scholarly journals Catalytic Performance of Spherical MCM-41 Modified with Copper and Iron as Catalysts of NH3-SCR Process

Molecules ◽  
2020 ◽  
Vol 25 (23) ◽  
pp. 5651
Author(s):  
Aleksandra Jankowska ◽  
Agata Chłopek ◽  
Andrzej Kowalczyk ◽  
Małgorzata Rutkowska ◽  
Marek Michalik ◽  
...  

Spherical MCM-41 with various copper and iron loadings was prepared by surfactant directed co-condensation method. The obtained samples were characterized with respect to their structure (X-ray diffraction, XRD), texture (N2 sorption), morphology (scanning electron microscopy, SEM), chemical composition (inductively coupled plasma optical emission spectrometry, ICP-OES), surface acidity (temperature programmed desorption of ammonia, NH3-TPD), form, and aggregation of iron and copper species (diffuse reflectance UV-Vis spectroscopy, UV-Vis DRS) as well as their reducibility (temperature programmed reduction with hydrogen, H2-TPR). The spherical MCM-41 samples modified with transition metals were tested as catalysts of selective catalytic reduction of NO with ammonia (NH3-SCR). Copper containing catalysts presented high catalytic activity at low-temperature NH3-SCR with a very high selectivity to nitrogen, which is desired reaction products. Similar results were obtained for iron containing catalysts, however in this case the loadings and forms of iron incorporated into silica samples very strongly influenced catalytic performance of the studied samples. The efficiency of the NH3-SCR process at higher temperatures was significantly limited by the side reaction of direct ammonia oxidation. The reactivity of ammonia molecules chemisorbed on the catalysts surface in NO reduction (NH3-SCR) and their selective oxidation (NH3-SCO) was verified by temperature-programmed surface reactions.

Molecules ◽  
2021 ◽  
Vol 26 (6) ◽  
pp. 1807
Author(s):  
Aleksandra Jankowska ◽  
Andrzej Kowalczyk ◽  
Małgorzata Rutkowska ◽  
Marek Michalik ◽  
Lucjan Chmielarz

Aluminum containing silica spherical MCM-41 was synthesized and modified with copper by the template ion-exchange method (TIE) and its modified version, including treatment of the samples with ammonia solution directly after template ion-exchange (TIE-NH3). The obtained samples were characterized with respect to their chemical composition (ICP-OES), structure (XRD), texture (low temperature N2 sorption), morphology (SEM-EDS), form and aggregation of deposited copper species (UV-vis DRS), reducibility of copper species (H2-TPR), and surface acidity (NH3-TPD). The deposition of copper by the TIE-NH3 method resulted in much better dispersion of this metal on the MCM-41 surface comparing to copper introduced by TIE method. It was shown that such highly dispersed copper species, mainly monomeric Cu2+ cations, deposited on aluminum containing silica spheres of MCM-41, are significantly more catalytically effective in the NH3-SCR process than analogous catalysts containing aggregated copper oxide species. The catalysts obtained by the TIE-NH3 method effectively operated in much broader temperature and were less active in the side process of direct ammonia oxidation by oxygen.


Catalysts ◽  
2021 ◽  
Vol 11 (4) ◽  
pp. 490
Author(s):  
Rudaviro Garidzirai ◽  
Phillimon Modisha ◽  
Innocent Shuro ◽  
Jacobus Visagie ◽  
Pieter van Helden ◽  
...  

The effects of Mg and Zn dopants on the catalytic performance of Pt/Al2O3 catalyst were investigated for dehydrogenation of perhydrodibenzyltoluene (H18-DBT) as a liquid organic hydrogen carrier. Al2O3 supports were modified with Mg and Zn to produce Mg-Al2O3 and Zn-Al2O3 with a target loading of 3.8 wt.% for dopants. The modified supports were impregnated with chloroplatinic acid solution to produce the catalysts Pt/Al2O3, Pt/Mg-Al2O3 and Pt/Zn-Al2O3 of 0.5 wt.% Pt loading. Thereafter, the catalysts were characterised using inductively coupled plasma- optical emission spectrometry, scanning electron microscopy-energy dispersive X-ray spectroscopy, hydrogen temperature-programmed reduction, carbon-monoxide pulse chemisorption, ammonia temperature-programmed desorption, X-ray diffraction and transmission electron microscopy. The dehydrogenation experiments were performed using a horizontal plug flow reactor system and the catalyst time-on-stream was 22 h. Pt/Mg-Al2O3 showed the highest average hydrogen flowrate of 29 nL/h, while an average of 27 nL/h was obtained for both Pt/Al2O3 and Pt/Zn-Al2O3. This has resulted in a hydrogen yield of 80% for Pt/Mg-Al2O3, 71% for Pt/Zn-Al2O3 and 73% for Pt/Al2O3. In addition, the conversion of H18-DBT ranges from 99% to 92%, Pt 97–90% and 96–90% for Pt/Mg-Al2O3, Pt/Zn-Al2O3 and Pt/Al2O3, respectively. Following the latter catalyst order, the selectivity to dibenzyltoluene (H0-DBT) ranges from 78% to 57%, 75–51% and 71–45%. Therefore, Pt/Mg-Al2O3 showed improved catalytic performance towards dehydrogenation of H18-DBT.


Catalysts ◽  
2021 ◽  
Vol 11 (1) ◽  
pp. 55
Author(s):  
Katarzyna Świrk ◽  
Ye Wang ◽  
Changwei Hu ◽  
Li Li ◽  
Patrick Da Costa ◽  
...  

Copper and iron promoted ZrO2 catalysts were prepared by one-pot synthesis using urea. The studied catalysts were characterized by XRD, N2 physisorption, XPS, temperature-programmed desorption of NH3 (NH3-TPD), and tested by the selective catalytic reduction by ammonia (NH3-SCR) of NO in the absence and presence of water vapor, under the experimental conditions representative of exhaust gases from stationary sources. The influence of SO2 on catalytic performance was also investigated. Among the studied catalysts, the Fe-Zr sample showed the most promising results in NH3-SCR, being active and highly selective to N2. The addition of SO2 markedly improved NO and NH3 conversions during NH3-SCR in the presence of H2O. The improvement in acidic surface properties is believed to be the cause.


2020 ◽  
Vol 534 ◽  
pp. 147592 ◽  
Author(s):  
Jing Li ◽  
Jiaxiu Guo ◽  
Xueke Shi ◽  
Xinru Wen ◽  
Yinghao Chu ◽  
...  

2018 ◽  
Vol 8 (12) ◽  
pp. 2430 ◽  
Author(s):  
Xinbo Zhu ◽  
Yaolin Wang ◽  
Yu Huang ◽  
Yuxiang Cai

In this work, a series of Ce-W-Ti catalysts were synthesized using a solution combustion method for the selective catalytic reduction (SCR) of NO with NH3 at low temperatures. The reaction performance of NH3-SCR of NO was significantly improved over the Ce-W-Ti catalysts compared to Ce0.4Ti and W0.4Ti catalysts, while Ce0.2W0.2Ti showed the best activity among all the samples. The Ce0.2W0.2Ti catalyst exhibited over 90% removal of NO and 100% N2 selectivity in the temperature range of 250–400 °C at a gas hourly space velocity (GHSV) of 120,000 mL·g−1·h−1. The Ce-W-Ti catalysts were characterized using N2 adsorption-desorption, X-ray diffraction, X-ray photoelectron spectrometry and temperature programmed desorption of NH3 to establish the structure-activity relationships of the Ce-W-Ti catalysts. The excellent catalytic performance of the Ce0.2W0.2Ti catalyst could be associated with the larger specific surface area, highly dispersed Ce and W species, increased amount of surface adsorbed oxygen (Oads) and enhanced total acidity on the catalyst surfaces.


2011 ◽  
Vol 396-398 ◽  
pp. 1851-1855
Author(s):  
Tian Si ◽  
Lin Hua Zhu

A series of new type acid catalyst samples based on mesoporous CaZr4(PO4)6(CZP) belonging to NZP family synthesized by sol-gel method was obtained by Al, La, B incorporation in CZP or by heteropoly acid H3PW12O7•xH2O(HPW) loading on CZP, and their acid catalytic activity and selectivity were investigated by using α-pinene isomerization as a probe reaction. The phase, pore structure and surface acidity of the catalyst samples were characterized by X-ray diffraction (XRD), N2 sorption and NH3 temperature programmed desorption (NH3-TPD) respectively. The results showed that the surface acidity of CZP modified by elements incorporation and HPW loading was improved in a different extent. The conversion of α-pinene at 150 °C reached to 41 % over the catalyst sample noted as Al-CZP-0.15 in which the mole ratio of Al to Zr was 0.15. Under the same reaction conditions, the conversion of α-pinene was above 95 % over the CZP supported with 20-30wt. %HPW.


Catalysts ◽  
2021 ◽  
Vol 11 (3) ◽  
pp. 361
Author(s):  
Ming Cai ◽  
Xue Bian ◽  
Feng Xie ◽  
Wenyuan Wu ◽  
Peng Cen

Selective catalytic reduction of nitrogen oxides with NH3 (NH3-SCR) is still the most commonly used control technology for nitrogen oxides emission. Specifically, the application of rare earth materials has become more and more extensive. CeO2 was widely developed in NH3-SCR reaction due to its good redox performance, proper surface acidity and abundant resource reserves. Therefore, a large number of papers in the literature have described the research of cerium-based catalysts. This review critically summarized the development of the different components of cerium-based catalysts, and characterized the preparation methods, the catalytic performance and reaction mechanisms of the cerium-based catalysts for NH3-SCR. The purpose of this review is to highlight: (1) the modification effect of the various metal elements for cerium-based catalysts; (2) various synthesis methods of the cerium-based catalysts; and (3) the physicochemical properties of the various catalysts and clarify their relations to catalytic performances, particularly in the presence of SO2 and H2O. Finally, we hope that this work can give timely technical guidance and valuable insights for the applications of NH3-SCR in the field of NOx control.


Author(s):  
Djamila Sellam ◽  
Kahina Ikkour ◽  
Sadia Dekkar ◽  
Hassiba Messaoudi ◽  
Taous Belaid ◽  
...  

The study presents the dry reforming of methane using natural Kaolin silica as catalyst support. The silica-supported LaNiO3 perovskite catalysts (20LaNiO3/SiO2 and 40LaNiO3/SiO2) and bulk LaNiO3 catalyst were synthesized by auto-combustion method. The resulting catalysts were characterized by X-ray diffraction (XRD), N2 adsorption - desorption isotherm measurement,  scanning electron microscopy (SEM) and temperature-programmed reduction (TPR). After reduction at 700 °C, they were used as catalysts for the reaction of dry reforming of methane into synthesis gas at atmospheric pressure at 800 °C. The reduced 40LaNiO3/SiO2 exhibited high catalytic activity. This result was attributed to the small Ni metallic particles obtained from the reduced perovskite highly dispersed on the support and the good reducibility. The increase of reduction temperature at 800 °C resulted in a further enhancement of the catalytic performance of 40LaNiO3/SiO2 catalyst. Copyright © 2019 BCREC Group. All rights reserved 


2013 ◽  
Vol 634-638 ◽  
pp. 377-381 ◽  
Author(s):  
Zhong Kui Zhao ◽  
Yi Tao Dai

The initial activity, selectivity, and especially catalytic stability of mesoporous MCM-41 supported phosphotungstic acid (HPW) prepared by ultrasonic-assisted impregnation (UAI) method and the HY zeolite were contrastively investigated for alkenylation of p-xylene with phenylacetylene in a fixed-bed continuous flow reactor. N2 adsorption-desorption, FT-IR, X-ray diffraction (XRD) and NH3 temperature-programmed (NH3-TPD) desorption characterization techniques were employed to explore the relationship of catalyst nature and catalytic performance in alkenylation. Results illustrate that the as-prepared HPW/MCM-41 catalyst exhibits notably superior catalytic activity, selectivity and stability to microporous HY zeolite, ascribed to its well-ordered mesoporous architecture, appropriate acidic sites and high dispersity of HPW phase.


Catalysts ◽  
2020 ◽  
Vol 10 (7) ◽  
pp. 734 ◽  
Author(s):  
Aneta Święs ◽  
Andrzej Kowalczyk ◽  
Małgorzata Rutkowska ◽  
Urbano Díaz ◽  
Antonio E. Palomares ◽  
...  

The main goal of the study was the development of effective catalysts for the low-temperature selective catalytic reduction of NO with ammonia (NH3-SCR), based on ferrierite (FER) and its delaminated (ITQ-6) and silica-intercalated (ITQ-36) forms modified with copper. The copper exchange zeolitic samples, with the intended framework Si/Al ratio of 30 and 50, were synthetized and characterized with respect to their chemical composition (ICP-OES), structure (XRD), texture (low-temperature N2 adsorption), form and aggregation of deposited copper species (UV-vis-DRS), surface acidity (NH3-TPD) and reducibility (H2-TPR). The samples of the Cu-ITQ-6 and Cu-ITQ-36 series were found to be significantly more active NH3-SCR catalysts compared to Cu-FER. The activity of these catalysts in low-temperature NH3-SCR was assigned to the significant contribution of highly dispersed copper species (monomeric cations and small oligomeric species) catalytically active in the oxidation of NO to NO2, which is necessary for fast-SCR. The zeolitic catalysts, with the higher framework alumina content, were more effective in high-temperature NH3-SCR due to their limited catalytic activity in the side reaction of ammonia oxidation.


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