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      • SCOPUSKCI등재

        실리카 담지 12-몰리브도인산 촉매상에서의 아산화질소에 의한 메탄의 부분산화반응

        홍성수,우희철,주창식,이근대,( Seong Soo Hong,Hee Chul Woo,Chang Sik Ju,Gun Dae Lee,J . B . Moffat ) 한국공업화학회 1994 공업화학 Vol.5 No.1

        실리카에 담지된 혜테로폴리산 촉매에서 아산화질소에 의한 메탄의 부분산화반응을 연구하였다. 여러 가지의 반응조건, 즉 반응온도, 반응물의 분압, 접촉시간, 촉매의 담지량 및 전처리온도 등이 전환율이나 생성물의 선택도 및 속도론에 미치는 영향이 연구되었다. 20wt%로 담지된 촉매가 전환율과 포름알데히드의 수율에 있어서 가장 높은 값을 보여 주었다. 메탄의 전환반응에서의 속도식을 구한 결과, 메탄에 대해서는 1차식을 보여 주었고, 아산화질소에 대한 반응차수는 약 0.4였다. 또한 전체반응의 겉보기 활성화에너지는 30.78 ㎉/mole 이었다. 반응물 중에 첨가된 소량의 사염화탄소는 메탄의 산화반응에서 실리카 담지 HPMo촉매의 활성을 증가시키는 반면에, 반응물에 첨가된 물은 오히려 활성을 감소시키는 것을 볼 수 있었다. The partial oxidation of methane with nitrous oxide on silica-supported metal-oxygen cluster compounds, known as heteropoly acids, has been studied. The effects of several variables such as reaction temperature, partial pressure of reactants, residence time, loading of the catalysts, and pretreatment temperature, on the conversion and product distribution were observed. The kinetics also has been studied. The conversion and yield of formaldehyde show maximum values at a loading of 20 wt%. The apparent reaction order of methane conversion is ca. 1.0 with respect to CH_4 and ca. 0.4 with respect to N_2O. In addition, the apparent activation energy is 30.78 ㎉/mole. The addition of small quantities of tetrachloromethane to the reactant stream enhanced the activity of the silica-supported HPMo in the oxidation of methane, whereas water introduced to the reactant decreased the activity of catalyst under present study.

      • The Oxidative Dehydrogenation of Ethane on Silica - Supported Metal - Oxygen Cluster Compounds

        홍성수 ( J. B. Moffat ) 한국공업화학회 1993 한국공업화학회 연구논문 초록집 Vol.1993 No.0

        The Oxidation of hydrocarbons is a subject of considerable industrial importance. While catalytic studies have focused on methane, for reasons of its predominance in natural gas, less work has been reported on ethane. Research on the oxidation of ethane is of value since products such as ethylene and acetaldehyde have applications as precursors to commercial materials. In addition, information on the oxidation of ethane may be useful in understanding other oxidation processes such as involving methane. In present work the partial oxidation of ethane on silica-supported MOCC, 12-molybdophosphoric, 12-molybdosilicic, 12-tungstophosphoric and 12- tungstosphoric acids has been studied. Particular emphasis has been placed on the effect of reaction variables, the rates of reaction and a comparison of N<sub>2</sub>O and O<sub>2</sub> as oxidants with silica-supported HPMo. In addition, the effect of TCM introduced into reactant was examined. As a result, the conversion of ethane and yield of acetaldehyde has maximum values at a loading of 20 wt%. With nitrous oxide as an oxidant, acetaldehyde and ethylene were the principal products, while carbon monoxide and ethylene were main products with oxygen. The reaction orders of C<sub>2</sub>H<sub>6</sub> and N<sub>2</sub>O were 0.8 and 0.6 respectively with nitrous oxide as an oxidant, the orders of C<sub>2</sub>H<sub>6</sub> and N<sub>2</sub>O were 0.7 and 0.4, respectively with oxygen as an oxidant. In addition, the addition of a small amount of TCM has shown the increment of catalytic activity.

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