scholarly journals Iron-Based Composite Oxide Catalysts Tuned by CTAB Exhibit Superior NH3–SCR Performance

Catalysts ◽  
2021 ◽  
Vol 11 (2) ◽  
pp. 224
Author(s):  
Wenshuo Zhang ◽  
Xiaoyan Shi ◽  
Meng Gao ◽  
Jingjing Liu ◽  
Zhihui Lv ◽  
...  

Iron-based oxide catalysts for the NH3–SCR (selective catalytic reduction of NOx by NH3) reaction have gained attention due to their high catalytic activity and structural adjustability. In this work, iron–niobium, iron–titanate and iron–molybdenum composite oxides were synthesized by a co-precipitation method with or without the assistance of hexadecyl trimethyl ammonium bromide (CTAB). The catalysts synthesized with the assistance of CTAB (FeM0.3Ox-C, M = Nb, Ti, Mo) showed superior SCR performance in an operating temperature range from 150 °C to 400 °C compared to those without CTAB addition (FeM0.3Ox, M = Nb, Ti, Mo). To reveal such enhancement, the catalysts were characterized by N2-physisorption, XRD (Powder X-ray diffraction), NH3-TPD (temperature-programmed desorption of ammonia), DRIFTS (Diffuse Reflectance Infrared Fourier Transform Spectroscopy), XPS (X-ray Photoelectron Spectroscopy), and H2-TPR (H2-Total Physical Response). It was found that the crystalline phase of Fe2O3 formed was influenced by the presence of CTAB in the preparation process, which favored the formation of crystalline γ-Fe2O3. Owing to the changed structure, the redox-acid properties of FeM0.3Ox-C catalysts were modified, with higher exposure of acid sites and improved ability of NO oxidation to NO2 at low-temperature, both of which also contributed to the improvement of NOx conversion. In addition, the weakened redox ability of Fe prevented the over-oxidation of NH3, thus accounting for the greatly improved high-temperature activity as well as N2 selectivity.

2020 ◽  
Vol 10 (1) ◽  
Author(s):  
Arunima Rajan ◽  
Madhulika Sharma ◽  
Niroj Kumar Sahu

Abstract This work reports the fabrication of magnetite (Fe3O4) nanoparticles (NPs) coated with various biocompatible surfactants such as glutamic acid (GA), citric acid (CA), polyethylene glycol (PEG), polyvinylpyrrolidine (PVP), ethylene diamine (EDA) and cetyl-trimethyl ammonium bromide (CTAB) via co-precipitation method and their comparative inductive heating ability for hyperthermia (HT) applications. X-ray and electron diffraction analyses validated the formation of well crystallined inverse spinel structured Fe3O4 NPs (crystallite size of ~ 8–10 nm). Magnetic studies confirmed the superparamagnetic (SPM) behaviour for all the NPs with substantial magnetisation (63–68 emu/g) and enhanced magnetic susceptibility is attributed to the greater number of occupations of Fe2+ ions in the lattice as revealed by X-ray photoelectron spectroscopy (XPS). Moreover, distinctive heating response (specific absorption rate, SAR from 130 to 44 W/g) of NPs with similar size and magnetisation is observed. The present study was successful in establishing a direct correlation between relaxation time (~ 9.42–15.92 ns) and heating efficiency of each surface functionalised NPs. Moreover, heat dissipated in different surface grafted NPs is found to be dependent on magnetic susceptibility, magnetic anisotropy and magnetic relaxation time. These results open very promising avenues to design surface functionalised magnetite NPs for effective HT applications.


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.


Catalysts ◽  
2019 ◽  
Vol 9 (2) ◽  
pp. 175 ◽  
Author(s):  
Yan Gao ◽  
Tao Luan ◽  
Shitao Zhang ◽  
Wenchao Jiang ◽  
Wenchen Feng ◽  
...  

The nanocatalysts of Mn−Co/TiO2 and Mn−Fe/TiO2 were synthesized by hydrothermal method and comprehensively compared from nanostructures, catalytic performance, kinetics, and thermodynamics. The physicochemical properties of the nanocatalysts were analyzed by N2 adsorption, transmission electron microscope (TEM), X-ray diffraction (XRD), H2-temperature-programmed reduction (TPR), NH3-temperature-programmed desorption (TPD), and X-ray photoelectron spectroscopy (XPS). Based on the multiple characterizations performed on Mn−Co/TiO2 and Mn−Fe/TiO2 nanocatalysts, it can be confirmed that the catalytic properties were decidedly dependent on the phase compositions of the nanocatalysts. The Mn−Co/TiO2 sample presented superior structure characteristics than Mn−Fe/TiO2, with the increased surface area, the promoted active components distribution, the diminished crystallinity, and the reduced nanoparticle size. Meanwhile, the Mn4+/Mnn+ ratios in the Mn−Co/TiO2 nanocatalyst were higher than Mn−Fe/TiO2, which further confirmed the better oxidation ability and the larger amount of Lewis acid sites and Bronsted acid sites on the sample surface. Compared to Mn−Fe/TiO2 nanocatalyst, Mn−Co/TiO2 nanocatalyst displayed the preferable catalytic property with higher catalytic activity and stronger selectivity in the temperature range of 75–250 °C. The results of mechanism and kinetic study showed that both Eley-Rideal mechanism and Langmuir-Hinshelwood mechanism reactions contributed to selective catalytic reduction of NO with NH3 (NH3-SCR) over Mn−Fe/TiO2 and Mn−Co/TiO2 nanocatalysts. In this test condition, the NO conversion rate of Mn−Co/TiO2 nanocatalyst was always higher than that of Mn−Fe/TiO2. Furthermore, comparing the reaction between doping transition metal oxides and NH3, the order of temperature−Gibbs free energy under the same reaction temperature is as follows: Co3O4 < CoO < Fe2O3 < Fe3O4, which was exactly consistent with nanostructure characterization and NH3-SCR performance. Meanwhile, the activity difference of MnOx exhibited in reducibility properties and Ellingham Diagrams manifested the promotion effects of cobalt and iron dopings. Generally, it might offer a theoretical method to select superior doping metal oxides for NO conversion by comprehensive comparing the catalytic performance with the insight from nanostructure, catalytic performance, reaction kinetics, and thermodynamics.


Nanomaterials ◽  
2021 ◽  
Vol 11 (2) ◽  
pp. 366
Author(s):  
Margarita Gabrovska ◽  
Ivan Ivanov ◽  
Dimitrinka Nikolova ◽  
Jugoslav Krstić ◽  
Anna Maria Venezia ◽  
...  

Supported gold on co-precipitated nanosized NiAl layered double hydroxides (LDHs) was studied as an effective catalyst for medium-temperature water–gas shift (WGS) reaction, an industrial catalytic process traditionally applied for the reduction in the amount of CO in the synthesis gas and production of pure hydrogen. The motivation of the present study was to improve the performance of the Au/NiAl catalyst via modification by CeO2. An innovative approach for the direct deposition of ceria (1, 3 or 5 wt.%) on NiAl-LDH, based on the precipitation of Ce3+ ions with 1M NaOH, was developed. The proposed method allows us to obtain the CeO2 phase and to preserve the NiAl layered structure by avoiding the calcination treatment. The synthesis of Au-containing samples was performed through the deposition–precipitation method. The as-prepared and WGS-tested samples were characterized by X-ray powder diffraction, N2-physisorption and X-ray photoelectron spectroscopy in order to clarify the effects of Au and CeO2 loading on the structure, phase composition, textural and electronic properties and activity of the catalysts. The reduction behavior of the studied samples was evaluated by temperature-programmed reduction. The WGS performance of Au/NiAl catalysts was significantly affected by the addition of CeO2. A favorable role of ceria was revealed by comparison of CO conversion degree at 220 °C reached by 3 wt.% CeO2-modified and ceria-free Au/NiAl samples (98.8 and 83.4%, respectively). It can be stated that tuning the properties of Au/NiAl LDH via CeO2 addition offers catalysts with possibilities for practical application owing to innovative synthesis and improved WGS performance.


2020 ◽  
Vol 9 (1) ◽  
pp. 734-743
Author(s):  
Ran Zhao ◽  
ZiChen Tian ◽  
Zengwu Zhao

AbstractBayan Obo tailings are rich in rare earth elements (REEs), iron, and other catalytic active substances. In this study, mine tailings were calcined at different temperatures and tested for the catalytic combustion of low-concentration methane. Upon calcination at 600°C, high catalytic activity was revealed, with 50% CH4 conversion at 587°C (space velocity of 12,000 mL/g h). The physicochemical properties of catalysts were characterized using thermogravimetric analysis, X-ray diffraction, scanning electron microscopy, hydrogen temperature-programmed reduction (H2-TPR), and X-ray photoelectron spectroscopy (XPS). Compared to the raw ore sample, the diffraction peak intensity of Fe2O3 increased post calcination, whereas that of CeCO3F decreased. A porous structure appeared after the catalyst was calcined at 600°C. Additionally, Fe, Ce, Ti, and other metal elements were more highly dispersed on the catalyst surface. H2-TPR results revealed a broadening of the reduction temperature range for the catalyst calcined at 600°C and an increase in the reduction peak. XPS analysis indicated the presence of Ce in the form of Ce3+ and Ce4+ oxidation states and the coexistence of Fe in the form of Fe2+ and Fe3+. Moreover, XPS revealed a higher surface Oads/Olatt ratio. This study provides evidence for the green reuse of Bayan Obo mine tailings in secondary resources.


Catalysts ◽  
2018 ◽  
Vol 8 (11) ◽  
pp. 541 ◽  
Author(s):  
Haiping Xiao ◽  
Chaozong Dou ◽  
Hao Shi ◽  
Jinlin Ge ◽  
Li Cai

A series of poisoned catalysts with various forms and contents of sodium salts (Na2SO4 and Na2S2O7) were prepared using the wet impregnation method. The influence of sodium salts poisoned catalysts on SO2 oxidation and NO reduction was investigated. The chemical and physical features of the catalysts were characterized via NH3-temperature programmed desorption (NH3-TPD), H2-temperature programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), and Fourier Transform Infrared Spectroscopy (FT-IR). The results showed that sodium salts poisoned catalysts led to a decrease in the denitration efficiency. The 3.6% Na2SO4 poisoned catalyst was the most severely deactivated with denitration efficiency of only 50.97% at 350 °C. The introduction of SO42− and S2O72− created new Brønsted acid sites, which facilitated the adsorption of NH3 and NO reduction. The sodium salts poisoned catalysts significantly increased the conversion of SO2–SO3. 3.6%Na2S2O7 poisoned catalyst had the strongest effect on SO2 oxidation and the catalyst achieved a maximum SO2–SO3-conversion of 1.44% at 410 °C. Characterization results showed sodium salts poisoned catalysts consumed the active ingredient and lowered the V4+/V5+ ratio, which suppressed catalytic performance. However, they increased the content of chemically adsorbed oxygen and the strength of V5+=O bonds, which promoted SO2 oxidation.


Reactions ◽  
2021 ◽  
Vol 2 (4) ◽  
pp. 457-472
Author(s):  
Jasmine Kaur ◽  
Sundaramurthy Vedachalam ◽  
Philip Boahene ◽  
Ajay K. Dalai

Pyrolysis oil derived from waste tires consists of sulfur content in the range of 7000 to 9000 ppm. For use in diesel engines, its sulfur content must be lowered to 10 to 15 ppm. Though conventional hydrodesulfurization is suitable for the removal of sulfur from tire pyrolysis oil, its high cost provides an avenue for alternative desulfurization technologies to be explored. In this study, oxidative desulfurization (ODS), a low-cost technology, was explored for the desulfurization of tire pyrolysis oil. Two categories of titanium-incorporated mesoporous supports with 20 wt% loaded heteropoly molybdic acid catalyst (HPMo/Ti-Al2O3 and HPMo/Ti-TUD-1) were developed and tested for ODS of tire pyrolysis oil at mild process conditions. Catalysts were characterized by X-ray diffraction, BET-N2 physisorption, and X-ray photoelectron spectroscopy (XPS). The incorporation of Ti into Al2O3 and TUD-1 frameworks was confirmed by XPS. The surface acidity of catalysts was studied by the temperature-programmed desorption of NH3 and pyridine FTIR analyses. HPMo/Ti-Al2O3 and HPMo/Ti-TUD-1 catalysts contained both Lewis and Brønsted acid sites. The presence of titanium in catalysts was found to promote the ODS activity of phosphomolybdic acid. The Ti-TUD-1-supported catalysts performed better than the Ti-Al2O3-supported catalysts for the ODS of tire pyrolysis oil. Hydrogen peroxide and cumene peroxide were found to be better oxidants than tert-butyl hydroperoxide for oxidizing sulfur compounds of tire pyrolysis oil. Process parameter optimization by the design of experiments was conducted with an optimal catalyst along with the catalyst regeneration study. An ANOVA statistical analysis demonstrated that the oxidant/sulfur and catalyst/oil ratios were more significant than the reaction temperature for the ODS of tire pyrolysis oil. It followed the pseudo-first-order kinetics over HPMo/Ti-TUD-1.


2011 ◽  
Vol 197-198 ◽  
pp. 919-925 ◽  
Author(s):  
Min Wang ◽  
Qiong Liu

Silver (Ag+) doped iron (III) vanadate (FeVO4) samples are prepared by the precipitation method and then characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), and X-ray photoelectron spectroscopy(XPS). The photocatalytic activity under visible light is evaluated by photocatalytic degradation of methyl orange (MO) in the solution. The results show that both FeVO4 and Ag+ doped FeVO4 samples are triclinic, the later have different surface morphology, and some needle-shaped materials appear in the later. From XPS, there are more Fe2+ ions in Ag+ doped FeVO4 sample than that in FeVO4 one without Ag+. It indicates that Ag+ doping can increase the density of the surface oxygen vacancies of catalysts, which can act as electron traps promoting the electron-hole separation and then increase the photo-activity. The decoloration rate after Ag+ doping against methyl orange solution can reach about 81%, and be more about 20% than that of pure FeVO4.


2011 ◽  
Vol 63 (5) ◽  
pp. 917-923 ◽  
Author(s):  
Jun Hu ◽  
Donglin Zhao ◽  
Xiangke Wang

Multiwalled carbon nanotubes (MWCNTs)/iron oxide magnetic composites (named as MCs) were prepared by co-precipitation method, and were characterised by scanning electron microscope (SEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) in detail. The prepared MCs were employed as an adsorbent for the removal of Pb(II) and Cu(II) ions from wastewater in heavy metal ion pollution cleanup. The results demonstrated that the sorption of Pb(II) and Cu(II) ions was strongly dependent on pH and temperature. The experimental data were well described by Langmuir model, and the monolayer sorption capacity of MCs was found to vary from 10.02 to 31.25 mg/g for Pb(II) and from 3.11 to 8.92 mg/g for Cu(II) at temperature increasing from 293.15 to 353.15 K at pH 5.50. The sorption capacity of Pb(II) on MCs was higher than that of Cu(II), which was attributed to their ionic radius, hydration energies and hydrolysis of their hydroxides. The thermodynamic parameters (i.e., ΔH0, ΔS0 and ΔG0) were calculated from temperature dependent sorption isotherms, and the results indicated that the sorption of Pb(II) and Cu(II) ions on MCs were spontaneous and endothermic processes.


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