Heterochirality restricts the self-assembly of phenylalanine dipeptides capped with highly aromatic groups

The influence of stereochemistry on the self-assembly of phenylalanine (Phe) dipeptides bearing aromatic fluorenyl groups at both the N- and C-termini (Fmoc, OFm) has been investigated. For this purpose, Fmoc–d-Phe–l-Phe–OFm and Fmoc–l-Phe–l-Phe–OFm have been examined considering a wide variety of s...

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Detalles Bibliográficos
Autores: Gil, Ana M., Casanovas Salas, Jordi|||0000-0002-4914-9194, Jimenez Sanz, Ana Isabel, Puiggalí Bellalta, Jordi|||0000-0002-0640-4474, Alemán Llansó, Carlos|||0000-0003-4462-6075
Tipo de recurso: artículo
Fecha de publicación:2020
País:España
Institución:Universitat Politècnica de Catalunya (UPC)
Repositorio:UPCommons. Portal del coneixement obert de la UPC
Idioma:inglés
OAI Identifier:oai:upcommons.upc.edu:2117/335756
Acceso en línea:https://hdl.handle.net/2117/335756
https://dx.doi.org/10.1021/acs.jpcb.0c04513
Access Level:acceso abierto
Palabra clave:Chemistry, Physical and theoretical
Fisicoquímica
Àrees temàtiques de la UPC::Enginyeria química
Descripción
Sumario:The influence of stereochemistry on the self-assembly of phenylalanine (Phe) dipeptides bearing aromatic fluorenyl groups at both the N- and C-termini (Fmoc, OFm) has been investigated. For this purpose, Fmoc–d-Phe–l-Phe–OFm and Fmoc–l-Phe–l-Phe–OFm have been examined considering a wide variety of solvents, which differ in dielectric constant and volatility. Results reveal that replacement of l-Phe by d-Phe has a major impact on the self-assembly propensities, restricting drastically the structural diversity and polymorphism shown by the homochiral dipeptide. Thus, the analogous heterochiral dipeptide shows a great propensity to form micro/nanofibers, independently of the environmental conditions. Theoretical calculations revealed that the stability of antiparallel disposition is much higher (a factor of ca. 15) for Fmoc–d-Phe–l-Phe–OFm than that for Fmoc–l-Phe–l-Phe–OFm, which has been attributed to the hydrophobic core formed in the former. Overall, results suggest that control of the backbone chirality is a potent and versatile strategy to drive and finely tune the self-assembly propensities of highly aromatic peptides.