Autor según el artículo: Sole-Daura, Albert; Poblet, Josep M.; Carbo, Jorge J.;

Departamento: Química Física i Inorgànica

Autor/es de la URV: Carbó Martin, Jorge Juan / Poblet Rius, Josep Maria

Palabras clave: Water Structure–activity relationships Structure-activity relationships Selective hydrolysis Protein interactions Polyoxometalates Molecular-dynamics simulations Molecular dynamics Inhibitors Human serum-albumin Egg-white lysozyme Crystallography Charge Chaotropic anions Bond hydrolysis Binding-affinity protein interactions polyoxometalates molecular dynamics chaotropic anions

Resumen: The influence of the composition of chaotropic polyoxometalate (POM) anions on their affinity to biological systems was studied by means of atomistic molecular dynamics (MD) simulations. The variations in the affinity to hen egg-white lysozyme (HEWL) were analyzed along two series of POMs whereby the charge or the size and shape of the metal cluster are modified systematically. Our simulations revealed a quadratic relationship between the charge of the POM and its affinity to HEWL as a consequence of the parabolic growth of POM...water interaction with the charge. As the charge increases, POMs become less chaotropic (more kosmotropic) increasing the number and the strength of POM-water hydrogen bonds and structuring the solvation shell around the POM. This atomistic description explains the proportionally larger desolvation energies and less protein affinity for highly charged POMs, and consequently, the preference for moderate charge densities (q/M=0.33). Also, our simulations suggest that POM...protein interactions are size-specific. The cationic pockets of HEWL protein show a preference for Keggin-like structures, which display the optimal dimensions (approximate to 1 nm). Finally, we developed a quantitative multidimensional model for protein affinity with predictive ability (r(2)=0.97; q(2)=0.88) using two molecular descriptors that account for the charge density (charge per metal atom ratio; q/M) and the size and shape (shape weighted-volume; V-S).

Áreas temáticas: Química Organic chemistry Medicina i Materiais Interdisciplinar General medicine General chemistry Farmacia Engenharias iii Engenharias ii Ciências biológicas iii Ciências biológicas ii Ciências biológicas i Ciências agrárias i Chemistry, multidisciplinary Chemistry (miscellaneous) Chemistry (all) Chemistry Catalysis Biotecnología Biodiversidade Astronomia / física

Acceso a la licencia de uso: https://creativecommons.org/licenses/by/3.0/es/

ISSN: 15213765

Direcció de correo del autor: j.carbo@urv.cat josepmaria.poblet@urv.cat

Identificador del autor: 0000-0002-3945-6721 0000-0002-4533-0623

Fecha de alta del registro: 2023-07-31

Versión del articulo depositado: info:eu-repo/semantics/acceptedVersion

Enlace a la fuente original: https://chemistry-europe.onlinelibrary.wiley.com/doi/abs/10.1002/chem.201905533

URL Documento de licencia: http://repositori.urv.cat/ca/proteccio-de-dades/

Referencia al articulo segun fuente origial: Chemistry-A European Journal. 26 (26): 5799-5809

Referencia de l'ítem segons les normes APA: Sole-Daura, Albert; Poblet, Josep M.; Carbo, Jorge J.; (2020). Structure-Activity Relationships for the Affinity of Chaotropic Polyoxometalate Anions towards Proteins. Chemistry-A European Journal, 26(26), 5799-5809. DOI: 10.1002/chem.201905533

DOI del artículo: 10.1002/chem.201905533

Entidad: Universitat Rovira i Virgili

Año de publicación de la revista: 2020

Tipo de publicación: Journal Publications