scholarly journals Promotional Effect of Cerium and/or Zirconium Doping on Cu/ZSM-5 Catalysts for Selective Catalytic Reduction of NO by NH3

Catalysts ◽  
2018 ◽  
Vol 8 (8) ◽  
pp. 306 ◽  
Author(s):  
Ye Liu ◽  
Chonglin Song ◽  
Gang Lv ◽  
Chenyang Fan ◽  
Xiaodong Li

The cerium and/or zirconium-doped Cu/ZSM-5 catalysts (CuCexZr1−xOy/ZSM-5) were prepared by ion exchange and characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), temperature-programmed reduction by hydrogen (H2-TPR). Activities of the catalysts obtained on the selective catalytic reduction (SCR) of nitric oxide (NO) by ammonia were measured using temperature programmed reactions. Among all the catalysts tested, the CuCe0.75Zr0.25Oy/ZSM-5 catalyst presented the highest catalytic activity for the removal of NO, corresponding to the broadest active window of 175–468 °C. The cerium and zirconium addition enhanced the activity of catalysts, and the cerium-rich catalysts exhibited more excellent SCR activities as compared to the zirconium-rich catalysts. XRD and TEM results indicated that zirconium additions improved the copper dispersion and prevented copper crystallization. According to XPS and H2-TPR analysis, copper species were enriched on the ZSM-5 grain surfaces, and part of the copper ions were incorporated into the zirconium and/or cerium lattice. The strong interaction between copper species and cerium/zirconium improved the redox abilities of catalysts. Furthermore, the introduction of zirconium abates N2O formation in the tested temperature range.

Catalysts ◽  
2020 ◽  
Vol 10 (2) ◽  
pp. 202
Author(s):  
Long Lu ◽  
Xueman Wang ◽  
Chunhua Hu ◽  
Ying Liu ◽  
Xiongbo Chen ◽  
...  

Nanosized V-Ce oxides supported on TiO2 (VCT) were prepared and utilized in the low-temperature selective catalytic reduction (SCR) of NO with NH3. Compared with the other V-Ce oxides-based catalysts supported on Al2O3, ZrO2, and ZSM-5, VCT showed the best SCR activity in a low-temperature range. The NOx conversion of 90% could be achieved at 220 °C. Characterizations including X-ray diffraction (XRD), scanning election micrograph (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), temperature-programmed desorption with NH3 (NH3-TPD), and temperature-programmed reduction with H2 (H2-TPR) showed that V1.05Ce1/TiO2 exhibited a good dispersion of V2O5, enrichment of surface Ce3+ and chemical-absorbed oxygen, and excellent redox capacity and acidity, which resulted in the best SCR performance at low temperature.


Catalysts ◽  
2021 ◽  
Vol 11 (2) ◽  
pp. 259
Author(s):  
Siva Sankar Reddy Putluru ◽  
Leonhard Schill ◽  
Anker Degn Jensen ◽  
Bernard Siret ◽  
Frank Tabaries ◽  
...  

Preparation of Mn/TiO2, Mn-Fe/TiO2, and Mn-Fe-Ce/TiO2 by the deposition-precipitation (DP) method can afford very active catalysts for low-temperature NH3-SCR (selective catalytic reduction of NO with NH3). The effect of precursor choice (nitrate vs. acetate) of Mn, Fe, and Ce on the physiochemical properties including thermal stability and the resulting SCR activity were investigated. The resulting materials were characterized by N2-Physisorption, XRD (Powder X-ray diffraction), XPS (X-ray photoelectron spectroscopy), H2-TPR (temperature-programmed reduction with hydrogen), and the oxidation of NO to NO2 measured at 300 °C. Among all the prepared catalysts 5MnAce/Ti, 25Mn0.75AceFe0.25Nit/Ti, and 25Mn0.75AceFe0.20NitCe0.05Ace/Ti showed superior SCR activity at low temperature. The superior activity of the latter two materials is likely attributable to the presence of amorphous active metal oxide phases (manganese-, iron- and cerium-oxide) and the ease of the reduction of metal oxides on TiO2. Enhanced ability to convert NO to NO2, which can promote fast-SCR like pathways, could be another reason. Cerium was found to stabilize amorphous manganese oxide phases when exposed to high temperatures.


Catalysts ◽  
2019 ◽  
Vol 9 (11) ◽  
pp. 956 ◽  
Author(s):  
Husnain ◽  
Wang ◽  
Fareed

The selective catalytic reduction of NO with NH3 at low temperatures has been investigated with natural iron ore catalysts. Four iron ore raw materials from different locations were taken and processed to be used as catalysts. The methods of X-ray diffraction (XRD), X-ray fluorescence (XRF), Brunauer-Emmett-Teller (BET), X-ray photoelectron spectroscopy (XPS), hydrogen temperature-programmed reduction (H2-TPR), ammonia temperature-programmed desorption (NH3-TPD), scanning electron microscopy (SEM) and Fourier-transform infrared spectroscopy (FTIR) were used to characterize the materials. The results showed that the sample A (comprised mainly of α-Fe2O3 and γ-Fe2O3), calcined at 250 °C, achieved excellent selective catalytic reduction (SCR) activity (above 80% at 170–350 °C) and N2 selectivity (above 90% up to 250 °C) at low temperatures. Suitable calcination temperature, large surface area, high concentration of surface-adsorbed oxygen, good reducibility, lots of acid sites and adsorption of the reactants were responsible for the excellent SCR performance of the iron ore. However, the addition of H2O and SO2 in the feed gas showed some adverse effects on the SCR activity. The FT-IR analysis indicated the formation of sulfate salts on the surface of the catalyst during the SCR reaction in the presence of SO2, which could cause pore plugging and result in the suppression of the catalytic activity.


Author(s):  
Vahid Zabihi ◽  
Mohammad Hasan Eikani ◽  
Mehdi Ardjmand ◽  
Seyed Mahdi Latifi ◽  
Alireza Salehirad

Abstract One of the most significant aspects in selective catalytic reduction (SCR) of nitrogen oxides (NOx) is developing suitable catalysts by which the process occurs in a favorable way. At the present work SCR reaction by ammonia (NH3-SCR) was conducted using Co-Mn spinel and its composite with Fe-Mn spinel, as nanocatalysts. The nanocatalysts were fabricated through liquid routes and then their physicochemical properties such as phase composition, degree of agglomeration, particle size distribution, specific surface area and also surface acidic sites have been investigated by X-ray diffraction, Field Emission Scanning Electron Microscope, Energy-dispersive X-ray spectroscopy, energy dispersive spectroscopy mapping, Brunauer–Emmett–Teller, temperature-programmed reduction (H2-TPR) and temperature-programmed desorption of ammonia (NH3-TPD) analysis techniques. The catalytic activity tests in a temperature window of 150–400 °C and gas hourly space velocities of 10,000, 18,000 and 30,000 h−1 revealed that almost in all studied conditions, CoMn2O4/FeMn2O4 nanocomposite exhibited better performance in SCR reaction than CoMn2O4 spinel.


Catalysts ◽  
2019 ◽  
Vol 9 (4) ◽  
pp. 357 ◽  
Author(s):  
Huang ◽  
Li ◽  
Qiu ◽  
Chen ◽  
Cheng ◽  
...  

In the present study, a series of CeO2/TiO2 catalysts were fabricated by dry ball milling method in the absence and presence of organic assistants, and their catalytic performances for the selective catalytic reduction (SCR) of NO by NH3 were investigated. It was found that the addition of organic assistants in the ball milling process and the calcining ambience exerted a significant influence on the catalytic performances of CeO2/TiO2 catalysts. The nitrogen sorption isotherm measurement (BET), powder X-ray diffraction (XRD), Raman spectra, high-resolution transmission electron microscopy (HR-TEM), hydrogen temperature-programmed reduction (H2-TPR), ammonia temperature-programmed desorption (NH3-TPD), sulfur dioxide temperature-programmed desorption (SO2-TPD), thermogravimetric analysis (TG), Fourier transform infrared (FT-IR) and X-ray photoelectron spectra (XPS) characterizations showed that the introduction of citric acid in the ball milling process could significantly change the decomposition process of the precursor mixture, which can lead to improved dispersion and reducibility of cerium species, surface acidity as well as the surface microstructure, all which were responsible for the high low temperature activity of CeTi-C-N in an NH3-SCR reaction. In contrast, the addition of sucrose in the milling process showed an inhibitory effect on the catalytic performance of CeO2/TiO2 catalyst in an NH3-SCR reaction, possibly due to the decrease of the crystallinity of the TiO2 support and the carbon residue covering the active sites.


Catalysts ◽  
2019 ◽  
Vol 9 (1) ◽  
pp. 62 ◽  
Author(s):  
Gunugunuri K. Reddy ◽  
Torin C. Peck ◽  
Charles A. Roberts

Direct decomposition of NO into N2 and O2 (2NO→N2 + O2) is recognized as the “ideal” reaction for NOx removal because it needs no reductant. It was reported that the spinel Co3O4 is one of the most active single-element oxide catalysts for NO decomposition at higher reaction temperatures, however, activity remains low below 650 °C. The present study aims to investigate new promoters for Co3O4, specifically PdO vs. PtO. Interestingly, the PdO promoter effect on Co3O4 was much greater than the PtO effect, yielding a 4 times higher activity for direct NO decomposition at 650 °C. Also, Co3O4 catalysts with the PdO promoter exhibit higher selectivity to N2 compared to PtO/Co3O4 catalysts. Several characterization measurements, including X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), H2-temperature programmed reduction (H2-TPR), and in situ FT-IR, were performed to understand the effect of PdO vs. PtO on the properties of Co3O4. Structural and surface analysis measurements show that impregnation of PdO on Co3O4 leads to a greater ease of reduction of the catalysts and an increased thermal stability of surface adsorbed NOx species, which contribute to promotion of direct NO decomposition activity. In contrast, rather than remaining solely as a surface species, PtO enters the Co3O4 structure, and it promotes neither redox properties nor NO adsorption properties of Co3O4, resulting in a diminished promotional effect compared to PdO.


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.


2010 ◽  
Vol 224 (06) ◽  
pp. 907-920 ◽  
Author(s):  
Fei Li ◽  
Dehai Xiao ◽  
Jing Li ◽  
Xiangguang Yang

AbstractSelective catalytic reduction (SCR) of NO with propane using bimetals (3Co2Ce, 3Co2Sr, 3Co2Sn and 3Co2In) loaded on HMCM-49 zeolite was studied under lean-burn condition. Only 3Co2In/HMCM-49 exhibited higher deNOx activity in a wide temperature range. The catalysts were characterized by N2-adsoption, X-ray diffraction (XRD), temperature-programmed surface reactions (TPSR) and temperature-programmed desorption (TPD) of NO. TPSR and TPD results exhibited that the addition of In inhibited the oxidation ability of Co on 3Co2In/HMCM-49 catalyst, but enhanced NOx adsorption.


2020 ◽  
Vol 218 ◽  
pp. 03032
Author(s):  
Chenxi Li ◽  
Fanwei Meng ◽  
Qing Ye

A series of xCe-Fe/ZSM-5 (x = 0, 0.25, 0.5 wt%) samples were prepared by the impregnation method, and the catalytic activity was evaluated by the selective catalytic reduction of NOx with ammonia (NH3-SCR). The physicochemical properties of prepared samples were characterized by various techniques such as X-ray diffraction (XRD), Brunner-Emmet-Teller (BET) measurement, hydrogen temperatureprogrammed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), ammonia temperatureprogrammed desorption (NH3-TPD) and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS). XRD and BET results demonstrated that Ce and Fe species were uniform dispersed on the surface of the ZSM-5 zeolite and the micropore structure of ZSM-5 was still maintained. H2-TPR analysis indicated that the doping of Ce created more isolated Ce4+ and Fe3+ on the surface of catalysts, and the abundant Ce4+ and Fe3+ could enhance the reduction ability of catalysts. XPS analysis suggested that the doping of Ce could generate more oxygen vacancies, thereby increasing the number of chemisorption oxygen. According to the in-situ DRIFTS and NH3-TPD results, Ce species provided more acidic sites, which is beneficial to the NH3 adsorption ability of ZSM-5 zeolite. Additionally, the abundant chemisorption oxygen, medium and strong Brønsted acid sites, excellent NH3 adsorption ability and outstanding reduction property are beneficial to the NH3-SCR reaction. Among all prepared samples, the 0.25Ce-Fe/ZSM-5 sample possessed the widest reaction temperature window and the best catalytic performance (NO conversion over 98% at 350-450 °C), which was associated with the abundant acid sites and remarkable adsorption ability of NH3, outstanding redox ability and abundant chemisorption oxygen after the doping of Ce.


NANO ◽  
2015 ◽  
Vol 10 (04) ◽  
pp. 1550050 ◽  
Author(s):  
Yanbing Zhang ◽  
Zhe Xu ◽  
Xie Wang ◽  
Xiulian Lu ◽  
Yuying Zheng

Mn - FeO x/carbon nanotubes (CNTs) catalysts were firstly prepared via simple incipient wetness method and used for low-temperature selective catalytic reduction (SCR) of NO with NH 3. The structure and surface properties of the catalysts were characterized by N 2 sorption, X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS) and temperature-programmed reduction by hydrogen ( H 2-TPR). It was found that Mn - FeO x/CNTs catalyst exhibited excellent low-temperature SCR activity and SO 2 resistance. XRD patterns revealed that metal oxides catalysts were possessed of amorphous structure. FESEM and TEM images showed that metal oxides catalysts were successfully supported on CNTs. The XPS results indicated that the obtained catalyst presented high Mn 4+/ Mn 3+ and OS/(OS + OL) ratios. The H 2-TPR profiles showed that Mn - FeO x/CNTs catalyst possessed better low-temperature reducibility. Besides, the obtained catalyst exhibited better SO 2 resistance.


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