Computational Modeling of Supramolecular Metallo-organic Cages-Challenges and Opportunities

[EN] Self-assembled metallo-organic cages have emerged as promising biomimetic platforms that can encapsulate whole substrates akin to an enzyme active site. Extensive experimental work has enabled access to a variety of structures, with a few notable examples showing catalytic behavior. However, co...

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Autores: Piskorz, Tomasz K., Young, Tom A., Lusby, Paul J., Duarte, Fernanda, Martí-Centelles, Vicente|||0000-0002-9142-9392
Formato: artículo
Fecha de publicación:2022
País:España
Recursos:Universitat Politècnica de València (UPV)
Repositorio:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
Idioma:inglés
OAI Identifier:oai:riunet.upv.es:10251/192036
Acesso em linha:https://riunet.upv.es/handle/10251/192036
Access Level:acceso abierto
Palavra-chave:Supramolecular chemistry
Metallo-organic cages
Computational modeling
Biomimetic catalysis
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spelling Computational Modeling of Supramolecular Metallo-organic Cages-Challenges and OpportunitiesPiskorz, Tomasz K.Young, Tom A.Lusby, Paul J.Duarte, FernandaMartí-Centelles, Vicente|||0000-0002-9142-9392Supramolecular chemistryMetallo-organic cagesComputational modelingBiomimetic catalysis[EN] Self-assembled metallo-organic cages have emerged as promising biomimetic platforms that can encapsulate whole substrates akin to an enzyme active site. Extensive experimental work has enabled access to a variety of structures, with a few notable examples showing catalytic behavior. However, computational investigations of metallo-organic cages are scarce, not least due to the challenges associated with their modeling and the lack of accurate and efficient protocols to evaluate these systems. In this review, we discuss key molecular principles governing the design of functional metallo-organic cages, from the assembly of building blocks through binding and catalysis. For each of these processes, computational protocols will be reviewed, considering their inherent strengths and weaknesses. We will demonstrate that while each approach may have its own specific pitfalls, they can be a powerful tool for rationalizing experimental observables and to guide synthetic efforts. To illustrate this point, we present several examples where modeling has helped to elucidate fundamental principles behind molecular recognition and reactivity. We highlight the importance of combining computational and experimental efforts to speed up supramolecular catalyst design while reducing time and resources.T.K.P., P.J.L., and F.D. acknowledge the financial support from EPSRC (EP/W010666/1 and EP/W009803/1). T.K.P. and F.D. acknowledge the financial support from the John Fell Fund (ref 0006752). V.M.-C. acknowledges the financial support from Generalitat Valenciana (CIDEGENT/2020/031). T.A.Y. acknowledges the impact acceleration account (IAA) grant (EP/R511742/1).American Chemical SocietyEscuela Técnica Superior de Ingeniería Aeroespacial y Diseño IndustrialDepartamento de QuímicaInstituto Interuniversitario de Investigación de Reconocimiento Molecular y Desarrollo TecnológicoGENERALITAT VALENCIANAEngineering and Physical Sciences Research Council, Reino UnidoRepositorio Institucional de la Universitat Politècnica de València Riunet20222022-05-20journal articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttps://riunet.upv.es/handle/10251/192036reponame:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valénciainstname:Universitat Politècnica de València (UPV)InglésengGeneralitat Valenciana https://doi.org/10.13039/501100003359 CIDEGENT%2F2020%2F031 CAJAS ORGANICAS COMO CONTENEDORES PARA LIBERACION DIRIGIDA DE FARMACOS EN TERAPIA CONTRA EL CANCEREngineering and Physical Sciences Research Council, Reino Unido https://doi.org/10.13039/501100000266 EP%2FW010666%2F1Engineering and Physical Sciences Research Council, Reino Unido https://doi.org/10.13039/501100000266 EP%2FW009803%2F1Engineering and Physical Sciences Research Council, Reino Unido https://doi.org/10.13039/501100000266 EP%2FR511742%2F1open accesshttp://purl.org/coar/access_right/c_abf2Reconocimiento (by)http://creativecommons.org/licenses/by/4.0/info:eu-repo/semantics/openAccessoai:riunet.upv.es:10251/1920362026-06-13T07:49:27Z
dc.title.none.fl_str_mv Computational Modeling of Supramolecular Metallo-organic Cages-Challenges and Opportunities
title Computational Modeling of Supramolecular Metallo-organic Cages-Challenges and Opportunities
spellingShingle Computational Modeling of Supramolecular Metallo-organic Cages-Challenges and Opportunities
Piskorz, Tomasz K.
Supramolecular chemistry
Metallo-organic cages
Computational modeling
Biomimetic catalysis
title_short Computational Modeling of Supramolecular Metallo-organic Cages-Challenges and Opportunities
title_full Computational Modeling of Supramolecular Metallo-organic Cages-Challenges and Opportunities
title_fullStr Computational Modeling of Supramolecular Metallo-organic Cages-Challenges and Opportunities
title_full_unstemmed Computational Modeling of Supramolecular Metallo-organic Cages-Challenges and Opportunities
title_sort Computational Modeling of Supramolecular Metallo-organic Cages-Challenges and Opportunities
dc.creator.none.fl_str_mv Piskorz, Tomasz K.
Young, Tom A.
Lusby, Paul J.
Duarte, Fernanda
Martí-Centelles, Vicente|||0000-0002-9142-9392
author Piskorz, Tomasz K.
author_facet Piskorz, Tomasz K.
Young, Tom A.
Lusby, Paul J.
Duarte, Fernanda
Martí-Centelles, Vicente|||0000-0002-9142-9392
author_role author
author2 Young, Tom A.
Lusby, Paul J.
Duarte, Fernanda
Martí-Centelles, Vicente|||0000-0002-9142-9392
author2_role author
author
author
author
dc.contributor.none.fl_str_mv Escuela Técnica Superior de Ingeniería Aeroespacial y Diseño Industrial
Departamento de Química
Instituto Interuniversitario de Investigación de Reconocimiento Molecular y Desarrollo Tecnológico
GENERALITAT VALENCIANA
Engineering and Physical Sciences Research Council, Reino Unido
Repositorio Institucional de la Universitat Politècnica de València Riunet
dc.subject.none.fl_str_mv Supramolecular chemistry
Metallo-organic cages
Computational modeling
Biomimetic catalysis
topic Supramolecular chemistry
Metallo-organic cages
Computational modeling
Biomimetic catalysis
description [EN] Self-assembled metallo-organic cages have emerged as promising biomimetic platforms that can encapsulate whole substrates akin to an enzyme active site. Extensive experimental work has enabled access to a variety of structures, with a few notable examples showing catalytic behavior. However, computational investigations of metallo-organic cages are scarce, not least due to the challenges associated with their modeling and the lack of accurate and efficient protocols to evaluate these systems. In this review, we discuss key molecular principles governing the design of functional metallo-organic cages, from the assembly of building blocks through binding and catalysis. For each of these processes, computational protocols will be reviewed, considering their inherent strengths and weaknesses. We will demonstrate that while each approach may have its own specific pitfalls, they can be a powerful tool for rationalizing experimental observables and to guide synthetic efforts. To illustrate this point, we present several examples where modeling has helped to elucidate fundamental principles behind molecular recognition and reactivity. We highlight the importance of combining computational and experimental efforts to speed up supramolecular catalyst design while reducing time and resources.
publishDate 2022
dc.date.none.fl_str_mv 2022
2022-05-20
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://riunet.upv.es/handle/10251/192036
url https://riunet.upv.es/handle/10251/192036
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.relation.none.fl_str_mv Generalitat Valenciana https://doi.org/10.13039/501100003359 CIDEGENT%2F2020%2F031 CAJAS ORGANICAS COMO CONTENEDORES PARA LIBERACION DIRIGIDA DE FARMACOS EN TERAPIA CONTRA EL CANCER
Engineering and Physical Sciences Research Council, Reino Unido https://doi.org/10.13039/501100000266 EP%2FW010666%2F1
Engineering and Physical Sciences Research Council, Reino Unido https://doi.org/10.13039/501100000266 EP%2FW009803%2F1
Engineering and Physical Sciences Research Council, Reino Unido https://doi.org/10.13039/501100000266 EP%2FR511742%2F1
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
Reconocimiento (by)
http://creativecommons.org/licenses/by/4.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
Reconocimiento (by)
http://creativecommons.org/licenses/by/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
instname:Universitat Politècnica de València (UPV)
instname_str Universitat Politècnica de València (UPV)
reponame_str RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
collection RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
repository.name.fl_str_mv
repository.mail.fl_str_mv
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