Single-molecule profiling of per- and polyfluoroalkyl substances by cyclodextrin mediated host-guest interactions within a biological nanopore

Autores
Wei, Xiaojun; Choudhary, Aditya; Wang, Leon Y.; Yang, Lixing; Uline, Mark J.; Tagliazucchi, Mario Eugenio; Wang, Qian; Bedrov, Dmitry; Liu, Chang
Año de publicación
2024
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Biological nanopores are increasingly used in molecular sensing due to their single-molecule sensitivity. Thedetection of per- and polyfluoroalkyl substances (PFAS) like perfluorooctanoic acid and perfluorooctane sulfonicacid is critical due to their environmental prevalence and toxicity. Here, we investigate selective interactionsbetween PFAS and four cyclodextrin (CD) variants (α- , β- , γ- , and 2- hydroxypropyl- γ-CD) within an α- hemolysinnanopore. We demonstrate that PFAS molecules can be electrochemically sensed by interacting with a γ-CD in ananopore. Using HP-γ- CDs with increased steric resistance, we can identify homologs of the perfluoroalkylcarboxylic acid and the perfluoroalkyl sulfonic acid families and detect common PFAS in drinking water at 0.4 to2 parts per million levels, which are further lowered to 400 parts per trillion by sample preconcentration. Moleculardynamics simulations reveal the underlying chemical mechanism of PFAS-CD interactions. These insights pave theway toward nanopore-based in situ detection with promises in environmental protection against PFAS pollution.
Fil: Wei, Xiaojun. University of South Carolina; Estados Unidos
Fil: Choudhary, Aditya. University of Utah; Estados Unidos
Fil: Wang, Leon Y.. University of South Carolina; Estados Unidos
Fil: Yang, Lixing. University of Melbourne; Australia
Fil: Uline, Mark J.. University of South Carolina; Estados Unidos
Fil: Tagliazucchi, Mario Eugenio. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; Argentina
Fil: Wang, Qian. University of South Carolina; Estados Unidos
Fil: Bedrov, Dmitry. University of Utah; Estados Unidos
Fil: Liu, Chang. University of South Carolina; Estados Unidos
Materia
Nanopore
Perfluoroalkyl sulfonic acid
Cyclodextrin
Ion transport
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/268476
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/268476
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Single-molecule profiling of per- and polyfluoroalkyl substances by cyclodextrin mediated host-guest interactions within a biological nanoporeWei, XiaojunChoudhary, AdityaWang, Leon Y.Yang, LixingUline, Mark J.Tagliazucchi, Mario EugenioWang, QianBedrov, DmitryLiu, ChangNanoporePerfluoroalkyl sulfonic acidCyclodextrinIon transporthttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Biological nanopores are increasingly used in molecular sensing due to their single-molecule sensitivity. Thedetection of per- and polyfluoroalkyl substances (PFAS) like perfluorooctanoic acid and perfluorooctane sulfonicacid is critical due to their environmental prevalence and toxicity. Here, we investigate selective interactionsbetween PFAS and four cyclodextrin (CD) variants (α- , β- , γ- , and 2- hydroxypropyl- γ-CD) within an α- hemolysinnanopore. We demonstrate that PFAS molecules can be electrochemically sensed by interacting with a γ-CD in ananopore. Using HP-γ- CDs with increased steric resistance, we can identify homologs of the perfluoroalkylcarboxylic acid and the perfluoroalkyl sulfonic acid families and detect common PFAS in drinking water at 0.4 to2 parts per million levels, which are further lowered to 400 parts per trillion by sample preconcentration. Moleculardynamics simulations reveal the underlying chemical mechanism of PFAS-CD interactions. These insights pave theway toward nanopore-based in situ detection with promises in environmental protection against PFAS pollution.Fil: Wei, Xiaojun. University of South Carolina; Estados UnidosFil: Choudhary, Aditya. University of Utah; Estados UnidosFil: Wang, Leon Y.. University of South Carolina; Estados UnidosFil: Yang, Lixing. University of Melbourne; AustraliaFil: Uline, Mark J.. University of South Carolina; Estados UnidosFil: Tagliazucchi, Mario Eugenio. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; ArgentinaFil: Wang, Qian. University of South Carolina; Estados UnidosFil: Bedrov, Dmitry. University of Utah; Estados UnidosFil: Liu, Chang. University of South Carolina; Estados UnidosScience Advances is the American Association for the Advancement of Science2024-11info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/268476Wei, Xiaojun; Choudhary, Aditya; Wang, Leon Y.; Yang, Lixing; Uline, Mark J.; et al.; Single-molecule profiling of per- and polyfluoroalkyl substances by cyclodextrin mediated host-guest interactions within a biological nanopore; Science Advances is the American Association for the Advancement of Science; Science Advances; 10; 45; 11-2024; 1-162375-2548CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://www.science.org/doi/10.1126/sciadv.adp8134info:eu-repo/semantics/altIdentifier/doi/10.1126/sciadv.adp8134info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-17T11:10:05Zoai:ri.conicet.gov.ar:11336/268476instacron: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:34982025-09-17 11:10:05.827CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Single-molecule profiling of per- and polyfluoroalkyl substances by cyclodextrin mediated host-guest interactions within a biological nanopore
title Single-molecule profiling of per- and polyfluoroalkyl substances by cyclodextrin mediated host-guest interactions within a biological nanopore
spellingShingle Single-molecule profiling of per- and polyfluoroalkyl substances by cyclodextrin mediated host-guest interactions within a biological nanopore
Wei, Xiaojun
Nanopore
Perfluoroalkyl sulfonic acid
Cyclodextrin
Ion transport
title_short Single-molecule profiling of per- and polyfluoroalkyl substances by cyclodextrin mediated host-guest interactions within a biological nanopore
title_full Single-molecule profiling of per- and polyfluoroalkyl substances by cyclodextrin mediated host-guest interactions within a biological nanopore
title_fullStr Single-molecule profiling of per- and polyfluoroalkyl substances by cyclodextrin mediated host-guest interactions within a biological nanopore
title_full_unstemmed Single-molecule profiling of per- and polyfluoroalkyl substances by cyclodextrin mediated host-guest interactions within a biological nanopore
title_sort Single-molecule profiling of per- and polyfluoroalkyl substances by cyclodextrin mediated host-guest interactions within a biological nanopore
dc.creator.none.fl_str_mv Wei, Xiaojun
Choudhary, Aditya
Wang, Leon Y.
Yang, Lixing
Uline, Mark J.
Tagliazucchi, Mario Eugenio
Wang, Qian
Bedrov, Dmitry
Liu, Chang
author Wei, Xiaojun
author_facet Wei, Xiaojun
Choudhary, Aditya
Wang, Leon Y.
Yang, Lixing
Uline, Mark J.
Tagliazucchi, Mario Eugenio
Wang, Qian
Bedrov, Dmitry
Liu, Chang
author_role author
author2 Choudhary, Aditya
Wang, Leon Y.
Yang, Lixing
Uline, Mark J.
Tagliazucchi, Mario Eugenio
Wang, Qian
Bedrov, Dmitry
Liu, Chang
author2_role author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Nanopore
Perfluoroalkyl sulfonic acid
Cyclodextrin
Ion transport
topic Nanopore
Perfluoroalkyl sulfonic acid
Cyclodextrin
Ion transport
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Biological nanopores are increasingly used in molecular sensing due to their single-molecule sensitivity. Thedetection of per- and polyfluoroalkyl substances (PFAS) like perfluorooctanoic acid and perfluorooctane sulfonicacid is critical due to their environmental prevalence and toxicity. Here, we investigate selective interactionsbetween PFAS and four cyclodextrin (CD) variants (α- , β- , γ- , and 2- hydroxypropyl- γ-CD) within an α- hemolysinnanopore. We demonstrate that PFAS molecules can be electrochemically sensed by interacting with a γ-CD in ananopore. Using HP-γ- CDs with increased steric resistance, we can identify homologs of the perfluoroalkylcarboxylic acid and the perfluoroalkyl sulfonic acid families and detect common PFAS in drinking water at 0.4 to2 parts per million levels, which are further lowered to 400 parts per trillion by sample preconcentration. Moleculardynamics simulations reveal the underlying chemical mechanism of PFAS-CD interactions. These insights pave theway toward nanopore-based in situ detection with promises in environmental protection against PFAS pollution.
Fil: Wei, Xiaojun. University of South Carolina; Estados Unidos
Fil: Choudhary, Aditya. University of Utah; Estados Unidos
Fil: Wang, Leon Y.. University of South Carolina; Estados Unidos
Fil: Yang, Lixing. University of Melbourne; Australia
Fil: Uline, Mark J.. University of South Carolina; Estados Unidos
Fil: Tagliazucchi, Mario Eugenio. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; Argentina
Fil: Wang, Qian. University of South Carolina; Estados Unidos
Fil: Bedrov, Dmitry. University of Utah; Estados Unidos
Fil: Liu, Chang. University of South Carolina; Estados Unidos
description Biological nanopores are increasingly used in molecular sensing due to their single-molecule sensitivity. Thedetection of per- and polyfluoroalkyl substances (PFAS) like perfluorooctanoic acid and perfluorooctane sulfonicacid is critical due to their environmental prevalence and toxicity. Here, we investigate selective interactionsbetween PFAS and four cyclodextrin (CD) variants (α- , β- , γ- , and 2- hydroxypropyl- γ-CD) within an α- hemolysinnanopore. We demonstrate that PFAS molecules can be electrochemically sensed by interacting with a γ-CD in ananopore. Using HP-γ- CDs with increased steric resistance, we can identify homologs of the perfluoroalkylcarboxylic acid and the perfluoroalkyl sulfonic acid families and detect common PFAS in drinking water at 0.4 to2 parts per million levels, which are further lowered to 400 parts per trillion by sample preconcentration. Moleculardynamics simulations reveal the underlying chemical mechanism of PFAS-CD interactions. These insights pave theway toward nanopore-based in situ detection with promises in environmental protection against PFAS pollution.
publishDate 2024
dc.date.none.fl_str_mv 2024-11
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/11336/268476
Wei, Xiaojun; Choudhary, Aditya; Wang, Leon Y.; Yang, Lixing; Uline, Mark J.; et al.; Single-molecule profiling of per- and polyfluoroalkyl substances by cyclodextrin mediated host-guest interactions within a biological nanopore; Science Advances is the American Association for the Advancement of Science; Science Advances; 10; 45; 11-2024; 1-16
2375-2548
CONICET Digital
CONICET
url http://hdl.handle.net/11336/268476
identifier_str_mv Wei, Xiaojun; Choudhary, Aditya; Wang, Leon Y.; Yang, Lixing; Uline, Mark J.; et al.; Single-molecule profiling of per- and polyfluoroalkyl substances by cyclodextrin mediated host-guest interactions within a biological nanopore; Science Advances is the American Association for the Advancement of Science; Science Advances; 10; 45; 11-2024; 1-16
2375-2548
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.science.org/doi/10.1126/sciadv.adp8134
info:eu-repo/semantics/altIdentifier/doi/10.1126/sciadv.adp8134
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv Science Advances is the American Association for the Advancement of Science
publisher.none.fl_str_mv Science Advances is the American Association for the Advancement of Science
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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score 13.001348

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