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Physicochemical properties and NH3-SCR catalytic performance of intercalated layered aluminosilicates

Szymaszek-Wawryca Agnieszka, Díaz Urbano, Samojeden Bogdan, Motak Monika

Physicochemical Problems of Mineral Processing

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2023

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Vol. 59, iss. 4

art. no. 171381

EN

The representative of natural layered clays, bentonite, was modified according to two routes and tested as a new catalyst for selective catalytic reduction of nitrogen oxides with ammonia (NH3-SCR). The natural acid-activated clay was ion-exchanged with Na+ or remained in H-form and pillared with metal oxides. In order to limit the number of synthesis steps, iron as an active phase was introduced simultaneously with Al2O3 during the intercalation procedure. Additionally, the samples were doped with 0.5 wt% of copper to promote low-temperature activity. It was found that the performed modifications resulted in disorganization of the ordered layered arrangement of bentonite. Nevertheless, acid activation and pillaring improved structural and textural parameters. The results of catalytic tests indicated that the samples containing Fe2O3 pillars promoted with Cu exhibited the highest NO conversion of 85% at 250°C (H-Bent-AlFe-Cu) and 75% at 300°C (Na-Bent-AlFe-Cu). What is important, activity of the protonated samples in the high-temperature region was noticeably affected by the side reaction of ammonia oxidation, correlated with the production of NO and resulting in N2O emission during the process comparing to Na-Bentonite catalysts.

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

Szymaszek Agnieszka, Motak Monika, Samojeden Bogdan

Polish Journal of Chemical Technology

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2020

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Vol. 22, nr 1

61--67

EN

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.

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Selective catalytic reduction of NO with ammoniaat low temperature over Cu-promotedand N-modified activated carbon

Saad Marwa, Białas Anna, Grzywacz Przemysław, Czosnek Cezary, Samojeden Bogdan, Motak Monika

Chemical and Process Engineering

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2020

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Vol. 41, nr 1

59–-67

EN

Catalytic properties of activated carbons oxidized, treated with N-compounds, and promoted withcopper were studied in selective catalytic reduction NOXby ammonia (NH3-SCR). The modificationof the catalysts consisted of a series of steps (pre-oxidation of activated carbon, impregnation with urea,impregnation with copper). The physicochemical properties of the obtained samples were determinedusing X-ray diffraction, FT-IR spectroscopy, and low-temperature N2sorption. The modification withcopper improved the catalytic activity and stability of the catalysts. All the functionalized carbon dopedwith copper reached more than 90% of NO conversion and CO2did not exceed 240 ppm at 220◦C.The sample doped with 5 wt.% Cu had the maximum NO conversion of 98% at 300◦C. The maximum N2O concentration detected for the same sample was only 55 ppm, which confirmed its selectivity.

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Modified bentonite-derived materials as catalystsfor selective catalytic reduction of nitrogen oxides

Szymaszek Agnieszka, Kubeł Maciej, Samojeden Bogdan, Motak Monika

Chemical and Process Engineering

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2020

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Vol. 41, nr 1

13–-24

EN

In the last few years, cationic layered clays, including bentonites have been investigated as potentialcatalysts for SCR DeNOxsystems. In this work, bentonite as the representative of layered clays wasmodified in order to obtain an alternative, low-cost NH3–SCR catalyst. Samples of raw clay wereactivated with HCl or HNO3, treated with C2H2O4and subsequently pillared with alumina by the ion-exchange. Afterwards, the modified materials were impregnated with iron and copper. The obtainedcatalysts were characterized by XRD and FT-IR. SCR catalytic tests carried out over analyzed samplesindicated the conversion of NO of approximately 90% for the most active sample. The type of acidused for modification and the type of active phase strongly influenced the catalytic properties of theanalyzed materials.

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Zastosowanie cenosfer promowanych jonami żelaza i miedzi jako katalizatorów w reakcji selektywnej redukcji katalitycznej tlenku azotu(II) amoniakiem

Samojeden Bogdan, Drużkowska Joanna, Duraczyńska Dorota, Poddębniak Magdalena, Motak Monika

Przemysł Chemiczny

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2019

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T. 98, nr 4

541--545

PL

Cenosfery (składniki popiołów lotnych) modyfikowano żelazem i miedzią. Właściwości fizykochemiczne otrzymanych katalizatorów określono metodami spektroskopii w podczerwienie (FTIR), dyfrakcji promieniami X (XRD), skaningowej mikroskopii elektronowej i niskotemperaturową sorpcją azotu. Uzyskane katalizatory przebadano w reakcji selektywnej redukcji katalitycznej NO amoniakiem w temp. 150-500°C. Najlepszymi testowanymi materiałami okazały się katalizatory żelazowe, dla których stopień konwersji osiągnął 90% przy niskich stężeniach N₂O w gazach odlotowych. Cenosfery modyfikowane Cu wykazywały wprawdzie wyższą aktywność (prawie 100% konwersję NO), ale zanotowano większe stężenia tlenku azotu(I).

EN

Cenospheres were promoted with Fe or Cu ions and studied for phys.-chem. properties by FTIR spectroscopy, X-ray diffraction, scanning electron microscopy and nitrogen sorption. The cenospheres were tested as catalysts for selective catalytic reduction of NO with NH₃. They were promising catalysts in medium and high temp. region (350-500°C).

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Dry and steam reforming of methane. Comparison and analysis of recently investigated catalytic materials. A short review.

Summa Paulina, Samojeden Bogdan, Motak Monika

Polish Journal of Chemical Technology

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2019

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Vol. 21, nr 2

31--37

EN

In order to produce valuable syngas, industrial processes of dry reforming of methane and steam reforming of methane must be further developed. This paper is focused on reviewing recently examined catalysts, supporting the mentioned technologies. In both processes the most popular active material choice is usually nickel, due to its good availability. On the other hand, noble metals, such as ruthenium, rhodium or platinum, provide better performance, however the solution is not cost-effective. Materials used as a support influence the catalytic activity. Oxides with basic properties, such as MgO, Al2 O3 , CeO2 , are frequently used as carriers. One of the most promising materials for reforming of methane technologies are hydrotalcites, due to adjustable composition, acid-base properties and possibility of incorporation of various metals and complexes.

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The influence of holmium on catalytic properties of Fe or Cu-modified vermiculites

Samojeden Bogdan, Grzybek Teresa, Kowal Joanna, Szymaszek Agnieszka, Jabłońska Magdalena, Gläser Roger, Motak Monika

Physicochemical Problems of Mineral Processing

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2019

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Vol. 55, iss. 6

1484--1495

EN

Natural layered clay, vermiculite, was modified and tested as catalyst for the selective catalytic reduction of NOx with ammonia (NH3-SCR). Its modification included the application of the blowing agent (azodicarbonamide), acid treatment and pillaring with Al2O3. Active phase (transition metals: Cu or Fe) was introduced via impregnation. The obtained materials were characterized by N2 sorption (texture), XRD (structure), DR-UV-Vis (oxidation state and aggregation of the active phase), H2-TPR (reducibility of the active phase), in situ DRIFTS (types of adsorbed species due to contact of the sample NH3) and NH3-TPD (type/strength of the acidic sites). The initial modification procedures (treatment with azodicarboamide) resulted in the increase of specific surface area of vermiculite. The introduction of transition metal ions provided a significant amount of acidic sites. The promoting impact of holmium was confirmed by the increased strength of the sites. The highest catalytic activity was exhibited by the sample Fe-containing vermiculite and doped with Ho.

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Selective catalytic reduction of NOX with ammonia NH3-SCR over transition metal-based catalysts -influence of the catalysts support

Szymaszek Agnieszka, Samojeden Bogdan, Motak Monika

Physicochemical Problems of Mineral Processing

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2019

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Vol. 55, iss. 6

1429-1441

EN

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.