Tunable Self-Assembly of YF3 Nanoparticles by Citrate-Mediated Ionic Bridges

Ligand-to-surface interactions are critical factors in surface and interface chemistry to control the mechanisms governing nanostructured colloidal suspensions. In particular, molecules containing carboxylate moieties (such as citrate anions) have been extensively investigated to stabilize metal, me...

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Autores: Martínez Esaín, Jordi, Faraudo, Jordi, Puig Molina, Teresa, Obradors, Xavier, Ros, Josep, Ricart, Susagna, Yáñez, Ramón
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2018
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/159985
Acceso en línea:http://hdl.handle.net/10261/159985
Access Level:acceso abierto
Palabra clave:Self-assembly
Nanoparticles
YF3
Citrate bridge
Ionic interaction in solution
Molecular dynamics simulations
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dc.title.none.fl_str_mv Tunable Self-Assembly of YF3 Nanoparticles by Citrate-Mediated Ionic Bridges
title Tunable Self-Assembly of YF3 Nanoparticles by Citrate-Mediated Ionic Bridges
spellingShingle Tunable Self-Assembly of YF3 Nanoparticles by Citrate-Mediated Ionic Bridges
Martínez Esaín, Jordi
Self-assembly
Nanoparticles
YF3
Citrate bridge
Ionic interaction in solution
Molecular dynamics simulations
title_short Tunable Self-Assembly of YF3 Nanoparticles by Citrate-Mediated Ionic Bridges
title_full Tunable Self-Assembly of YF3 Nanoparticles by Citrate-Mediated Ionic Bridges
title_fullStr Tunable Self-Assembly of YF3 Nanoparticles by Citrate-Mediated Ionic Bridges
title_full_unstemmed Tunable Self-Assembly of YF3 Nanoparticles by Citrate-Mediated Ionic Bridges
title_sort Tunable Self-Assembly of YF3 Nanoparticles by Citrate-Mediated Ionic Bridges
dc.creator.none.fl_str_mv Martínez Esaín, Jordi
Faraudo, Jordi
Puig Molina, Teresa
Obradors, Xavier
Ros, Josep
Ricart, Susagna
Yáñez, Ramón
author Martínez Esaín, Jordi
author_facet Martínez Esaín, Jordi
Faraudo, Jordi
Puig Molina, Teresa
Obradors, Xavier
Ros, Josep
Ricart, Susagna
Yáñez, Ramón
author_role author
author2 Faraudo, Jordi
Puig Molina, Teresa
Obradors, Xavier
Ros, Josep
Ricart, Susagna
Yáñez, Ramón
author2_role author
author
author
author
author
author
dc.contributor.none.fl_str_mv Ministerio de Economía y Competitividad (España)
European Commission
Generalitat de Catalunya
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Self-assembly
Nanoparticles
YF3
Citrate bridge
Ionic interaction in solution
Molecular dynamics simulations
topic Self-assembly
Nanoparticles
YF3
Citrate bridge
Ionic interaction in solution
Molecular dynamics simulations
description Ligand-to-surface interactions are critical factors in surface and interface chemistry to control the mechanisms governing nanostructured colloidal suspensions. In particular, molecules containing carboxylate moieties (such as citrate anions) have been extensively investigated to stabilize metal, metal oxide, and metal fluoride nanoparticles. Using YF3 nanoparticles as a model system, we show here the self-assembly of citrate-stabilized nanostructures (supraparticles) with a size tunable by temperature. Results from several experimental techniques and molecular dynamics simulations show that the self-assembly of nanoparticles into supraparticles is due to ionic bridges between different nanoparticles. These interactions were caused by cations (e.g., ammonium) strongly adsorbed onto the nanoparticle surface that also interact strongly with nonbonded citrate anions, creating ionic bridges in solution between nanoparticles. Experimentally, we observe self-assembly of nanoparticles into supraparticles at 25 and 100 °C. Interestingly, at high temperatures (100 °C), this citrate-bridge self-assembly mechanism is more efficient, giving rise to larger supraparticles. At low temperatures (5 °C), this mechanism is not observed, and nanoparticles remain stable. Molecular dynamics simulations show that the free energy of a single citrate bridge between nanoparticles in solution is much larger than the thermal energy and in fact is much larger than typical adsorption free energies of ions on colloids. Summarizing our experiments and simulations, we identify as key aspects of the self-assembly mechanism the requirement of NPs with a surface able to adsorb anions and cations and the presence of multidentate ions in solution. This indicates that this new ion-mediated self-assembly mechanism is not specific of YF3 and citrate anions, as supported by preliminary experimental results in other systems.
publishDate 2018
dc.date.none.fl_str_mv 2018
2018
2018
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dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/159985
url http://hdl.handle.net/10261/159985
dc.language.none.fl_str_mv Inglés
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dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
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spelling Tunable Self-Assembly of YF3 Nanoparticles by Citrate-Mediated Ionic BridgesMartínez Esaín, JordiFaraudo, JordiPuig Molina, TeresaObradors, XavierRos, JosepRicart, SusagnaYáñez, RamónSelf-assemblyNanoparticlesYF3Citrate bridgeIonic interaction in solutionMolecular dynamics simulationsLigand-to-surface interactions are critical factors in surface and interface chemistry to control the mechanisms governing nanostructured colloidal suspensions. In particular, molecules containing carboxylate moieties (such as citrate anions) have been extensively investigated to stabilize metal, metal oxide, and metal fluoride nanoparticles. Using YF3 nanoparticles as a model system, we show here the self-assembly of citrate-stabilized nanostructures (supraparticles) with a size tunable by temperature. Results from several experimental techniques and molecular dynamics simulations show that the self-assembly of nanoparticles into supraparticles is due to ionic bridges between different nanoparticles. These interactions were caused by cations (e.g., ammonium) strongly adsorbed onto the nanoparticle surface that also interact strongly with nonbonded citrate anions, creating ionic bridges in solution between nanoparticles. Experimentally, we observe self-assembly of nanoparticles into supraparticles at 25 and 100 °C. Interestingly, at high temperatures (100 °C), this citrate-bridge self-assembly mechanism is more efficient, giving rise to larger supraparticles. At low temperatures (5 °C), this mechanism is not observed, and nanoparticles remain stable. Molecular dynamics simulations show that the free energy of a single citrate bridge between nanoparticles in solution is much larger than the thermal energy and in fact is much larger than typical adsorption free energies of ions on colloids. Summarizing our experiments and simulations, we identify as key aspects of the self-assembly mechanism the requirement of NPs with a surface able to adsorb anions and cations and the presence of multidentate ions in solution. This indicates that this new ion-mediated self-assembly mechanism is not specific of YF3 and citrate anions, as supported by preliminary experimental results in other systems.This work was supported by Spanish Ministry of Economy and Competitiveness through the “Severo Ochoa” Programme for Centres of Excellence in R&D (SEV-2015-0496), CONSOLIDER Excellence Network (MAT2015-68994-REDC), COACHSUPENERGY project (MAT2014-51778-C2-1-R, co-financed by the European Regional Development Fund) and SUPERINKS project (RTC-2015-3640-3, cofinanced by the European Regional Development Fund). We also thank support from the European Union for EUROTAPES project (FP7-NMP-Large-2011-280432) and ULTRASUPERTAPE project (H2020 ERC-2014-ADG-669504) and from the Catalan Government with 2014-SGR-753 and Xarmae. The authors acknowledge the technical support of Servei de Microscòpia, NMR Service and Servei de Difracció de Raigs-X, all at the UAB, to the Soft Materials Service and Dr. Judit Oró (Microscope Service) at the ICMAB-CSIC, Dr. Guillaume Sauthier for his support in XPS analysis, and Dr. Eduardo Solano for his scientific discussions. J.M.E. acknowledges the PIF predoctoral fellowship from the Universitat Autònoma de Barcelona. J.F. thanks CESGA Supercomputing Center for technical support and the use of computational resources. We thank Justin J. Charette for help with English usage.Peer reviewedAmerican Chemical SocietyMinisterio de Economía y Competitividad (España)European CommissionGeneralitat de CatalunyaConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]201820182018info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionhttp://hdl.handle.net/10261/159985reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/SEV-2015-0496info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/MAT2015-68994-REDCinfo:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/MAT2014-51778-C2-1-Rinfo:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/RTC-2015-3640-3info:eu-repo/grantAgreement/EC/FP7/280432info:eu-repo/grantAgreement/EC/H2020/669504http://dx.doi.org/10.1021/jacs.7b09821Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/1599852026-05-22T06:33:51Z
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