Defect-Engineered Ruthenium MOFs as Versatile Heterogeneous Hydrogenation Catalysts

dc.contributor.affiliationInstituto Universitario Mixto de Tecnología Química
dc.contributor.authorEpp, Konstantines_ES
dc.contributor.authorLuz, Ignacioes_ES
dc.contributor.authorHeinz, Werner R.es_ES
dc.contributor.authorRapeyko, Anastasia
dc.contributor.authorLlabrés i Xamena, Francesc Xavier
dc.contributor.authorFischer, Roland A.es_ES
dc.contributor.funderDeutsche Forschungsgemeinschaftes_ES
dc.contributor.funderGesellschaft Deutscher Chemikeres_ES
dc.contributor.funderTechnische Universität Münchenes_ES
dc.contributor.funderMinisterio de Economía y Competitividades_ES
dc.contributor.funderAgencia Estatal de Investigaciónes_ES
dc.date.accessioned2021-04-17T03:33:09Z
dc.date.available2021-04-17T03:33:09Z
dc.date.issued2020-03-19es_ES
dc.description.abstract[EN] Ruthenium MOF [Ru-3(BTC)(2)Y-y] . G(g) (BTC=benzene-1,3,5-tricarboxylate; Y=counter ions=Cl-, OH-, OAc-; G=guest molecules=HOAc, H2O) is modified via a mixed-linker approach, using mixtures of BTC and pyridine-3,5-dicarboxylate (PYDC) linkers, triggering structural defects at the distinct Ru-2 paddlewheel (PW) nodes. This defect-engineering leads to enhanced catalytic properties due to the formation of partially reduced Ru-2-nodes. Application of a hydrogen pre-treatment protocol to the Ru-MOFs, leads to a further boost in catalytic activity. We study the benefits of (1) defect engineering and (2) hydrogen pre-treatment on the catalytic activity of Ru-MOFs in the Meerwein-Ponndorf-Verley reaction and the isomerization of allylic alcohols to saturated ketones. Simple solvent washing could not avoid catalyst deactivation during recycling for the latter reaction, while hydrogen treatment prior to each catalytic run proved to facilitate materials recyclability with constant activity over five runs.en_EN
dc.description.accrualMethodSes_ES
dc.description.bibliographicCitationEpp, K.; Luz, I.; Heinz, WR.; Rapeyko, A.; Llabrés I Xamena, FX.; Fischer, RA. (2020). Defect-Engineered Ruthenium MOFs as Versatile Heterogeneous Hydrogenation Catalysts. ChemCatChem. 12(6):1720-1725. https://doi.org/10.1002/cctc.201902079es_ES
dc.description.issue6es_ES
dc.description.referencesGascon, J., Corma, A., Kapteijn, F., & Llabrés i Xamena, F. X. (2013). Metal Organic Framework Catalysis: Quo vadis? ACS Catalysis, 4(2), 361-378. doi:10.1021/cs400959kes_ES
dc.description.referencesHasegawa, S., Horike, S., Matsuda, R., Furukawa, S., Mochizuki, K., Kinoshita, Y., & Kitagawa, S. (2007). Three-Dimensional Porous Coordination Polymer Functionalized with Amide Groups Based on Tridentate Ligand:  Selective Sorption and Catalysis. Journal of the American Chemical Society, 129(9), 2607-2614. doi:10.1021/ja067374yes_ES
dc.description.referencesWang, Z., & Cohen, S. M. (2009). Postsynthetic modification of metal–organic frameworks. Chemical Society Reviews, 38(5), 1315. doi:10.1039/b802258pes_ES
dc.description.referencesVermoortele, F., Bueken, B., Le Bars, G., Van de Voorde, B., Vandichel, M., Houthoofd, K., … De Vos, D. E. (2013). Synthesis Modulation as a Tool To Increase the Catalytic Activity of Metal–Organic Frameworks: The Unique Case of UiO-66(Zr). Journal of the American Chemical Society, 135(31), 11465-11468. doi:10.1021/ja405078ues_ES
dc.description.referencesZheng, J., Ye, J., Ortuño, M. A., Fulton, J. L., Gutiérrez, O. Y., Camaioni, D. M., … Lercher, J. A. (2019). Selective Methane Oxidation to Methanol on Cu-Oxo Dimers Stabilized by Zirconia Nodes of an NU-1000 Metal–Organic Framework. Journal of the American Chemical Society, 141(23), 9292-9304. doi:10.1021/jacs.9b02902es_ES
dc.description.referencesRogge, S. M. J., Bavykina, A., Hajek, J., Garcia, H., Olivos-Suarez, A. I., Sepúlveda-Escribano, A., … Gascon, J. (2017). Metal–organic and covalent organic frameworks as single-site catalysts. Chemical Society Reviews, 46(11), 3134-3184. doi:10.1039/c7cs00033bes_ES
dc.description.referencesFarrusseng, D., Aguado, S., & Pinel, C. (2009). Metal-Organic Frameworks: Opportunities for Catalysis. Angewandte Chemie International Edition, 48(41), 7502-7513. doi:10.1002/anie.200806063es_ES
dc.description.referencesValvekens, P., Vermoortele, F., & De Vos, D. (2013). Metal–organic frameworks as catalysts: the role of metal active sites. Catalysis Science & Technology, 3(6), 1435. doi:10.1039/c3cy20813ces_ES
dc.description.referencesDoonan, C. J., & Sumby, C. J. (2017). Metal–organic framework catalysis. CrystEngComm, 19(29), 4044-4048. doi:10.1039/c7ce90106bes_ES
dc.description.referencesDhakshinamoorthy, A., Li, Z., & Garcia, H. (2018). Catalysis and photocatalysis by metal organic frameworks. Chemical Society Reviews, 47(22), 8134-8172. doi:10.1039/c8cs00256hes_ES
dc.description.referencesWang, Y., & Wöll, C. (2018). Chemical Reactions at Isolated Single-Sites Inside Metal–Organic Frameworks. Catalysis Letters, 148(8), 2201-2222. doi:10.1007/s10562-018-2432-2es_ES
dc.description.referencesGenna, D. T., Pfund, L. Y., Samblanet, D. C., Wong-Foy, A. G., Matzger, A. J., & Sanford, M. S. (2016). Rhodium Hydrogenation Catalysts Supported in Metal Organic Frameworks: Influence of the Framework on Catalytic Activity and Selectivity. ACS Catalysis, 6(6), 3569-3574. doi:10.1021/acscatal.6b00404es_ES
dc.description.referencesChen, H., He, Y., Pfefferle, L. D., Pu, W., Wu, Y., & Qi, S. (2018). Phenol Catalytic Hydrogenation over Palladium Nanoparticles Supported on Metal-Organic Frameworks in the Aqueous Phase. ChemCatChem, 10(12), 2558-2570. doi:10.1002/cctc.201800211es_ES
dc.description.referencesMarx, S., Kleist, W., Huang, J., Maciejewski, M., & Baiker, A. (2010). Tuning functional sites and thermal stability of mixed-linker MOFs based on MIL-53(Al). Dalton Transactions, 39(16), 3795. doi:10.1039/c002483jes_ES
dc.description.referencesFang, Z., Bueken, B., De Vos, D. E., & Fischer, R. A. (2015). Defect-Engineered Metal-Organic Frameworks. Angewandte Chemie International Edition, 54(25), 7234-7254. doi:10.1002/anie.201411540es_ES
dc.description.referencesDissegna, S., Epp, K., Heinz, W. R., Kieslich, G., & Fischer, R. A. (2018). Defective Metal-Organic Frameworks. Advanced Materials, 30(37), 1704501. doi:10.1002/adma.201704501es_ES
dc.description.referencesZhang, Y.-B., Furukawa, H., Ko, N., Nie, W., Park, H. J., Okajima, S., … Yaghi, O. M. (2015). Introduction of Functionality, Selection of Topology, and Enhancement of Gas Adsorption in Multivariate Metal–Organic Framework-177. Journal of the American Chemical Society, 137(7), 2641-2650. doi:10.1021/ja512311aes_ES
dc.description.referencesDrache, F., Cirujano, F. G., Nguyen, K. D., Bon, V., Senkovska, I., Llabrés i Xamena, F. X., & Kaskel, S. (2018). Anion Exchange and Catalytic Functionalization of the Zirconium-Based Metal–Organic Framework DUT-67. Crystal Growth & Design, 18(9), 5492-5500. doi:10.1021/acs.cgd.8b00832es_ES
dc.description.referencesZhang, W., Kauer, M., Halbherr, O., Epp, K., Guo, P., Gonzalez, M. I., … Fischer, R. A. (2016). Ruthenium Metal-Organic Frameworks with Different Defect Types: Influence on Porosity, Sorption, and Catalytic Properties. Chemistry - A European Journal, 22(40), 14297-14307. doi:10.1002/chem.201602641es_ES
dc.description.referencesKozachuk, O., Yusenko, K., Noei, H., Wang, Y., Walleck, S., Glaser, T., & Fischer, R. A. (2011). Solvothermal growth of a ruthenium metal–organic framework featuring HKUST-1 structure type as thin films on oxide surfaces. Chemical Communications, 47(30), 8509. doi:10.1039/c1cc11107hes_ES
dc.description.referencesKozachuk, O., Luz, I., Llabrés i Xamena, F. X., Noei, H., Kauer, M., Albada, H. B., … Fischer, R. A. (2014). Multifunctional, Defect-Engineered Metal-Organic Frameworks with Ruthenium Centers: Sorption and Catalytic Properties. Angewandte Chemie International Edition, 53(27), 7058-7062. doi:10.1002/anie.201311128es_ES
dc.description.referencesAgirrezabal-Telleria, I., Luz, I., Ortuño, M. A., Oregui-Bengoechea, M., Gandarias, I., López, N., … Soukri, M. (2019). Gas reactions under intrapore condensation regime within tailored metal–organic framework catalysts. Nature Communications, 10(1). doi:10.1038/s41467-019-10013-6es_ES
dc.description.referencesZhang, W., Kozachuk, O., Medishetty, R., Schneemann, A., Wagner, R., Khaletskaya, K., … Fischer, R. A. (2015). Controlled SBU Approaches to Isoreticular Metal-Organic Framework Ruthenium-Analogues of HKUST-1. European Journal of Inorganic Chemistry, 2015(23), 3913-3920. doi:10.1002/ejic.201500478es_ES
dc.description.referencesHeinz, W. R., Kratky, T., Drees, M., Wimmer, A., Tomanec, O., Günther, S., … Fischer, R. A. (2019). Mixed precious-group metal–organic frameworks: a case study of the HKUST-1 analogue [RuxRh3−x(BTC)2]. Dalton Transactions, 48(32), 12031-12039. doi:10.1039/c9dt01198fes_ES
dc.description.referencesBäckvall, J.-E. (2002). Transition metal hydrides as active intermediates in hydrogen transfer reactions. Journal of Organometallic Chemistry, 652(1-2), 105-111. doi:10.1016/s0022-328x(02)01316-5es_ES
dc.description.referencesChowdhury, R. L., & Bäckvall, J.-E. (1991). Efficient ruthenium-catalysed transfer hydrogenation of ketones by propan-2-ol. J. Chem. Soc., Chem. Commun., 0(16), 1063-1064. doi:10.1039/c39910001063es_ES
dc.description.referencesAhlsten, N., Bartoszewicz, A., & Martín-Matute, B. (2012). Allylic alcohols as synthetic enolate equivalents: Isomerisation and tandem reactions catalysed by transition metal complexes. Dalton Transactions, 41(6), 1660. doi:10.1039/c1dt11678aes_ES
dc.description.referencesAhlsten, N., Lundberg, H., & Martín-Matute, B. (2010). Rhodium-catalysed isomerisation of allylic alcohols in water at ambient temperature. Green Chemistry, 12(9), 1628. doi:10.1039/c004964fes_ES
dc.description.referencesCahard, D., Gaillard, S., & Renaud, J.-L. (2015). Asymmetric isomerization of allylic alcohols. Tetrahedron Letters, 56(45), 6159-6169. doi:10.1016/j.tetlet.2015.09.098es_ES
dc.description.referencesXia, T., Wei, Z., Spiegelberg, B., Jiao, H., Hinze, S., & de Vries, J. G. (2018). Isomerization of Allylic Alcohols to Ketones Catalyzed by Well-Defined Iron PNP Pincer Catalysts. Chemistry - A European Journal, 24(16), 4043-4049. doi:10.1002/chem.201705454es_ES
dc.description.referencesScalambra, F., Lorenzo-Luis, P., de los Rios, I., & Romerosa, A. (2019). Isomerization of allylic alcohols in water catalyzed by transition metal complexes. Coordination Chemistry Reviews, 393, 118-148. doi:10.1016/j.ccr.2019.04.012es_ES
dc.description.referencesYamaguchi, K., Koike, T., Kotani, M., Matsushita, M., Shinachi, S., & Mizuno, N. (2005). Synthetic Scope and Mechanistic Studies of Ru(OH)x/Al2O3-Catalyzed Heterogeneous Hydrogen-Transfer Reactions. Chemistry - A European Journal, 11(22), 6574-6582. doi:10.1002/chem.200500539es_ES
dc.description.referencesMitchell, R. W., Spencer, A., & Wilkinson, G. (1973). Carboxylato-triphenylphosphine complexes of ruthenium, cationic triphenylphosphine complexes derived from them, and their behaviour as homogeneous hydrogenation catalysts for alkenes. Journal of the Chemical Society, Dalton Transactions, (8), 846. doi:10.1039/dt9730000846es_ES
dc.description.sponsorshipFunding by the Spanish Government is acknowledged through projects MAT2017-82288-C2-1-P and Severo Ochoa (SEV-2016-0683). This project is further funded by the Deutsche Forschungsgemeinschaft grant no. FI-502/32-1 ("DEMOFs"). KE and WRH would like to thank TUM Graduate School and the Gesellschaft Deutscher Chemiker (GDCh) for financial support. KE gratefully acknowledges support from the colleagues Olesia Halbherr (nee Kozachuk) and Wenhua Zhang.es_ES
dc.description.upvformatpfin1725es_ES
dc.description.upvformatpinicio1720es_ES
dc.description.volume12es_ES
dc.identifier.doi10.1002/cctc.201902079es_ES
dc.identifier.issn1867-3880es_ES
dc.identifier.urihttps://riunet.upv.es/handle/10251/165293
dc.languageIngléses_ES
dc.publisherJohn Wiley & Sonses_ES
dc.relation.ispartofChemCatChemes_ES
dc.relation.pasarelaS\409743es_ES
dc.relation.projectIDinfo:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/MAT2017-82288-C2-1-P/ES/MATERIALES HIBRIDOS MULTIFUNCIONALES BASADOS EN NANO-UNIDADES ESTRUCTURALES ACTIVAS/es_ES
dc.relation.projectIDinfo:eu-repo/grantAgreement/DFG//FI-502%2F32-1/es_ES
dc.relation.projectIDinfo:eu-repo/grantAgreement/MINECO//SEV-2016-0683/es_ES
dc.relation.publisherversionhttps://doi.org/10.1002/cctc.201902079es_ES
dc.relation.references10.1021/cs400959kes_ES
dc.relation.references10.1021/ja067374yes_ES
dc.relation.references10.1039/b802258pes_ES
dc.relation.references10.1021/ja405078ues_ES
dc.relation.references10.1021/jacs.9b02902es_ES
dc.relation.references10.1039/C7CS00033Bes_ES
dc.relation.references10.1002/anie.200806063es_ES
dc.relation.references10.1039/c3cy20813ces_ES
dc.relation.references10.1039/C7CE90106Bes_ES
dc.relation.references10.1039/C8CS00256Hes_ES
dc.relation.references10.1007/s10562-018-2432-2es_ES
dc.relation.references10.1021/acscatal.6b00404es_ES
dc.relation.references10.1002/cctc.201800211es_ES
dc.relation.references10.1039/c002483jes_ES
dc.relation.references10.1002/anie.201411540es_ES
dc.relation.references10.1002/adma.201704501es_ES
dc.relation.references10.1021/ja512311aes_ES
dc.relation.references10.1021/acs.cgd.8b00832es_ES
dc.relation.references10.1002/chem.201602641es_ES
dc.relation.references10.1039/c1cc11107hes_ES
dc.relation.references10.1002/anie.201311128es_ES
dc.relation.references10.1038/s41467-019-10013-6es_ES
dc.relation.references10.1002/ejic.201500478es_ES
dc.relation.references10.1039/C9DT01198Fes_ES
dc.relation.references10.1016/S0022-328X(02)01316-5es_ES
dc.relation.references10.1039/C39910001063es_ES
dc.relation.references10.1039/c1dt11678aes_ES
dc.relation.references10.1039/c004964fes_ES
dc.relation.references10.1016/j.tetlet.2015.09.098es_ES
dc.relation.references10.1002/chem.201705454es_ES
dc.relation.references10.1016/j.ccr.2019.04.012es_ES
dc.relation.references10.1002/chem.200500539es_ES
dc.relation.references10.1039/dt9730000846es_ES
dc.rightsReconocimiento - No comercial - Sin obra derivada (by-nc-nd)es_ES
dc.rights.accessRightsAbiertoes_ES
dc.subjectMetal-Organic Frameworkses_ES
dc.subjectDefectses_ES
dc.subjectRutheniumes_ES
dc.subjectRu-BTCes_ES
dc.subjectRu-MOFes_ES
dc.subjectHKUST-1es_ES
dc.subjectDefect-Engineeringes_ES
dc.subjectMOF catalysises_ES
dc.subjectDEMOFes_ES
dc.titleDefect-Engineered Ruthenium MOFs as Versatile Heterogeneous Hydrogenation Catalystses_ES
dc.typeArtículoes_ES
dc.type.versioninfo:eu-repo/semantics/publishedVersiones_ES
dspace.entity.typePublication
person.identifier451417
person.identifier319450
person.identifier.orcid0000-0002-8309-3702
person.identifier.orcid0000-0002-4238-5784
relation.isAuthorOfPublication1d44cf8d-c018-49c3-9fd4-b3a62e5e6795
relation.isAuthorOfPublication77bb60c6-de77-40ff-b724-ea8f51106ed8
relation.isAuthorOfPublication.latestForDiscovery1d44cf8d-c018-49c3-9fd4-b3a62e5e6795
relation.isOrgUnitOfPublicationb97c2806-5147-442a-a1a8-a2c75cc2a941
relation.isOrgUnitOfPublication.latestForDiscoveryb97c2806-5147-442a-a1a8-a2c75cc2a941
upv.uuid74ba2fdc-467e-4337-b426-4b33a3a3afc3es_ES

Archivos

Bloque original

Mostrando 1 - 1 de 1
Cargando...
Miniatura
Nombre:
Epp;Luz;Henz - Defect-Engneered Ruthenum MOFs as Versatle Heterogeneous Hydrogenaton Catalysts.pdf
Tamaño:
556.33 KB
Formato:
Adobe Portable Document Format
Descripción:
Versión editorial