Catalytic Performance of One-Pot Synthesized Fe-MWW Layered Zeolites (MCM-22, MCM-36, and ITQ-2) in Selective Catalytic Reduction of Nitrogen Oxides with Ammonia

[EN] The application of layered zeolites of MWW topology in environmental catalysis has attracted growing attention in recent years; however, only a few studies have explored their performance in selective catalytic reduction with ammonia (NH3-SCR). Thus, our work describes, for the first time, the one-pot synthesis of Fe-modified NH3-SCR catalysts supported on MCM-22, MCM-36, and ITQ-2. The calculated chemical composition of the materials was Si/Al of 30 and 5 wt.% of Fe. The reported results indicated a correlation between the arrangement of MWW layers and the form of iron in the zeolitic structure. We have observed that one-pot synthesis resulted in high dispersion of Fe3+ sites, which significantly enhanced low-temperature activity and prevented N2O generation during the reaction. All of the investigated samples exhibited almost 100% NO conversion at 250 degrees C. The most satisfactory activity was exhibited by Fe-modified MCM-36, since 50% of NO reduction was obtained at 150 degrees C for this catalyst. This effect can be explained by the abundance of isolated Fe3+ species, which are active in low-temperature NH3-SCR. Additionally, SiO2 pillars present in MCM-36 provided an additional surface for the deposition of the active phase.Agnieszka Szymaszek-Wawryca gratefully acknowledges the financial support of the research from the National Science Centre Grant, Preludium 19 (no. 2020/37/N/ST5/00186). Monika Motak would like to kindly acknowledge AGH Grant "Excellence Initiative-Research University" (no. 501.696.7996) for the financial support. Bogdan Samojeden is thankful to AGH Grant (no. 16.16.210.476) for the foundation of the publication. Urbano Diaz acknowledges the support from the Government of Spain through the project PID2020-112590GB-C21/AEI/10.13039/501100011033.Szymaszek-Wawryca, A.; Díaz Morales, UM.; Samojeden, B.; Motak, M. (2022). Catalytic Performance of One-Pot Synthesized Fe-MWW Layered Zeolites (MCM-22, MCM-36, and ITQ-2) in Selective Catalytic Reduction of Nitrogen Oxides with Ammonia. Molecules. 27(9):1-24. https://doi.org/10.3390/molecules2709298312427

MCM-22, MCM-36, and ITQ-2 Zeolites with Different Si/Al Molar Ratios as Effective Catalysts of Methanol and Ethanol Dehydration

[EN] MCM-22, MCM-36, and ITQ-2 zeolites with the intended Si/Al molar ratios of 15, 25, and 50 were synthetized and tested as catalysts for dehydration of methanol to dimethyl ether and dehydration of ethanol to diethyl ether and ethylene. The surface concentration of acid sites was regulated by the synthesis of zeolite precursors with different aluminum content in the zeolite framework, while the influence of porous structure on the overall efficiency of alcohol conversion was analyzed by application of zeolitic materials with different types of porosity-microporous MCM-22 as well as microporous-mesoporous MCM-36 and ITQ-2. The zeolitic samples were characterized with respect to their: chemical composition (ICP-OES), structure (XRD, FT-IR), texture (N-2 sorption), and surface acidity (NH3-TPD). Comparison of the catalytic activity of the studied zeolitic catalysts with other reported catalytic systems, including zeolites with the similar Si/Al ratio as well as gamma-Al2O3 (one of the commercial catalysts for methanol dehydration), shows a great potential of MCM-22, MCM-36, and ITQ-2 in the reactions of alcohols dehydration.This research was funded by National Science Centre-Poland grant number 2016/21/B/ST5/00242. U.D. acknowledges to the Spanish Government grant number MAT2017-82288-C2-1-P. The research was partially done using the equipment purchased from the funds of European Regional Development Fund, Polish Innovation Economy Operational Program, grant numberPOIG.02.01.00-12-023/08.Marosz, M.; Samojeden, B.; Kowalczyk, A.; Rutkowska, M.; Motak, M.; Díaz Morales, UM.; Palomares Gimeno, AE.... (2020). MCM-22, MCM-36, and ITQ-2 Zeolites with Different Si/Al Molar Ratios as Effective Catalysts of Methanol and Ethanol Dehydration. 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The effect of La in PdCe-zeolite catalysts for NOx-SCR with CH4

Communication presented at the International Symposium on Air & Water Pollution Abatement Catalysis - AWPAC 2014. Kraków, Poland, 1-5 September 2014Fundação para a Ciência e a Tecnologia. GDF Sue

Meta-analysis of CO2 conversion, energy efficiency, and other performance data of plasma-catalysis reactors with the open access PIONEER database

This paper brings the comparison of performances of CO2 conversion by plasma and plasma-assisted catalysis based on the data collected from literature in this field, organised in an open access online database. This tool is open to all users to carry out their own analyses, but also to contributors who wish to add their data to the database in order to improve the relevance of the comparisons made, and ultimately to improve the efficiency of CO2 conversion by plasma-catalysis. The creation of this database and database user interface is motivated by the fact that plasma-catalysis is a fast-growing field for all CO2 conversion processes, be it methanation, dry reforming of methane, methanolisation, or others. As a result of this rapid increase, there is a need for a set of standard procedures to rigorously compare performances of different systems. However, this is currently not possible because the fundamental mechanisms of plasma-catalysis are still too poorly understood to define these standard procedures. Fortunately however, the accumulated data within the CO2 plasma-catalysis community has become large enough to warrant so-called “big data” studies more familiar in the fields of medicine and the social sciences. To enable comparisons between multiple data sets and make future research more effective, this work proposes the first database on CO2 conversion performances by plasma-catalysis open to the whole community. This database has been initiated in the framework of a H2020 European project and is called the “PIONEER DataBase”. The database gathers a large amount of CO2 conversion performance data such as conversion rate, energy efficiency, and selectivity for numerous plasma sources coupled with or without a catalyst. Each data set is associated with metadata describing the gas mixture, the plasma source, the nature of the catalyst, and the form of coupling with the plasma. Beyond the database itself, a data extraction tool with direct visualisation features or advanced filtering functionalities has been developed and is available online to the public. The simple and fast visualisation of the state of the art puts new results into context, identifies literal gaps in data, and consequently points towards promising research routes. More advanced data extraction illustrates the impact that the database can have in the understanding of plasma-catalyst coupling. Lessons learned from the review of a large amount of literature during the setup of the database lead to best practice advice to increase comparability between future CO2 plasma-catalytic studies. Finally, the community is strongly encouraged to contribute to the database not only to increase the visibility of their data but also the relevance of the comparisons allowed by this tool

Formation of ammonia bisulfate in coal-fired power plant equipped with SCR reactors and the effect of reduced load operation

Coal fired power plant are still responsible for vast amount of electricity and heat production in Poland in 2019. Increasing number of units is equipped with SCR reactors in order to mitigate NOx emission. Older units have been designed to work in a base load operation· however increasing number of intermittent energy sources on the market· forces power plant owners to operate such units in reduced load for significant number of hours in a year. Most of parameters in coal-fired boiler would change in reduced load operation· particularly flue gas parameters. That would affect the formation of ammonia bisulfate (NH4HSO4) as well as operation of SCR reactors in the boiler. The NH4HSO4 formation is highly undesired as it can plug the catalyst or heating surfaces in the boiler. To investigate this phenomenon· the NH4HSO4 formation was comprehensively studied. Moreover· reduced load operation of boiler in a medium size CHP plant was simulated· using computer modelling tools. Obtained parameters were used to analyse· how different flue gas parameters affect NH4HSO4 formation and what consequences does it have for boiler operation. In particular, effect related with operation of SCR reactors equipped with V2O5-WO3/TiO2 catalyst was deeply studied

Selective catalytic reduction of NO,sub>x</sub> with ammonia (NH₃-SCR) over transition metal-based catalysts -influence of the catalysts support

Natural layered clays (bentonite and vermiculite) and natural zeolite (clinoptilolite) were tested and compared as the supports of the catalysts forselective catalytic reduction withammonia (NH3-SCR). The raw materials were modified in order to improve their catalytic properties. Layered clays were treated with HNO3 and intercalated with Al2O3 pillars to enhance their acidity, porosity and specific surface area. Clinoptilolite was ion-exchanged with NH4NO3 in order to increase the content of Brönsted acid sites, indispensablefor NH3 adsorptionduring the reaction. Subsequently, iron as an active phase was deposited on the modified supports by various methods, including incipient wetness impregnation, ion-exchange and co-precipitation. The efficiency of these methods was compared as NOx conversionobtained for each material. XRD analysis indicated that the initial modifications affected the structure of the raw aluminosilicates. FT-IR measurement confirmed the presence of characteristic Si-O and Al-O bonds and H2O molecules that occurnaturally in the materials. UV-Vis spectroscopy results indicated that different types of Fe species were deposited on the catalysts surface and theirform strongly depends on the type of the support. NH3-SCR catalytic tests showedthat all of the analyzed materials exhibitsatisfactory level of NO conversion and negligible concentration of by-product (N2O) in the exhaust gas. The highest catalytic activity (ca. 50% at 170°C and over 95% above 250°C) was obtained for Fe-Bent. The lowest concentration of N2O in the flue gas (less than 5 ppm in the whole temperature range) was observed for Fe-Clin

The application of modified layered double hydroxides in selective catalytic reduction of nitrogen oxides by ammonia (NH3-SCR)

Selective catalytic reduction with ammonia (NH3-SCR) is very efficient DeNOx technique. According to some problems with the commercial catalyst, novel one should be prepared. Hydrotalcites are potential precursors of the new catalysts of NH3-SCR. In this paper, several attempts to apply these materials in NH3-SCR are presented

Tri-reforming as a process of CO

Methane tri-reforming process is a combination of three reactions: steam methane reforming (SRM), dry methane reforming (DRM), and partial oxidation of methane (POM). The first two reactions have endothermic character, while the POM is the exothermic reaction, which allows to obtain the energy necessary for the other two processes in situ. CH4 reacts with H2O, CO2, O2, and synthesis gas is produced with desired H2/CO ratios (1.5 – 2.0). The presence of H2O and O2 in the reaction environment can positively influence the stability of the used catalyst, by the inhibition of coke formation. In this paper two scenarios for methane tri-reforming implementation are discussed: (i) Tri-reforming as a effective way for chemical CO2 utilization, without the separation of carbon dioxide from flue gases from fossil fuel-fired power stations, and (ii) dry reforming of methane improved by the addition of water and oxygen, which may be applied as a chemical energy storage process. The literature on the subject of trireforming is shortly reviewed, including thermodynamics of the process, the possible conversions of methane and carbon dioxide, and proposed catalysts, both studied in tri-reforming, and in single processes (SRM, DRM and POM)