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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 NH3
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dc.contributor.author | Turrina, Alessandro | |
dc.contributor.author | Eschenroeder, Eike Christian Viktor | |
dc.contributor.author | Bode, Bela Ernest | |
dc.contributor.author | Collier, Jillian E. | |
dc.contributor.author | Apperley, David C. | |
dc.contributor.author | Cox, Paul A. | |
dc.contributor.author | Casci, John L. | |
dc.contributor.author | Wright, Paul Anthony | |
dc.date.accessioned | 2016-05-26T23:32:26Z | |
dc.date.available | 2016-05-26T23:32:26Z | |
dc.date.issued | 2015-10-01 | |
dc.identifier | 188962731 | |
dc.identifier | 89fc98c5-f539-4d57-8527-456475a7ff7c | |
dc.identifier | 84930959331 | |
dc.identifier | 000358393900019 | |
dc.identifier.citation | Turrina , 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.2015.05.038 | en |
dc.identifier.issn | 1387-1811 | |
dc.identifier.other | ORCID: /0000-0002-3384-271X/work/27582727 | |
dc.identifier.other | ORCID: /0000-0002-4243-9957/work/62668264 | |
dc.identifier.uri | https://hdl.handle.net/10023/8882 | |
dc.description | This work has been supported by Johnson Matthey PLC, UK. | en |
dc.description.abstract | Cu2+ 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.format.extent | 1463025 | |
dc.format.extent | 431350 | |
dc.language.iso | eng | |
dc.relation.ispartof | Microporous and Mesoporous Materials | en |
dc.subject | One-pot synthesis | en |
dc.subject | Metal- polyamine complexes | en |
dc.subject | Cu-SAPO-34 | en |
dc.subject | Cu-SAPO-18 | en |
dc.subject | NH3-SCR | en |
dc.subject | QD Chemistry | en |
dc.subject | DAS | en |
dc.subject.lcc | QD | en |
dc.title | 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 NH3 | en |
dc.type | Journal article | en |
dc.contributor.institution | University of St Andrews. School of Chemistry | en |
dc.contributor.institution | University of St Andrews. Centre of Magnetic Resonance | en |
dc.contributor.institution | University of St Andrews. Biomedical Sciences Research Complex | en |
dc.contributor.institution | University of St Andrews. EaSTCHEM | en |
dc.identifier.doi | 10.1016/j.micromeso.2015.05.038 | |
dc.description.status | Peer reviewed | en |
dc.date.embargoedUntil | 2016-05-27 | |
dc.identifier.url | http://www.sciencedirect.com/science/article/pii/S1387181115003078#appd001 | en |
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