File Download

There are no files associated with this item.

  Links for fulltext
     (May Require Subscription)
Supplementary

Article: Electrochemically addressable trisradical rotaxanes organized within a metal-organic framework

TitleElectrochemically addressable trisradical rotaxanes organized within a metal-organic framework
Authors
KeywordsMechanically interlocked molecules
Metal-organic framework
Molecular switches
Radicals
Rotaxanes
Issue Date2015
Citation
Proceedings of the National Academy of Sciences of the United States of America, 2015, v. 112, n. 36, p. 11161-11168 How to Cite?
AbstractThe organization of trisradical rotaxanes within the channels of a Zr6-based metal-organic framework (NU-1000) has been achieved postsynthetically by solvent-assisted ligand incorporation. Robust ZrIV-carboxylate bonds are forged between the Zr clusters of NU-1000 and carboxylic acid groups of rotaxane precursors (semirotaxanes) as part of this building block replacement strategy. Ultraviolet-visible-near-infrared (UV-Vis-NIR), electron paramagnetic resonance (EPR), and 1H nuclear magnetic resonance (NMR) spectroscopies all confirm the capture of redox-active rotaxanes within the mesoscale hexagonal channels of NU-1000. Cyclic voltammetry measurements performed on electroactive thin films of the resulting material indicate that redox-active viologen subunits located on the rotaxane components can be accessed electrochemically in the solid state. In contradistinction to previous methods, this strategy for the incorporation of mechanically interlocked molecules within porousmaterials circumvents the need for de novo synthesis of a metal-organic framework, making it a particularly convenient approach for the design and creation of solid-state molecular switches and machines. The results presented here provide proof-of-concept for the application of postsynthetic transformations in the integration of dynamic molecular machines with robust porous frameworks.
Persistent Identifierhttp://hdl.handle.net/10722/333686
ISSN
2023 Impact Factor: 9.4
2023 SCImago Journal Rankings: 3.737
ISI Accession Number ID

 

DC FieldValueLanguage
dc.contributor.authorMcGonigal, Paul R.-
dc.contributor.authorDeria, Pravas-
dc.contributor.authorHod, Idan-
dc.contributor.authorMoghadam, Peyman Z.-
dc.contributor.authorAvestro, Alyssa Jennifer-
dc.contributor.authorHorwitz, Noah E.-
dc.contributor.authorGibbs-Hall, Ian C.-
dc.contributor.authorBlackburn, Anthea K.-
dc.contributor.authorChen, Dongyang-
dc.contributor.authorBotros, Youssry Y.-
dc.contributor.authorWasielewski, Michael R.-
dc.contributor.authorSnurr, Randall Q.-
dc.contributor.authorHupp, Joseph T.-
dc.contributor.authorFarha, Omar K.-
dc.contributor.authorStoddart, J. Fraser-
dc.date.accessioned2023-10-06T05:21:36Z-
dc.date.available2023-10-06T05:21:36Z-
dc.date.issued2015-
dc.identifier.citationProceedings of the National Academy of Sciences of the United States of America, 2015, v. 112, n. 36, p. 11161-11168-
dc.identifier.issn0027-8424-
dc.identifier.urihttp://hdl.handle.net/10722/333686-
dc.description.abstractThe organization of trisradical rotaxanes within the channels of a Zr<inf>6</inf>-based metal-organic framework (NU-1000) has been achieved postsynthetically by solvent-assisted ligand incorporation. Robust Zr<sup>IV</sup>-carboxylate bonds are forged between the Zr clusters of NU-1000 and carboxylic acid groups of rotaxane precursors (semirotaxanes) as part of this building block replacement strategy. Ultraviolet-visible-near-infrared (UV-Vis-NIR), electron paramagnetic resonance (EPR), and <sup>1</sup>H nuclear magnetic resonance (NMR) spectroscopies all confirm the capture of redox-active rotaxanes within the mesoscale hexagonal channels of NU-1000. Cyclic voltammetry measurements performed on electroactive thin films of the resulting material indicate that redox-active viologen subunits located on the rotaxane components can be accessed electrochemically in the solid state. In contradistinction to previous methods, this strategy for the incorporation of mechanically interlocked molecules within porousmaterials circumvents the need for de novo synthesis of a metal-organic framework, making it a particularly convenient approach for the design and creation of solid-state molecular switches and machines. The results presented here provide proof-of-concept for the application of postsynthetic transformations in the integration of dynamic molecular machines with robust porous frameworks.-
dc.languageeng-
dc.relation.ispartofProceedings of the National Academy of Sciences of the United States of America-
dc.subjectMechanically interlocked molecules-
dc.subjectMetal-organic framework-
dc.subjectMolecular switches-
dc.subjectRadicals-
dc.subjectRotaxanes-
dc.titleElectrochemically addressable trisradical rotaxanes organized within a metal-organic framework-
dc.typeArticle-
dc.description.naturelink_to_subscribed_fulltext-
dc.identifier.doi10.1073/pnas.1514485112-
dc.identifier.scopuseid_2-s2.0-84941242282-
dc.identifier.volume112-
dc.identifier.issue36-
dc.identifier.spage11161-
dc.identifier.epage11168-
dc.identifier.eissn1091-6490-
dc.identifier.isiWOS:000360994900028-

Export via OAI-PMH Interface in XML Formats


OR


Export to Other Non-XML Formats