Plasma-Enhanced Catalytic Reduction of SO2: Decoupling Plasma-Induced Surface Reaction from Plasma-Phase Reaction

Author(s):  
Mohammad S. AlQahtani ◽  
Xiaoxing Wang ◽  
Sean D. Knecht ◽  
Sven G. Bilén ◽  
Chunshan Song
2016 ◽  
Vol 852 ◽  
pp. 293-299 ◽  
Author(s):  
Rong Liu ◽  
Yi Fan Xu ◽  
Fei Ye ◽  
Ling Chen Ji ◽  
Hao Guan ◽  
...  

The MnOx-CeO2/t-ZrO2 catalyst was prepared by impregnation with nano t-ZrO2 as the support. The influence of active component and reaction temperature on denitration performance of catalyst was investigated. The results showed that denitration efficiency improved as active component increased and reaction temperature rose. The denitration efficiency of 2.5% MnOx-CeO2/t-ZrO2 at 100°C was 68.1% while 15% MnOx-CeO2/t-ZrO2 was 97.4%. The results of XRD, BET and H2-TPR showed that surface structure of loaded catalyst was good for oxidation-reduction and denigration. NH3-TPD test demonstrated that NH3 was mainly adsorbed at Lewis acid sites on the surface of catalysts and became coordination NH3. Intermediate product NH2NO generated from reactions between coordination NH3 and NO which finally changed into N2 and H2O.NOx are potentially harmful to humans as a kind of primary pollutants. And NOx are the main cause of many environment problems, such as acid rain, surface ozone pollution and Particulate Matter 2.5[1]. The emission of NOx was 2337.8 tons in China in 2011 and that was 2275.4 tons[2]. The environmental situation is grim although the emission of NOx had begun decreasing. Emission standard of air pollutants for thermal power plants which came into effect on January 1, 2012 require the emission concentration of NOx under 100mg·m-3. The task is arduous.Selective catalytic reduction (SCR) of NOx with NH3 is the most promising method to remove NOx and catalysts with high activity play a decisive part in low temperature SCR technology. Many researches about metal oxide as SCR catalyst support have been reported recently, such as TiO2[3], Al2O3[4], activated carbon[5] and molecular sieve[6]. Zirconium oxide has attracted considerable attention recently as a catalyst support because of its special characteristics. Takahashi et al.[7] investigated the influence of the various compositions of TiO2 and ZrO2 on the NOx removal ability over a sulfur-treated NSR catalyst and came to a conclusion that ZrO2 support suppressed the solid phase reaction with potassium. Reddy et al.[8, 9] investigated structural characteristics of nanosized ceria-silica, ceria-titania, and ceria-zirconia mixed oxide catalysts and found these mixed oxides exhibit better redox properties than pure CeO2. YAN Zhi-yong et al.[10] reported that the existence of ZrO2 in catalysts can raise its specific area and enhance the dispersion of CeO2 on catalysts which results in high activity of the catalysts. CeO2/TiO2-ZrO2 catalyst has strong tolerance to water vapor and sulfur dioxide.It is well known that ZrO2 exists mainly in three polymorphs with monoclinic (m-ZrO2), tetragonal (t-ZrO2) and (c-ZrO2) cubic structures[11]. ZrO2 polymorphs have different amphoteric character of its surface hydroxyl groups. The crystalline phase of ZrO2 has a great effect on the structure, activity and selectivity of catalysts. Therefore, it is valuable to investigate the effects of nanocrystalline zirconia polymorphs on catalytic properties of MnOx-CeO2/t-ZrO2 Catalysts which few researchers have concerned about. In this study, we try to investigate catalytic activity and microstructure of SCR catalysts with manganese oxide and cerium oxide supported on t-ZrO2.


2002 ◽  
Vol 17 (6) ◽  
pp. 1536-1542 ◽  
Author(s):  
Chih-Yi Pan ◽  
Yin-Lang Chen ◽  
Dah-Shyang Tsai

Ferroelectric PZT thin films were deposited on Pt and SrRuO3 substrates in a cold-wall reactor, using the Pb(C2H5)4/Zr(OBu)4/Ti(OPri)4/O2 reaction system. In comparison with Pt substrate, the growth rate of lead zirconate titanate (PZT) thin film was higher on SrRuO3. Lead content of the thin film deposited on either substrate at low temperatures (723–863 K) was much more temperature dependent than the other two metal contents. The strong temperature dependence originated from the high activation energy in the initial decomposition of Pb(C2H5)4 vapor, which was 54 kcal/mol. The surface reaction constant of lead precursor had much lower temperature dependence. The activation energy of surface reaction for PbO, estimated from deposition in a mini-chamber, was 6 kcal/mol on Pt and 9 kcal/mol on the SrRuO3 substrate. Therefore, the incorporation path of component oxide PbO, whose apparent activation energy was 31 kcal/mol on Pt and 29 kcal/mol on SrRuO3, essentially involved considerable gas-phase reaction. The PZT (50/50) thin film on SrRuO3 bottom electrode possessed a lower coercive field and a smaller remnant polarization than that on Pt. The PZT capacitor on SrRuO3 was also less vulnerable to polarization fatigue.


1964 ◽  
Vol 42 (1) ◽  
pp. 1-9 ◽  
Author(s):  
Nick Demchuk ◽  
H. Gesser

The gas-phase reaction of atomic hydrogen with ketene has been investigated over a temperature range of −130° to 232 °C using a low-pressure, fast-flow system. In most cases methane, carbon monoxide, and ethane were the major products, but trace amounts of glyoxal were also detected. Above −96 °C. considerable evidence exists for the occurrence of a chain reaction carried by HCO radicals. The surface reaction at −196 °C produced methane and glyoxal predominantly with only a minor amount of carbon monoxide.


2016 ◽  
Vol 195 ◽  
pp. 69-80 ◽  
Author(s):  
Sonia Álvarez-Barcia ◽  
Marie-Sophie Russ ◽  
Jan Meisner ◽  
Johannes Kästner

The title reaction is involved in the formation of ammonia in the interstellar medium. We have calculated thermal rates including atom tunnelling using different rate theories. Canonical variational theory with microcanonically optimised multidimensional tunnelling was used for bimolecular rates, modelling the gas-phase reaction and also a surface-catalysed reaction of the Eley–Rideal type. Instanton theory provided unimolecular rates, which model the Langmuir–Hinshelwood type surface reaction. The potential energy was calculated on the CCSD(T)-F12 level of theory on the fly. We report thermal rates and H/D kinetic isotope effects. The latter have implications for observed H/D fractionation in molecular clouds. Tunnelling causes rate constants to be sufficient for the reaction to play a role in interstellar chemistry even at cryogenic temperature. We also discuss intricacies and limitations of the different tunnelling approximations to treat this reaction, including its pre-reactive minimum.


1994 ◽  
Vol 337 ◽  
Author(s):  
P. J. Chen ◽  
C. M. Truong ◽  
J. S. Corneille ◽  
W. S. Oh ◽  
D. W. Goodman

ABSTRACTThe adsorption and thermal behavior of tetrakis-(dimethylamido)-titaniurn (TDMAT), Ti[NMe2]4, were investigated by surface spectroscopic techniques in the temperature range 100-1100K. A metallic Ti substrate readily dissociates TDMAT even below 300 K, producing a carbon-rich interface. When the substrate is exposed to a continuous flux of TDMAT at growth temperatures (550-700K), deposition of carbon-rich TiCxNy films readily occurs with a high precursor reactive sticking coefficient. With the addition of sufficient NH3 flux, we demonstrate the existence of a direct surface-reaction-driven deposition mechanism which involves reaction(s) between adsorbed TDMAT and NHX species on the film surface and thus leads to growth of substantially cleaner TiNx films. This growth mechanism dominates at low pressures (≤10-4Torr) where gas-phase reaction between the precursor gases becomes insignificant.


Author(s):  
Kazuhiro Hayashida ◽  
Kenji Amagai ◽  
Masataka Arai

Exhaust gas from the catalytic combustion of methane mixture was analyzed experimentally. A palladium catalyst supported on a cordierite honeycomb was used. The methane/air mixture, which was pre-heated to 530K, was introduced into the catalyst. Combustion states were investigated under various conditions of the equivalence ratio. In the case of lean mixture, homogeneous surface reaction in the catalyst was observed, and combustion reaction was completed within the catalyst. However, in the case of rich mixture, a thermal combustion flame appeared after the catalyst with the homogeneous surface reaction. In order to investigate exhaust gas composition, exhaust gas was sampled by a quartz probe, and was analyzed by a FTIR. Furthermore, low level NO in the exhaust gas was detected by a LIF method. In order to obtain the NO concentration from the NO fluorescence, temperature dependency of the fluorescence was obtained by using a NO/N2 mixture. NO concentration in a exhaust gas just after the catalyst was highest when the equivalence ratio was 0.3. When the thermal combustion flame appeared after the catalyst, CO and CH4 were detected just after the catalyst. These concentrations decreased around the thermal combustion flame. This result suggests that unburnt CH4 and CO which was produced by a partial combustion in the catalyst were converted in a gas phase reaction. In this case, although NO was hardly detected just after the catalyst, it was detected around the thermal flame.


RSC Advances ◽  
2015 ◽  
Vol 5 (110) ◽  
pp. 90235-90244 ◽  
Author(s):  
Shuangshuang Lai ◽  
Dongmei Meng ◽  
Wangcheng Zhan ◽  
Yun Guo ◽  
Yanglong Guo ◽  
...  

Ce doped Cu/ZSM-5 catalysts were prepared by the incipient-wetness-impregnation method, and the effect of Ce doping on the structure and the catalytic performance was investigated in detail for the selective catalytic reduction of NO with NH3


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