scholarly journals Deactivation of Cu/SSZ-13 NH3-SCR Catalyst by Exposure to CO, H2, and C3H6

Catalysts ◽  
2019 ◽  
Vol 9 (11) ◽  
pp. 929 ◽  
Author(s):  
Auvray ◽  
Mihai ◽  
Lundberg ◽  
Olsson
Keyword(s):  
Flow Reactor ◽  
Catalytic Reduction ◽  
Plug Flow ◽  
Acid Sites ◽  
Drift Spectroscopy ◽  
Scr Catalyst ◽  
Nh3 Scr ◽  
Scr Catalysts ◽  
Nh3 Oxidation ◽  
Diffuse Reflectance Infrared

Lean nitric oxide (NOx)-trap (LNT) and selective catalytic reduction (SCR) are efficient systems for the abatement of NOx. The combination of LNT and SCR catalysts improves overall NOx removal, but there is a risk that the SCR catalyst will be exposed to high temperatures and rich exhaust during the LNTs sulfur regeneration. Therefore, the effect of exposure to various rich conditions and temperatures on the subsequent SCR activity of a Cu-exchanged chabazite catalyst was studied. CO, H2, C3H6, and the combination of CO + H2 were used to simulate rich conditions. Aging was performed at 800 °C, 700 °C, and, in the case of CO, 600 °C, in a plug-flow reactor. Investigation of the nature of Cu sites was performed with NH3-temperature-programed desorption (TPD) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFT) of probe molecules (NH3 and NO). The combination of CO and H2 was especially detrimental to SCR activity and to NH3 oxidation. Rich aging with low reductant concentrations resulted in a significantly larger deactivation compared to lean conditions. Aging in CO at 800 °C caused SCR deactivation but promoted high-temperature NH3 oxidation. Rich conditions greatly enhanced the loss of Brønsted and Lewis acid sites at 800 °C, indicating dealumination and Cu migration. However, at 700 °C, mainly Brønsted sites disappeared during aging. DRIFT spectroscopy analysis revealed that CO aging modified the Cu2+/CuOH+ ratio in favor of the monovalent CuOH+ species, as opposed to lean aging. To summarize, we propose that the reason for the increased deactivation observed for mild rich conditions is the transformation of the Cu species from Z2Cu to ZCuOH, possibly in combination with the formation of Cu clusters.

scholarly journals Cu-IM-5 as the Catalyst for Selective Catalytic Reduction of NOx with NH3: Role of Cu Species and Reaction Mechanism

Catalysts ◽  
2021 ◽  
Vol 11 (2) ◽  
pp. 221
Author(s):  
Guangying Fu ◽  
Junwen Chen ◽  
Yuqian Liang ◽  
Rui Li ◽  
Xiaobo Yang ◽  
...  
Keyword(s):  
Reaction Mechanism ◽  
Selective Catalytic Reduction ◽  
Low Temperatures ◽  
Catalytic Reduction ◽  
Oxidation Activity ◽  
Paramagnetic Resonance ◽  
Nh3 Scr ◽  
Nh3 Oxidation ◽  
Diffuse Reflectance Infrared

The role of Cu species in Cu ion-exchanged IM-5 zeolite (Cu-IM-5) regarding the performance in selective catalytic reduction (SCR) of NOx with NH3 (NH3-SCR) and the reaction mechanism was studied. Based on H2 temperature-programmed reduction (H2-TPR) and electron paramagnetic resonance (EPR) results, Cu–O–Cu and isolated Cu species are suggested as main Cu species existing in Cu-IM-5 and are active for SCR reaction. Cu–O–Cu species show a good NH3-SCR activity at temperatures below 250 °C, whereas their NH3 oxidation activity at higher temperatures hinders the SCR performance. At low temperatures, NH4NO3 and NH4NO2 are key reaction intermediates. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) suggests a mixed Eley–Rideal (E–R) and Langmuir–Hinshelwood (L–H) mechanism over Cu-IM-5 at low temperatures.

NO2 Reaction Pathways With NH3 on an Fe-Zeolite SCR Catalyst

2011 ◽  
Author(s):  
Michael A. Smith ◽  
Christopher D. Depcik ◽  
Stefan Klinkert ◽  
John W. Hoard ◽  
Stanislav V. Bohac ◽  
...  
Keyword(s):  
Flow Reactor ◽  
Catalytic Reduction ◽  
Nox Reduction ◽  
Catalyst System ◽  
Lean Nox Trap ◽  
Scr Catalyst ◽  
Nh3 Scr ◽  
Nox Conversion ◽  
Lean Nox ◽  
System Part

One approach for nitrogen oxides (NOx) emission control of medium duty diesel engines is through the use of a combination Lean NOx Trap and Selective Catalytic Reduction (LNT-SCR) catalyst system. In this system, part of the NOx conversion occurs via an NH3 SCR catalyst that is dependent on the NO2 to NOx ratio of the feed gas with NO2 being a more advantageous oxidizer. One benefit of using this system is the conversion of NO to NO2 over the LNT which increases the NO2:NOx ratio of the feed gas to the SCR catalyst. An experimental study has been performed to investigate the NO2-NH3 reaction for an Fe-based zeolite SCR catalyst using a bench top flow reactor. The increase in NO2 concentration at the inlet of the SCR results in the formation of large quantities of N2O from 200°C to 400°C. Further experiments determined that N2O and NH3 react above 350°C. This has led to a hypothesis that one primary SCR reaction (Slow SCR) can be replaced with two reaction steps featuring NH3, NO2, and N2O. As a result, this paper proposes five NOx reduction reactions as part of a global mechanism, which would account for the observed experimental behavior.

scholarly journals Comparision on the Low-Temperature NH3-SCR Performance of γ-Fe2O3 Catalysts Prepared by Two Different Methods

Catalysts ◽  
2019 ◽  
Vol 9 (12) ◽  
pp. 1018
Author(s):  
Naveed Husnain ◽  
Enlu Wang ◽  
Shagufta Fareed ◽  
Muhammad Tuoqeer Anwar
Keyword(s):  
Photoelectron Spectroscopy ◽  
Catalytic Reduction ◽  
Acid Sites ◽  
High Concentration ◽  
X Ray ◽  
Nh3 Scr ◽  
Transmission Electron ◽  
Temperature Programmed ◽  
Diffuse Reflectance Infrared

Maghemite (γ-Fe2O3) catalysts were prepared by two different methods, and their activities and selectivities for selective catalytic reduction of NO with NH3 were investigated. The methods of X-ray powder diffraction (XRD), Brunauer–Emmett–Teller (BET), X-ray photoelectron spectroscopy (XPS), hydrogen temperature-programmed reduction (H2-TPR), ammonia temperature-programmed desorption (NH3-TPD), transmission electron microscopy (TEM), Energy-dispersive X-ray spectroscopy (EDS), and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) were used to characterize the catalysts. The resulted demonstrated that the γ-Fe2O3 nanoparticles prepared by the facile method (γ-Fe2O3–FM) not only exhibited better NH3-SCR activity and selectivity than the catalyst prepared by the coprecipitation method but also showed improved SO2 tolerance. This superior NH3-SCR performance was credited to the existence of the larger surface area, better pore structure, a high concentration of lattice oxygen and surface-adsorbed oxygen, good reducibility, a lot of acid sites, lower activation energy, adsorption of the reactants, and the existence of unstable nitrates on the surface of the γ-Fe2O3–FM.

scholarly journals Promoting Effect of Mn on In Situ Synthesized Cu-SSZ-13 for NH3-SCR

Catalysts ◽  
2020 ◽  
Vol 10 (12) ◽  
pp. 1375
Author(s):  
Jinpeng Du ◽  
Jingyi Wang ◽  
Xiaoyan Shi ◽  
Yulong Shan ◽  
Yan Zhang ◽  
...  
Keyword(s):  
Low Temperature ◽  
Active Sites ◽  
Catalytic Reduction ◽  
Acid Sites ◽  
Promoting Effect ◽  
Nh3 Scr ◽  
Temperature Programmed ◽  
Diffuse Reflectance Infrared ◽  
Redox Ability

The effect of Mn impregnation on the NH3-SCR (selective catalytic reduction of NOx by NH3) activity of in situ synthesized Cu-SSZ-13 was investigated in this work. It was found that Mn addition could efficiently improve the low-temperature activity of Cu-SSZ-13. The optimal amount of Mn was 5 wt.%, and NOx conversion was improved by more than 20% over a temperature range of 120 °C to 150 °C. SEM (scanning electron microscopy), XRD (X-ray diffraction), N2 adsorption-desorption, H2-TPR (temperature programmed reduction of H2), NH3-TPD (temperature programmed desorption of NH3) and in situ DRIFTS (diffuse reflectance infrared Fourier transform spectroscopy) experiments were conducted to investigate the changes in the zeolite structure, active sites, acid sites and reaction mechanism. The impregnated MnOx species caused a decline in the crystallinity of Cu-SSZ-13 but markedly improved the redox ability. Nitrate and nitrite species were observed in the Mn-modified Cu-SSZ-13, and the formation of these species was thought to cause the observed increase in low-temperature NH3-SCR activity. The results show that the addition of Mn is a promising method for promoting the low-temperature catalytic activity of Cu-SSZ-13.

scholarly journals Preparation of Mesoporous Mn–Ce–Ti–O Aerogels by a One-Pot Sol–Gel Method for Selective Catalytic Reduction of NO with NH3

Materials ◽  
2020 ◽  
Vol 13 (2) ◽  
pp. 475
Author(s):  
Yabin Wei ◽  
Shuangling Jin ◽  
Rui Zhang ◽  
Weifeng Li ◽  
Jiangcan Wang ◽  
...  
Keyword(s):  
Selective Catalytic Reduction ◽  
Lewis Acid ◽  
Catalytic Reduction ◽  
Sol Gel ◽  
Acid Sites ◽  
Lewis Acid Sites ◽  
One Pot ◽  
Gel Method ◽  
Nh3 Scr ◽  
Composite Aerogels

Novel Mn–Ce–Ti–O composite aerogels with large mesopore size were prepared via a one-pot sol–gel method by using propylene oxide as a network gel inducer and ethyl acetoacetate as a complexing agent. The effect of calcination temperature (400, 500, 600, and 700 °C) on the NH3–selective catalytic reduction (SCR) performance of the obtained Mn–Ce–Ti–O composite aerogels was investigated. The results show that the Mn–Ce–Ti–O catalyst calcined at 600 °C exhibits the highest NH3–SCR activity and lowest apparent activation energy due to its most abundant Lewis acid sites and best reducibility. The NO conversion of the MCTO-600 catalyst maintains 100% at 200 °C in the presence of 100 ppm SO2, showing the superior resistance to SO2 poisoning as compared with the MnOx–CeO2–TiO2 catalysts reported the literature. This should be mainly attributed to its large mesopore sizes with an average pore size of 32 nm and abundant Lewis acid sites. The former fact facilitates the decomposition of NH4HSO4, and the latter fact reduces vapor pressure of NH3. The NH3–SCR process on the MCTO-600 catalyst follows both the Eley–Rideal (E–R) mechanism and the Langmuir–Hinshelwood (L–H) mechanism.

scholarly journals The Effect of Tourmaline on SCR Denitrification Activity of MnOx/TiO2 at Low Temperature

Catalysts ◽  
2020 ◽  
Vol 10 (9) ◽  
pp. 1020
Author(s):  
Yizhe Helian ◽  
Suping Cui ◽  
Xiaoyu Ma
Keyword(s):  
Low Temperature ◽  
Catalytic Reduction ◽  
Catalytic Performance ◽  
Scr Catalyst ◽  
Highly Efficient ◽  
Nh3 Scr ◽  
Catalytic Material ◽  
Acidic Sites ◽  
Denitrification Activity ◽  
The Stability

Selective catalytic reduction (SCR) technology is the most widely used flue gas denitration technology at present. The stability of a catalyst is the main factor limiting the development of this technology. In this study, an environmentally friendly and highly efficient NH3-SCR catalyst was prepared by coprecipitation method from acidolysis residue of industrial waste and tourmaline. We found that the addition of tourmaline has an important impact on the denitration activity of the catalytic material. The NOx conversion exceeded 97% at 200 °C with the dosage of 10% tourmaline, which is about 7% higher than that without doping. The improvement of catalytic performance was mostly attributed to the permanent electrodes of tourmaline, which effectively promotes the dispersion of MnOx/TiO2 catalytic materials, increases the number of acidic sites and changes the valence distribution of manganese ions in products, which speeds up the diffusion of protons and ions, resulting in the acceleration of redox reaction. These as-developed tourmaline-modified MnOx/TiO2 materials have been demonstrated to be promising as a new type of highly efficient low-temperature NH3-SCR catalyst.

scholarly journals Mechanism and Performance of the SCR of NO with NH3 over Sulfated Sintered Ore Catalyst

Catalysts ◽  
2019 ◽  
Vol 9 (1) ◽  
pp. 90 ◽  
Author(s):  
Wangsheng Chen ◽  
Fali Hu ◽  
Linbo Qin ◽  
Jun Han ◽  
Bo Zhao ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Catalytic Reduction ◽  
Nox Reduction ◽  
Space Velocity ◽  
Acid Sites ◽  
X Ray Diffraction ◽  
X Ray ◽  
Diffuse Reflectance Infrared Spectroscopy ◽  
And Performance ◽  
Diffuse Reflectance Infrared

A sulfated sintered ore catalyst (SSOC) was prepared to improve the denitration performance of the sintered ore catalyst (SOC). The catalysts were characterized by X-ray Fluorescence Spectrometry (XRF), Brunauer–Emmett–Teller (BET) analyzer, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and diffuse reflectance infrared spectroscopy (DRIFTS) to understand the NH3-selective catalytic reduction (SCR) reaction mechanism. Moreover, the denitration performance and stability of SSOC were also investigated. The experimental results indicated that there were more Brønsted acid sites at the surface of SSOC after the treatment by sulfuric acid, which lead to the enhancement of the adsorption capacity of NH3 and NO. Meanwhile, Lewis acid sites were also observed at the SSOC surface. The reaction between −NH2, NH 4 + and NO (E-R mechanism) and the reaction of the coordinated ammonia with the adsorbed NO2 (L-H mechanism) were attributed to NOx reduction. The maximum denitration efficiency over the SSOC, which was about 92%, occurred at 300 °C, with a 1.0 NH3/NO ratio, and 5000 h−1 gas hourly space velocity (GHSV).

scholarly journals The Keggin Structure: An Important Factor in Governing NH3–SCR Activity Over the V2O5–MoO3/TiO2 Catalyst

2018 ◽  
Vol 148 (4) ◽  
pp. 1228-1235 ◽  
Author(s):  
Rui Wu ◽  
Ningqiang Zhang ◽  
Xiaojun Liu ◽  
Lingcong Li ◽  
Liyun Song ◽  
...  
Keyword(s):  
Low Temperature ◽  
Catalytic Reduction ◽  
Physicochemical Characteristics ◽  
Acid Sites ◽  
Keggin Structure ◽  
Lewis Acid Sites ◽  
Nh3 Scr ◽  
Strong Acidity ◽  
Ft Ir ◽  
Brønsted And Lewis Acid

Abstract Heteropolyacids and their salts have been effectively used in selective catalytic reduction because of the Keggin structure and extraordinarily strong acidity. Catalysts with and without the Keggin structure were synthesized to further investigate the effects of heteropolyoxometallate on low temperature NH3–SCR. XRD, BET, Raman, H2–TPR, NH3–TPD, FT-IR, and SO2–TPD techniques were used to characterize the physicochemical characteristics of the catalysts. Results indicate that catalysts with the Keggin structure had more surface Brönsted and Lewis acid sites, and these catalysts had significantly improved performances in the SCR reaction and in SO2 poisoning resistance. Graphical Abstract

Iron-exchanged high-silica LTA zeolites as hydrothermally stable NH3-SCR catalysts

2019 ◽  
Vol 4 (6) ◽  
pp. 1050-1058 ◽  
Author(s):  
Taekyung Ryu ◽  
Yonjoo Kang ◽  
In-Sik Nam ◽  
Suk Bong Hong
Keyword(s):  
High Activity ◽  
Selective Catalytic Reduction ◽  
Catalytic Reduction ◽  
Hydrothermal Aging ◽  
Reduction Of No ◽  
Nh3 Scr ◽  
Scr Catalysts ◽  
High Silica

Iron-exchanged high-silica LTA zeolites exhibit high activity for selective catalytic reduction of NOx by NH3, even after hydrothermal aging at 900 °C.

scholarly journals Experimental Study on the Deactivating Effect of KNO3, KCl, and K2SO4on Nanosized Ceria/Titania SCR Catalyst

2015 ◽  
Vol 2015 ◽  
pp. 1-10
Author(s):  
Xiongbo Chen ◽  
Ping Fang ◽  
Wenhao Zeng ◽  
Kunyuan Liu ◽  
Zhixiong Tang ◽  
...  
Keyword(s):  
Oxygen Diffusion ◽  
Surface Defects ◽  
Catalytic Reduction ◽  
Surface Acidity ◽  
Acid Sites ◽  
Ammonia Adsorption ◽  
Scr Catalyst ◽  
No Conversion ◽  
Ceria Reduction ◽  
Potassium Addition

Nanosized Ce/TiO2is effective in selective catalytic reduction of NO with NH3. The NO conversion of Ce/TiO2is 93% at 370°C. However, addition of potassium using KNO3, KCl, or K2SO4as precursors effectively deactivates Ce/TiO2. NO conversion at 370°C is reduced to 45%, 24%, and 16% after addition of KNO3, KCl, and K2SO4, respectively, with a controlled K/Ce molar ration at 0.25. The deactivation may be attributed to the changes in the structural and chemical state of ceria and the degradation of surface acidity. The transformation of amorphous ceria into ceria crystals after potassium addition, together with the decrease of surface defects, is also determined. Oxygen diffusion in the process of ceria reduction is slow, and the redox cycle is slowed down. Moreover, the surface acid sites are markedly destroyed, leading to the reduced capacity of ammonia adsorption. These results may provide useful information for the application and life management of CeO2/TiO2in potassium-rich environments such as biofuel-fired boilers.

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