Chemically Tailored Metal-Organic Frameworks for Enhanced Capture of Short- and Long-Chain Per- and Polyfluoroalkyl Substances from Water

Per- and polyfluoroalkyl substances (PFAS) are emerging as bioaccumulative and toxic water pollutants, posing a large threat to human and aquatic organisms. This threat is aggravated by their extreme persistence to common degradation methods. Adsorption is regarded as the most conventional method to...

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Autores: Loukopoulos, Edward, Marugán-Benito, Sergio, Raptis, Dionysios, Tylianakis, Emmanuel, Froudakis, George E., Mavrandonakis, Andreas, Platero-Prats, Ana E.
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2024
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/383432
Acceso en línea:http://hdl.handle.net/10261/383432
https://api.elsevier.com/content/abstract/scopus_id/85200207069
Access Level:acceso abierto
Palabra clave:computational modelling
metal-organic frameworks
per-/polyfluoroalkyl substances
post-synthetic functionalization
water decontamination
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oai_identifier_str oai:digital.csic.es:10261/383432
network_acronym_str ES
network_name_str España
repository_id_str
dc.title.none.fl_str_mv Chemically Tailored Metal-Organic Frameworks for Enhanced Capture of Short- and Long-Chain Per- and Polyfluoroalkyl Substances from Water
title Chemically Tailored Metal-Organic Frameworks for Enhanced Capture of Short- and Long-Chain Per- and Polyfluoroalkyl Substances from Water
spellingShingle Chemically Tailored Metal-Organic Frameworks for Enhanced Capture of Short- and Long-Chain Per- and Polyfluoroalkyl Substances from Water
Loukopoulos, Edward
computational modelling
metal-organic frameworks
per-/polyfluoroalkyl substances
post-synthetic functionalization
water decontamination
title_short Chemically Tailored Metal-Organic Frameworks for Enhanced Capture of Short- and Long-Chain Per- and Polyfluoroalkyl Substances from Water
title_full Chemically Tailored Metal-Organic Frameworks for Enhanced Capture of Short- and Long-Chain Per- and Polyfluoroalkyl Substances from Water
title_fullStr Chemically Tailored Metal-Organic Frameworks for Enhanced Capture of Short- and Long-Chain Per- and Polyfluoroalkyl Substances from Water
title_full_unstemmed Chemically Tailored Metal-Organic Frameworks for Enhanced Capture of Short- and Long-Chain Per- and Polyfluoroalkyl Substances from Water
title_sort Chemically Tailored Metal-Organic Frameworks for Enhanced Capture of Short- and Long-Chain Per- and Polyfluoroalkyl Substances from Water
dc.creator.none.fl_str_mv Loukopoulos, Edward
Marugán-Benito, Sergio
Raptis, Dionysios
Tylianakis, Emmanuel
Froudakis, George E.
Mavrandonakis, Andreas
Platero-Prats, Ana E.
author Loukopoulos, Edward
author_facet Loukopoulos, Edward
Marugán-Benito, Sergio
Raptis, Dionysios
Tylianakis, Emmanuel
Froudakis, George E.
Mavrandonakis, Andreas
Platero-Prats, Ana E.
author_role author
author2 Marugán-Benito, Sergio
Raptis, Dionysios
Tylianakis, Emmanuel
Froudakis, George E.
Mavrandonakis, Andreas
Platero-Prats, Ana E.
author2_role author
author
author
author
author
author
dc.contributor.none.fl_str_mv Agencia Estatal de Investigación (España)
European Commission
European Synchrotron Radiation Facility
0000-0001-9067-9499
#NODATA#
0009-0002-6777-5364
0000-0002-1747-2106
0000-0002-6907-1822
0000-0002-5053-8154
0000-0002-2248-2739
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv computational modelling
metal-organic frameworks
per-/polyfluoroalkyl substances
post-synthetic functionalization
water decontamination
topic computational modelling
metal-organic frameworks
per-/polyfluoroalkyl substances
post-synthetic functionalization
water decontamination
description Per- and polyfluoroalkyl substances (PFAS) are emerging as bioaccumulative and toxic water pollutants, posing a large threat to human and aquatic organisms. This threat is aggravated by their extreme persistence to common degradation methods. Adsorption is regarded as the most conventional method to treat these contaminants, however, existing sorbents present considerable limitations on performance. The development of more efficient PFAS adsorbents is therefore of urgent need. The class of metal-organic frameworks (MOFs) can hold great promise for these purposes, featuring porous materials with high tailoring potential. Herein, a series of functionalized Zr-MOFs have been designed with boosted capacities for the adsorption of short- and long-chain perfluorinated carboxylic acids of environmental interest. The approach relies on chemistry-based concepts to introduce targeted post-synthetic modifications that promote PFAS···MOF interactions, specifically through coordinative bonding and hydrophobic effects. In particular, the framework TFA-MOF-808 (TFA = trifluoroacetic acid) displays the highest capture capacities reported for MOF materials in this pollutant class. Mechanistic studies, assisted by advanced synchrotron characterization techniques and theoretical calculations, support a ligand exchange process occurring during the adsorption phenomena. The results demonstrate the potential of this design approach in developing advanced PFAS sorbents with optimal performance.
publishDate 2024
dc.date.none.fl_str_mv 2024
2025
2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Publisher's version
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/383432
https://api.elsevier.com/content/abstract/scopus_id/85200207069
url http://hdl.handle.net/10261/383432
https://api.elsevier.com/content/abstract/scopus_id/85200207069
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Advanced Functional Materials
https://doi.org/10.1002/adfm.202409932
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv John Wiley & Sons
publisher.none.fl_str_mv John Wiley & Sons
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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spelling Chemically Tailored Metal-Organic Frameworks for Enhanced Capture of Short- and Long-Chain Per- and Polyfluoroalkyl Substances from WaterLoukopoulos, EdwardMarugán-Benito, SergioRaptis, DionysiosTylianakis, EmmanuelFroudakis, George E.Mavrandonakis, AndreasPlatero-Prats, Ana E.computational modellingmetal-organic frameworksper-/polyfluoroalkyl substancespost-synthetic functionalizationwater decontaminationPer- and polyfluoroalkyl substances (PFAS) are emerging as bioaccumulative and toxic water pollutants, posing a large threat to human and aquatic organisms. This threat is aggravated by their extreme persistence to common degradation methods. Adsorption is regarded as the most conventional method to treat these contaminants, however, existing sorbents present considerable limitations on performance. The development of more efficient PFAS adsorbents is therefore of urgent need. The class of metal-organic frameworks (MOFs) can hold great promise for these purposes, featuring porous materials with high tailoring potential. Herein, a series of functionalized Zr-MOFs have been designed with boosted capacities for the adsorption of short- and long-chain perfluorinated carboxylic acids of environmental interest. The approach relies on chemistry-based concepts to introduce targeted post-synthetic modifications that promote PFAS···MOF interactions, specifically through coordinative bonding and hydrophobic effects. In particular, the framework TFA-MOF-808 (TFA = trifluoroacetic acid) displays the highest capture capacities reported for MOF materials in this pollutant class. Mechanistic studies, assisted by advanced synchrotron characterization techniques and theoretical calculations, support a ligand exchange process occurring during the adsorption phenomena. The results demonstrate the potential of this design approach in developing advanced PFAS sorbents with optimal performance.This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement N°101034324. This work was supported by the grants PID2021- 123839OB-I00, RYC2018-024328-I, CNS2022-135261, and CNS2023- 143965 funded by MICIU/AEI/10.13039/501100011033 and the NextGenerationEU/ PRTR. The authors acknowledge the financial support from the Spanish Ministry of Science and Innovation, through the “María de Maeztu” Programme forUnits of Excellence in R&D(CEX2018-000805-M). The authors acknowledge the computing facilities of CSUC for providing resources that contributed to the research results reported within this paper. This work was carried out with the support of Diamond Light Source, instrument I15-1 (proposal CY34409-1) and the authors thank Dr Philip Chater for his assistance on PDF experiments. The authors acknowledge the European Synchrotron Radiation Facility (ESRF) for provision of synchrotron radiation facilities (PDF experiments, proposal MA-5852), and the authors would like to thank Stefano Checcia for assistance and support in using beamline ID15A. The authors acknowledge DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, for the provision of experimental facilities. Parts of this research were carried out at PETRAIII and the authors would like to thank Dr. Alba San Jose Mendez for assistance in using beamline P02.1. Beamtime was allocated for proposal I-20230444 EC. Spanish Ministry of Science and Innovation. Grant Number: CEX2018-000805-M European Synchrotron Radiation Facility HORIZON EUROPE Reforming and enhancing the European Research and Innovation system. Grant Number: 101034324 Agencia Estatal de Investigación. Grant Numbers: PID2021-123839OB-I00, RYC2018-024328-I, CNS2022-135261, CNS2023-143965Peer reviewedJohn Wiley & SonsAgencia Estatal de Investigación (España)European CommissionEuropean Synchrotron Radiation Facility0000-0001-9067-9499#NODATA#0009-0002-6777-53640000-0002-1747-21060000-0002-6907-18220000-0002-5053-81540000-0002-2248-2739Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202520252024info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionhttp://hdl.handle.net/10261/383432https://api.elsevier.com/content/abstract/scopus_id/85200207069reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)InglésAdvanced Functional Materialshttps://doi.org/10.1002/adfm.202409932Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3834322026-05-22T06:33:51Z
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