• Title/Summary/Keyword: 촉매 표면 반응

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Heterogeneous Oxidation of Liquid-phase TCE over $CoO_x/TiO_2$ Catalysts (액상 TCE 제거반응을 위한 $CoO_x/TiO_2$ 촉매)

  • Kim, Moon-Hyeon;Choo, Kwang-Ho
    • Journal of Korean Society of Environmental Engineers
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    • v.27 no.3
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    • pp.253-261
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    • 2005
  • Catalytic wet oxidation of ppm levels of trichloroethylene (TCE) in water has been conducted using $TiO_2$-supported cobalt oxides at a given temperature and weight hourly space velocity. 5% $CoO_x/TiO_2$ might be the most promising catalyst for the wet oxidation at $36^{\circ}C$ although it exhibited a transient behavior in time on-stream activity. Not only could the bare support be inactive for the wet decomposition reaction, but no TCE removal also occurred by the process of adsorption on $TiO_2$ surface. The catalytic activity was independent of all particle sizes used, thereby representing no mass transfer limitation in intraparticle diffusion. Characterization of the $CoO_x$ catalyst by acquiring XPS spectra of both fresh and used Co surfaces gave different surface spectral features of each $CoO_x$. Co $2p_{3/2}$ binding energy of Co species exposed predominantly onto the outermost surface of the fresh catalyst appeared at 781.3 eV, which is very similar to the chemical states of $CoTiO_x$ such as $Co_2TiO_4$ and $CoTiO_3$. The spent catalyst possessed a 780.3 eV main peak with a satellite structure at 795.8 eV. Based on XPS spectra of reference Co compound, the TCE-exposed Co surfaces could be assigned to be in the form of mainly $Co_3O_4$. XRD measurements indicated that the phase structure of Co species in 5% $CoO_x/TiO_2$ catalyst even before reaction is quite comparable to the diffraction lines of external $Co_3O_4$ standard. A model structure of $CoO_x$ present on titania surfaces would be $Co_3O_4$, encapsulated in thin-film $CoTiO_x$ species consisting of $Co_2TiO_4$ and $CoTiO_3$, which may be active for the decomposition of TCE in a flow of water.

Synthesis and characterization of 60 wt.% RGO(reduced graphite oxide) supported PtSn series catalysts for methanol electrooxidation (RGO(reduced graphite oxide)에 담지된 PtSn 시리즈 촉매의 합성 및 특성분석과 메탄올 산화 반응)

  • Choe, Seung-Mok;Kim, Won-Bae;Lee, Ju-Yeol
    • Proceedings of the Korean Institute of Surface Engineering Conference
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    • 2013.05a
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    • pp.159-159
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    • 2013
  • 넓은 비표면적과 높은 전기전도성을 갖는 표면에 관능기가 도입된 RGO(reduced graphite oxide)를 modified Hummers method 와 thermal exfoliation 을 통해하여 합성하였으며 합성된 RGO를 PtSn alloy 촉매의 담지체로 도입하여 impregnation method를 통해 PtSn/RGO 시리즈 촉매를 합성하였다. XRD, SEM, TEM, XPS 분석을 통해 촉매의 특성을 분석하였고 methanol electrooxidation 활성을 확인하였다.

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고분자 촉매 집합체 제조를 위한 Surface Coating 특성연구.

  • 이성호;조해동;김용성;정흥석
    • Proceedings of the Korean Nuclear Society Conference
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    • 1995.05b
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    • pp.957-963
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    • 1995
  • 촉매탑에서 수소와 물 사이의 수소동위원소 교환반응에 사용되는 소수성 고분자 촉매 집합체제조 기술개발을 위하여, 촉매담체를 소수성 수지를 이용하여 충전물 표면에 효과적으로 Binding 시키기 위한 Surface coating 특성에 대하여 연구하였다. 실험에서 먼저 Teflon 수지에 잘 혼합된 Activated carbon을 Ceramic berl - saddle 등의 3가지 형태의 충전물 표면에 Coating시켜 소결 온도, 충전물의 형태 및 표면 위치에 따른 Coating 특성에 대하여 연구하였다.

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고에너지 전자빔으로 처리된 Ni/Al$_{2}$O$_{3}$ 촉매에서 메탄의 dry reforming

  • Sin, Jung-Hyeok;Lee, Jeong-Hwan;Jeon, Jin
    • Proceedings of the Korean Environmental Sciences Society Conference
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    • 2005.05a
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    • pp.284-285
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    • 2005
  • Ni/${\gamma}$-Al$_{2}$O$_{3}$의 촉매능 향상을 위하여 고에너지의 전자빔을 사용하여 처리한 후 촉매반응과 표면상태 변화를 관찰하였다. XRD와 XPS 분석 결과로부터 전자빔 처리된 촉매에서 표면의 상대적인 O/Ni의 비가 감소되고 Ni의 산화상태가 변화하였음을 관찰하였다. 2MeV의 준위에서 600 kGy의 선량으로 전자빔을 조사한 촉매에서 가장 높은 전환율과 수득율을 보임으로써 고준위 고선량의 전자빔 처리가 촉매능 향상에 유리함을 알 수 있었다.

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Continuous Wet Oxidation of TCE over Supported Metal Oxide Catalysts (금속산화물 담지촉매상에서 연속 습식 TCE 분해반응)

  • Kim, Moon Hyeon;Choo, Kwang-Ho
    • Korean Chemical Engineering Research
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    • v.43 no.2
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    • pp.206-214
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    • 2005
  • Heterogeneously-catalyzed oxidation of aqueous phase trichloroethylene (TCE) over supported metal oxides has been conducted to establish an approach to eliminate ppm levels of organic compounds in water. A continuous flow reactor system was designed to effect predominant reaction parameters in determining catalytic activity of the catalysts for wet TCE decomposition as a model reaction. 5 wt.% $CoO_x/TiO_2$ catalyst exhibited a transient period in activity vs. on-stream time behavior, suggesting that the surface structure of the $CoO_x$ might be altered with on-stream hours; regardless, it is probable to be the most promising catalyst. Not only could the bare support be inactive for the wet decomposition reaction at $36^{\circ}C$, but no TCE removal also occurred by the process of adsorption on $TiO_2$ surface. The catalytic activity was independent of all particle sizes used, thereby representing no mass transfer limitation in intraparticle diffusion. Very low TCE conversion appeared for $TiO_2$-supported $NiO_x$ and $CrO_x$ catalysts. Wet oxidation performance of supported Cu and Fe catalysts, obtained through an incipient wetness and ion exchange technique, was dependent primarily on the kinds of the metal oxides, in addition to the acidic solid supports and the preparation routes. 5 wt.% $FeO_x/TiO_2$ catalyst gave no activity in the oxidation reaction at $36^{\circ}C$, while 1.2 wt.% Fe-MFI was active for the wet decomposition depending on time on-stream. The noticeable difference in activity of the both catalysts suggests that the Fe oxidation states involved to catalytic redox cycle during the course of reaction play a significant role in catalyzing the wet decomposition as well as in maintaining the time on-stream activity. Based on the results of different $CoO_x$ loadings and reaction temperatures for the decomposition reaction at $36^{\circ}C$ with $CoO_x/TiO_2$, the catalyst possessed an optimal $CoO_x$ amount at which higher reaction temperatures facilitated the catalytic TCE conversion. Small amounts of the active ingredient could be dissolved by acidic leaching but such a process gave no appreciable activity loss of the $CoO_x$ catalyst.

A Study on Oxidative Decomposition of CFC-113 over TiO2-SiO2 Catalysts Prepared by the Sol-Gel Method (솔-젤법으로 제조된 TiO2-SiO2 촉매상에서 CFC-113의 산화분해반응에 관한 연구)

  • Chang, Won-Chul;Lee, Doo-Hyoung;Lee, Tae-Jin
    • Applied Chemistry for Engineering
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    • v.10 no.7
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    • pp.963-968
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    • 1999
  • The global environmental problems have been caused by the release of CFCs. Therefore, methods for safe destruction of recoverd CFCs will be eventually needed. The objective of this study was to develop and test a catalyst operating at a mild condition for the decomposition of CFC-113. In this work, catalytic oxidative decomposition of CFC-113 was carried out over aerosol $TiO_2/SiO_2(ATS)$ catalysts prepared by the sol-gel method. All ATS catalysts(Ti/Si mol ratio=1, 2, 2.33, 4) showed high initial activity. However, the deactivation of ATS catalysts was found that more remarkable due to an attack of fluorine and the destruction of ATS structure(Si-F reaction) from analyses of SEM-EDX, XRD than $TiO_2/SiO_2(ATS)$ catalyst prepared by the precipitation method. ATS catalysts prepared by more acidic prehydrolysis condition were found to have still more activity and longer life-time by increasing of acidity. The activity of ATS catalyst also depend on the content of $TiO_2$. There was reason that the acidity of the ATS catalyst was increased with the increased content of $TiO_2$ from 50 to 80 mol %. Solid superacid catalyst ($ATX/SO_4{^{2-}}$) modified with $H_2SO_4$ solution was prepared for high activity and lower deactivation. The reaction of $ATS/SO_4{^{2-}}$ catalyst also exhibited even higher activity and lower deactivation than the original ATS catalyst. It is suggested that the addition of the sulphate species clearly inhibit the deactivation.

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Preparation and Reactivity of Cu-Zn-Al Based Hybrid Catalysts for Direct Synthesis of Dimethyl Ether by Physical Mixing and Precipitation Methods (물리혼합 및 침전법에 의한 DME 직접 합성용 Cu-Zn-Al계 혼성촉매의 제조 및 반응특성)

  • Bang, Byoung Man;Park, No-Kuk;Han, Gi Bo;Yoon, Suk Hoon;Lee, Tae Jin
    • Korean Chemical Engineering Research
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    • v.45 no.6
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    • pp.566-572
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    • 2007
  • Two hybrid catalysts for the direct synthesis of DME were prepared and the catalytic activity of these catalysts were investigated. The hybrid catalyst for the direct synthesis of DME was composed as the catalytic active components of methanol synthesis and dehydration. The methanol synthesis catalyst was formed from the precursor contained Cu and Zn, the methanol dehydration catalyst was used ${\gamma}-Al_2O_3$. As PM-CZ+D and CP-CZA/D, Two hybrid catalysts were prepared by physical mixing method (PM-CZ+D) and precipitation method (CP-CZA/D), respectively. PM-CZ+D was prepared by physically mixing methanol synthesis catalyst and methanol dehydration catalyst, CP-CZA/D was prepared by depositing Cu-Zn or Cu-Zn-Al components on ${\gamma}-Al_2O_3$. The crystallinity and the surface morphology of synthesized catalyst were analyzed by X-ray diffraction (XRD) and scanning electron microscope (SEM) to investigate the physical property of prepared catalyst. And BET surface area by $N_2$ adsorption and the surface area of Cu by $N_2O$ chemisorption were investigated about the hybrid catalysts. In addition, catalytic activity of these hybrid catalysts was examined with varying reaction conditions. At that time, the reaction temperature of $250{\sim}290^{\circ}C$, the reaction pressure of 50~70 atm, the $[H_2]/[CO]$ mole ratio of 0.5~2.0 and the space velocity of $1,500{\sim}6,000h^{-1}$ were investigated the catalytic activity. From these results, it was confirmed that the reactivity of CP-CZA/D was higher than that of PM-CZ+D. When the conditions of reaction temperature, pressure, $[H_2]/[CO]$ ratio and space velocity were $260^{\circ}C$, 50 atm and 1.0, $3,000h^{-1}$ respectively, CO conversion using CP-CZA/D hybrid catalyst was 72% and the CO conversion of CP-CZA/D was more than 20% compared with the CO conversion of PM-CZ+D. It was known that Cu surface area of CP-CZA/D hybrid catalyst was higher than that of hybrid PM-CZ+D catalyst using $N_2O$ chemisorption. It was assumed that the catalytic activity was improved because Cu particle of hybrid catalyst prepared by precipitation method was well dispersed.

Preparation and Reaction Studies of $Pt/Al_2O_3$ Model Catalysts

  • Kim, Chang-Min;Gabor A. Somorjai
    • Journal of the Korean Vacuum Society
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    • v.3 no.4
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    • pp.414-419
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    • 1994
  • Surface of Pt/$Al_2O_3$ model catalyst was produced on an aluminum foil with surface area of 1 $cm^2$ The aluminum surface was oxidized under $10 ^5Torr$Torr oxygen and platinum was deposited on top of the oxide layer using a plasma evaporation source. Conversion of I-butene was performed on the model catalyst surface. Isomerization was the major reaction in I-butene conversion on the aluminum oxide layer. Addition of Pt on the aluminum oxide layer induces hydrogenation of I-butene. Selectivity for the hydrogenation increases as the amount of Pt on alumina increases.

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Study of fabrication of anodic TiO2 nanotube and transition metal catalyst doping on its surface (양극산화 타이타늄 나노튜브 제작 및 전이금속 촉매 표면처리에 대한 연구)

  • O, Gi-Seok;Yu, Hyeon-Seok;Choe, Jin-Seop
    • Proceedings of the Korean Institute of Surface Engineering Conference
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    • 2015.11a
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    • pp.336-337
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    • 2015
  • $TiO_2$는 표면적이 넓고 안정성이 높아 자체의 높은 밴드갭(3.0~3.2 eV)에도 불구하고 산업적으로 염소분해 전극으로써 사용되며, 최근 물분해 전극 적용 연구가 진행되고 있다. 전기화학적 물분해 반응을 위해서는 높은 과전압이 요구되므로 산업적으로 이용하기 위해 전도성을 향상시키기 위한 연구가 필요하다. 이러한 문제를 해결하기 위해 촉매제의 도핑이 연구되고 있으며 본 연구에서는 표면에 촉매를 도핑시키기 위한 두가지 방법을 연구하였다. 일반적으로 촉매로 사용되는 금속은 루테늄과 이리듐 등의 귀금속이며 촉매가 균일하게 도핑이 될수록 성능은 향상된다. 본 연구에서는 루테늄을 촉매로 선택하였으며 서로 다른 도핑 방법과 용매 하에서 물분해 실험을 진행하여 두 가지 방법의 물분해 효율을 비교하였다.

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Pd/Pd3Fe Alloy Catalyst for Enhancing Hydrogen Production Rate from Formic Acid Decomposition: Density Functional Theory Study (개미산 분해 반응에서 수소 생산성 증대를 위한 Pd/Pd3Fe 합금 촉매: 범밀도 함수 이론 연구)

  • Cho, Jinwon;Han, Jonghee;Yoon, Sung Pil;Nam, Suk Woo;Ham, Hyung Chul
    • Korean Chemical Engineering Research
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    • v.55 no.2
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    • pp.270-274
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    • 2017
  • Formic acid has been known as one of key sources of hydrogen. Among various monometallic catalysts, hydrogen can be efficiently produced on Pd catalyst. However, the catalytic activity of Pd is gradually reduced by the blocking of active sites by CO, which is formed from the unwanted indirect oxidation of formic acid. One of promising solutions to overcome such issue is the design of alloy catalyst by adding other metal into Pd since alloying effect (such as ligand and strain effect) can increase the chance to mitigate CO poisoning issue. In this study, we have investigated formic acid deposition on the bimetallic $Pd/Pd_3Fe$ core-shell nanocatalyst using DFT (density functional theory) calculation. In comparison to Pd catalyst, the activation energy of formic acid dehydrogenation is greatly reduced on $Pd/Pd_3Fe$ catalyst. In order to understand the importance of alloying effects in catalysis, we decoupled the strain effect from ligand effect. We found that both strain effect and ligand effect reduced the binding energy of HCOO by 0.03 eV and 0.29 eV, respectively, compared to the pure Pd case. Our DFT analysis of electronic structure suggested that such decrease of HCOO binding energy is related to the dramatic reduction of density of state near the fermi level.