LEV type zeolites were synthesized with four different structure-directing agents and converted to copper loaded NH3-SCR catalysts. The synthesis recipe was found to impact the respective Al population in the two topologically different framework sites in double and single 6-rings, resolvable by 27Al MAS NMR spectroscopy. Hydrothermal stability was found to be related to the silanol concentration, Si/Al ratio, particle size, crystal morphology, crystal defects, external surface area, and microporosity. Catalytic activity in NH3-SCR was dependent on preferential Al siting in the double 6-rings. Levinite synthesized using adamantylamine showed the strongest preference for Al atoms sitting in double 6-ring sites, and showed the highest catalytic turnover frequency. Unfortunately, because of the large crystal size, copper loading of this sample was limited to 0.6 wt% while other samples could be loaded with copper up to 3.3 wt%. An optimum combination of hydrothermal stability and catalytic activity was obtained with N,N'-bis-dimethylpentanediyldiammonium dibromide as structure-directing agent.
Low temperature performance is key for catalysts used in selective catalytic reduction of NOx with ammonia (NH3-SCR). The best performing NH3-SCR catalysts are based on small pore copper loaded zeolites. A key question remains which structural and compositional parameters make a copper zeolite catalytically active in this application. In this work a collection of 83 different zeolite samples having 25 different frameworks and compositional variations was evaluated to uncover the critical structural and compositional parameters governing catalytic activity at 150 degrees C. The Si/Al ratio, the content of double six-ring building units, the framework density and pore dimensionality were identified as having a strong impact on the catalytic activity of zeolites. A critical value for each of these parameters was determined. This knowledge was used to predict MOZ, SZR and GME as active NH3-SCR catalysts. They were synthesized respecting the compositional prerequisites and their catalytic evaluation confirmed the predicted high catalytic activity. (C) 2020 Elsevier Inc. All rights reserved.
EU-7 is identified as BIK topology and proves stable to withstand steaming at 900 °C relevant to DeNOx catalysis.
Zeolites are microporous materials driving industrial scale adsorption, ion exchange, and catalytic processes. Their water content dramatically impacts their properties, but its quantification with Karl Fisher titration or thermal gravimetric analysis is problematic. When standard addition of water is combined with 1H magic angle spinning (MAS) NMR detection, absolute quantification of water in microporous materials becomes possible. The method was demonstrated on five different, commercially available zeolites.