/2.5/ar/ |
dc.format.none.fl_str_mv |
application/pdf application/pdf |
dc.publisher.none.fl_str_mv |
MDPI |
publisher.none.fl_str_mv |
MDPI |
dc.source.none.fl_str_mv |
reponame:CONICET Digital (CONICET) instname:Consejo Nacional de Investigaciones Científicas y Técnicas |
reponame_str |
CONICET Digital (CONICET) |
collection |
CONICET Digital (CONICET) |
instname_str |
Consejo Nacional de Investigaciones Científicas y Técnicas |
repository.name.fl_str_mv |
CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas |
repository.mail.fl_str_mv |
dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar |
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1842269800534900736 |
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13.13397 |