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함형원,배종욱 한국공업화학회 2018 한국공업화학회 연구논문 초록집 Vol.2018 No.0
The ferrierite (FER) zeolite, which is a candidate for a stable dehydration catalyst due to its proper acid property, was investigated for a direct DME synthesis from syngas containing CO or CO<sub>2</sub> with the impregnated copper-based catalyst (Cu-ZnO-Al<sub>2</sub>O<sub>3</sub>, CZA). The acidity and surface properties of FER zeolite can be easily modified by changing the synthesis condition like hydrothermal time, synthesis temperature, and Si/Al ratio, which can make a large influence to the dehydration activity of methanol. The hybrid catalysts which are copper based catalyst loaded on the as-prepared ferrierite having various Si/Al ratio were tested for a direct DME synthesis to confirm the effects of the Si/Al ratios to the activity. NH<sub>3</sub>-TPD, H<sub>2</sub>-TPR, XRD, and methanol dehydration test were performed to verify effects of the Si/Al ratio and the results showed that a high crystallinity was one of the key factors for a higher catalytic activity.
함형원,배종욱 한국공업화학회 2018 한국공업화학회 연구논문 초록집 Vol.2018 No.0
The valuable chemicals such as ethanol or acetic acid, which are widely used as petrochemical intermediates or alcohol fuels, can be synthesized through indirect multi-step reactions such as DME synthesis from syngas, DME carbonylation to methyl acetate and MA hydration or hydrogenation reactions to EtOH or AA. These multi-step reactions can produce a higher yield of EtOH compared to the direct routes using Rh, Co, Fe or Mo-based catalysts. Copper-based hybrid catalyst and highly crystalline ferrierite were applied for an indirect conversion technology of syngas, and dual-bed catalytic reactions were preliminarily investigated to optimize the reaction conditions and an order of catalyst loading and so on. This preliminary test can be further applied for the design of an integrated fluidized-bed reactor with two-phase segregation concept, which can be further used in order to simplify two cascade reactions in one reactor by efficiently controlling highly exothermic reactions.
함형원,배종욱 한국공업화학회 2019 한국공업화학회 연구논문 초록집 Vol.2019 No.0
A highly crystalline ferrierite (FER), which was prepared by seed-derived hydrothermal synthesis method, was utilized for dimethyl ether (DME) carbonylation to methyl acetate (MA). The seed-derived FER showed a higher catalytic activity and stability due to a larger amount of Brønsted acid sites with smaller defect sites. The superior carbonylation activity was originated from a proper aluminum distribution on the 10-membered ring (MR) and 8-MR channels on the seed-derived FER, however, excess aluminum distributions in the 8-MR channels seems to weaken the acidic strengths by increasing the repetition of seed-derived hydrothermal synthesis, which is responsible for a decreased activity. It is essential to control the aluminum concentration in 8-MR channels with their distribution to get a higher activity as well as long-term stability.
Syngas conversions to clean fuels and petrochemicals
배종욱,함형원,구현모,조재민,박용민 한국공업화학회 2018 한국공업화학회 연구논문 초록집 Vol.2018 No.0
Syngas conversion technologies to useful petrochemical intermediates and clean fuels by CO (or CO<sub>2</sub>) hydrogenation have been largely attracted to efficiently utilize many waste feedstocks such as byproduct gases from steel refinery industries. The chemical products of methanol, dimethyl ether (DME) and methyl acetate and paraffinic hydrocarbons such as diesel and gasoline can be used as many petrochemical intermediates or clean fuels directly. The newly developed highly ordered mesoporous structures of the binary metal oxides such as Co<sub>3</sub>O<sub>4</sub>-Al<sub>2</sub>O<sub>3</sub>, Co<sub>3</sub>O<sub>4</sub>-ZrO<sub>2</sub> and Fe<sub>2</sub>O<sub>3</sub>-ZrO<sub>2</sub> after a proper zeolite-encapsulation with additional promoters were applied for Fischer-Tropsch synthesis (FTS) reaction to produce clean hydrocarbon fuels. In addition, the effects of highly crystalline ferrierite zeolite on the hybrid catalysts was also intensively investigated for an enhanced catalytic activity and stability for CO hydrogenation reaction as well.
배종욱,함형원,김지현 한국공업화학회 2016 한국공업화학회 연구논문 초록집 Vol.2016 No.1
Oxygenates such as alcohols and dimethylether (DME), which has similar physical properties with LPG, are attractive alternative fuels to possibly replace conventional petroleum-based hydrocarbon fuels due to its lower emission of air-pollutants. In the present study, a direct formation of oxygenates from syngas including CO<sub>2</sub> was investigated using hybrid heterogeneous catalysts containing copper crystallites with metal (Ga, Zn, Ti)-incorporated ordered mesoporous Al<sub>2</sub>O<sub>3</sub> with 10wt%Cu. The ordered mesoporous structures enhanced the catalytic stability for CO (or CO<sub>2</sub>) hydrogenation to oxygenates by confining copper crystallites in the mesopores of Al<sub>2</sub>O<sub>3</sub> efficiently. Some characterizations such as H2-TPR, XRD, NH<sub>3</sub>-TPD, N2-physisorption, XPS, and XAFS were applied to characterize the catalytic properties and activities before and after reaction.
Seed-mediated synthesized FER for dimethyl ether carbonylation to methyl acetate
정현승,함형원,박경수,배종욱 한국공업화학회 2018 한국공업화학회 연구논문 초록집 Vol.2018 No.0
Dimethyl ether (DME) can be utilized to produce methyl acetate (MA) by carbonylation of DME, which can be transformed to ethanol or acetic acid through a subsequent hydrogenation or hydration reaction. To insert the carbon monoxide into the DME, zeolite can be used as a heterogeneous catalyst since its acidic sites can efficiently form methoxy and acetyl intermediates from the adsorbed DME and CO molecules. Nowadays, the seed-derived ferrierite (FER) was investigated to observe the effects of crystallinity and acidic natures to catalytic activity and stability. Seed-mediated synthesis of FER was applied using an as-synthesized FER as a seeding material to tune the crystallinity of the final FER zeolite at different seed concentration. A pristine FER and seed-mediated FER were tested for DME carbonylation, and the FER seed contents were optimized to find out the best catalyst by showing a higher stability originated from a less deposition of coke precursors during DME carbonylation.
Effects of W/C ratio on Mn-Rh/WxC catalysts to synthesize mixed alcohols by CO hydrogenation
원바다,함형원,배종욱 한국공업화학회 2016 한국공업화학회 연구논문 초록집 Vol.2016 No.1
Higher alcohol synthesis by direct CO hydrogenation was investigated using mesoporous Rh-Mn/WxC catalysts having a different C/W ratio to verify the roles of WxC supports to CO conversion and product distribution. The Rh-Mn/WxC catalyst was synthesized by using hard-template of SBA-15 with different weight ratios of C/W from 1 to 20 with a fixed 5 wt%Rh and 3 wt%Mn. The catalysts prepared by using C/W ratio of 10 showed a higher productivity of mixed alcohols, and the superior activity seems to be attributed to a high dispersion of active metals on the WxC support having an optimal C/W ratio. The surface properties of Rh-Mn/WxC catalysts were characterized by XRD, N<sub>2</sub>-sorption, TEM-EDS and XPS analysis.
Confinement effects of Ni nanoparticles in ordered mesoporous materials for dry reforming of methane
박경수,조재민,함형원,배종욱 한국공업화학회 2019 한국공업화학회 연구논문 초록집 Vol.2019 No.0
For a dry reforming of methane (DRM), Ni-based catalysts have a lot of problems due to their thermal instability by a sintering of supported Ni nanoparticles (NPs) to form less active larger agglomerates at a high temperature as well as significant coke formation compared to the novel metal-based catalysts. In order to suppress those limitations for a commercial application, the ordered mesoporous materials of SiO<sub>2</sub> and Al<sub>2</sub>O<sub>3</sub> were used to solve the deactivation of Ni nanoparticles, which were synthesized by a chemical reduction method by using nickel (II) acetylacetonate with borane tertbutylamine. The Ni nanoparticles were successfully confined in the ordered mesoporous structures, which suppressed the aggregations of the confined Ni nanoparticles thus showed a stable production of syngas at a high temperature without any significant aggregation and coke deposition.