dc.contributor.author | Broto-Ribas, Anna | |
dc.contributor.author | Vignatti, Claudia | |
dc.contributor.author | Jimenez-Almarza, Alicia | |
dc.contributor.author | Luis Barrera, Javier | |
dc.contributor.author | Dolatkhah, Zahra | |
dc.contributor.author | Gándara, Felipe | |
dc.contributor.author | Imaz, Inhar | |
dc.contributor.author | Mas Ballesté, Rubén | |
dc.contributor.author | Alemán Lara, José Julián | |
dc.contributor.author | Maspoch, Daniel | |
dc.contributor.other | UAM. Departamento de Química Inorgánica | es_ES |
dc.contributor.other | UAM. Departamento de Química Orgánica | es_ES |
dc.date.accessioned | 2021-10-27T14:56:52Z | |
dc.date.available | 2021-10-27T14:56:52Z | |
dc.date.issued | 2020-04-15 | |
dc.identifier.citation | Nano Research 14.2 (2020): 458-465 | en_US |
dc.identifier.issn | 1998-0124 (print) | en_US |
dc.identifier.issn | 1998-0000 (online) | en_US |
dc.identifier.uri | http://hdl.handle.net/10486/698454 | |
dc.description | Título del post-print: Rational design of heterogeneous catalysts with programmable topologies by reticulation of organocatalysts into metal-organic frameworks: the case of squaramide | en_US |
dc.description.abstract | A well-established strategy to synthesize heterogeneous, metal-organic framework (MOF) catalysts that exhibit nanoconfinement effects, and specific pores with highly-localized catalytic sites, is to use organic linkers containing organocatalytic centers. Here, we report that by combining this linker approach with reticular chemistry, and exploiting three-dimensioanl (3D) MOF-structural data from the Cambridge Structural Database, we have designed four heterogeneous MOF-based catalysts for standard organic transformations. These programmable MOFs are isoreticular versions of pcu IRMOF-16, fcu UiO-68 and pillared-pcu SNU-8X, the three most common topologies of MOFs built from the organic linker p,p’-terphenyldicarboxylic acid (tpdc). To synthesize the four squaramide-based MOFs, we designed and synthesized a linker, 4,4’-((3,4‐dioxocyclobut‐1‐ene‐1,2‐diyl)bis(azanedyil))dibenzoic acid (Sq_tpdc), which is identical in directionality and length to tpdc but which contains organocatalytic squaramide centers. Squaramides were chosen because their immobilization into a framework enhances its reactivity and stability while avoiding any self-quenching phenomena. Therefore, the four MOFs share the same organocatalytic squaramide moiety, but confine it within distinct pore environments. We then evaluated these MOFs as heterogeneous H-bonding catalysts in organic transformations: a Friedel-Crafts alkylation and an epoxide ring-opening. Some of them exhibited good performance in both reactions but all showed distinct catalytic profiles that reflect their structural differences | en_US |
dc.description.sponsorship | This work was supported by the Spanish MINECO (projects RTI2018-095622-B-I00 and RTI2018-095038-B-I00), the Catalan AGAUR (project 2017 SGR 238), the ERC under the EU FP7 (ERC−Co 615954), European Union’s Horizon 2020 research and innovation program under grant agreement No. 685727, and European Structural Funds (S2018/NMT-4367). It was also funded by the CERCA Program/Generalitat de Catalunya. ICN2 is supported by the Severo Ochoa program from the Spanish MINECO (Grant No. SEV-2017-0706) | en_US |
dc.format.extent | 23 pag. | es_ES |
dc.format.mimetype | application/pdf | es_ES |
dc.language.iso | eng | es_ES |
dc.publisher | Springer Verlag | es_ES |
dc.relation.ispartof | Nano Research | en_US |
dc.rights | © 2020 Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature | en_US |
dc.subject.other | Friedel-Crafts | en_US |
dc.subject.other | H-bond catalysis | en_US |
dc.subject.other | Epoxide ring-opening | en_US |
dc.subject.other | Metal-organic frameworks | en_US |
dc.subject.other | Reticular chemistry | en_US |
dc.subject.other | Squaramide | en_US |
dc.title | Heterogeneous catalysts with programmable topologies generated by reticulation of organocatalysts into metal-organic frameworks: the case of squaramide | en_US |
dc.type | article | en_US |
dc.subject.eciencia | Química | es_ES |
dc.date.embargoend | 2021-04-15 | |
dc.relation.publisherversion | https://doi.org/10.1007/s12274-020-2779-8 | es_ES |
dc.identifier.doi | 10.1007/s12274-020-2779-8 | es_ES |
dc.identifier.publicationfirstpage | 458 | es_ES |
dc.identifier.publicationissue | 2 | es_ES |
dc.identifier.publicationlastpage | 465 | es_ES |
dc.identifier.publicationvolume | 14 | es_ES |
dc.relation.projectID | Gobierno de España. RTI2018-095622-B-I00 | es_ES |
dc.relation.projectID | Gobierno de España. RTI2018-095038-B-I00 | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/EC/FP7/615954/EU//InanoMOF | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/EC/H2020/685727/EU//ProDIA | es_ES |
dc.relation.projectID | Comunidad de Madrid. S2018/NMT-4367/FotoArt-CM | es_ES |
dc.relation.projectID | Gobierno de España. SEV-2017-0706 | es_ES |
dc.type.version | info:eu-repo/semantics/acceptedVersion | en |
dc.rights.accessRights | openAccess | es_ES |
dc.authorUAM | Jiménez Almarza, Alicia (278945) | |
dc.authorUAM | Mas Balleste, Rubén (261764) | |
dc.authorUAM | Aleman Lara, José Julián (262855) | |
dc.facultadUAM | Facultad de Ciencias | |
dc.institutoUAM | Instituto de Investigación Avanzada en Ciencias Químicas (IAdChem) | |