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      • KCI등재

        Promotional effects of Sm2O3 on Mn-H4SiW12O40/SiO2 catalyst for dimethyl ether direct-oxidation to dimethoxymethane

        Qingde Zhang,Yizhuo Han,Yisheng Tan,Guangbo Liu,Caihong Yang 한국공업화학회 2014 Journal of Industrial and Engineering Chemistry Vol.20 No.4

        The promotional effects of Sm2O3 on Mn-H4SiW12O40/SiO2 for dimethyl ether (DME) direct-oxidation to dimethoxymethane (DMM) were investigated. The results showed that Sm2O3 introduction could significantly improve the activity of Mn-H4SiW12O40/SiO2 for DMM formation, and DMM selectivity was remarkably increased from 36.3% to 60.3% when the Sm2O3 content was 1%. The catalysts were characterized by ICP-AES, XRD, NH3-TPD, Pyridine-IR and XPS. The Sm2O3 introduction enhanced the number of Lewis acid sites and weak acid sites and also increased the amount of Mn4+ species of Mn-H4SiW12O40/SiO2, which is favorable for the formation of DMM.

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        Water-gas shift coupling with methanation over MO_x modified nanorod-NiO/γ-Al_2O_3 catalysts

        Shengli Ma,Yizhuo Han,Yisheng Tan 한국공업화학회 2011 Journal of Industrial and Engineering Chemistry Vol.17 No.4

        Water-gas shift coupling with methanation was carried out over metal oxide modified nanorod-NiO/γ-Al_2O_3 catalysts prepared by grind-mixing method in a continuous flow type fixed-bed reactor. The effects of promoter type, Co_3O_4 content, and reaction pressure were investigated. From the experimental results, Co_3O_4 modified nanorod-NiO/g-Al_2O_3 catalyst exhibited better activity than NiO–CuO/g-Al_2O_3and NiO–Fe_2O_3/g-Al_2O_3 with molar ratio of CO/H_2/H_2O = 3:1:1 at 593 K and atmospheric pressure. The addition of 10 wt%Co_3O_4 to nanorod-NiO/γ-Al_2O_3 catalyst was optimum. The CO conversion of 50 wt%NiO–10 wt%Co_3O_4/γ-Al_2O_3 catalyst was 7.8% and the CH_4 selectivity reached 83.2%. The NiO–MO_x/γ-Al_2O_3 catalysts were analyzed by X-ray diffraction, temperature programmed reduction and thermogravimetry techniques.

      • KCI등재

        The mechanism of higher alcohol formation on ZrO2-based catalyst from syngas

        Yingquan Wu,Hongjuan Xie,Yongli Kou,Noritatsu Tsubaki,Yizhuo Han,Yisheng Tan 한국화학공학회 2015 Korean Journal of Chemical Engineering Vol.32 No.3

        A chain growth scheme for the synthesis of alcohols from carbon monoxide and hydrogen is proposedbased on the chemical enrichment method on ZrO2-based catalyst. Methanol addition has no obvious effect on theSTY of C2+ alcohols, indicating that COH→CCOH is a slow initial growth step. Addition of ethanol and propanols canenhance the STY of isobutanol, especially n-propanol, revealing that n-propanol is largely the precursor of isobutanol. Results of large alcohols addition further reveal the relationship between small alcohols and large alcohols of formation. Also, addition of aldehydes has a similar effect on the formation of higher alcohols, indicating that alcohols existin the form of aldehydes before desorption. Anisole are introduced into syngas for confirmation of predicted intermediatesand the result indicates that formyl species is participated both in the formation of methanol and higher alcohols. Reaction temperature has a significant effect on the chain growth of alcohols synthesis. Under low temperature,chain growth occurs with CO insertion and alcohols are linear products. Isobutanol appears and becomes the mainproduct during C2+ alcohols undergo an aldo-condensation reaction at high temperature.

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