Fe and/or Mn oxides supported on fly ash-derived SBA-15 for low-temperature NH3-SCR

A series of CeOx catalysts supported by commercial porous cordierite ceramics (CPCC) and synthesized porous cordierite ceramics (SPCC) from fly ash were prepared for selective catalytic reduction of NOx with ammonia (NH3-SCR). A greater than 90% NOx conversion rate was achieved by the SPCC supported catalyst at 250–300 °C when the concentration of loading precursor was 0.6 mol/L (denoted as 0.6Ce/SPCC), which is more advantageous than the CPCC supported ones. The EDS mapping results reveal the existence of evenly distributed impurities on the surface of SPCC, which hence might be able to provide more attachment sites for CeOx particles. Further measurements with temperature programmed reduction by hydrogen (H2-TPR) demonstrate more reducible species on the surface of 0.6Ce/SPCC, thus giving rise to better NH3-SCR performance at a low-temperature range. The X-ray photoelectron spectroscopy (XPS) analyses reveal that the Ce atom ratio is higher in 0.6Ce/SPCC, indicating that a higher concentration of catalytic active sites could be found on the surface of 0.6Ce/SPCC. The in situ diffused reflectance infrared fourier transform spectroscopy (DRIFTS) results indicate that the SCR reactions over 0.6Ce/SPCC follow both Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) mechanisms. Hence, the SPCC might be a promising candidate to provide support for NH3-SCR catalysts, which also provide a valuable approach to recycling the fly ash.

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A Study on Mn-Fe Catalysts Supported on Coal Fly Ash for Low-Temperature Selective Catalytic Reduction of NOX in Flue Gas

Catalysts ◽

10.3390/catal10121399 ◽

2020 ◽

Vol 10 (12) ◽

pp. 1399

Author(s):

Xiaoxu Duan ◽

Jinxiao Dou ◽

Yongqi Zhao ◽

Salman Khoshk Rish ◽

Jianglong Yu

Keyword(s):

Reaction Mechanism ◽

Fly Ash ◽

Low Temperature ◽

Selective Catalytic Reduction ◽

Low Temperatures ◽

Catalytic Reduction ◽

Coal Fly Ash ◽

Fixed Bed Reactor ◽

Main Reaction ◽

Nh3 Scr

A series of Mn0.15Fe0.05/fly-ash catalysts have been synthesized by the co-precipitation method using coal fly ash (FA) as the catalyst carrier. The catalyst showed high catalytic activity for low-temperature selective catalytic reduction (LTSCR) of NO with NH3. The catalytic reaction experiments were carried out using a lab-scale fixed-bed reactor. De-NOx experimental results showed the use of optimum weight ratio of Mn/FA and Fe/FA, resulted in high NH3-SCR (selective catalytic reduction) activity with a broad operating temperature range (130–300 °C) under 50000 h−1. Various characterization methods were used to understand the role of the physicochemical structure of the synthesized catalysts on their De-NOx capability. The scanning electron microscopy, physical adsorption-desorption, and X-ray photoelectron spectroscopy showed the interaction among the MnOx, FeOx, and the substrate increased the surface area, the amount of high valence metal state (Mn4+, Mn3+, and Fe3+), and the surface adsorbed oxygen. Hence, redox cycles (Fe3+ + Mn2+ ↔ Mn3+ + Fe2+; Fe2+ + Mn4+ ↔ Mn3+ + Fe3+) were co-promoted over the catalyst. The balance between the adsorption ability of the reactants and the redox ability can promote the excellent NOx conversion ability of the catalyst at low temperatures. Furthermore, NH3/NO temperature-programmed desorption, NH3/NO- thermo gravimetric-mass spectrometry (NH3/NO-TG-MS), and in-situ DRIFTs (Diffuse Reflectance Infrared Fourier Transform Spectroscopy) results showed the Mn0.15Fe0.05/FA has relatively high adsorption capacity and activation capability of reactants (NO, O2, and NH3) at low temperatures. These results also showed that the Langmuir–Hinshelwood (L–H) reaction mechanism is the main reaction mechanism through which NH3-SCR reactions took place. This work is important for synthesizing an efficient and environmentally-friendly catalyst and demonstrates a promising waste-utilization strategy.

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Insight into the Promoting Role of Er Modification on SO2 Resistance for NH3-SCR at Low Temperature over FeMn/TiO2 Catalysts

Catalysts ◽

10.3390/catal11050618 ◽

2021 ◽

Vol 11 (5) ◽

pp. 618

Author(s):

Huan Du ◽

Zhitao Han ◽

Xitian Wu ◽

Chenglong Li ◽

Yu Gao ◽

...

Keyword(s):

Low Temperature ◽

Catalyst Surface ◽

Impregnation Method ◽

In Situ Drifts ◽

Tio2 Catalyst ◽

Nh3 Scr ◽

Nh3 Adsorption ◽

So2 Resistance ◽

Fast Scr

Er-modified FeMn/TiO2 catalysts were prepared through the wet impregnation method, and their NH3-SCR activities were tested. The results showed that Er modification could obviously promote SO2 resistance of FeMn/TiO2 catalysts at a low temperature. The promoting effect and mechanism were explored in detail using various techniques, such as BET, XRD, H2-TPR, XPS, TG, and in-situ DRIFTS. The characterization results indicated that Er modification on FeMn/TiO2 catalysts could increase the Mn4+ concentration and surface chemisorbed labile oxygen ratio, which was favorable for NO oxidation to NO2, further accelerating low-temperature SCR activity through the “fast SCR” reaction. As fast SCR reaction could accelerate the consumption of adsorbed NH3 species, it would benefit to restrain the competitive adsorption of SO2 and limit the reaction between adsorbed SO2 and NH3 species. XPS results indicated that ammonium sulfates and Mn sulfates formed were found on Er-modified FeMn/TiO2 catalyst surface seemed much less than those on FeMn/TiO2 catalyst surface, suggested that Er modification was helpful for reducing the generation or deposition of sulfate salts on the catalyst surface. According to in-situ DRIFTS the results of, the presence of SO2 in feeding gas imposed a stronger impact on the NO adsorption than NH3 adsorption on Lewis acid sites of Er-modified FeMn/TiO2 catalysts, gradually making NH3-SCR reaction to proceed in E–R mechanism rather than L–H mechanism. DRIFTS.

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