scholarly journals Modified Zeolite Catalyst for a NOx Selective Catalytic Reduction Process in Nitric Acid Plants

Catalysts ◽  
2021 ◽  
Vol 11 (4) ◽  
pp. 450
Author(s):  
Magdalena Saramok ◽  
Agnieszka Szymaszek ◽  
Marek Inger ◽  
Katarzyna Antoniak-Jurak ◽  
Bogdan Samojeden ◽  
...  

Natural zeolite of the heulandite-type framework was modified with iron and tested as a catalyst for the selective catalytic reduction of nitrogen oxides with ammonia (NH3-SCR) in the temperature range of 150–450 °C. The catalyst was prepared at a laboratory scale in a powder form and then the series of experiments of its shaping into tablets was conducted. Physicochemical studies of the catalyst (N2 sorption at −196 °C, FT-IR, XRD, UV-vis) were performed to determine the textural and structural properties and identify the surface functional groups, the crystalline structure of the catalysts and the form and aggregation of the active phase. The activity tests over the shaped catalyst were performed industry-reflecting conditions, using tail gases from the pilot nitric acid plant. The influence of a temperature, catalyst load, and the amount of reducing agent (ammonia) on the NOx reduction process were investigated. The results of catalytic tests that were performed on model gas mixture showed that non-modified clinoptilolite exhibited around 58% conversion of NO at 450 °C. The temperature window of the shaped catalyst shifted to a higher temperature range in comparison to the powder sample. The catalytic performance of the shaped Fe-clinoptilolite in the industry-reflecting conditions was satisfactory, especially at 450 °C. Additionally, it was observed that the ratio of N2O concentration downstream and upstream of the catalytic bed was below 1, which indicated that the catalyst exhibited activity in both DeNOx and DeN2O process.

2021 ◽  
Author(s):  
Cherif Larabi ◽  
Cuirong chen ◽  
Nicolas Merle ◽  
marc charlin ◽  
Kai Chung Szeto ◽  
...  

A novel well-defined precatalyst for ammonia selective catalytic reduction of NOx (NH3-SCR), [W(CtBu)(CH2tBu)3]/CeO2, was prepared by surface organometallic chemistry and characterized. Due to the high dispersion of the active phase,...


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.


Processes ◽  
2021 ◽  
Vol 9 (11) ◽  
pp. 1966
Author(s):  
Shiyong Yu ◽  
Jichao Zhang

A systematic modeling approach was scrutinized to develop a kinetic model and a novel monolith channel geometry was designed for NH3 selective catalytic reduction (NH3-SCR) over Cu-ZSM-5. The redox characteristic of Cu-based catalysts and the variations of NH3, NOx concentration, and NOx conversion along the axis in porous media channels were studied. The relative pressure drop in different channels, the variations of NH3 and NOx conversion efficiency were analyzed. The model mainly considers NH3 adsorption and desorption, NH3 oxidation, NO oxidation, and NOx reduction. The results showed that the model could accurately predict the NH3-SCR reaction. In addition, it was found that the Cu-based zeolite catalyst had poor low-temperature catalytic performance and good high-temperature activity. Moreover, the catalytic reaction of NH3-SCR was mainly concentrated in the upper part of the reactor. In addition, the hexagonal channel could effectively improve the diffusion rate of gas reactants to the catalyst wall, reduce the pressure drop and improve the catalytic conversion efficiencies of NH3 and NOx.


Catalysts ◽  
2020 ◽  
Vol 10 (3) ◽  
pp. 314
Author(s):  
Xing Ning ◽  
Zhi-bo Xiong ◽  
Bin Yang ◽  
Wei Lu ◽  
Shui-mu Wu

Sol-gel spread self-combustion is the burning of the complexing agent in dried gel and the oxidant. Meanwhile, high temperature takes place during the combustion process, which is harmful to the pore structure of the catalyst. The nitrate from metal nitrate precursors as an oxidant could participate in the spread of the self-combustion process. Therefore, the influence of nitrate from metal nitrate on the spread self-combustion of an iron–cerium–tungsten citric acid gel and its catalytic performance of NOx reduction were investigated by removing nitrate via the dissolution of washing co-precipitation with citric acid and re-introducing nitric acid into the former solution. It was found that the removal of nitrate contributes to enhancing the NH3–SCR activity of the magnetic mixed oxide catalyst. The NOx reduction efficiency was close to 100% for Fe85Ce10W5–CP–CA at 250 °C while the highest was only 80% for the others. The results of thermal analysis demonstrate that the spread self-combustion process of citric acid dried gel is enhanced by re-introducing nitric acid into the citric acid dissolved solution when compared with the removal of nitrate. In addition, the removal of nitrate helps in the formation of γ-Fe2O3 crystallite in the catalyst, refining the particle size of the catalyst and increasing its pore volume. The removal of nitrate also contributes to the formation of Lewis acid sites and Brønsted acid sites on the surface of the catalyst compared with the re-introduction of nitric acid. The in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) demonstrates that both Eley–Rideal (E–R) and Langmuir–Hinshelwood (L–H) mechanisms exist over Fe85Ce10W5–CP–CA at 250 °C with E–R as its main mechanism.


Materials ◽  
2018 ◽  
Vol 11 (8) ◽  
pp. 1307 ◽  
Author(s):  
Yaping Zhang ◽  
Xiupeng Yue ◽  
Tianjiao Huang ◽  
Kai Shen ◽  
Bin Lu

TiO2-ZrO2 (Ti-Zr) carrier was prepared by a co-precipitation method and 1 wt. % V2O5 and 0.2 CeO2 (the Mole ratio of Ce to Ti-Zr) was impregnated to obtain the V2O5-CeO2/TiO2-ZrO2 catalyst for the selective catalytic reduction of NOx by NH3. The transient activity tests and the in situ DRIFTS (diffuse reflectance infrared Fourier transform spectroscopy) analyses were employed to explore the NH3-SCR (selective catalytic reduction) mechanism systematically, and by designing various conditions of single or mixing feeding gas and pre-treatment ways, a possible pathway of NOx reduction was proposed. It was found that NH3 exhibited a competitive advantage over NO in its adsorption on the catalyst surface, and could form an active intermediate substance of -NH2. More acid sites and intermediate reaction species (-NH2), at lower temperatures, significantly promoted the SCR activity of the V2O5-0.2CeO2/TiO2-ZrO2 catalyst. The presence of O2 could promote the conversion of NO to NO2, while NO2 was easier to reduce. The co-existence of NH3 and O2 resulted in the NH3 adsorption strength being lower, as compared to tests without O2, since O2 could occupy a part of the active site. Due to CeO2’s excellent oxygen storage-release capacity, NH3 adsorption was weakened, in comparison to the 1 wt. % V2O5-0.2CeO2/TiO2-ZrO2 catalyst. If NOx were to be pre-adsorbed in the catalyst, the formation of nitrate and nitro species would be difficult to desorb, which would greatly hinder the SCR reaction. All the findings concluded that NH3-SCR worked mainly through the Eley-Rideal (E-R) mechanism.


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.


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.


Catalysts ◽  
2018 ◽  
Vol 8 (9) ◽  
pp. 384 ◽  
Author(s):  
Ruonan Wang ◽  
Xu Wu ◽  
Chunlei Zou ◽  
Xiaojian Li ◽  
Yali Du

A series of NiFe mixed oxide catalysts were prepared via calcining hydrotalcite-like precursors for the selective catalytic reduction of nitrogen oxides (NOx) with NH3 (NH3-SCR). Multiple characterizations revealed that catalytic performance was highly dependent on the phase composition, which was vulnerable to the calcination temperature. The MOx phase (M = Ni or Fe) formed at a lower calcination temperature would induce more favorable contents of Fe2+ and Ni3+ and as a result contribute to the better redox capacity and low-temperature activity. In comparison, NiFe2O4 phase emerged at a higher calcination temperature, which was expected to generate more Fe species on the surface and lead to a stable structure, better high-temperature activity, preferable SO2 resistance, and catalytic stability. The optimum NiFe-500 catalyst incorporated the above virtues and afforded excellent denitration (DeNOx) activity (over 85% NOx conversion with nearly 98% N2 selectivity in the region of 210–360 °C), superior SO2 resistance, and catalytic stability.


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