Degradation of Glyphosate to Benign N ‐Formyl Glycine Using MOF‐808 Nanocrystals

Autores
Peña Prada, Jhair A.; Huertas Navarro, Tatiana Alejandra; Chua, Stephanie L.; Granados, Alejandro Manuel; Pao, Chih Wen; Fracaroli, Alejandro Matías; Bedford, Nicholas M.
Año de publicación
2025
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Glyphosate (N-phosphonomethyl glycine, GPh) is an industrial herbicide used worldwide in modern agricultural practices. With the growing concerns about cumulative environmental and health ef-fects, pathways for catalytic GPh degradation to benign products are becoming a pressing societal need. This report demonstrates that Zr-based metal-organic framework (MOF-808) with different crystal sizes and designed defect sites can be employed as an efficient heterogeneous catalyst for the complete degradation of GPh at room temperature. Importantly, the degradation mechanism produces N−formyl glycine and hydroxymethyl-phosphonate, which are largely innocuous chemicals, especially when compared to more common decomposition products that typically result in GPh degradation. Nanocrystalline MOF−808 (nMOF−808) exhibits en-hanced reactivity than larger MOF-808 crystals, attributed to the higher coordination of hydroxyl and water molecules to the second-ary building units (SBU) as determined using a range of X-ray ab-sorption spectroscopy (XAS) techniques. These studies indicate that the crystal size-dependency in GPh degradation is related to structural modifications on coordinative unsaturated Zr site that promote the fast exchange of weakly bonded ligands. Taken to-gether, this study demonstrates that GPh degradation can be opti-mized through ligand field tuning in MOFs, which can help improve overall reactivity while also pushing the reaction toward desirable, non-toxic products.
Fil: Peña Prada, Jhair A.. University of New South Wales. Faculty of Science; Australia
Fil: Huertas Navarro, Tatiana Alejandra. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Departamento de Química Orgánica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Chua, Stephanie L.. University of New South Wales. Faculty of Science; Australia
Fil: Granados, Alejandro Manuel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Departamento de Química Orgánica; Argentina
Fil: Pao, Chih Wen. National Synchrotron Radiation Research Center; China
Fil: Fracaroli, Alejandro Matías. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Departamento de Química Orgánica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Bedford, Nicholas M.. University of New South Wales. Faculty of Science; Australia
Materia
Metal-Organic Frameworks
nMOF-808
Glyphosate Degradation
Heterogeneous Catalysis
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/279958
Acceder
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repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Degradation of Glyphosate to Benign N ‐Formyl Glycine Using MOF‐808 NanocrystalsPeña Prada, Jhair A.Huertas Navarro, Tatiana AlejandraChua, Stephanie L.Granados, Alejandro ManuelPao, Chih WenFracaroli, Alejandro MatíasBedford, Nicholas M.Metal-Organic FrameworksnMOF-808Glyphosate DegradationHeterogeneous Catalysishttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Glyphosate (N-phosphonomethyl glycine, GPh) is an industrial herbicide used worldwide in modern agricultural practices. With the growing concerns about cumulative environmental and health ef-fects, pathways for catalytic GPh degradation to benign products are becoming a pressing societal need. This report demonstrates that Zr-based metal-organic framework (MOF-808) with different crystal sizes and designed defect sites can be employed as an efficient heterogeneous catalyst for the complete degradation of GPh at room temperature. Importantly, the degradation mechanism produces N−formyl glycine and hydroxymethyl-phosphonate, which are largely innocuous chemicals, especially when compared to more common decomposition products that typically result in GPh degradation. Nanocrystalline MOF−808 (nMOF−808) exhibits en-hanced reactivity than larger MOF-808 crystals, attributed to the higher coordination of hydroxyl and water molecules to the second-ary building units (SBU) as determined using a range of X-ray ab-sorption spectroscopy (XAS) techniques. These studies indicate that the crystal size-dependency in GPh degradation is related to structural modifications on coordinative unsaturated Zr site that promote the fast exchange of weakly bonded ligands. Taken to-gether, this study demonstrates that GPh degradation can be opti-mized through ligand field tuning in MOFs, which can help improve overall reactivity while also pushing the reaction toward desirable, non-toxic products.Fil: Peña Prada, Jhair A.. University of New South Wales. Faculty of Science; AustraliaFil: Huertas Navarro, Tatiana Alejandra. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Departamento de Química Orgánica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; ArgentinaFil: Chua, Stephanie L.. University of New South Wales. Faculty of Science; AustraliaFil: Granados, Alejandro Manuel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Departamento de Química Orgánica; ArgentinaFil: Pao, Chih Wen. National Synchrotron Radiation Research Center; ChinaFil: Fracaroli, Alejandro Matías. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Departamento de Química Orgánica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; ArgentinaFil: Bedford, Nicholas M.. University of New South Wales. Faculty of Science; AustraliaWiley VCH Verlag2025-02info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/279958Peña Prada, Jhair A.; Huertas Navarro, Tatiana Alejandra; Chua, Stephanie L.; Granados, Alejandro Manuel; Pao, Chih Wen; et al.; Degradation of Glyphosate to Benign N ‐Formyl Glycine Using MOF‐808 Nanocrystals; Wiley VCH Verlag; Angewandte Chemie; 64; 21; 2-2025; 1-101433-7851CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://onlinelibrary.wiley.com/journal/15213773info:eu-repo/semantics/altIdentifier/doi/10.1002/anie.202424540info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2026-02-06T12:37:41Zoai:ri.conicet.gov.ar:11336/279958instacron: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:34982026-02-06 12:37:41.62CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Degradation of Glyphosate to Benign N ‐Formyl Glycine Using MOF‐808 Nanocrystals
title Degradation of Glyphosate to Benign N ‐Formyl Glycine Using MOF‐808 Nanocrystals
spellingShingle Degradation of Glyphosate to Benign N ‐Formyl Glycine Using MOF‐808 Nanocrystals
Peña Prada, Jhair A.
Metal-Organic Frameworks
nMOF-808
Glyphosate Degradation
Heterogeneous Catalysis
title_short Degradation of Glyphosate to Benign N ‐Formyl Glycine Using MOF‐808 Nanocrystals
title_full Degradation of Glyphosate to Benign N ‐Formyl Glycine Using MOF‐808 Nanocrystals
title_fullStr Degradation of Glyphosate to Benign N ‐Formyl Glycine Using MOF‐808 Nanocrystals
title_full_unstemmed Degradation of Glyphosate to Benign N ‐Formyl Glycine Using MOF‐808 Nanocrystals
title_sort Degradation of Glyphosate to Benign N ‐Formyl Glycine Using MOF‐808 Nanocrystals
dc.creator.none.fl_str_mv Peña Prada, Jhair A.
Huertas Navarro, Tatiana Alejandra
Chua, Stephanie L.
Granados, Alejandro Manuel
Pao, Chih Wen
Fracaroli, Alejandro Matías
Bedford, Nicholas M.
author Peña Prada, Jhair A.
author_facet Peña Prada, Jhair A.
Huertas Navarro, Tatiana Alejandra
Chua, Stephanie L.
Granados, Alejandro Manuel
Pao, Chih Wen
Fracaroli, Alejandro Matías
Bedford, Nicholas M.
author_role author
author2 Huertas Navarro, Tatiana Alejandra
Chua, Stephanie L.
Granados, Alejandro Manuel
Pao, Chih Wen
Fracaroli, Alejandro Matías
Bedford, Nicholas M.
author2_role author
author
author
author
author
author
dc.subject.none.fl_str_mv Metal-Organic Frameworks
nMOF-808
Glyphosate Degradation
Heterogeneous Catalysis
topic Metal-Organic Frameworks
nMOF-808
Glyphosate Degradation
Heterogeneous Catalysis
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Glyphosate (N-phosphonomethyl glycine, GPh) is an industrial herbicide used worldwide in modern agricultural practices. With the growing concerns about cumulative environmental and health ef-fects, pathways for catalytic GPh degradation to benign products are becoming a pressing societal need. This report demonstrates that Zr-based metal-organic framework (MOF-808) with different crystal sizes and designed defect sites can be employed as an efficient heterogeneous catalyst for the complete degradation of GPh at room temperature. Importantly, the degradation mechanism produces N−formyl glycine and hydroxymethyl-phosphonate, which are largely innocuous chemicals, especially when compared to more common decomposition products that typically result in GPh degradation. Nanocrystalline MOF−808 (nMOF−808) exhibits en-hanced reactivity than larger MOF-808 crystals, attributed to the higher coordination of hydroxyl and water molecules to the second-ary building units (SBU) as determined using a range of X-ray ab-sorption spectroscopy (XAS) techniques. These studies indicate that the crystal size-dependency in GPh degradation is related to structural modifications on coordinative unsaturated Zr site that promote the fast exchange of weakly bonded ligands. Taken to-gether, this study demonstrates that GPh degradation can be opti-mized through ligand field tuning in MOFs, which can help improve overall reactivity while also pushing the reaction toward desirable, non-toxic products.
Fil: Peña Prada, Jhair A.. University of New South Wales. Faculty of Science; Australia
Fil: Huertas Navarro, Tatiana Alejandra. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Departamento de Química Orgánica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Chua, Stephanie L.. University of New South Wales. Faculty of Science; Australia
Fil: Granados, Alejandro Manuel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Departamento de Química Orgánica; Argentina
Fil: Pao, Chih Wen. National Synchrotron Radiation Research Center; China
Fil: Fracaroli, Alejandro Matías. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Departamento de Química Orgánica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Bedford, Nicholas M.. University of New South Wales. Faculty of Science; Australia
description Glyphosate (N-phosphonomethyl glycine, GPh) is an industrial herbicide used worldwide in modern agricultural practices. With the growing concerns about cumulative environmental and health ef-fects, pathways for catalytic GPh degradation to benign products are becoming a pressing societal need. This report demonstrates that Zr-based metal-organic framework (MOF-808) with different crystal sizes and designed defect sites can be employed as an efficient heterogeneous catalyst for the complete degradation of GPh at room temperature. Importantly, the degradation mechanism produces N−formyl glycine and hydroxymethyl-phosphonate, which are largely innocuous chemicals, especially when compared to more common decomposition products that typically result in GPh degradation. Nanocrystalline MOF−808 (nMOF−808) exhibits en-hanced reactivity than larger MOF-808 crystals, attributed to the higher coordination of hydroxyl and water molecules to the second-ary building units (SBU) as determined using a range of X-ray ab-sorption spectroscopy (XAS) techniques. These studies indicate that the crystal size-dependency in GPh degradation is related to structural modifications on coordinative unsaturated Zr site that promote the fast exchange of weakly bonded ligands. Taken to-gether, this study demonstrates that GPh degradation can be opti-mized through ligand field tuning in MOFs, which can help improve overall reactivity while also pushing the reaction toward desirable, non-toxic products.
publishDate 2025
dc.date.none.fl_str_mv 2025-02
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/11336/279958
Peña Prada, Jhair A.; Huertas Navarro, Tatiana Alejandra; Chua, Stephanie L.; Granados, Alejandro Manuel; Pao, Chih Wen; et al.; Degradation of Glyphosate to Benign N ‐Formyl Glycine Using MOF‐808 Nanocrystals; Wiley VCH Verlag; Angewandte Chemie; 64; 21; 2-2025; 1-10
1433-7851
CONICET Digital
CONICET
url http://hdl.handle.net/11336/279958
identifier_str_mv Peña Prada, Jhair A.; Huertas Navarro, Tatiana Alejandra; Chua, Stephanie L.; Granados, Alejandro Manuel; Pao, Chih Wen; et al.; Degradation of Glyphosate to Benign N ‐Formyl Glycine Using MOF‐808 Nanocrystals; Wiley VCH Verlag; Angewandte Chemie; 64; 21; 2-2025; 1-10
1433-7851
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
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info:eu-repo/semantics/altIdentifier/doi/10.1002/anie.202424540
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 Wiley VCH Verlag
publisher.none.fl_str_mv Wiley VCH Verlag
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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