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

Low-temperature selective catalytic reduction of NOx with NH3 over metal oxide and zeolite catalysts—A review

A series of catalysts of manganese oxide supported on TiO 2 and iron–manganese oxide supported on TiO 2 with different amounts of manganese and iron were studied for low-temperature selective catalytic reduction (SCR) of NO with ammonia in the presence of excess oxygen. It was found that the addition of iron oxide not only increased the NO conversion and N 2 selectivity but also increased the resistance to H 2 O and SO 2 . The Fe–Mn/TiO 2 catalysts yield high activities and high N 2 product selectivity. The N 2 O product selectivity increased with the amount of MnO x as well as temperature. Crystalline phase of MnO x was present at ≥15% Mn on TiO 2 , and the amount increased with Mn content. In addition, SO 2 and H 2 O decreased the activities only slightly, while such effect was reversible. The Fe–Mn/TiO 2 with Mn/Fe=1 showed the highest activity. The results showed that this catalyst yielded nearly 100% NO conversion at 120 °C at a space velocity of 15,000 h −1 . The effect of oxygen was also studied. Reversible transient behaviors similar to that on other oxide catalysts, including vanadia and chromia, were observed for the Fe–Mn/TiO 2 catalyst.

Low-temperature selective catalytic reduction of NO with NH3 over iron and manganese oxides supported on titania

A series of high-activity manganese−cerium oxide catalysts for the low-temperature (373−453 K) selective catalytic reduction (SCR) of NOx with ammonia were prepared. They were prepared by using the...

Characterization and FTIR Studies of MnOx−CeO2 Catalyst for Low-Temperature Selective Catalytic Reduction of NO with NH3

Selective catalytic reduction (SCR) technology has been widely used for the removal of NOx from flue gas. However, it is still a challenge to develop novel low-temperature catalysts for SCR of NOx, especially at temperatures below 200 °C. This paper reviewed the recent progress on the Mn-based catalysts for low-temperature SCR de-NOx with NH3. Catalysts were divided into four categories, single MnOx, Mn-based multi-metal oxide, Mn-based multi-metal oxide with support, and Mn-based monolith catalyst. In the section of single MnOx, the effects of several factors, such as Mn oxidation state, crystallization state, specific surface area and morphology on catalytic activity were systematically reviewed. In the section of multi-metal oxide catalysts, the various roles played by the components of catalysts were intentionally summarized from four aspects, improving de-NOx efficiency, enhancing N2 selectivity, improving resistance to SO2 and H2O, extending operation temperature window, respectively. Moreover, the newly emerging morphology-dependent nanocatalysts were highlighted at the end of this section. In the introduction of supported metal oxide catalysts, the effects of supports were systematically analyzed according to their types, such as Al2O3, TiO2, carbon materials, etc. Considering the actual operation, Mn-based monolith catalysts were also introduced with regard to monolith supports, such as ceramics, metal wire mesh, etc. Subsequently, NH3-SCR mechanisms at low temperature, including E-R and L-H mechanisms, were discussed. At last, the perspective and the future direction of low-temperature SCR of NOx were proposed.

Manganese oxide-based catalysts for low-temperature selective catalytic reduction of NOx with NH3: A review

The selective catalytic reduction of NOx (NO + NO2) at low temperature with ammonia has been investigated with natural manganese ore, pure manganese dioxide, and manganese dioxide supported alumina. The catalysts showed high activities for NOx reduction with NH3 in the presence of O2 at temperatures below 250 °C. The decrease of SCR activity without oxygen in the gas phase differed among the three catalysts in accord with their differing amounts of lattice oxygen. The SCR activity of the catalysts, in that case, decreased in the order MnO2 > NMO > MnO2/γ-Al2O3. Small amounts of SO2 deactivated the catalysts in the low-temperature range. An XRD analysis of the sulfated catalysts with differing temperature provides evidence that the formation of ammonium sulfates is the main poisoning route. These results could restrict the practical application of these catalysts to sulfur-free conditions.

Selective catalytic reduction of nitrogen oxides with NH3 over natural manganese ore at low temperature

In this experiment, the simultaneous removal of SO2 and NO from flue gases was investigated through the use of natural manganese ore as a sorbent-catalyst in a fluidized bed reactor. Selective catalytic reduction behavior was determined as a function of the sulfation degree within the temperature range from 100 °C to 500 °C. The natural manganese ore showed a high activity in the production of nitrogen and water by the reaction of nitric oxide with ammonia and oxygen up to around 200 °C. At higher temperatures, the nitric oxide removal efficiency decreased due to the oxidation of ammonia by oxygen. With the increase of sulfation degree, the temperature at which the maximum selective catalytic reduction of nitric oxide appears gradually increased, however the maximum nitric oxide removal efficiency decreased. Additionally, we investigated the removal efficiency of sulfur dioxide and nitric oxide with reaction time in a batch fluidized bed reactor within a temperature range of 350 °C to 500 °C. As the reaction temperature increased, the adsorption capacity of sulfur dioxide increased, but the nitric oxide removal efficiency decreased.



© 2001 Society of Chemical Industry

Simultaneous SOx /NOx removal in a fluidized bed reactor using natural manganese ore

Simultaneous removal of SO2 and NOx from simulated gas was investigated using a continuously operating fluidized bed reactor with variables of gas velocity, sorbent/catalyst feeding rate, aspect ratio (L/D), temperature, sorbent/catalyst size. NMO (natural manganese ore) was used as a sorbent and catalyst of size from 0.715 mm to 0.194 mm in diameter. Particle size, aspect ratio, and sorbent feeding rate did not affect the reduction of NOx with ammonia, and NOx removal efficiency was about 94% at 350°C, gas velocity of 0.204 m/sec, L/D=1.0. SOx removal efficiency was affected by temperature, gas velocity, sorbent/catalyst feeding rate, aspect ratio and sorbent/catalyst size and it was about 92% at 450°C, gas velocity of 0.204 m/sec, sorbent/catalyst feeding rate of 8.54 g/min, L/D=1.0.

Soon Kwan Jeong

Papers

Selective catalytic reduction of nitrogen oxides with NH3 over natural manganese ore at low temperature

Simultaneous SOx /NOx removal in a fluidized bed reactor using natural manganese ore

Combined DeSOx/DeNOx reactions on a natural manganese ore in a fluidized bed reactor