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Article: Supramolecular Porous Organic Nanocomposites for Heterogeneous Photocatalysis of a Sulfur Mustard Simulant

TitleSupramolecular Porous Organic Nanocomposites for Heterogeneous Photocatalysis of a Sulfur Mustard Simulant
Authors
Keywordscyclophanes
nanocomposites
photocatalysis
photosensitizers
polymers
Issue Date2020
Citation
Advanced Materials, 2020, v. 32, n. 32, article no. 2001592 How to Cite?
AbstractEfficient heterogeneous photosensitizing materials require both large accessible surface areas and excitons of suitable energies and with well-defined spin structures. Confinement of the tetracationic cyclophane (ExBox4+) within a nonporous anionic polystyrene sulfonate (PSS) matrix leads to a surface area increase of up to 225 m2 g−1 in ExBox•PSS. Efficient intersystem crossing is achieved by combining the spin-orbit coupling associated to Br heavy atoms in 1,3,5,8-tetrabromopyrene (TBP), and the photoinduced electron transfer in a TBP⊂ExBox4+ supramolecular dyad. The TBP⊂ExBox4+ complex displays a charge transfer band at 450 nm and an exciplex emission at 520 nm, indicating the formation of new mixed-electronic states. The lowest triplet state (T1, 1.89 eV) is localized on the TBP and is close in energy with the charge separated state (CT, 2.14 eV). The homogeneous and heterogeneous photocatalytic activities of the TBP⊂ExBox4+, for the elimination of a sulfur mustard simulant, has proved to be significantly more efficient than TBP and ExBox+4, confirming the importance of the newly formed excited-state manifold in TBP⊂ExBox4+ for the population of the low-lying T1 state. The high stability, facile preparation, and high performance of the TBP⊂ExBox•PSS nanocomposites augur well for the future development of new supramolecular heterogeneous photosensitizers using host–guest chemistry.
Persistent Identifierhttp://hdl.handle.net/10722/333445
ISSN
2023 Impact Factor: 27.4
2023 SCImago Journal Rankings: 9.191
ISI Accession Number ID

 

DC FieldValueLanguage
dc.contributor.authorBeldjoudi, Yassine-
dc.contributor.authorAtilgan, Ahmet-
dc.contributor.authorWeber, Jacob A.-
dc.contributor.authorRoy, Indranil-
dc.contributor.authorYoung, Ryan M.-
dc.contributor.authorYu, Jierui-
dc.contributor.authorDeria, Pravas-
dc.contributor.authorEnciso, Alan E.-
dc.contributor.authorWasielewski, Michael R.-
dc.contributor.authorHupp, Joseph T.-
dc.contributor.authorStoddart, J. Fraser-
dc.date.accessioned2023-10-06T05:19:26Z-
dc.date.available2023-10-06T05:19:26Z-
dc.date.issued2020-
dc.identifier.citationAdvanced Materials, 2020, v. 32, n. 32, article no. 2001592-
dc.identifier.issn0935-9648-
dc.identifier.urihttp://hdl.handle.net/10722/333445-
dc.description.abstractEfficient heterogeneous photosensitizing materials require both large accessible surface areas and excitons of suitable energies and with well-defined spin structures. Confinement of the tetracationic cyclophane (ExBox4+) within a nonporous anionic polystyrene sulfonate (PSS) matrix leads to a surface area increase of up to 225 m2 g−1 in ExBox•PSS. Efficient intersystem crossing is achieved by combining the spin-orbit coupling associated to Br heavy atoms in 1,3,5,8-tetrabromopyrene (TBP), and the photoinduced electron transfer in a TBP⊂ExBox4+ supramolecular dyad. The TBP⊂ExBox4+ complex displays a charge transfer band at 450 nm and an exciplex emission at 520 nm, indicating the formation of new mixed-electronic states. The lowest triplet state (T1, 1.89 eV) is localized on the TBP and is close in energy with the charge separated state (CT, 2.14 eV). The homogeneous and heterogeneous photocatalytic activities of the TBP⊂ExBox4+, for the elimination of a sulfur mustard simulant, has proved to be significantly more efficient than TBP and ExBox+4, confirming the importance of the newly formed excited-state manifold in TBP⊂ExBox4+ for the population of the low-lying T1 state. The high stability, facile preparation, and high performance of the TBP⊂ExBox•PSS nanocomposites augur well for the future development of new supramolecular heterogeneous photosensitizers using host–guest chemistry.-
dc.languageeng-
dc.relation.ispartofAdvanced Materials-
dc.subjectcyclophanes-
dc.subjectnanocomposites-
dc.subjectphotocatalysis-
dc.subjectphotosensitizers-
dc.subjectpolymers-
dc.titleSupramolecular Porous Organic Nanocomposites for Heterogeneous Photocatalysis of a Sulfur Mustard Simulant-
dc.typeArticle-
dc.description.naturelink_to_subscribed_fulltext-
dc.identifier.doi10.1002/adma.202001592-
dc.identifier.pmid32602131-
dc.identifier.scopuseid_2-s2.0-85087204818-
dc.identifier.volume32-
dc.identifier.issue32-
dc.identifier.spagearticle no. 2001592-
dc.identifier.epagearticle no. 2001592-
dc.identifier.eissn1521-4095-
dc.identifier.isiWOS:000543976000001-

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