• Title/Summary/Keyword: Catalytic Surface Reaction

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Development of the Highly Dispersed Palladium-Nickel Catalysts for Catalytic Partial Oxidation of Methane (메탄 부분산화 반응을 위한 고분산된 팔라듐-니켈 촉매 합성 및 반응)

  • Lee, Seunghyun;Jeon, Jonghyun;Kim, Juchan;Ha, Kyoung-Su
    • Korean Chemical Engineering Research
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    • v.59 no.2
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    • pp.269-275
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    • 2021
  • In this study, ordered mesoporous silica-supported Ni catalysts were prepared for catalytic partial oxidation of methane (CPOM) by using electroless nickel plating method. Unlike conventionally impregnated catalysts, the electrolessly-plated nickel catalyst showed that nickel was highly dispersed and formed stably on silica-supported surface. It was verified by TEM-EDS analysis. During the activity tests, the electrolessly-plated nickel was barely sintered and the amount of carbon deposition was very small. Consequently, the catalyst was far less deactivated, while the sintering was significantly observed in the cases of the catalysts prepared by the conventional impregnation method. Regarding the palladium-promoted catalysts, the reducibility of nickel was increased, and the reaction performances were enhanced in terms of CH4 conversion and H2/CO ratio of produced syngas.

Investigation on CO Adsorption and Catalytic Oxidation of Commercial Impregnated Activated Carbons (상용 첨착활성탄의 일산화탄소 흡착성능 및 촉매산화반응 연구)

  • Ko, Sangwon;Kim, Dae Han;Kim, Young Dok;Park, Duckshin;Jeong, Wootae;Lee, Duck Hee;Lee, Jae-Young;Kwon, Soon-Bark
    • Applied Chemistry for Engineering
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    • v.24 no.5
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    • pp.513-517
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    • 2013
  • We investigated the properties of impregnated activated carbons, a commercial adsorbent for the individual protection equipment, and examined CO adsorption and oxidation to $CO_2$. The surface area, pore volume and pore size were measured for four commercial samples using Brunauer-Emmett-Teller/Barrett-Joyner-Halenda (BET/BJH), and atomic compositions of the sample surface were analyzed based on SEM/EDS and XPS. Impregnated activated carbons containing Mn and Cu for fire showed the catalytic CO oxidation to $CO_2$ with a high catalytic activity (up to 99% $CO_2$ yield), followed by the CO adsorption at an initial reaction time. On the other hand, C: for chemical biologial and radiological (CBR) samples, not including Mn, showed a lower CO conversion to $CO_2$ (up to 60% yield) compared to that of fire samples. It was also found that a heat-treated activated carbon has a higher removal capacity both for CO and $CO_2$ at room temperature than that of untreated carbon, which was probably due to the impurity removal in pores resulted in a detection-delay about 30 min.

Hydrogen Production by Catalytic Reforming of $CO_2$ by $CH_4$ over Ni Based Catalysts and It's Applications (Ni계 촉매상에서 메탄에 의한 이산화탄소의 개질반응에 의한 수소제조 및 응용)

  • Moon, Dong-Ju;Kang, Jung-Shik;Ryu, Jong-Woo;Kim, Dae-Hyun;Yoo, Kye-Sang;Lee, Hyun-Joo;Kim, Hong-Gon;Lee, Sang-Deuk;Ahn, Byoung-Sung;Lee, Byung-Gwon
    • Journal of Hydrogen and New Energy
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    • v.17 no.2
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    • pp.166-173
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    • 2006
  • Catalytic reforming of $CO_2$ by $CH_4$ over Ni-YSZ based catalysts was investigated to produce syngas as raw material of high valued chemicals and develop high performance catalyst electrode for an internal reforming of $CO_2$ in SOFC system. Ni-YSZ based catalysts were prepared using physical mixing and maleic acid methods to improve catalytic activity and inhibition of carbon deposition. The catalysts before and after the reaction were characterized by $N_2$ physisorption, TPR(temperature programed reduction), XRD and impedance analyzer. The conversions for $CO_2$ and $CH_4$ over Ni-MgO catalyst showed 90% but much amount of carbon deposition was detected on catalyst surface. On the other hand, the conversions for $CO_2$ and $CH_4$ over NiO-YSZ-$CeO_2$ catalyst showed 100% and 85% respectively, and carbon deposition on catalyst surface was inhibited under the tested condition. It was concluded that NiO-YSZ-$CeO_2$ catalyst is a promising candidate for the catalytic reforming of $CO_2$ and the internal reforming in SOFC system.

Preparation of Porous Ceramic Bead using Mine Tailings and Its Applications to Catalytic Converter (광미(鑛尾)를 활용(活用)한 다공성 세라믹 비드 제조(製造) 및 촉매(觸媒) 변환기(變換機)로의 응용(應用))

  • Seo, Junhyung;Kim, Seongmin;Han, Yosep;Kim, Yodeuk;Lee, Junhan;Park, Jaikoo
    • Resources Recycling
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    • v.22 no.4
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    • pp.38-45
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    • 2013
  • The porous ceramic beads using mine tailing were prepared and applied to catalytic converter for NOx/SOx removal. Catalytic support was used synthesized mesoporous silica (SBA-15) which coated on surface. Internal structure for porous ceramic beads was composed of three-dimensional network structure and porosity was about 80%. In addition, the specific surface area for mesoporous silica(SBA-15) coated on converter was significantly increased 55 $m^2/g$ compared with 0.8 $m^2/g$ before coating. NOx/SOx removal experiment was performed using $V_2O_5$ and $V_2O_5$/CuO converter. NOx conversion ratio for $V_2O_5$/CuO converter was approximately increased 10% compared to $V_2O_5$ converter. In addition, catalytic converter of $V_2O_5$/CuO was shown to remove 95% of NOx and 90% of SOx at reaction temperature of $350^{\circ}C$, space velocity of 10000 $h^{-1}$ and $O_2$ concentrations of 5%, respectively.

Characteristics of Rh- Pd- Pt Three-Way Catalysts with Double-Layer Washcoat on the Hydrothermal Aging (이중층 워시코트 Rh-Pd-Pt 삼원촉매의 열적 열하에 따른 반응 특성)

  • Choi Byungchul;Jeong Jongwoo;Son Geonseog;Jung Myunggun
    • Transactions of the Korean Society of Automotive Engineers
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    • v.14 no.1
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    • pp.8-16
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    • 2006
  • The research was conducted to characterize of Rh-Pd-Pt TWC with a double-layer washcoat for gasoline vehicle. The physical characteristics on surface of catalyst were inspected by BET, SEM and TEM. The characteristics of catalytic reaction were examined by the TPD/TPR and CO-pulse chemisorption. The catalyst $6Hx(0.35\times11\times3)$ showed superior conversion performance after hydrothermal aging process, which was due to small difference of the surface area between. the fresh and the aged catalyst. The CO-chemisorption and surface area were superior in the 600 cpsi catalyst than other catalysts, this catalyst also shown the higher conversion efficiency of the exhaust emissions. From the TPR test, the conversion performance of the aged catalyst was decreased by the agglomeration and sintering of the PM and metal oxides. From the TPD result, it was found that the NO chemisorption was happed on the bottom-layer washcoat with Pd, and the NO chemisorption was re-happened on the upper-layer washcoat with Pt and Rh in the desorption process.

Control of Molecular Weight, Stereochemistry and Higher Order Structure of Siloxane-containing Polymers and Their Functional Design

  • Yusuke Kawakami;Yuning Li;Yang Liu;Makoto Seino;Chitsakon Pakjamsai;Motoi Oishi;Cho, Yeong-Bee;Ichiro Imae
    • Macromolecular Research
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    • v.12 no.2
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    • pp.156-171
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    • 2004
  • We describe the precision synthesis schemes of siloxane-containing polymers, i.e., the control of their molecular weight, stereoregularity, and higher-order structures. First, we found a new catalytic dehydrocoupling reaction of water with bis(dimethylsilyl)benzene to give poly(phenylene-disiloxane). Together with this reaction, we applied hetero-condensations to the synthesis of thermally stable poly(arylene-siloxane)s. The dehydrocoupling reaction was applied to the synthesis of syndiotactic poly(methylphenylsiloxane) and poly(silsesquioxane)s, which we also prepared by hydrolysis and deaminative condensation reactions. We discuss the tendency for loop formation to occur in the synthesis of poly(silsesquioxane) by hydrolysis, and provide comments on the design of functionality of the polymers produced. By taking advantage of the low energy barrier to rotation in the silicon-oxygen bond, we designed selective oxygen-permeable membrane materials and liquid crystalline materials. The low surface free energy of siloxane-containing systems allows surface modification of a blend film and the design of holographic grating materials.

Studies on Activity and Characteristics of CuO/ZnO/TiO2 Catalysts for Methanol Steam Reforming (메탄올 수증기 개질반응을 위한 CuO/ZnO/TiO2계 촉매의 활성 및 특성에 관한 연구)

  • Koh, Hyoung-Lim;Kim, Tae-Won;Lee, Jihn-Koo;Kim, Kyung-Lim
    • Applied Chemistry for Engineering
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    • v.9 no.7
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    • pp.956-960
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    • 1998
  • Cu-Zn and Cu-Zn-Ti catalysts for the steam reforming of methanol were prepared. This reaction was carried out at atmospheric pressure, $250^{\circ}C$, steam/methanol molar ratio 1.5, and contact time 0.1 g-cat.hr/mL-feed. In case of the catalyst with 3 mol% of $TiO_2$, the activity was superior to that of catalysts without $TiO_2$. The reaction products were mainly hydrogen and carbon dioxide. It was found that catalytic activity was not related to specific surface area but affected by metallic copper area which was measured by $N_2O$ decomposition and increased with the addition of $TiO_2$ content. XPS and XRD showed that the oxidation state of zinc was not changed during reaction, but oxidation states of copper existed in Cu(0) or Cu(I).

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Excess proton catalyzed H/D exchange reaction at the ice surface

  • Moon, Eui-Seong;Kang, Heon
    • Proceedings of the Korean Vacuum Society Conference
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    • 2011.02a
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    • pp.333-333
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    • 2011
  • We studied the H/D exchange kinetics of pure and acid dopped water-ice film by using the techniques of reactive ions scattering (RIS) and low energy sputtering (LES) with low kinetic energy cesium ion beam (<35 eV). From RIS, neutral water isotopomers were detected in the form of cesium-molecule ion clusters, $CsX^+$ (X= $H_2O$, HDO, $D_2O$). Ionic species, like $H_3O^+$, $DH_2O^+$, $D_2HO^+$, $D_3O^+$, adsorbed on the surface were ejected via LES process. Those techniques allowed us to trace the isotopomeric populations of water-ice film. To show the catalytic effect of excess proton in the H/D exchange reaction, our study was conducted with two types of water-ice films. In film 1, about 0.5 BL of $H_2O$ was adsorbed on HCl (0.1 ML) dopped $D_2O$ (8 BL) film. In film 2, similar amount of $H_2O$ used in film 1 was adsorbed on pure $D_2O$ film. Kinetic data were obtained from each film type for 90-110 K (film 1) and 110-130 K (film 2) and fitted with numerically integrated lines. Through the Arrhenius plot of kinetic coefficient deduced from fitting of the H/D exchange reaction, the activation energy of film 1 and 2 were estimated to be $10{\pm}3kJmol^{-1}$ and $17{\pm}4kJmol^{-1}$. This activation barrier difference could be understood from detailed pictures of H/D exchange. In film 2, both the formation of ion pair, $H_3O^+$ and OH. and proton transfer were needed for the H/D exchange. However, in film 1, only proton transfer was necessary but ion pair formation was not, so this might reduce the activation energy.

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Kinetics of Hydrogen Rich Ethanol as Reductant for HC-SCR over $Al_2O_3$ Supported Ag Catalyst (Ag/$Al_2O_3$ 촉매하의 HC-SCR에서 수소 풍부 에탄올의 반응 특성)

  • Lee, Ju-Heon;Park, Jeong-Whan;Kim, Seong-Soo;Yoo, Seung-Joon;Kim, Jin-Gul
    • Journal of Hydrogen and New Energy
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    • v.21 no.6
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    • pp.519-525
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    • 2010
  • Ethanol was used as reductant to remove $NO_x$ over Ag/$Al_2O_3$ catalyst via SCR from stationary emission source. Among the tested hydrocarbon reductants, ethanol showed highest de-$NO_x$ performance over the Ag/$Al_2O_3$ catalyst. De-$NO_x$ efficiency of about 83% was obtained in the condition of GHSV 20,000 $hr^{-1}$, $NO_x$ 200 ppm, CO 200 ppm, $O_2$ 13%, $H_2O$ 5% and mole ratio of ethanol/$NO_x$ = 2 between temperature of $300^{\circ}C$ and $400^{\circ}C$. While $SO_2$ presence in the $NO_x$ exhaust suppressed the catalytic activity, catalyst with acid (0.7% $H_2SO_4$) treatment of catalyst showed higher catalytic activity, where In-Situ DRIFT showed S presence over catalyst surface was increased after acid treatment of catalyst. From in-situ DRIFT and SCR results, it was concluded that sulfur presence over the surface of Ag/$Al_2O_3$ catalyst was the dominant factor to control the de-$NO_x$ reaction yield via HC-SCR from the exhausted gas including $SO_2$.

Morphology-dependent Nanocatalysis: Rod-shaped Oxides

  • Shen, Wenjie
    • Proceedings of the Korean Vacuum Society Conference
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    • 2013.02a
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    • pp.130-131
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    • 2013
  • Nanostructured oxides are widely used in heterogeneous catalysis where their catalytic properties are closely associated with the size and morphology at nanometer level. The effect of particle size has been well decumented in the past two decades, but the shape of the nanoparticles has rarely been concerned. Here we illustrate that the redox and acidic-basic properties of oxides are largely dependent on their shapes by taking $Co_3O_4$, $Fe_2O_3$, $CeO_2$ and $La_2O_3$ nanorods as typical examples. The catalytic activities of these rod-shaped oxides are mainly governed by the nature of the exposed crystal planes. For instance, the predominant presence of {110} planes which are rich in active $Co^{3+}$ on $Co_3O_4$ nanorods led to a much higher activity for CO oxidation than the nanoparticles that mainly exposed the {111} planes. The simultaneous exposure of iron and oxygen ions on the surface of $Fe_2O_3$ nanorods have significantly enhanced the adsorption and activation of NO and thereby promoted the efficiency of DeNOx process. Moreover, the exposed surface planes of these rod-shaped oxides mediated the reaction performance of the integrated metal-oxide catalysts. Au/$CeO_2$ catalysts exhibited outstanding stability under water-gas shift conditions owing to the strong bonding of gold particle on the $CeO_2$ nanorods where the formed gold-ceria interface was resistant towards sintering. Cu nanoparticles dispersed on $La_2O_3$ nanorods efficiently catalyzed transfer dehydrogenation of primary aliphatic alcohols based on the uniue role of the exposed {110} planes on the support. Morphology control at nanometer level allows preferential exposure of the catalytically active sites, providing a new stragegy for the design of highly efficient nanostructured catalysts.

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