Insights into mechanochemical reactions at the molecular level: Simulated indentations of aspirin and meloxicam crystals

Autores
Ferguson, Michael; Moyano, María Silvina; Tribello, Gareth A.; Crawford, Deborah E.; Bringa, Eduardo Marcial; James, Stuart L.; Kohanoff, Jorge; del Popolo, Mario Gabriel
Año de publicación
2019
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Although solvent-free mechanochemical synthesis continues to gain ever greater importance, the molecular scale processes that occur during such reactions remain largely uncharacterised. Here, we apply computational modelling to indentations between particles of crystals of aspirin and meloxicam under a variety of conditions to mimic the early stages of their mechanochemical cocrystallisation reaction. The study also extends to the effects of the presence of small amounts of solvent. It is found that, despite the solid crystalline nature of the reactants and the presence of little or no solvent, mixing occurs readily at the molecular level even during relatively low-energy collisions. When indented crystals are subsequently drawn apart, a connective neck formed by a mixture of the reactant molecules is observed, suggesting plastic-like behaviour of the reacting materials. Overall the work reveals some striking new insights including (i) relatively facile mixing of crystals under solvent-free conditions, (ii) no appreciable local temperature increases, (iii) localised amorphisation at the contact region and neck of the reacting crystals, and (iv) small amounts of solvent have relatively little effect during this early stage of the reaction, suggesting that their accelerating effect on the reaction may be exerted at later stages.
Fil: Ferguson, Michael. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; Argentina. The Queens University of Belfast; Irlanda
Fil: Moyano, María Silvina. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; Argentina
Fil: Tribello, Gareth A.. The Queens University of Belfast; Irlanda
Fil: Crawford, Deborah E.. The Queens University of Belfast; Irlanda
Fil: Bringa, Eduardo Marcial. Universidad de Mendoza. Facultad de Ingenieria; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; Argentina
Fil: James, Stuart L.. The Queens University of Belfast; Irlanda
Fil: Kohanoff, Jorge. The Queens University of Belfast; Irlanda
Fil: del Popolo, Mario Gabriel. The Queens University of Belfast; Irlanda. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; Argentina
Materia
MECHANOCHEMISTRY
CO-CRYSTALLISATION
MOLECULAR DYNAMICS
COMPUTER SIMULATION
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/136639
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/136639
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Insights into mechanochemical reactions at the molecular level: Simulated indentations of aspirin and meloxicam crystalsFerguson, MichaelMoyano, María SilvinaTribello, Gareth A.Crawford, Deborah E.Bringa, Eduardo MarcialJames, Stuart L.Kohanoff, Jorgedel Popolo, Mario GabrielMECHANOCHEMISTRYCO-CRYSTALLISATIONMOLECULAR DYNAMICSCOMPUTER SIMULATIONhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Although solvent-free mechanochemical synthesis continues to gain ever greater importance, the molecular scale processes that occur during such reactions remain largely uncharacterised. Here, we apply computational modelling to indentations between particles of crystals of aspirin and meloxicam under a variety of conditions to mimic the early stages of their mechanochemical cocrystallisation reaction. The study also extends to the effects of the presence of small amounts of solvent. It is found that, despite the solid crystalline nature of the reactants and the presence of little or no solvent, mixing occurs readily at the molecular level even during relatively low-energy collisions. When indented crystals are subsequently drawn apart, a connective neck formed by a mixture of the reactant molecules is observed, suggesting plastic-like behaviour of the reacting materials. Overall the work reveals some striking new insights including (i) relatively facile mixing of crystals under solvent-free conditions, (ii) no appreciable local temperature increases, (iii) localised amorphisation at the contact region and neck of the reacting crystals, and (iv) small amounts of solvent have relatively little effect during this early stage of the reaction, suggesting that their accelerating effect on the reaction may be exerted at later stages.Fil: Ferguson, Michael. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; Argentina. The Queens University of Belfast; IrlandaFil: Moyano, María Silvina. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; ArgentinaFil: Tribello, Gareth A.. The Queens University of Belfast; IrlandaFil: Crawford, Deborah E.. The Queens University of Belfast; IrlandaFil: Bringa, Eduardo Marcial. Universidad de Mendoza. Facultad de Ingenieria; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; ArgentinaFil: James, Stuart L.. The Queens University of Belfast; IrlandaFil: Kohanoff, Jorge. The Queens University of Belfast; IrlandaFil: del Popolo, Mario Gabriel. The Queens University of Belfast; Irlanda. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; ArgentinaRoyal Society of Chemistry2019-01info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/136639Ferguson, Michael; Moyano, María Silvina; Tribello, Gareth A.; Crawford, Deborah E.; Bringa, Eduardo Marcial; et al.; Insights into mechanochemical reactions at the molecular level: Simulated indentations of aspirin and meloxicam crystals; Royal Society of Chemistry; Chemical Science; 10; 10; 1-2019; 2924-29292041-6520CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://xlink.rsc.org/?DOI=C8SC04971Hinfo:eu-repo/semantics/altIdentifier/doi/10.1039/c8sc04971hinfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T15:15:33Zoai:ri.conicet.gov.ar:11336/136639instacron: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:34982025-10-15 15:15:33.481CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Insights into mechanochemical reactions at the molecular level: Simulated indentations of aspirin and meloxicam crystals
title Insights into mechanochemical reactions at the molecular level: Simulated indentations of aspirin and meloxicam crystals
spellingShingle Insights into mechanochemical reactions at the molecular level: Simulated indentations of aspirin and meloxicam crystals
Ferguson, Michael
MECHANOCHEMISTRY
CO-CRYSTALLISATION
MOLECULAR DYNAMICS
COMPUTER SIMULATION
title_short Insights into mechanochemical reactions at the molecular level: Simulated indentations of aspirin and meloxicam crystals
title_full Insights into mechanochemical reactions at the molecular level: Simulated indentations of aspirin and meloxicam crystals
title_fullStr Insights into mechanochemical reactions at the molecular level: Simulated indentations of aspirin and meloxicam crystals
title_full_unstemmed Insights into mechanochemical reactions at the molecular level: Simulated indentations of aspirin and meloxicam crystals
title_sort Insights into mechanochemical reactions at the molecular level: Simulated indentations of aspirin and meloxicam crystals
dc.creator.none.fl_str_mv Ferguson, Michael
Moyano, María Silvina
Tribello, Gareth A.
Crawford, Deborah E.
Bringa, Eduardo Marcial
James, Stuart L.
Kohanoff, Jorge
del Popolo, Mario Gabriel
author Ferguson, Michael
author_facet Ferguson, Michael
Moyano, María Silvina
Tribello, Gareth A.
Crawford, Deborah E.
Bringa, Eduardo Marcial
James, Stuart L.
Kohanoff, Jorge
del Popolo, Mario Gabriel
author_role author
author2 Moyano, María Silvina
Tribello, Gareth A.
Crawford, Deborah E.
Bringa, Eduardo Marcial
James, Stuart L.
Kohanoff, Jorge
del Popolo, Mario Gabriel
author2_role author
author
author
author
author
author
author
dc.subject.none.fl_str_mv MECHANOCHEMISTRY
CO-CRYSTALLISATION
MOLECULAR DYNAMICS
COMPUTER SIMULATION
topic MECHANOCHEMISTRY
CO-CRYSTALLISATION
MOLECULAR DYNAMICS
COMPUTER SIMULATION
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Although solvent-free mechanochemical synthesis continues to gain ever greater importance, the molecular scale processes that occur during such reactions remain largely uncharacterised. Here, we apply computational modelling to indentations between particles of crystals of aspirin and meloxicam under a variety of conditions to mimic the early stages of their mechanochemical cocrystallisation reaction. The study also extends to the effects of the presence of small amounts of solvent. It is found that, despite the solid crystalline nature of the reactants and the presence of little or no solvent, mixing occurs readily at the molecular level even during relatively low-energy collisions. When indented crystals are subsequently drawn apart, a connective neck formed by a mixture of the reactant molecules is observed, suggesting plastic-like behaviour of the reacting materials. Overall the work reveals some striking new insights including (i) relatively facile mixing of crystals under solvent-free conditions, (ii) no appreciable local temperature increases, (iii) localised amorphisation at the contact region and neck of the reacting crystals, and (iv) small amounts of solvent have relatively little effect during this early stage of the reaction, suggesting that their accelerating effect on the reaction may be exerted at later stages.
Fil: Ferguson, Michael. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; Argentina. The Queens University of Belfast; Irlanda
Fil: Moyano, María Silvina. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; Argentina
Fil: Tribello, Gareth A.. The Queens University of Belfast; Irlanda
Fil: Crawford, Deborah E.. The Queens University of Belfast; Irlanda
Fil: Bringa, Eduardo Marcial. Universidad de Mendoza. Facultad de Ingenieria; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; Argentina
Fil: James, Stuart L.. The Queens University of Belfast; Irlanda
Fil: Kohanoff, Jorge. The Queens University of Belfast; Irlanda
Fil: del Popolo, Mario Gabriel. The Queens University of Belfast; Irlanda. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; Argentina
description Although solvent-free mechanochemical synthesis continues to gain ever greater importance, the molecular scale processes that occur during such reactions remain largely uncharacterised. Here, we apply computational modelling to indentations between particles of crystals of aspirin and meloxicam under a variety of conditions to mimic the early stages of their mechanochemical cocrystallisation reaction. The study also extends to the effects of the presence of small amounts of solvent. It is found that, despite the solid crystalline nature of the reactants and the presence of little or no solvent, mixing occurs readily at the molecular level even during relatively low-energy collisions. When indented crystals are subsequently drawn apart, a connective neck formed by a mixture of the reactant molecules is observed, suggesting plastic-like behaviour of the reacting materials. Overall the work reveals some striking new insights including (i) relatively facile mixing of crystals under solvent-free conditions, (ii) no appreciable local temperature increases, (iii) localised amorphisation at the contact region and neck of the reacting crystals, and (iv) small amounts of solvent have relatively little effect during this early stage of the reaction, suggesting that their accelerating effect on the reaction may be exerted at later stages.
publishDate 2019
dc.date.none.fl_str_mv 2019-01
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/11336/136639
Ferguson, Michael; Moyano, María Silvina; Tribello, Gareth A.; Crawford, Deborah E.; Bringa, Eduardo Marcial; et al.; Insights into mechanochemical reactions at the molecular level: Simulated indentations of aspirin and meloxicam crystals; Royal Society of Chemistry; Chemical Science; 10; 10; 1-2019; 2924-2929
2041-6520
CONICET Digital
CONICET
url http://hdl.handle.net/11336/136639
identifier_str_mv Ferguson, Michael; Moyano, María Silvina; Tribello, Gareth A.; Crawford, Deborah E.; Bringa, Eduardo Marcial; et al.; Insights into mechanochemical reactions at the molecular level: Simulated indentations of aspirin and meloxicam crystals; Royal Society of Chemistry; Chemical Science; 10; 10; 1-2019; 2924-2929
2041-6520
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://xlink.rsc.org/?DOI=C8SC04971H
info:eu-repo/semantics/altIdentifier/doi/10.1039/c8sc04971h
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv Royal Society of Chemistry
publisher.none.fl_str_mv Royal Society of Chemistry
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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score 13.22299

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