Ultrasound-Enhanced Gelation of Stimuli-Responsive and Biocompatible Phenylalanine-Derived Hydrogels

Autores
Buxaderas, Eduardo; Moglie, Yanina Fernanda; Figueroa, Aarón Baz; Alegre Requena, Juan Vicente; Grijalvo, Santiago; Saldías, César; Pérez Herrera, Raquel; Marqués López, Eugenia; Díaz Oviedo, Christian David
Año de publicación
2025
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Stimuli-responsive materials, particularly supramolecular hydrogels, exhibit a dynamic adaptability to external factors such as pH and ultrasound. Among these, phenylalanine (Phe)-derived hydrogels are promising due to their biocompatibility, biodegradability, and tunable properties, making them ideal for biomedical applications. This study explores the effects of pH and ultrasound on the gelation properties of N-substituted Phe derivatives, with a primary focus on the role of ultrasound in optimizing the gelation process. A series of N-substituted Phe derivatives were synthesized via reductive amination and hydrolysis. Hydrogel formation was possible with two of these compounds, namely G1 and G2, using the following two methods: heating–cooling (H–C) and heating–ultrasound–cooling (H–US–C). The critical gelation concentration (CGC), gelation kinetics, thermal stability (Tgel), and viscoelastic properties were assessed. Morphological and cytotoxicity analyses were performed to confirm the suitability of these gels for biomedical applications. Both G1 and G2 derivatives demonstrated enhanced gelation under the H–US–C protocol compared to H–C, with notable reductions in CGC (up to 47%) and gelation time (by over 90%). Ultrasound-induced gels led to an improved network density and stability, while maintaining thermal reversibility and mechanical properties comparable to those of hydrogels formed without ultrasound. Cytotoxicity studies confirmed a high biocompatibility, with cell viability rates above 95% across the tested concentrations. Given the similar rheological and morphological properties of the hydrogels regardless of the preparation method, drug release experiments were performed with representative gel samples and demonstrated the efficient encapsulation and controlled release of 5-fluorouracil and methotrexate from the hydrogels, supporting their potential as pH-responsive drug delivery platforms. This study highlights the role of ultrasound as a powerful tool for accelerating and optimizing the gelation process of supramolecular hydrogels, which is particularly relevant for applications requiring rapid gel formation. The developed Phe-based hydrogels also demonstrate promising characteristics as drug delivery systems.
Fil: Buxaderas, Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; Argentina. Universidad de la Laguna. Departamento de Química Orgánica. Instituto Universitario de Bio-Orgánica "Antonio González"; España
Fil: Moglie, Yanina Fernanda. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; Argentina. Universidad de la Laguna. Departamento de Química Orgánica. Instituto Universitario de Bio-Orgánica "Antonio González"; España. Universidad de la Laguna. Departamento de Química Orgánica; España
Fil: Figueroa, Aarón Baz. Universidad de la Laguna. Departamento de Química Orgánica. Instituto Universitario de Bio-Orgánica "Antonio González"; España. Universidad de la Laguna. Departamento de Química Orgánica; España
Fil: Alegre Requena, Juan Vicente. Universidad de Zaragoza; España. Consejo Superior de Investigaciones Científicas; España
Fil: Grijalvo, Santiago. Instituto de Salud Carlos III; España
Fil: Saldías, César. Pontificia Universidad Católica de Chile; Chile
Fil: Pérez Herrera, Raquel. Universidad de Zaragoza; España. Consejo Superior de Investigaciones Científicas; España
Fil: Marqués López, Eugenia. Consejo Superior de Investigaciones Científicas; España. Universidad de Zaragoza; España
Fil: Díaz Oviedo, Christian David. Universitat Regensburg; Alemania
Materia
SUPRAMOLECULAR HYDROGEL
AMINO ACID
PHENYLALANINE
SONOGELATION
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:11336/289938
Acceder
id CONICETDig_8f144e24029a0f0e91af82233942d95d
oai_identifier_str oai:ri.conicet.gov.ar:11336/289938
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Ultrasound-Enhanced Gelation of Stimuli-Responsive and Biocompatible Phenylalanine-Derived HydrogelsBuxaderas, EduardoMoglie, Yanina FernandaFigueroa, Aarón BazAlegre Requena, Juan VicenteGrijalvo, SantiagoSaldías, CésarPérez Herrera, RaquelMarqués López, EugeniaDíaz Oviedo, Christian DavidSUPRAMOLECULAR HYDROGELAMINO ACIDPHENYLALANINESONOGELATIONhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Stimuli-responsive materials, particularly supramolecular hydrogels, exhibit a dynamic adaptability to external factors such as pH and ultrasound. Among these, phenylalanine (Phe)-derived hydrogels are promising due to their biocompatibility, biodegradability, and tunable properties, making them ideal for biomedical applications. This study explores the effects of pH and ultrasound on the gelation properties of N-substituted Phe derivatives, with a primary focus on the role of ultrasound in optimizing the gelation process. A series of N-substituted Phe derivatives were synthesized via reductive amination and hydrolysis. Hydrogel formation was possible with two of these compounds, namely G1 and G2, using the following two methods: heating–cooling (H–C) and heating–ultrasound–cooling (H–US–C). The critical gelation concentration (CGC), gelation kinetics, thermal stability (Tgel), and viscoelastic properties were assessed. Morphological and cytotoxicity analyses were performed to confirm the suitability of these gels for biomedical applications. Both G1 and G2 derivatives demonstrated enhanced gelation under the H–US–C protocol compared to H–C, with notable reductions in CGC (up to 47%) and gelation time (by over 90%). Ultrasound-induced gels led to an improved network density and stability, while maintaining thermal reversibility and mechanical properties comparable to those of hydrogels formed without ultrasound. Cytotoxicity studies confirmed a high biocompatibility, with cell viability rates above 95% across the tested concentrations. Given the similar rheological and morphological properties of the hydrogels regardless of the preparation method, drug release experiments were performed with representative gel samples and demonstrated the efficient encapsulation and controlled release of 5-fluorouracil and methotrexate from the hydrogels, supporting their potential as pH-responsive drug delivery platforms. This study highlights the role of ultrasound as a powerful tool for accelerating and optimizing the gelation process of supramolecular hydrogels, which is particularly relevant for applications requiring rapid gel formation. The developed Phe-based hydrogels also demonstrate promising characteristics as drug delivery systems.Fil: Buxaderas, Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; Argentina. Universidad de la Laguna. Departamento de Química Orgánica. Instituto Universitario de Bio-Orgánica "Antonio González"; EspañaFil: Moglie, Yanina Fernanda. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; Argentina. Universidad de la Laguna. Departamento de Química Orgánica. Instituto Universitario de Bio-Orgánica "Antonio González"; España. Universidad de la Laguna. Departamento de Química Orgánica; EspañaFil: Figueroa, Aarón Baz. Universidad de la Laguna. Departamento de Química Orgánica. Instituto Universitario de Bio-Orgánica "Antonio González"; España. Universidad de la Laguna. Departamento de Química Orgánica; EspañaFil: Alegre Requena, Juan Vicente. Universidad de Zaragoza; España. Consejo Superior de Investigaciones Científicas; EspañaFil: Grijalvo, Santiago. Instituto de Salud Carlos III; EspañaFil: Saldías, César. Pontificia Universidad Católica de Chile; ChileFil: Pérez Herrera, Raquel. Universidad de Zaragoza; España. Consejo Superior de Investigaciones Científicas; EspañaFil: Marqués López, Eugenia. Consejo Superior de Investigaciones Científicas; España. Universidad de Zaragoza; EspañaFil: Díaz Oviedo, Christian David. Universitat Regensburg; AlemaniaMultidisciplinary Digital Publishing Institute2025-02-23info: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/11336/289938Buxaderas, Eduardo; Moglie, Yanina Fernanda; Figueroa, Aarón Baz; Alegre Requena, Juan Vicente; Grijalvo, Santiago; et al.; Ultrasound-Enhanced Gelation of Stimuli-Responsive and Biocompatible Phenylalanine-Derived Hydrogels; Multidisciplinary Digital Publishing Institute; Gels; 11; 3; 23-2-2025; 1-212310-2861CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://www.mdpi.com/2310-2861/11/3/160info:eu-repo/semantics/altIdentifier/doi/ 10.3390/gels11030160info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2026-08-25T14:44:03Zoai:ri.conicet.gov.ar:11336/289938instacron: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:34982026-08-25 14:44:03.858CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Ultrasound-Enhanced Gelation of Stimuli-Responsive and Biocompatible Phenylalanine-Derived Hydrogels
title Ultrasound-Enhanced Gelation of Stimuli-Responsive and Biocompatible Phenylalanine-Derived Hydrogels
spellingShingle Ultrasound-Enhanced Gelation of Stimuli-Responsive and Biocompatible Phenylalanine-Derived Hydrogels
Buxaderas, Eduardo
SUPRAMOLECULAR HYDROGEL
AMINO ACID
PHENYLALANINE
SONOGELATION
title_short Ultrasound-Enhanced Gelation of Stimuli-Responsive and Biocompatible Phenylalanine-Derived Hydrogels
title_full Ultrasound-Enhanced Gelation of Stimuli-Responsive and Biocompatible Phenylalanine-Derived Hydrogels
title_fullStr Ultrasound-Enhanced Gelation of Stimuli-Responsive and Biocompatible Phenylalanine-Derived Hydrogels
title_full_unstemmed Ultrasound-Enhanced Gelation of Stimuli-Responsive and Biocompatible Phenylalanine-Derived Hydrogels
title_sort Ultrasound-Enhanced Gelation of Stimuli-Responsive and Biocompatible Phenylalanine-Derived Hydrogels
dc.creator.none.fl_str_mv Buxaderas, Eduardo
Moglie, Yanina Fernanda
Figueroa, Aarón Baz
Alegre Requena, Juan Vicente
Grijalvo, Santiago
Saldías, César
Pérez Herrera, Raquel
Marqués López, Eugenia
Díaz Oviedo, Christian David
author Buxaderas, Eduardo
author_facet Buxaderas, Eduardo
Moglie, Yanina Fernanda
Figueroa, Aarón Baz
Alegre Requena, Juan Vicente
Grijalvo, Santiago
Saldías, César
Pérez Herrera, Raquel
Marqués López, Eugenia
Díaz Oviedo, Christian David
author_role author
author2 Moglie, Yanina Fernanda
Figueroa, Aarón Baz
Alegre Requena, Juan Vicente
Grijalvo, Santiago
Saldías, César
Pérez Herrera, Raquel
Marqués López, Eugenia
Díaz Oviedo, Christian David
author2_role author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv SUPRAMOLECULAR HYDROGEL
AMINO ACID
PHENYLALANINE
SONOGELATION
topic SUPRAMOLECULAR HYDROGEL
AMINO ACID
PHENYLALANINE
SONOGELATION
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Stimuli-responsive materials, particularly supramolecular hydrogels, exhibit a dynamic adaptability to external factors such as pH and ultrasound. Among these, phenylalanine (Phe)-derived hydrogels are promising due to their biocompatibility, biodegradability, and tunable properties, making them ideal for biomedical applications. This study explores the effects of pH and ultrasound on the gelation properties of N-substituted Phe derivatives, with a primary focus on the role of ultrasound in optimizing the gelation process. A series of N-substituted Phe derivatives were synthesized via reductive amination and hydrolysis. Hydrogel formation was possible with two of these compounds, namely G1 and G2, using the following two methods: heating–cooling (H–C) and heating–ultrasound–cooling (H–US–C). The critical gelation concentration (CGC), gelation kinetics, thermal stability (Tgel), and viscoelastic properties were assessed. Morphological and cytotoxicity analyses were performed to confirm the suitability of these gels for biomedical applications. Both G1 and G2 derivatives demonstrated enhanced gelation under the H–US–C protocol compared to H–C, with notable reductions in CGC (up to 47%) and gelation time (by over 90%). Ultrasound-induced gels led to an improved network density and stability, while maintaining thermal reversibility and mechanical properties comparable to those of hydrogels formed without ultrasound. Cytotoxicity studies confirmed a high biocompatibility, with cell viability rates above 95% across the tested concentrations. Given the similar rheological and morphological properties of the hydrogels regardless of the preparation method, drug release experiments were performed with representative gel samples and demonstrated the efficient encapsulation and controlled release of 5-fluorouracil and methotrexate from the hydrogels, supporting their potential as pH-responsive drug delivery platforms. This study highlights the role of ultrasound as a powerful tool for accelerating and optimizing the gelation process of supramolecular hydrogels, which is particularly relevant for applications requiring rapid gel formation. The developed Phe-based hydrogels also demonstrate promising characteristics as drug delivery systems.
Fil: Buxaderas, Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; Argentina. Universidad de la Laguna. Departamento de Química Orgánica. Instituto Universitario de Bio-Orgánica "Antonio González"; España
Fil: Moglie, Yanina Fernanda. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; Argentina. Universidad de la Laguna. Departamento de Química Orgánica. Instituto Universitario de Bio-Orgánica "Antonio González"; España. Universidad de la Laguna. Departamento de Química Orgánica; España
Fil: Figueroa, Aarón Baz. Universidad de la Laguna. Departamento de Química Orgánica. Instituto Universitario de Bio-Orgánica "Antonio González"; España. Universidad de la Laguna. Departamento de Química Orgánica; España
Fil: Alegre Requena, Juan Vicente. Universidad de Zaragoza; España. Consejo Superior de Investigaciones Científicas; España
Fil: Grijalvo, Santiago. Instituto de Salud Carlos III; España
Fil: Saldías, César. Pontificia Universidad Católica de Chile; Chile
Fil: Pérez Herrera, Raquel. Universidad de Zaragoza; España. Consejo Superior de Investigaciones Científicas; España
Fil: Marqués López, Eugenia. Consejo Superior de Investigaciones Científicas; España. Universidad de Zaragoza; España
Fil: Díaz Oviedo, Christian David. Universitat Regensburg; Alemania
description Stimuli-responsive materials, particularly supramolecular hydrogels, exhibit a dynamic adaptability to external factors such as pH and ultrasound. Among these, phenylalanine (Phe)-derived hydrogels are promising due to their biocompatibility, biodegradability, and tunable properties, making them ideal for biomedical applications. This study explores the effects of pH and ultrasound on the gelation properties of N-substituted Phe derivatives, with a primary focus on the role of ultrasound in optimizing the gelation process. A series of N-substituted Phe derivatives were synthesized via reductive amination and hydrolysis. Hydrogel formation was possible with two of these compounds, namely G1 and G2, using the following two methods: heating–cooling (H–C) and heating–ultrasound–cooling (H–US–C). The critical gelation concentration (CGC), gelation kinetics, thermal stability (Tgel), and viscoelastic properties were assessed. Morphological and cytotoxicity analyses were performed to confirm the suitability of these gels for biomedical applications. Both G1 and G2 derivatives demonstrated enhanced gelation under the H–US–C protocol compared to H–C, with notable reductions in CGC (up to 47%) and gelation time (by over 90%). Ultrasound-induced gels led to an improved network density and stability, while maintaining thermal reversibility and mechanical properties comparable to those of hydrogels formed without ultrasound. Cytotoxicity studies confirmed a high biocompatibility, with cell viability rates above 95% across the tested concentrations. Given the similar rheological and morphological properties of the hydrogels regardless of the preparation method, drug release experiments were performed with representative gel samples and demonstrated the efficient encapsulation and controlled release of 5-fluorouracil and methotrexate from the hydrogels, supporting their potential as pH-responsive drug delivery platforms. This study highlights the role of ultrasound as a powerful tool for accelerating and optimizing the gelation process of supramolecular hydrogels, which is particularly relevant for applications requiring rapid gel formation. The developed Phe-based hydrogels also demonstrate promising characteristics as drug delivery systems.
publishDate 2025
dc.date.none.fl_str_mv 2025-02-23
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/11336/289938
Buxaderas, Eduardo; Moglie, Yanina Fernanda; Figueroa, Aarón Baz; Alegre Requena, Juan Vicente; Grijalvo, Santiago; et al.; Ultrasound-Enhanced Gelation of Stimuli-Responsive and Biocompatible Phenylalanine-Derived Hydrogels; Multidisciplinary Digital Publishing Institute; Gels; 11; 3; 23-2-2025; 1-21
2310-2861
CONICET Digital
CONICET
url http://hdl.handle.net/11336/289938
identifier_str_mv Buxaderas, Eduardo; Moglie, Yanina Fernanda; Figueroa, Aarón Baz; Alegre Requena, Juan Vicente; Grijalvo, Santiago; et al.; Ultrasound-Enhanced Gelation of Stimuli-Responsive and Biocompatible Phenylalanine-Derived Hydrogels; Multidisciplinary Digital Publishing Institute; Gels; 11; 3; 23-2-2025; 1-21
2310-2861
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://www.mdpi.com/2310-2861/11/3/160
info:eu-repo/semantics/altIdentifier/doi/ 10.3390/gels11030160
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
application/pdf
application/pdf
dc.publisher.none.fl_str_mv Multidisciplinary Digital Publishing Institute
publisher.none.fl_str_mv Multidisciplinary Digital Publishing Institute
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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