Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 6, Issue 6, Pages 1011-1017Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.5b00069
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Funding
- Spanish Ministry of Economy and Competitiveness through the Severo Ochoa program [SEV-2012-0267]
- operating grants Consolider Ingenio Multicat [CSD-2009-00050, MAT-2012-3856-C02-01]
- Generalitat Valenciana [PROMETEOII/2013/011]
- ITQ
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Nowadays, the most attractive technology for the elimination of nitric oxides from the exhaust gas of diesel vehicles is the selective catalytic reduction with ammonia (NH3-SCR-NOx) using Cu zeolite with the chabazite structure as the catalyst. Isolated copper species are the active sites, but the reaction intermediates and the overall reaction mechanism are still under debate. Here, we study the interaction of ammonia with zeolite Cu-SSZ-13 (CHA topology) with a uniform distribution of Cu2+ sites prepared in one pot and a conventional Cu-ZSM-5 (MFI topology) for comparison. In situ EPR and solid-state NMR spectroscopies combined with DFT calculations have allowed the identification of NH4+, [Cu(NH3)(5)](2+), [Cu(Of)(2)(NH3)(2)](2+), [Cu(Of)(3)NH3](2+), [Cu(NH3)(2)](+), and [CuOf(NH3)](+) (Of being framework oxygen) under different conditions. The results demonstrate that ammonia is able to reduce Cu2+ to Cu+ and provide new information on the species formed in Cu-SSZ-13, which have important implications for the elucidation of the SCR reaction mechanism.
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