• Title/Summary/Keyword: Catalytic Surface Reaction

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Development of Pd/TiO2 Catalysts with La2O3 Addition and Study on the Performance Improvement of H2 Oxidation at Room Temperature (La2O3가 첨가된 Pd/TiO2 촉매의 개발 및 H2 상온산화 반응에서의 성능 향상 연구)

  • Lee, Dong Yoon;Kim, Sung Chul;Lee, Sang Moon;Kim, Sung Su
    • Applied Chemistry for Engineering
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    • v.31 no.6
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    • pp.674-678
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    • 2020
  • In this study, a Pd/TiO2 catalyst which oxidized H2 at room temperature without an additional energy source was prepared. And a specific surface area of TiO2 as a support was not proportional to H2 oxidation reaction performance of Pd/TiO2 catalyst. In addition La2O3 was added to Pd/TiO2 catalyst in order to evaluate the performance effect due to the change of catalysts physical properties. A Pd/La2O3-TiO2 was prepared by adding different amounts of La2O3 to TiO2 and CO chemisorption analysis was performed. Compared to the conversion rate (14% at 0.5% H2) of the Pd/TiO2(G) catalyst, the Pd/La2O3-TiO2 catalyst showed 74% which was improved by more than five times. It was found that the larger the metal dispersion of Pd as an active metal is, the more favorable to H2 oxidation reaction is. However, when the added La2O3 amount exceeded 10%, the catalyst performance decreased again. Finally, it was concluded that the physical properties of the Pd/La2O3-TiO2 catalyst have a dominant influence on the catalytic activity until 0.3~0.5% of injected H2 concentrations and the catalyst reaction rate was controlled by substance transfer from 1% or more concentrations of H2.

A Study on the Catalytic Characteristics of Oxygen Reduction in an Alkaline Fuel Cell I. Synthesis of La0.6Sr0.4Co1-xFexO3 and Reduction Reaction of Oxygen (알칼리형 연료전지에서 산소환원에 미치는 촉매 특성 연구 I. La0.6Sr0.4Co1-xFexO3의 합성과 산소환원반응)

  • Moon, Hyeung-Dae;Lee, Ho-In
    • Applied Chemistry for Engineering
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    • v.7 no.3
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    • pp.543-553
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    • 1996
  • Oxygen reduction in an alkaline fuel cell was studied by using perovskite type oxides as an oxygen electrode catalyst. The high surface area catalysts were prepared by malic acid method and had a formula of $La_{0.6}Sr_{0.4}Co_{1-x}Fe_xO_3$(x=0.00, 0.01, 0.10, 0.20, 0.35 and 0.50). From the result of XRD pattern and specific surface area due to the amount of Fe substitution and the consumption of ammonia-water, the complex formation of Fe ion with $NH_3$ was the main factor for both the phase stability of perovskite and the increase of specific surface area. Multi-step calcination was necessary to give a single phase of perovskite in catalyst precursor. The crystal structure of the catalysts was simple cubic perovskite, which was verified from the XRD patterns of the catalysts. The activity of oxygen reduction was monitored by the techniques of cyclic voltammetry, static voltage-current method, and current interruption method. The activity(current density) of oxygen reduction showed its minimum at x=0.01 and its maximum between 0.20 and 0.35 of x-value in $La_{0.6}Sr_{0.4}Co_{1-x}Fe_xO_3$. This tendency was independent of the change of surface area.

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Effect of Sludge Pellets on $NO_x$ REmoval in $BaTiO_3$-sludge Packed-bed Reactor ($BaTiO_3$-슬러지 Packed-bed형 반응기에서 $NO_x$제거에 미치는 슬러지의 영향)

  • 박재윤;송원섭;고희석;박상현
    • Journal of the Korean Institute of Electrical and Electronic Material Engineers
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    • v.14 no.10
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    • pp.861-867
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    • 2001
  • In this paper, in order to investigate the catalytic effect of the sludge exhausted from waterworks on NO$_{x}$ removal, we measure NO removal characteristics with and without sludge pellets in BaTiO$_3$-sludge packed-bed reactor of plate-plate geometry. NO initial concentration is 50 ppm balanced with air and a gas flow rate is 5ι/min. Gas temperature is changed from 25 to 10$0^{\circ}C$ to investigate the role of sludge pellet on removing active oxygen species and NO$_2$. BaTiO$_3$pellets is filled for coronal discharge at upstream of reactor and sludge pellets is filled for catalytic effect at downstream of reactor. The volume percent of sludge pellets to BaTiO$_3$pellets is changed from 0% to 100% and AC voltage is supplied to the reactor for discharging simulated gases. In the results, when sludge pellets is put at the downstream of plasma reactor, NO removal rate is slightly increased. However, NO$_2$and $O_3$ as by-products during NO removal is significantly decreased from 51ppm without sludge pellets to 5 ppm with sludge pellets and from 50 ppm without sludge pellets to 0.004ppm with sludge pellets, respectively. Therefore, NO$_{x}$(NO+NO$_2$) removal rate is increased up to 93%. It is thought that sludge pellet maybe react with active oxygen species and NO$_2$ generated by corona discharge in surface of BaTiO$_3$pellets, the then NO$_2$O$_3$as by-products are considerably decreased. When we increase gas temperature from room temperature to 10$0^{\circ}C$, NO removal rate is decreased, while NO$_2$ concentration is independent on gas temperature. These result suggest that the removal mechanism of active oxygen species and NO$_2$in sludge pellet is not absorption, but chemical reaction. Therefore we expect that sludge pellets exhausted for waterworks could be used as catalyst for NO$_{x}$ removal with high removal rate and low by-product.oduct.

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The Adsorption of COS with a Modified-Activated Carbon for Ultra-Cleanup of Coal Gas (석탄가스의 초정밀 정제를 위한 변형된 활성탄의 흡착특성 연구)

  • Lee, You-Jin;Park, No-Kuk;Lee, Tae-Jin
    • Clean Technology
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    • v.13 no.4
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    • pp.266-273
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    • 2007
  • The adsorption properties of the activated carbon-based adsorbents were studied to remove COS emitted from $SO_2$ catalytic reduction process on the integrated gasification combined cycle (IGCC) system in this work. Transition metal supported catalysts and mixed metal oxide catalysts were used for the $SO_2$ catalytic reduction. The mechanism of COS produced from the $SO_2$ reduction and the COS concentration s according to the reaction temperature were investigated. In this study, an activated carbon and a modified activated carbon doped with KOH were used to remove the very low concentration of COS effectively. The adsorption rate and the breakthrough time of COS were measured by a thermo gravity analyzer (TGA, Cahn Balance) and a fixed bed flow reactor equipped with GC-pulsed flammable photometric detector (PFPD), respectively. It was confirmed that the COS breakthrough time of the activated carbon doped with KOH was longer than that of an activated carbon. In conclusion, the modified-activated carbon having a high surface area showed a high adsorption rate of COS produced from the $SO_2$ reduction.

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Selective Synthesis of Acetonitrile via Direct Amination of Ethanol Over Ni/SiO2-Al2O3 Mixed Oxide Catalysts (Ni/SiO2-Al2O3 복합 산화물 촉매 상에서 에탄올의 직접 아민화 반응에 의한 선택적 아세토니트릴 합성)

  • Kim, Hanna;Shin, Chae-Ho
    • Korean Chemical Engineering Research
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    • v.59 no.2
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    • pp.281-295
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    • 2021
  • In this study, the direct amination of ethanol was performed over impregnated Ni on SiO2-Al2O3 mixed oxide catalysts prepared by varying Si/(Si + Al) molar ratio to 30 mol%. To characterize the physico-chemical properties of the catalysts used, X-ray diffraction (XRD), N2-physisorption, temperature-programmed desorption of iso-propyl alcohol (IPA-TPD), temperature-programmed desorption of ethanol (EtOH-TPD), temperature-programmed reduction with H2 (H2-TPR), H2-chemisorption and transmission electron microscopy (TEM) were used. The acidic property was continuously increased until Si/(Si + Al) = 30 mol% in SiO2-Al2O3 mixed oxides used. The dispersion of Ni metal and surface area, acid characteristics of the supported Ni catalyst have a complex effect on the catalytic reaction activity. The low reduction temperature of nickel oxide and acidic properties were beneficial to the formation of acetonitrile. In terms of conversion of ethanol, Ni/SiO2-Al2O3 catalyst with a molar ratio of 10 mol% Si/(Si+Al) showed the highest activity and a volcanic curve based on it. The tendency of results were consistent in the metal dispersion and catalytic activity.

Synthesis of Ethylamines for the Reductive Amination of Ethanol over Ni Catalysts: Effect of Supports (니켈 촉매상에서 에탄올의 환원성 아민화반응에 의한 에틸아민 제조 : 담체의 영향)

  • Jeong, Ye-Seul;Shin, Chae-Ho
    • Korean Chemical Engineering Research
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    • v.57 no.5
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    • pp.714-722
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    • 2019
  • Catalysts were prepared by using incipient wetness impregnation method with 17 wt% Ni on a support ($SiO_2-Y_2O_3$, $Al_2O_3$, $SiO_2-ZrO_2$, $SiO_2$, $TiO_2$, MgO) and the catalytic activity in the reductive amination of ethanol with ammonia in the presence of hydrogen was compared and evaluated. The catalysts used before and after the reaction were characterized using X-ray diffraction, nitrogen adsorption, ethanol-temperature programmed desorption (EtOH-TPD), isopropanol-temperature programmed desorption (IPA-TPD), and hydrogen chemisorption etc. In the case of preparing $ZrO_2$ and $Y_2O_3$ supports, the small amount of Si dissolution from the Pyrex reactor surface provoked the formation of mixed oxides $SiO_2-ZrO_2$ and $SiO_2-Y_2O_3$. Among the catalysts used, $Ni/SiO_2-Y_2O_3$ catalyst showed the best activity, and this good activity was closely related to the highest nickel dispersion, and low desorption temperature in EtOH-TPD and IPA-TPD. The low catalytic activity on Ni/MgO catalysts showed low activity due to the formation of NiO-MgO solid-solutions. In the case of $Ni/TiO_2$, the reactivity was low due to the low nickel metal phase due to strong metal-support interaction. In the case of using a support as $SiO_2-Y_2O_3$, $Al_2O_3$, $SiO_2-ZrO_2$, and $SiO_2$, the selectivities of ethylamines and acetonitrile were not significantly different at similar ethanol conversion.

Selective Catalytic Reduction (SCR) of NOx with NH3 on Sb-promoted VWTi Catalysts (Sb 첨가에 따른 VWTi 촉매의 암모니아 선택적 촉매 환원(SCR)을 통한 질소산화물 저감)

  • Kim, Su Bin;Choi, Gyeong Ryun;Shin, Jung Hun;Hong, Sung Chang
    • Applied Chemistry for Engineering
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    • v.32 no.1
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    • pp.35-41
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    • 2021
  • VWTi, which is used as a commercial catalyst in NH3-SCR, exhibits excellent denitrification performance at 300 to 400 ℃, but there is a problem that efficiency decreases at low temperatures below 300 ℃. Research on catalysts containing promoter to increase low-temperature denitrification efficiency is steadily progressing. However, research on the cause of the improvement in low-temperature denitrification efficiency of the catalyst and the catalyst properties is insufficient. In this study, it was confirmed that by adding Sb to VWTi, denitrification performance was improved by more than 10% in NH3-SCR reaction below 300 ℃. At this time, the space velocity and the size of the catalyst particles were controlled to exclude the influence of external/internal diffusion. In addition, the catalytic properties according to the presence or absence of Sb were investigated by performing BET, TEM/EDS, O2-TPD, H2-TPR and DRIFTs analysis. It was judged that the addition of Sb increased the adsorbed oxygen species on the surface of the catalyst, thereby enhancing the redox properties of the catalyst at low temperature and exhibiting excellent denitrification performance.

Catalytic Hydrodeoxygenation of Biomass-Derived Oxygenates: a Review (바이오매스 유래 함산소 화합물의 수첨탈산소 촉매 반응: 총설)

  • Ha, Jeong-Myeong
    • Clean Technology
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    • v.28 no.2
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    • pp.174-181
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    • 2022
  • Biomass is a sustainable alternative resource for production of liquid fuels and organic compounds that are currently produced from fossil fuels including petroleum, natural gas, and coal. Because the use of fossil fuels can increase the production of greenhouse gases, the use of carbon-neutral biomass can contribute to the reduction of global warming. Although biological and chemical processes have been proposed to produce petroleum-replacing chemicals and fuels from biomass feedstocks, it is difficult to replace completely fossil fuels because of the high oxygen content of biomass. Production of petroleum-like fuels and chemicals from biomass requires the removal of oxygen atoms or conversion of the oxygen functionalities present in biomass derivatives, which can be achieved by catalytic hydrodeoxygenation. Hydrodeoxygenation has been used to convert raw biomass-derived materials, such as biomass pyrolysis oils and lignocellulose-derived chemicals and lipids, into deoxygenated fuels and chemicals. Multifunctional catalysts composed of noble metals and transition metals supported on high surface area metal oxides and carbons, usually selected as supports of heterogeneous catalysts, have been used as efficient hydrodeoxygenation catalysts. In this review, the catalysts proposed in the literature are surveyed and hydrodeoxygenation reaction systems using these catalysts are discussed. Based on the hydrodeoxygenation methods reported in the literature, an insight for feasible hydrodeoxygenation process development is also presented.

Heterogeneous Porous WO3@SnO2 Nanofibers as Gas Sensing Layers for Chemiresistive Sensory Devices

  • Bulemo, Peresi Majura;Lee, Jiyoung;Kim, Il-Doo
    • Journal of Sensor Science and Technology
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    • v.27 no.5
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    • pp.345-351
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    • 2018
  • We employed an unprecedented technique to synthesize porous $WO_3@SnO_2$ nanofibers exhibiting core-shell and fiber-in-tube configurations. Firstly, 2-methylimidazole was uniformly incorporated in as-spun nanofibers containing ammonium metatungstate hydrate and the sacrificial polymer (polyacrylonitrile). Secondly, the 2-methylimidazole on the surfaces of nanofibers was complexed with tin(II) chloride ($SnCl_2$) via simple impregnation of the as-spun nanofibers in ethanol containing tin(II) chloride dihydrate ($SnCl_2{\cdot}2H_2O$). The presence of vacant p-orbitals in tin (Sn) and the nucleophilic nitrogen on the imidazole ring allowed for the reaction between $SnCl_2$ and 2-methylimidazole, forming adducts on the surfaces of the as-spun nanofibers. The calcination of these nanofibers resulted in porous $WO_3@SnO_2$ nanofibers with a higher surface area ($55.3m^2{\cdot}g^{-1}$) and a better response to 1-5 ppm of acetone than pristine $SnO_2$ NFs synthesized using a similar method. An improved response to acetone was achieved upon functionalization of the $WO_3@SnO_2$ nanofibers with catalytic palladium nanoparticles. This work demonstrates the potential application of $WO_3@SnO_2$ nanofibers as sensing layers for chemiresistive sensory devices for the detection of acetone in exhaled breath.

Experimental Study of Hydrogen and Syngas Production over Ni/Ce-ZrO2/Al2O3 Catalysts with Additives (Ni/Ce-ZrO2/Al2O3 촉매의 첨가제에 따른 수소 및 합성가스 생성에 대한 실험적 연구)

  • Cho, Wonjun;Yu, Hyejin;Mo, Yonggi;Ahn, Whaseung
    • Transactions of the Korean hydrogen and new energy society
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    • v.25 no.2
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    • pp.105-113
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    • 2014
  • Performance tests on $Ni/Ce-ZrO_2/Al_2O_3$ catalysts with additives (MgO, $La_2O_3$) were investigated in the combined reforming processes (SCR, ATR, TRM) in order to produce hydrogen and carbon monoxide (it is called "syngas".). The catalyst characterization was conducted using the BET surface analyzer, X-ray diffraction (XRD), SEM, TPR and TGA. The combined reforming process was developed to adjust the syngas ratio depending on the synthetic fuel (methanol, DME and GTL) manufacturing processes. Ni-based catalysts supported on alumina has been generally recommended as a combined reforming reaction catalyst. It was found that both free NiO and complexed NiO species were responsible for the catalytic activity in the combined reforming of methane conversion, and the $Ce-ZrO_2$ binary support employed had improved the oxygen storage capacity and thermal stability. The additives, MgO and $La_2O_3$, also seemed to play an important role to prevent the formation of the carbon deposition over the catalysts. The experimental results were compared with the equilibrium data using a commercial simulation tool (PRO/II).