• Applied Chemistry for Engineering
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• v.27 no.1
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• pp.92-100
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• 2016

Low-temperature conversion of nitrogen oxides using plasma-assisted hydrocarbon selective catalytic reduction of (HC-SCR) was investigated. Plasma was created in the catalyst-packed bed so that it could directly interact with the catalyst. The effect of the reaction temperature, the shape of catalyst, the concentration of n-heptane as a reducing agent, the oxygen content, the water vapor content and the energy density on $NO_x$ removal was examined. $NO_x$ conversion efficiencies achieved with the plasma-catalytic hybrid process at a temperature of $250^{\circ}C$ and an specific energy input (SIE) of $42J\;L^{-1}$ were 83% and 69% for one-dimensional Ag catalyst ($Ag\;(nanowire)/{\gamma}-Al_2O_3$) and spherical Ag catalyst ($Ag\;(sphere)/{\gamma}-Al_2O_3$), respectively, whereas that obtained with the catalyst-alone was considerably lower (about 30%) even with $Ag\;(nanowire)/{\gamma}-Al_2O_3$ under the same condition. The enhanced catalytic activity towards $NO_x$ conversion in the presence of plasma can be explained by the formation of more reactive $NO_2$ species and partially oxidized hydrocarbon intermediates from the oxidation of NO and n-heptane under plasma discharge. Increasing the SIE tended to improve $NO_x$ conversion efficiency, and so did the increase in the n-heptane concentration; however, a further increase in the n-heptane concentration beyond $C_1/NO_x$ ratio of 5 did not improve the $NO_x$ conversion efficiency any more. The increase in the humidity affected negatively the $NO_x$ conversion efficiency, resulting in lowering the $NO_x$ conversion efficiency at the higher water vapor content, because water molecules competed with $NO_x$ species for the same active site. The $NO_x$ conversion efficiency increased with increasing the oxygen content from 3 to 15%, in particular at low SIE values, because the formation of $NO_2$ and partially oxidized hydrocarbon intermediates was facilitated.

• Applied Chemistry for Engineering
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• v.29 no.1
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• pp.103-111
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• 2018

A plasma-catalytic combined process was used as an attempt to improve the conversion efficiency of nitrogen oxides ($NO_x$) over a wide temperature range ($150{\sim}500^{\circ}C$) to cope with the exhaust gas whose temperature varies greatly. Since the catalytic $NO_x$ reduction is effective at high temperatures where the activity of the catalyst itself is high, the $NO_x$ reduction was carried out without plasma generation in the high temperature region. On the other hand, in the low temperature region, the plasma was created in the catalyst bed to make up for the decreased catalytic activity, thereby increasing the $NO_x$ conversion efficiency. Effects of the types of catalysts, the reaction temperature, the concentration of the reducing agent (n-heptane), and the energy density on $NO_x$ conversion efficiency were examined. As a result of comparative analysis of various catalysts, the catalytic $NO_x$ conversion efficiency in the high temperature region was the highest in the case of the $Ag-Zn/{\gamma}-Al_2O_3$ catalyst of more than 90%. In the low temperature region, $NO_x$ was hardly removed by the hydrocarbon selective reduction process, but when the plasma was generated in the catalyst bed, the $NO_x$ conversion sharply increased to about 90%. The $NO_x$ conversion can be maintained high at temperatures of $150{\sim}500^{\circ}C$ by the combination of plasma in accordance with the temperature change of the exhaust gas.

• Journal of the Korean Institute of Gas
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• v.19 no.5
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• pp.20-28
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• 2015

This work investigated the size and shape effect of ${\gamma}$-alumina-supported metal oxides on the hydrocarbon selective catalytic reduction of nitrogen oxides. Several metal oxides including Ag, Cu and Ru were used as the catalysts, and n-heptane as the reducing agent. For the Ag/${\gamma}$-alumina catalyst, the $NO_x$ reduction efficiency in the range of $250{\sim}400^{\circ}C$ increased as the size of Ag decreased (20 nm>50 nm>80 nm). The shape effect of metal oxides on the $NO_x$ reduction was examined with spherical- and wire-shape nanoparticles. Under identical condition, higher catalytic activity for $NO_x$ reduction was observed with Ag and Cu wires than with the spheres, while spherical- and wire-shape Ru exhibited similar $NO_x$ reduction efficiency to each other. Among the metal oxides examined, the best catalytic activity for $NO_x$ reduction was obtained with Ag wire, showing almost complete $NO_x$ removal at a temperature of $300^{\circ}C$. For Cu and Ru catalysts, considerable amount of NO was oxidized to $NO_2$, rather than reduced to $N_2$, leading to lower $NO_x$ reduction efficiency.

• Transactions of the Korean Society of Automotive Engineers
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• v.21 no.6
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• pp.64-71
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• 2013

In this study we designed a lean $NO_x$ trap (LNT) model with $GT-POWER^{TM}$ program and then the LNT model was compared to the bench flow reactor test results. This model consists of 9 kinetic reactions to represent the main steps of NO oxidation, $NO_x$ adsorption, $NO_x$ release and then its reduction. The comparison was performed on the operating conditions at the space velocity of 50,000 1/hr and 80,000 1/hr with the temperature range of $200^{\circ}C{\sim}500^{\circ}C$ with the even spaced temperature step of $50^{\circ}C$. The experimental results show that the $NO_x$ conversion efficiency was enhanced by the temperature up to $350^{\circ}C$ and then decayed at higher temperatures. The LNT model predicts the similar trend of the $NO_x$ conversion efficiency to the experimental results below $350^{\circ}C$, but overestimates above $350^{\circ}C$. This overestimation comes from the higher reduction efficiency which was obtained by the different reduction gas composition such as $C_3H_6$ in the model to replace $CH_4$, $C_2H_4$ in the bench test.

• Applied Chemistry for Engineering
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• v.24 no.3
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• pp.333-336
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• 2013

Experimental investigation to estimate the feasibility of fast selective catalytic reduction (SCR) or oxidation catalyst combined ammonia SCR system to abate NOx in low temperature condition ($150{\sim}250^{\circ}C$) is reported. Because the conversion of NO to $NO_2$ is pre-requisite of the fast SCR process, the effect of the amount of oxidation catalyst to NO conversion to $NO_2$ was tested. 37, 45 and 51% of conversion rates were obtained for the OCV of 563000, 375000 and 281000 h, respectively. $De-NO_x$ performance in the case of $NO_2/NO_x$ ratio of 45% showed the best result in all tested temperature conditions. Comparison of the fast SCR and standard SCR with the condition of $NO_2/NO_x$ ratio of 45%, $200{\sim}250^{\circ}C$ and space velocity of 10000~30000 h showed that the fast SCR does not show much difference according to the variance of space velocity. Also it was shown that using the fast SCR, the volume of SCR catalyst can be reduced less than half of the standard SCR condition by increasing space velocity without the loss of $De-NO_x$ performance.

• Journal of the Korea Academia-Industrial cooperation Society
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• v.17 no.7
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• pp.713-719
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• 2016

The NOx conversion properties of Mn-Cu-$TiO_2$ and $V_2O_5$/$TiO_2$ catalysts were studied for the selective catalytic reduction (SCR) of NOx with ammonia. The performance of the catalysts was investigated in terms of their $NOx$ conversion activity as a function of the reaction temperature and space velocity. The activity of the Mn-Cu-$TiO_2$ catalyst decreased with increasing reaction temperature and space velocity. However, the activity of the $V_2O_5$/$TiO_2$ catalyst increased with increasing reaction temperature. High activity of the Mn-Cu-$TiO_2$ catalyst was observed at temperatures below $200^{\circ}C$. H2-TPR and XPS analyses were conducted to explain these results. It was found that the activity of the Mn-Cu-$TiO_2$ catalyst was influenced by the thermal shock caused by the change of the initial reaction temperature, whereas the $V_2O_5$/$TiO_2$ catalyst was not affected by the initial reaction temperature. In the case of catalyst C, the $NO_x$ conversion efficiency decreased with increasing space velocity. The decrease in the $NO_x$ conversion efficiency with increasing space velocity was much less for catalyst D than for catalyst C.

• Journal of Industrial Technology
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• v.18
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• pp.249-258
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• 1998

In this paper, we investigated the post-combustion removal of nitrogen oxide($NO_x$) and sulfur oxide($SO_x$) which is based on the gas to particle conversion process by the pulsed corona discharge. Under normal pressure, the pulsed corona discharge produces the energetic free electrons which dissociate gas molecules to form the active radicals. These radicals cause the chemical reactions that convert $SO_x$ and $NO_x$ into acid mists and these mists react with $NH_3$ to form solid particles. Those particles can be removed from the gas stream by conventional devices such as electrostatic precipitator or bag filter. The reactor geometry was coaxial with an inner wire discharge electrode and an outer ground electrode wrapped on a glass tube. The simulated flue gas with $SO_x$ and $NO_x$ was used in the experiment. The corona discharge reactor was more efficient in removing $SO_x$ and $NO_x$ by adding $NH_3$ and $H_2O$ in the gas stream. We also measured the removal efficiency of $SO_x$ and $NO_x$ in a cylinder type corona discharge reactor and obtained more than 90 % of removal efficiency in these experimental conditions. The effects of process variables such as the inlet concentrations of $SO_x$, $NH_3$ and $H_2O$, residence time, pulse frequencies and applied voltages were investigated.

• Applied Chemistry for Engineering
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• v.34 no.5
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• pp.507-514
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• 2023

The selective catalytic reduction (SCR) of nitrogen oxides (NO_x) was investigated in a catalyst (Ag/γ-Al₂O₃) packed dielectric barrier discharge plasma reactor. The intermittent generation of plasma in the catalyst bed partially oxidized the hydrocarbon reductant for NO_x removal to several aldehydes. Compared to using the catalyst alone, higher NO_x conversion was observed with the intermittent generation of plasma due to the formation of highly reductive aldehydes. Under the same operating conditions (temperature: 250 ℃; C/N: 8), the NO_x reduction efficiencies were 47.5%, 92%, and 96% for n-heptane, propionaldehyde, and butyraldehyde, respectively, demonstrating the high NO_x reduction capability of aldehydes. To determine the optimal condition for intermittent plasma generation, the high voltage on/off cycle was adjusted from 0.5 to 3 min. The NO_x reduction performance was compared between continuous and intermittent plasma generation on the same energy density basis. The highest NO_x reduction efficiency was achieved at 2-min high voltage on/off intervals. The reason that the intermittent plasma discharge exhibited higher NO_x reduction efficiency even at the same energy density, compared to the continuous plasma generation case, is that the intermediate products, such as aldehydes generated from hydrocarbon, were more efficiently utilized for the reduction of nitrogen oxides.

• Journal of the Korea Academia-Industrial cooperation Society
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• v.13 no.11
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• pp.5610-5614
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• 2012

Performance of catalyst was studied with various operating conditions for selective catalytic reduction of $NO_x$ with $NH_3$. It is confirmed that catalysts containing Mn and Cu have a good efficiency in the usage of oxygen by the $H_2$-TPR analysis. In the case of catalyst #1, $NO_x$ conversion was decrease with the increase of reaction temperature. But in the case of catalyst #2, $NO_x$ conversion was increased and then remained constant with the increase of reaction temperature. This phenomenon is due to the difference of the $NH_3$ oxidation of both catalysts.

• Transactions of the Korean Society of Automotive Engineers
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• v.24 no.3
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• pp.345-351
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• 2016

This study was carried out to determine an optimal lean $NO_x$ trap (LNT) regeneration condition based on a $NO_x$ storage fraction. The LNT regeneration was performed by an in-cylinder post fuel injection method. A $NO_x$ storage fraction is defined by the ratio of current cumulated $NO_x$ amount in the LNT to the $NO_x$ storage capacity: 0 means empty and 1 fully loaded. In this study five engine operating conditions were chosen to represent the New European Driving Cycle. With various $NO_x$ storage fractions each engine operating condition, the LNT regeneration was executed and then $NO_x$ conversion efficiency, additional fuel consumption, CO and THC slip, peak catalyst temperature were measured. The results showed that there exist an optimal condition to regenerate the LNT, eg. 1500 rpm 6 bar BMEP with below 0.7 $NO_x$ storage fraction in this experimental constraint.