scholarly journals Modification of V2O5-WO3/TiO2 Catalyst by Loading of MnOx for Enhanced Low-Temperature NH3-SCR Performance

Nanomaterials ◽  
2020 ◽  
Vol 10 (10) ◽  
pp. 1900
Author(s):  
Xianlong Zhang ◽  
Qinchao Diao ◽  
Xiaorui Hu ◽  
Xueping Wu ◽  
Kesong Xiao ◽  
...  

V2O5-WO3/TiO2 as a commercial selective catalytic reduction (SCR) catalyst usually used at middle-high temperatures was modified by loading of MnOx for the purpose of enhancing its performance at lower temperatures. Manganese oxides were loaded onto V-W/Ti monolith by the methods of impregnation (I), precipitation (P), and in-situ growth (S), respectively. SCR activity of each modified catalyst was investigated at temperatures in the range of 100–340 °C. Catalysts were characterized by specific surface area and pore size determination (BET), X-ray diffraction (XRD), temperature programmed reduction (TPR), etc. Results show that the loading of MnOx remarkably enhanced the SCR activity at a temperature lower than 280 °C. The catalyst prepared by the in-situ growth method was found to be most active for SCR.

Author(s):  
Chiara Negri ◽  
Elisa Borfecchia ◽  
Andrea Martini ◽  
Gabriele Deplano ◽  
Kirill A. Lomachenko ◽  
...  

AbstractAmmonia-mediated selective catalytic reduction (NH3-SCR) using Cu-exchanged chabazite zeolites as catalysts is one of the leading technologies for NOx removal from exhaust gases, with CuII/CuI redox cycles being the basis of the catalytic reaction. The amount of CuII ions reduced by NO/NH3 can be quantified by the consumption of NO during temperature-programmed reduction experiments (NO-TPR). In this article, we show the capabilities of in situ X-ray absorption near-edge spectroscopy (XANES), coupled with multivariate curve resolution (MCR) and principal component analysis (PCA) methods, in following CuII/CuI speciation during reduction in NO/NH3 after oxidation in NO/O2 at 50 °C on samples with different copper loading and pretreatment conditions. Our XANES results show that during the NO/NH3 ramp CuII ions are fully reduced to CuI in the 50–290 °C range. The number of species involved in the process, their XANES spectra and their concentration profiles as a function of the temperature were obtained by MCR and PCA. Mixed ligand ammonia solvated complexes [CuII(NH3)3(X)]+ (X = OH−/O− or NO3−) are present at the beginning of the experiment, and are transformed into mobile [CuI(NH3)2]+ complexes: these complexes lose an NH3 ligand and become framework-coordinated above 200 °C. In the process, multiple CuII/CuI reduction events are observed: the first one around 130 °C is identified with the reduction of [CuII(NH3)3(OH/O)]+ moieties, while the second one occurs around 220–240 °C and is associated with the reduction of the ammonia-solvated Cu-NO3− species. The nitrate concentration in the catalysts is found to be dependent on the zeolite Cu loading and on the applied pretreatment conditions. Ammonia solvation increases the number of CuII sites available for the formation of nitrates, as confirmed by infrared spectroscopy.


Catalysts ◽  
2019 ◽  
Vol 9 (12) ◽  
pp. 1018
Author(s):  
Naveed Husnain ◽  
Enlu Wang ◽  
Shagufta Fareed ◽  
Muhammad Tuoqeer Anwar

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.


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 (9) ◽  
pp. 768 ◽  
Author(s):  
Shuang Ding ◽  
Jiankang Zhao ◽  
Qiang Yu

Vapor-phase ketonization of propionic acid derived from biomass was studied at 300–375 °C over ZrO2 with different zirconia polymorph. The tetragonal ZrO2 (t-ZrO2) are more active than monoclinic ZrO2 (m-ZrO2). The results of characterizations from X-ray diffraction (XRD) and Raman suggest m-ZrO2 and t-ZrO2 are synthesized by the solvothermal method. NH3 and CO2 temperature-programmed desorption (NH3-TPD and CO2-TPD) measurements show that there were more medium-strength Lewis acid base sites with lower coordination exposed on m-ZrO2 relative to t-ZrO2, increasing the adsorption strength of propionic acid. The in situ DRIFTS (Diffuse reflectance infrared Fourier transform spectroscopy) of adsorbed propionic acid under ketonization reaction reveal that as the most abundant surface intermediates, the monodentate propionates are more active than bidentate propionates. In comparison with m-ZrO2, the t-ZrO2 surface favors monodentate adsorption over bidentate adsorption. Additionally, the adsorption strength of monodentate propionate is weaker on t-ZrO2. These differences in adsorption configuration and adsorption strength of propionic acid are affected by the zirconia structure. The higher surface concentration and weaker adsorption strength of monodentate propionates contribute to the higher ketonization rate in the steady state.


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 ◽  
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.


Catalysts ◽  
2020 ◽  
Vol 10 (7) ◽  
pp. 807
Author(s):  
Zen Maeno ◽  
Xiaopeng Wu ◽  
Shunsaku Yasumura ◽  
Takashi Toyao ◽  
Yasuharu Kanda ◽  
...  

In this study, the characterization of In-exchanged CHA zeolite (In-CHA (SiO2/Al2O3 = 22.3)) was conducted by in-situ X-ray diffraction (XRD) and ammonia temperature-programmed desorption (NH3-TPD). We also prepared other In-exchanged zeolites with different zeolite structures (In-MFI (SiO2/Al2O3 = 22.3), In-MOR (SiO2/Al2O3 = 20), and In-BEA (SiO2/Al2O3 = 25)) and different SiO2/Al2O3 ratios (In-CHA(Al-rich) (SiO2/Al2O3 = 13.7)). Their catalytic activities in nonoxidative ethane dehydrogenation were compared. Among the tested catalysts, In-CHA(Al-rich) provided the highest conversion. From kinetic experiments and in-situ Fourier transform infrared (FTIR) spectroscopy, [InH2]+ ions are formed regardless of SiO2/Al2O3 ratio, serving as the active sites.


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.


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