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
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/136639
Ver los metadatos del registro completo
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CONICET Digital (CONICET) |
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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 |
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CONICET Digital (CONICET) |
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CONICET Digital (CONICET) |
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Consejo Nacional de Investigaciones Científicas y Técnicas |
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CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas |
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dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar |
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13.22299 |