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dc.contributor.author | Zhang, Wenhua | es_ES |
dc.contributor.author | Kauer, Max | es_ES |
dc.contributor.author | Halbherr, Olesia | es_ES |
dc.contributor.author | Epp, Konstantin | es_ES |
dc.contributor.author | Guo, Penghu | es_ES |
dc.contributor.author | Gonzalez, Miguel I. | es_ES |
dc.contributor.author | Xiao, Dianne J. | es_ES |
dc.contributor.author | Wiktor, Christian | es_ES |
dc.contributor.author | Llabrés i Xamena, Francesc Xavier | es_ES |
dc.contributor.author | Woell, Christof | es_ES |
dc.contributor.author | Wang, Yuemin | es_ES |
dc.contributor.author | Muhler, Martin | es_ES |
dc.contributor.author | Fischer, Roland A. | es_ES |
dc.date.accessioned | 2017-05-23T12:04:01Z | |
dc.date.available | 2017-05-23T12:04:01Z | |
dc.date.issued | 2016-09 | |
dc.identifier.issn | 0947-6539 | |
dc.identifier.uri | http://hdl.handle.net/10251/81653 | |
dc.description.abstract | By employing the mixed-component, solid-solution approach, various functionalized ditopic isophthalate (ip) defect-generating linkers denoted 5-X-ipH(2), where X = OH (1), H (2), NH2 (3), Br (4), were introduced into the mixed-valent ruthenium analogue of [Cu-3(btc)(2)](n) (HKUST-1, btc = benzene-1,3,5-tricarboxylate) to yield Ru-DEMOFs (defect-engineered metal-organic frameworks) of the general empirical formula [Ru-3(btc)(2-x)(5-X-ip)(x)Y-y](n). Framework incorporation of 5-X-ip was confirmed by powder XRD, FTIR spectroscopy, ultrahigh-vacuum IR spectroscopy, thermogravimetric analysis, H-1 NMR spectroscopy, N-2 sorption, and X-ray absorption near edge structure. Interestingly, Ru-DEMOF 1c with 32% framework incorporation of 5-OH-ip shows the highest BET surface area (approximate to 1300 m(2) g(-1), N-2 adsorption, 77 K) among all materials (including the parent framework [Ru-3(btc)(2)Y-y](n)). The characterization data are consistent with two kinds of structural defects induced by framework incorporation of 5-X-ip: modified paddlewheel nodes featuring reduced ruthenium sites (Ru delta+, 0 < delta < 2, type A) and missing nodes leading to enhanced porosity (type B). Their relative abundances depend on the choice of the functional group X in the defect linkers. Defects A and B also appeared to play a key role in sorption of small molecules (i.e., CO2, CO, H-2) and the catalytic properties of the materials (i.e., ethylene dimerization and the Paal-Knorr reaction). | es_ES |
dc.description.sponsorship | This research was partially supported by the DFG project FI-502/32-1. W.Z. is thankful for a PhD fellowship from the China Scholarship Council (CSC). W.Z. is also grateful to the Research School<SUP>Plus</SUP> at Ruhr-University Bochum for the support of her PhD project and funding of an internship at UC Berkeley at the group of Prof. Jeffrey. R. Long and collaboration with D.J.X. and M.I.G. including Douglas Reed for the collection of CO isotherms (298 K). W.Z. also thanks Dr. Raghavender Medishetty for the fruitful discussions. P.G. acknowledges the support of the EU innovative Training Network "DEFect NETwork materials science and engineering" (DEFNET). The authors further thank the team at DELTA synchrotron facility at the TU Dortmund for the support with the X-ray absorption spectroscopy experiments performed at beam lines BL8 and the PXRD data collection at beam lines BL9. | en_EN |
dc.language | Inglés | es_ES |
dc.publisher | Wiley | es_ES |
dc.relation.ispartof | Chemistry - A European Journal | es_ES |
dc.rights | Reserva de todos los derechos | es_ES |
dc.title | Ruthenium Metal–Organic Frameworks with Different Defect Types: Influence on Porosity, Sorption, and Catalytic Properties | es_ES |
dc.type | Artículo | es_ES |
dc.identifier.doi | 10.1002/chem.201602641 | |
dc.relation.projectID | info:eu-repo/grantAgreement/DFG//FI-502%2F32-1/ | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/EC/H2020/641887/EU/DEFect NETwork materials science and engineering/ | es_ES |
dc.rights.accessRights | Abierto | es_ES |
dc.contributor.affiliation | Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química | es_ES |
dc.description.bibliographicCitation | Zhang, W.; Kauer, M.; Halbherr, O.; Epp, K.; Guo, P.; Gonzalez, MI.; Xiao, DJ.... (2016). Ruthenium Metal–Organic Frameworks with Different Defect Types: Influence on Porosity, Sorption, and Catalytic Properties. Chemistry - A European Journal. 22(40):14297-14307. https://doi.org/10.1002/chem.201602641 | es_ES |
dc.description.accrualMethod | S | es_ES |
dc.relation.publisherversion | http://dx.doi.org/10.1002/chem.201602641 | es_ES |
dc.description.upvformatpinicio | 14297 | es_ES |
dc.description.upvformatpfin | 14307 | es_ES |
dc.type.version | info:eu-repo/semantics/publishedVersion | es_ES |
dc.description.volume | 22 | es_ES |
dc.description.issue | 40 | es_ES |
dc.relation.senia | 324338 | es_ES |
dc.contributor.funder | European Commission | es_ES |
dc.contributor.funder | Deutsche Forschungsgemeinschaft | es_ES |
dc.contributor.funder | China Scholarship Council | es_ES |
dc.contributor.funder | Ruhr University Bochum, Alemania | es_ES |