0000000000267743
AUTHOR
Andrei-nicolae Parvulescu
Direct Synthesis of Aluminosilicate IWR Zeolite from a Strong Interaction between Zeolite Framework and Organic Template.
A large amount of zeolite structures are still not synthetically available or not available in the form of aluminosilicate currently. Despite significant progress in the development of predictive concepts for zeolite synthesis, accessing some of these new materials is still challenging. One example is the IWR structure as well. Despite successful synthesis of Ge-based IWR zeolites, direct synthesis of aluminosilicate IWR zeolite is still not successful. In this report we show how a suitable organic structure directing agent (OSDA), through modeling of an OSDA/zeolite cage interaction, could access directly the aluminum-containing IWR structure (denoted as COE-6), which might allow access to…
Recent advances in the preparation of zeolites for the selective catalytic reduction of NOx in diesel engines
Metal-exchanged zeolites with small pore sizes have attracted much attention in recent years due to their application in the selective catalytic reduction (SCR) of NOx in diesel engines. Typically, copper-chabazite (e.g. Cu-SSZ-13) has been gradually used as an SCR catalyst in heavy-duty diesel vehicles over the last decade due to its relatively excellent catalytic performance and stability. However, most SSZ-13 zeolites are still prepared via the traditional hydrothermal process in the presence of organic templates, requiring consecutive solid separation and thermal treatment steps to achieve the final zeolite products. In recent years, several strategies for the environmentally friendly p…
The effect of trivalent framework heteroatoms in Cu-CHA on the Selective Catalytic Reduction of NO
Abstract The effect of the trivalent framework atoms (Si4+/M3+ = 13-105) in Cu exchanged CHA-type zeolites was investigated for the selective catalytic reduction of NO with NH3. While the increased hydrophobicity of B-CHA compared to Al-CHA could make it a good candidate for low temperature SCR, the material was too unstable under reaction conditions and the exchanged Cu2+ did not remain isolated. Consequently a lower activity and selectivity than for Al-CHA were observed. Ga-CHA on the other hand showed a similar Cu2+ speciation as Al-CHA at similar Si4+/M3+ ratios. The difference in catalytic activity was remarkably small. While Ga-CHA was less stable upon hydrothermal aging, this was mar…
Rare-earth ion exchanged Cu-SSZ-13 zeolite from organotemplate-free synthesis with enhanced hydrothermal stability in NH3-SCR of NOx
The relatively low hydrothermal stability of Al-rich Cu-SSZ-13 catalysts hinders their practical application in ammonia selective catalytic reduction (NH3-SCR) reaction. Rare-earth ions were introduced into the Al-rich SSZ-13 zeolite using an organotemplate-free synthesis prior to the exchange of Cu2+ ions. Among the rare-earth ions tested (Ce, La, Sm, Y, Yb), Y shows significant enhancement of the hydrothermal stability and NH3-SCR activities after severe hydrothermal aging at 800 °C for 16 h when compared with Cu-SSZ-13 without Y. Cu–Y-SSZ-13 catalysts with various amounts of Y were prepared, and it is found that with increasing Y content, the low temperature NO conversions can be improve…
Transformation synthesis of aluminosilicate SSZ-39 zeolite from ZSM-5 and beta zeolite
Aluminosilicate SSZ-39 zeolite has been successfully prepared by transformation from ZSM-5 and beta zeolite in the presence of N,N-diethyl-cis-2,6-dimethylpiperidinium hydroxide (DMPOH) under hydrothermal conditions. Catalytic tests in the selective catalytic reduction of NOx with NH3 (NH3-SCR) show that the copper-exchanged products synthesized from the interzeolite transformation exhibit excellent catalytic performance.
A Cationic Oligomer as an Organic Template for Direct Synthesis of Aluminosilicate ITH Zeolite
There are a large number of zeolites, such as ITH, that cannot be prepared in the aluminosilicate form. Now, the successful synthesis of aluminosilicate ITH zeolite using a simple cationic oligomer as an organic template is presented. Key to the success is that the cationic oligomer has a strong complexation ability with aluminum species combined with a structural directing ability for the ITH structure similar to that of the conventional organic template. The aluminosilicate ITH zeolite has very high crystallinity, nanosheet-like crystal morphology, large surface area, fully four-coordinated Al species, and abundant acidic sites. Methanol-to-propylene (MTP) tests reveal that the Al-ITH zeo…
Cu-Exchanged CHA-Type Zeolite from Organic Template-Free Synthesis: An Effective Catalyst for NH3-SCR
A Cu-containing CHA-type zeolite was prepared via aqueous ion exchange of the CHA zeolite from organic template-free synthesis. The thus-obtained template-free Cu-CHA showed the best catalytic perf...