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dc.contributor.authorTurrina, Alessandro
dc.contributor.authorEschenroeder, Eike Christian Viktor
dc.contributor.authorBode, Bela Ernest
dc.contributor.authorCollier, Jillian E.
dc.contributor.authorApperley, David C.
dc.contributor.authorCox, Paul A.
dc.contributor.authorCasci, John L.
dc.contributor.authorWright, Paul Anthony
dc.date.accessioned2016-05-26T23:32:26Z
dc.date.available2016-05-26T23:32:26Z
dc.date.issued2015-10-01
dc.identifier.citationTurrina , A , Eschenroeder , E C V , Bode , B E , Collier , J E , Apperley , D C , Cox , P A , Casci , J L & Wright , P A 2015 , ' Understanding the structure directing action of copper-polyamine complexes in the direct synthesis of Cu-SAPO-34 and Cu-SAPO-18 catalysts for the selective catalytic reduction of NO with NH 3 ' , Microporous and Mesoporous Materials , vol. 215 , pp. 154-167 . https://doi.org/10.1016/j.micromeso.2015.05.038en
dc.identifier.issn1387-1811
dc.identifier.otherPURE: 188962731
dc.identifier.otherPURE UUID: 89fc98c5-f539-4d57-8527-456475a7ff7c
dc.identifier.otherScopus: 84930959331
dc.identifier.otherORCID: /0000-0002-3384-271X/work/27582727
dc.identifier.otherWOS: 000358393900019
dc.identifier.otherORCID: /0000-0002-4243-9957/work/62668264
dc.identifier.urihttp://hdl.handle.net/10023/8882
dc.descriptionThis work has been supported by Johnson Matthey PLC, UK.en
dc.description.abstractCu2+ cations complexed by linear polyamines have been studied as structure-directing agents (SDAs) for the direct synthesis of copper-containing microporous silicoaluminophosphate (SAPO) materials. The complexing ligands diethylenetriamine (DETA), N-(2-hydroxyethyl)ethylenediamine (HEEDA), triethylenetetramine (TETA), N,N′-bis(2-aminoethyl)-1,3-propanediamine (232), 1,2-bis(3-aminopropylamino)ethane (323), tetraethylenepentamine (TEPA) and pentaethylenehexamine (PEHA) have been investigated. For comparison, syntheses have been performed using the analogous nickel-polyamine complexes. Cu2+ and Ni2+ forms of both SAPO-18 and SAPO-34 materials have been prepared. While most polyamine complexes direct crystallisation to SAPO-34, SAPO-18 has been prepared with Cu2+(232), Ni2+(232) and Ni2+(TETA). The coordination geometry of the included metal complexes was studied by UV-visible and EPR spectroscopy and computer simulation. SAPO-18 is favoured by the smaller square planar complexes or octahedral species (with 2 water molecules) of 232 and TETA. Calcination leaves extra-framework Cu2+ and Ni2+ cations within SAPO-18 and SAPO-34 frameworks. In situ synchrotron IR spectroscopy of Ni-SAPO-18 has shown thermal template degradation occurs via nitrile intermediates. Rietveld structural analysis located extra-framework Cu2+ and Ni2+ cations released by calcination. In SAPO-34, Cu2+ and Ni2+ were located in the 8R window of the cha cage. A second site was found for Ni2+ at the centre of the six-membered rings (6Rs) of the double-six-ring (D6R) sub-units. In SAPO-18 both Cu2+ and Ni2+ cations were located only in the 6Rs of the D6R sub-units. Selected copper SAPO-18 and SAPO-34 samples were tested in the selective catalytic reduction of NO with ammonia (NH3-SCR); both showed high activity.
dc.language.isoeng
dc.relation.ispartofMicroporous and Mesoporous Materialsen
dc.rightsCopyright 2015 Elsevier Inc. All rights reserved. This work is made available online in accordance with the publisher’s policies. This is the author created, accepted version manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at http://dx.doi.org/10.1016/j.micromeso.2015.05.038en
dc.rightsCopyright 2015 Elsevier Inc. All rights reserved. This work is made available online in accordance with the publisher’s policies. This is the author created, accepted version manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at http://dx.doi.org/10.1016/j.micromeso.2015.05.038en
dc.subjectOne-pot synthesisen
dc.subjectMetal- polyamine complexesen
dc.subjectCu-SAPO-34en
dc.subjectCu-SAPO-18en
dc.subjectNH3-SCRen
dc.subjectQD Chemistryen
dc.subjectDASen
dc.subject.lccQDen
dc.titleUnderstanding the structure directing action of copper-polyamine complexes in the direct synthesis of Cu-SAPO-34 and Cu-SAPO-18 catalysts for the selective catalytic reduction of NO with NH3en
dc.typeJournal articleen
dc.description.versionPostprinten
dc.description.versionPostprinten
dc.contributor.institutionUniversity of St Andrews.School of Chemistryen
dc.contributor.institutionUniversity of St Andrews.Centre of Magnetic Resonanceen
dc.contributor.institutionUniversity of St Andrews.Biomedical Sciences Research Complexen
dc.contributor.institutionUniversity of St Andrews.EaSTCHEMen
dc.identifier.doihttps://doi.org/10.1016/j.micromeso.2015.05.038
dc.description.statusPeer revieweden
dc.date.embargoedUntil2016-05-27
dc.identifier.urlhttp://www.sciencedirect.com/science/article/pii/S1387181115003078#appd001en


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