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Qingde Zhang,Yisheng Tan,Caihong Yang,Hongjuan Xie 한국공업화학회 2013 Journal of Industrial and Engineering Chemistry Vol.19 No.3
The conversion of syngas to aromatics via dimethyl ether was investigated over MnCl2 modified HZSM-5zeolites. The results demonstrated that 2%MnCl2 modified HZSM-5 (SiO2/Al2O3 = 38) exhibited higher pxylene selectivity than other catalysts and further decreased 1,2,4,5-tetramethylbenzene selectivity. The CO conversion was obviously increased after 5%MnCl2 modification to HZSM-5. The catalysts were characterized by XRD, BET, XPS, FT-IR, NH3-TPD, SEM, element analysis and O2-TPO. The loading amount of MnCl2 affected the adsorption and reaction of DME molecules on zeolites. Appropriate amount of MnCl2 introduction could adjust the acidity and pore volume of HZSM-5 to increase p-xylene selectivity and CO conversion.
Synthesis of light olefins from syngas over Fe–Mn–V–K catalysts in the slurry phase
Gencun Wang,Yisheng Tan,Kan Zhang,Ping Liu,Haitao Hui 한국공업화학회 2013 Journal of Industrial and Engineering Chemistry Vol.19 No.3
Fe–Mn–V–K catalysts for the synthesis of light olefins from CO hydrogenation were prepared by a specially controlled degradation method. The effect of the V content on the structure and the catalytic performance of the catalysts were investigated in a continuously stirred tank slurry reactor. Mo¨ssbauer spectra (MES) results show that the incorporation of V with appropriate contents can improve the dispersion of the a-Fe2O3 phase. CO hydrogenation results indicate that a small addition of V can improve the product distribution. The addition can also increase the selectivity to light olefins by inhibiting the secondary hydrogenation reaction of the initial olefin. The best catalytic performance was obtained at the Fe/Mn/V molar ratio of 3/1/0.2. The total C2–C4 content in all hydrocarbons and O/P in the C2–C4 fraction were 49.15 wt% and 3.95, respectively.
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.
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.
Zhenmin Liu,Junwei Wang,Mao-qing Kang,Ning Yin,Xin-kui Wang,Yisheng Tan,Yulei Zhu 한국공업화학회 2015 Journal of Industrial and Engineering Chemistry Vol.21 No.1
MgAl hydrotalcite synthesized via co-precipitation method from magnesium and aluminum nitrateswas calcined to produce Mg4AlO5.5 mixed oxides. The oxides were modified by introducing LiNO3 andapplied to the synthesis of glycerol carbonate from glycerol and dimethyl carbonate. The research resultsindicated that LiNO3/Mg4AlO5.5 was an efficient catalyst for the synthesis of glycerol carbonate. The fullconversion of glycerol and 96.28% yield of glycerol carbonate were obtained after reacting at 80 8C for1.5 h in the presence of LiNO3/Mg4AlO5.5. The structure and properties of the catalysts were studied bymeans of XRD, TGA, BET, CO2-TPD and Hammett indicator method. It was found that the basic strengthand the basicity of the catalysts were enhanced after addition of LiNO3. Over Mg4AlO5.5 oxides, LiNO3 waseasily converted to LiAlO2 which constituted new strong basic sites. Too high basic strength and basicityof catalysts may improve the conversion of glycerol at the cost of GC selectivity reduction.
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.
Zixiang Cui,Jie Fan,Huijuan Duan,Junfeng Zhang,Yongqiang Xue,Yisheng Tan 한국화학공학회 2017 Korean Journal of Chemical Engineering Vol.34 No.1
Nano-CeO2 was prepared through the calcination of Ce(OH)3 precursor in different atmospheres (H2, Ar, air, O2), which was prepared by a hydrothermal method, and then used as catalysts in the direct synthesis of dimethyl carbonate (DMC) from methanol and CO2. The results indicated that the catalyst calcined in O2 (CeO2-O2) showed an optimum catalytic performance, and the yield of DMC reached to 1.304mmol/mmolcat. In addition, reaction temperature and weight of catalyst were optimized. Based on characterizations of the catalysts, the ratio of Ce(IV)/Ce(III) and Lewis acid-base property of nano-CeO2 catalyst could be adjusted through different calcination atmosphere treatment. It was determined that the higher activity of CeO2-O2 catalyst is mainly attributed to its higher ratio of Ce(IV)/Ce(III) as well as abundant and moderate intensity Lewis acid base sites.