The open literature concerning chemical and mechanistic aspects of the selective catalytic reduction of NO by ammonia (SCR process) on metal oxide catalysts is reviewed. Catalytic systems based on supported V2O5 (including the industrial TiO2-supported V2O5–WO3 and/or V2O5–MoO3 catalysts) and catalysts containing Fe2O3, CuO, MnOx and CrOx are considered. The results of spectroscopic studies of the adsorbed surface species, adsorption–desorption measurements, flow reactor and kinetic experiments are analyzed. The proposed reaction mechanisms are described and critically discussed. Points of convergence and of disagreement are underlined.

Chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts: A review

The infrared spectral performance of the N x O y species observed on oxide surfaces [N2O, NO−, NO, (NO)2, N2O3, NO+, NO2 − (different nitro and nitrito anions), NO2, N2O4, N2O5, NO2, and NO3 − (bridged, bidentate, and monodentate nitrates)] is considered. The spectra of related compounds (N2, H-, and C-containing nitrogen oxo species, C─N species, NH x species) are also briefly discussed. Some guidelines for spectral identification of N x O y adspecies are proposed and the transformation of the nitrogen oxo species on catalyst surfaces are regarded.

Identification of Neutral and Charged N x O y Surface Species by IR Spectroscopy

A series of manganese-cerium oxide catalysts were prepared by co-precipitation method and used for low temperature selective catalytic reduction (SCR) of NO x with ammonia in the presence of excess O 2 . These catalysts were characterized by X-ray diffraction (XRD), surface area measurement and FTIR. The experimental results showed that the best Mn-Ce mixed-oxide catalyst yielded 95% NO conversion at 150 °C at a space velocity of 42,000 h −1 . As the manganese content was increased from 0 to 40% (i.e. the molar ratio of Mn/(Mn+Ce)), NO conversion increased significantly, but decreased at higher manganese contents. The most active catalyst was obtained with a molar Mn/(Mn+Ce) ratio of 0.4. Only N 2 rather than N 2 O was found in the product when the temperature was below 150 °C. At higher temperatures, trace amounts of N 2 O were detected. A mechanistic pathway for this reaction was proposed based on earlier findings and FTIR results obtained in this work. The initial step was the adsorption of NH 3 on Lewis acid sites of catalyst, followed by reaction with nitrite species to produce N 2 and H 2 O. Possible intermediates are proposed and all the intermediates could transform into NH 2 NO, which could further react to produce N 2 and H 2 O.

MnOx-CeO2 mixed oxides prepared by co-precipitation for selective catalytic reduction of NO with NH3 at low temperatures

An overview is given of the selective catalytic reduction of NOx by ammonia (NH3‐SCR) over metal‐exchanged zeolites. The review gives a comprehensive overview of NH3‐SCR chemistry, including undesired side‐reactions and aspects of the reaction mechanism over zeolites and the active sites involved. The review attempts to correlate catalyst activity and stability with the preparation method, the exchange metal, the exchange degree, and the zeolite topology. A comparison of Fe‐ZSM‐5 catalysts prepared by different methods and research groups shows that the preparation method is not a decisive factor in determining catalytic activity. It seems that decreased turnover frequency (TOF) is an oft‐neglected effect of increasing Fe content, and this oversight may have led to the mistaken conclusion that certain production methods produce highly active catalysts. The available data indicate that both isolated and bridged iron species participate in the NH3‐SCR reaction over Fe‐ZSM‐5, with isolated species being the ...

https://www.tandfonline.com/doi/pdf/10.1080/01614940802480122

The State of the Art in Selective Catalytic Reduction of NOx by Ammonia Using Metal‐Exchanged Zeolite Catalysts

This paper surveys the present status and the perspective of de-NO x SCR catalysis for stationary sources, that is based on the reduction of NO x by NH 3 to form water and nitrogen. After a brief description of the SCR chemistry the characteristics of commercial SCR catalysts, their physico-chemical properties and reactivity, and their performances in both NO x reduction and SO 2 oxidation are presented. The mechanism of the SCR reactions, the mathematical modeling of the reactor and the arrangements of the reactor and process are then described. Finally the emerging technologies for NO x removal and the future perspectives of the SCR catalysis are outlined.

Present status and perspectives in de-NOx SCR catalysis

Adsorption, Activation, and Oxidation of Ammonia over SCR Catalysts

Ammonia activation over catalysts for the selective catalytic reduction of NOx and the selective catalytic oxidation of NH3. An FT-IR study

Silicated titanias have been prepared by reaction of commercial anatase-based TiO2 powders with tetraethylorthosilicate, followed by calcination. At low loadings orthosilicate species are found, that interact mainly with surface defects of anatase where surface hydroxy groups are located. At higher loadings polysilicate species are found, while amorphous silica is observed if the nominal loading is comparable to that allowing the coverage of the entire TiO2 surface with a silicate layer. Surface silicate species progressively mask the TiO2 surface, and do not generate Bronsted acidity that is sufficiently strong to protonate pyridine. Silication strongly hinders anatase crystal growth and loss of surface area upon heating, as well as the anatase-to-rutile phase transformation. Thus, supported silica in small amounts can act as an efficient morphology and structure promoter of anatase TiO2-based catalysts, although it also perturbs the TiO2 surface chemistry significantly.

Li Yi

Papers

Adsorption, Activation, and Oxidation of Ammonia over SCR Catalysts

Ammonia activation over catalysts for the selective catalytic reduction of NOx and the selective catalytic oxidation of NH3. An FT-IR study

Characterization of silicated anatase powders

Characterization of Silicated Anatase Powders.