• Title/Summary/Keyword: Mesoporous catalyst

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Knoevenagel Condensation Reaction Using Amine-functionalized MCM-41 Base Catalysts (아민고정화 MCM-41 염기촉매를 이용한 Knoevenagel 축합반응)

  • Choi, Jung-Sik;Ahn, Wha-Seung
    • Korean Chemical Engineering Research
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    • v.44 no.4
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    • pp.417-423
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    • 2006
  • A series of amine functionalized MCM-41 catalysts were prepared by aminopropyltrimethoxysilane grafting and their catalytic performance in Knoevenagel reaction of selected substrates was investigated. Water resistant and catalytically active amine grafted MCM-41 was prepared by post-synthetic silylation using methyltrimethoxysilane ; hydrogen bonding of the water molecules formed during the condensation reaction to the active N group was suppressed, which led to high TON of the reaction. Amine functionalized MCM-41 prepared by coating method produced high conversion, but the TON of the catalyst was much lower than that of the amine grafted MCM-41; pore volume of the functionalized MCM-41 decreased substantially and large portion of the immobilized amine is believed to be hydrogen bonded to each other, which can result in decrease in the basicity of the N group. A secondary amine group was prepared by room temperature condensation between aminopropylsilane and chloropropylsilane, and the MCM-41 grafted with the secondary amine group demonstrated the highest catalytic activity among the catalysts prepared.

Ultrathin Titania Coating for High-temperature Stable $SiO_2$/Pt Nanocatalysts

  • Reddy, A. Satyanarayana;Kim, S.;Jeong, H.Y.;Jin, S.;Qadir, K.;Jung, K.;Jung, C.H.;Yun, J.Y.;Cheon, J.Y.;Joo, S.H.;Terasaki, O.;Park, Jeong-Young
    • Proceedings of the Korean Vacuum Society Conference
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    • 2011.08a
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    • pp.217-217
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    • 2011
  • Recently, demand for thermally stable metal nanoparticles suitable for chemical reactions at high temperatures has increased to the point to require a solution to nanoparticle coalescence. Thermal stability of metal nanoparticles can be achieved by adopting core-shell models and encapsulating supported metal nanoparticles with mesoporous oxides [1,2]. However, to understand the role of metal-support interactions on catalytic activity and for surface analysis of complex structures, we developed a novel catalyst design by coating an ultra-thin layer of titania on Pt supported silica ($SiO_2/Pt@TiO_2$). This structure provides higher metal dispersion (~52% Pt/silica), high thermal stability (~600$^{\circ}C$) and maximization of the interaction between Pt and titania. The high thermal stability of $SiO_2/Pt@TiO_2$ enabled the investigation of CO oxidation studies at high temperatures, including ignition behavior, which is otherwise not possible on bare Pt nanoparticles due to sintering [3]. It was found that this hybrid catalyst exhibited a lower activation energy for CO oxidation because of the metal-support interaction. The concept of an ultra-thin active metal oxide coating on supported nanoparticles opens-up new avenues for synthesis of various hybrid nanocatalysts with combinations of different metals and oxides to investigate important model reactions at high-temperatures and in industrial reactions.

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Synthesis and Characterization of Fe-Co/mesoHZSM-5 : Effect of Desilication Agent and Iron-cobalt Composition

  • Jimmy, Jimmy;Roesyadi, Achmad;Suprapto, Suprapto;Kurniawansyah, Firman
    • Korean Chemical Engineering Research
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    • v.58 no.1
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    • pp.163-169
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    • 2020
  • Synthesis of Fe-Co/meso-HZSM5 catalyst, intended to be applied in Fischer-Tropsch (FT) reaction was investigated. The study emphasized the effect of desilication agents, NaOH and KOH, on the catalyst materials properties. Impregnation composition of active metal (Fe and Co) was also examined. HZSM-5, converted from ammonium ZSM-5 through calcination, was treated with NaOH and KOH for desilication, followed by impregnation with 10% metal loading. Fe composition in the initial mixture was varied at 10-50% from total composition. After impregnation, reduction was applied by flowing hydrogen gas at 400 ℃ for 10 hours. The use of KOH solution induced greater mesoporous volumes; however, it had a detrimental effect on zeolite crystal structure. NaOH solutions, on the other hand, increased mesopore area as high as 100%, indicated from surface area increase from 266.28 m2/g of HZSM-5, to 526.03 m2/g of NaOH-desilicated HZSM-5. In addition, the application of NaOH solution increased pore volume from 0.14 cc/g to 0.486 cc/g. Further, more Fe-Co alloys and less oxide of iron (Fe2O3) as well cobalt (Co3O4) had been commonly observed in the produced catalysts. The largest Fe-Co alloys could be found in 50Fe-50Co/HZSM-5

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.

Effect of Sulfation on Physicochemical Properties of ZrO2 and TiO2 Nanoparticles

  • Wijaya, Karna;Pratika, Remi Ayu;Fitri, Edhita Rahmawati;Prabani, Prisnu Fadilah;Candrasasi, Yufinta;Saputri, Wahyu Dita;Mulijani, Sri;Patah, Aep;Wibowo, Arief Cahyo
    • Korean Journal of Materials Research
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    • v.32 no.3
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    • pp.125-131
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    • 2022
  • Effect of sulfation processes on the physicochemical properties of ZrO2 and TiO2 nanoparticles were thoroughly investigated. SO4/ZrO2 and SO4/TiO2 catalysts were synthesized to identify the acidity character of each. The wet impregnation method of ZrO2 and TiO2 nanoparticles was employed using H2SO4 with various concentrations of 0.5, 0.75, and 1 M, followed by calcination at 400, 500, and 600 ℃ to obtain optimum conditions of the catalyst synthesis process. The highest total acidity was found when using 1 M SO4/ZrO2-500 and 1 M SO4/TiO2-500 catalysts, with total acidity values of 2.642 and 6.920 mmol/g, respectively. Sulfation increases titania particles via agglomeration. In contrast, sulfation did not practically change the size of zirconia particles. The sulfation process causes color of both catalyst particles to brighten due to the presence of sulfate. There was a decrease in surface area and pore volume of catalysts after sulfation; the materials' mesoporous structural properties were confirmed. The 1 M SO4/ZrO2 and 1 M SO4/TiO2 catalysts calcined at 500 ℃ are the best candidate heterogeneous acid catalysts synthesized in thus work.

Oxidative Desulfurization of Marine Diesel Using WOx/SBA-15 Catalyst and Hydrogen Peroxide (WOx/SBA-15 촉매와 과산화수소를 이용한 선박용 경유의 산화 탈황 연구)

  • Oh, Hyeonwoo;Kim, Ji Man;Huh, Kwang-Sun;Woo, Hee Chul
    • Korean Chemical Engineering Research
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    • v.55 no.4
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    • pp.567-573
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    • 2017
  • In this work, tungsten oxide ($WO_x$) supported on SBA-15 (mesoporous silica) were prepared and applied for oxidative desulfurization of sulfur compounds in marine diesel containing about 230 ppmw of sulfur concentration. Prepared catalysts were examined by two steps; at first step, oxidation reaction carried out with hydrogen peroxide as oxidant and then the oxidized sulfur compounds were extracted by acetonitrile as solvent. Catalysts were characterized by using X-ray diffraction, X-ray fluorescence, X-ray photoelectron spectroscopy and $N_2$ adsorption-desorption isotherms. Tungsten oxide exists as monoclinic crystal system on SBA-15 and over about 10 wt% of the $WO_x$ loading took the form of multi-layers on SBA-15. The 13 wt% $WO_x$/SBA-15 catalyst exhibite highest activity, achieving about 76.3% sulfur removal in the reaction conditions, such as catalyst amount of 0.1 g, reaction temperature at $90^{\circ}C$, reaction time for 3 h and O/S molar ratio of 10. One time oxidation reaction is enough oxidize the sulfur compounds in marine diesel completely. The repetition experiment of extraction process indicated that sulfur removal could reach 94.4% after 5 times.

Synthesis of Mesoporous SAPO-34 Catalyst Using Chitosan and Its DTO Reaction (키토산을 이용한 메조 세공 SAPO-34 촉매의 합성 및 DTO 반응)

  • Yoon, Young-Chan;Song, Kang;Lim, Jeong-Hyeon;Park, Chu-Sik;Kim, Young-Ho
    • Applied Chemistry for Engineering
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    • v.32 no.3
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    • pp.305-311
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    • 2021
  • Effects of chitosan as a mesopore directing agent of SAPO-34 catalysts were investigated to improve the catalytic lifetime in DTO reaction. The synthesized catalysts were characterized by XRD, SEM, N2 adsorption-desorption isotherm and NH3-temperature programmed desorption (TPD). The modified SAPO-34 catalysts prepared by varying the added amount of chitosan showed the same cubic morphology and chabazite structure as the conventional SAPO-34 catalyst. As the added amount of chitosan increased to 3 wt%, the surface area, mesopore volume and concentration of weak acid sites of modified SAPO-34 catalysts increased. The modified SAPO-34 catalysts showed enhanced catalytic lifetime and high selectivity for light olefins in the DTO reaction. In particular, the SAPO-CHI 3 catalyst (3 wt%) exhibited the longest catalytic lifetime than that of the conventional SAPO-34. Therefore, it was confirmed that chitosan was a suitable material as a mesopore directing agent to delay deactivation of the SAPO-34 catalyst.

Effect of Conductive Additive Amount on Electrochemical Performances of Organic Supercapacitors (유기계 슈퍼커패시터에서 도전재의 양이 전기화학적 특성에 미치는 영향)

  • Yang, Inchan;Lee, Gihoon;Jung, Ji Chul
    • Korean Journal of Materials Research
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    • v.26 no.12
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    • pp.696-703
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    • 2016
  • In this study, we intensively investigated the effect of conductive additive amount on electrochemical performance of organic supercapacitors. For this purpose, we assembled coin-type organic supercapacitor cells with a variation of conductive additive(carbon black) amount; carbon aerogel and polyvinylidene fluoride were employed as active material and binder, respectively. Carbon aerogel, which is a highly mesoporous and ultralight material, was prepared via pyrolysis of resorcinol-formaldehyde gels synthesized from polycondensation of two starting materials using sodium carbonate as the base catalyst. Successful formation of carbon aerogel was well confirmed by Fourier-transform infrared spectroscopy and $N_2$ adsorption-desorption analysis. Electrochemical performances of the assembled organic supercapacitor cells were evaluated by cyclic voltammetry, galvanostatic charge/discharge, and electrochemical impedance spectroscopy measurements. Amount of conductive additive was found to strongly affect the charge transfer resistance of the supercapacitor electrodes, leading to a different optimal amount of conductive additive in organic supercapacitor electrodes depending on the applied charge-discharge rate. A high-rate charge-discharge process required a relatively high amount of conductive additive. Through this work, we came to conclude that determining the optimal amount of conductive additive in developing an efficient organic supercapacitor should include a significant consideration of supercapacitor end use, especially the rate employed for the charge-discharge process.

Conversion of Cellulose over Ni Loaded Mesoporous MSU-F Catalysts via Air Gasification

  • Park, Young-Kwon;Park, Kyung Sun;Kim, Seong-Soo;Park, Sung Hoon;Jung, Sang-Chul;Kim, Sang Chai;Jeon, Jong-Ki;Jeon, Ki-Joon
    • Bulletin of the Korean Chemical Society
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    • v.35 no.11
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    • pp.3205-3208
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    • 2014
  • Catalytic gasification of cellulose was carried out in a U-type fixed reactor with Ni loaded MSU-F catalyst (Ni/MSU-F) and Ni loaded ${\gamma}-Al_2O_3$ (Ni/${\gamma}-Al_2O_3$). The characteristics of the catalysts were analyzed by using X-ray diffraction, $H_2$-temperature programmed reduction, and Brunauer-Emmett-Teller analyses. The operation conditions of catalytic gasification reactions were $750^{\circ}$ and 0.2 equivalence ratio. Air was used as gasification agent. Catalytic gasification characteristics, such as gas yield and gas composition ($H_2$, CO, $CO_2$, $C_1-C_4$), were measured and calculated. The gas yield of Ni/MSU-F was much higher than that of Ni/${\gamma}-Al_2O_3$. Especially high amount of hydrogen was produced by Ni/MSU-F.

Photocatalytic Decomposition of Methylene Blue over Sm Ion Doped Ti-SBA-15 Catalysts (Sm이온이 도핑된 Ti-SBA-15 촉매에서의 메틸렌블루의 광촉매 분해 반응)

  • Jung, Won-Young;Lee, Seong-Hun;Hong, Seong-Soo
    • Journal of Environmental Science International
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    • v.20 no.4
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    • pp.511-517
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    • 2011
  • Ti-SBA-15 catalysts doped with samarium ion were synthesized using conventional hydrothermal method. The physical properties of Sm/Ti-SBA-15 catalysts have been characterized by XRD, FT-IR, DRS and PL. In addition, we have also examined the activity of these materials on the photocatalytic decomposition of methylene blue. The Sm/ Ti-SBA-15 was shown to have the mesoporous structure regardless of Sm ion doping. With doping amount of 1% lanthanide ion, the pore size and pore volume of Sm(Er, Cs)/Ti-SBA-15 decreased and the surface area increased. For the purpose of vibration characteristics on the Ti-SBA-15 and Sm/Ti-SBA-15 photocatalysts, the IR absorption at 960 $cm^{-1}$ commonly accepted the characteristic vibration of Ti-O-Si bond. 1% of Sm/Ti-SBA-15 had the highest photocatalytic activity on the decomposition of methylene blue but the catalysts doped with Er ions had lower activity in comparison with pure Ti-SBA-15 catalyst.