铁基催化剂对胜利褐煤液化的影响
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摘要
考察了不同温度下,α-FeOOH、FeSO4·7H2O及其混合物对蒙东胜利褐煤液化性能的影响。结果表明:α-FeOOH在450℃时液化转化率达到97.47%,FeSO4·7H2O在425℃时液化转化率达到97.21%;当温度低于400℃时,α-FeOOH和FeSO4·7H2O之间存在协同作用,α-FeOOH和FeSO4·7H2O混合可能生成类似Fe2O3/SO42-超强酸的活性组分,促进煤转化成前沥青烯,同时α-FeOOH的存在促进了前沥青烯向沥青烯和油气转变,提高了油气产率;当温度高于400℃时,α-FeOOH和FeSO4·7H2O混合可能会加剧前沥青烯结焦,导致转化率比α-FeOOH与FeSO4·7H2O单独作催化剂时低。
Effects of synthesized catalysts,α-FeOOH,ferrous sulfated and their mixture,on the liquefaction conversion and oil and gas yield of Shengli lignite from East Inner Mongolia at different temperature were investigated.Results indicated that the conversion of Shengli lignite reached 97.47%at 450℃ withα-FeOOH and 97.21% at 425 ℃ with ferrous sulfated.During the process of liquefaction at temperature lower than 400 ℃,there existed synergistic effect betweenα-FeOOH and ferrous sulfated. The mixture ofα-FeOOH and ferrous sulfated might form one superacid similar with Fe2O3 /SO4 2-which promoted the thermal pyrolysis of coal to preasphaltenes.At the same time,the presence ofα-FeOOH promoted the transformation of preasphaltenes to asphaltenes,oil and gas,and increased the yield of oil and gas.At temperature higher than 400℃,the coking of preasphaltenes was intensified,which led to the lower liquefaction conversion by the mixture ofα-FeOOH and FeSO4 ·7H2O than alone.
Effects of synthesized catalysts,α-FeOOH,ferrous sulfated and their mixture,on the liquefaction conversion and oil and gas yield of Shengli lignite from East Inner Mongolia at different temperature were investigated.Results indicated that the conversion of Shengli lignite reached 97.47%at 450℃ withα-FeOOH and 97.21% at 425 ℃ with ferrous sulfated.During the process of liquefaction at temperature lower than 400 ℃,there existed synergistic effect betweenα-FeOOH and ferrous sulfated. The mixture ofα-FeOOH and ferrous sulfated might form one superacid similar with Fe2O3 /SO4 2-which promoted the thermal pyrolysis of coal to preasphaltenes.At the same time,the presence ofα-FeOOH promoted the transformation of preasphaltenes to asphaltenes,oil and gas,and increased the yield of oil and gas.At temperature higher than 400℃,the coking of preasphaltenes was intensified,which led to the lower liquefaction conversion by the mixture ofα-FeOOH and FeSO4 ·7H2O than alone.
引文
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[18]Liu Z,Yang J,Zondlo J W,et al.In situimpregnated ironbased catalyst for direct coal liquefaction[J].Fuel,1996,75(1):51-57.
[19]张立安,杨建丽,刘振宇,等.硫酸亚铁基催化剂对两种中国烟煤直接液化的催化作用[J].燃料化学学报,1999,27(12):35-36.
[2]朱晓苏.中国煤炭直接液化优选煤种的研究[J].煤化工,1997,25(3):32-39
[3]Bacaud R,Besson M,Djega-Mariadassou G.Development of a new iron catalyst for the direct liquefaction of coal[J].Energy&Fuels,1994,8(1):3-9.
[4]Cebolla V L,Diack M,Oberson M,et al.Effect of various catalysts on the chemical structure of oils and asphaltenes obtained from the hydroliquefaction of a highly volatile bituminous coal[J].Fuel Processing Technology,1991,28(2):183-201.
[5]Hager G T,Compton A L,Givens E N,et al.The effect of promoter metal concentration on the catalytic activity of sulfated hematite for the liquefaction of a subbituminous coal[J].American Chemical Society:Division of Fuel Chemistry,1994,39(1):1083-1087.
[6]Tian Dacheng,Sharma R K,Stiller A H,et al.Direct liquefaction of coal using ferric-sulfide-based,mixed-metal catalysts containing Mg or Mo[J].Fuel,1996,75(6):751-758.
[7]Zhao Jianmin,Zheng Feng,Huggins F E,et al.Binary iron oxide catalysts for direct coal liquefaction[J].Energy&Fuels,1994,8(1),38-43.
[8]Zhu Jisheng,Yang Jianli,Liu Zhenyu,et al.Improvement and characterization of an impregnated iron-based catalyst for direct coal liquefaction[J].Fuel Processing Technology,2001,72(3):199-214.
[9]郭劼蘅,杨建丽,刘振宇.原位担载型铁系煤直接液化催化剂的研究[J].煤炭转化,2000,23(3):53-58.
[10]Kaneko T,Tazawa K,Koyama T,et al.Transformation of iron catalyst to the active phase in coal liquefaction[J].Energy&Fuels,1998,12(5):897-904.
[11]Artoka L,Schobert H H,Davis A.Temperature-staged liquefaction of coals impregnated with ferrous sulfate[J].Fuel Process Technology,1992,32(1-2):87-100.
[12]Yokoyama S,Yamamoto M,Yoshida R,et al.Catalytic behaviour of sulphate and sulphide in S-promoted iron oxide catalysts for liquefaction of bituminous coal and lignite[J].Fuel,1991,70(2):163-168.
[13]Gaboriaud F,Ehrhardt J.Effects of different crystal faces on the surface charge of colloidal goethite(α-FeOOH)particles[J].Geochimica et Cosmochimica Acta,2003,67(5):967-983.
[14]水恒福,刘健龙,王知彩,等.小龙潭褐煤不同气氛下液化性能的研究[J].燃料化学学报,2009,37(3):257-261.
[15]穆平,杨正宇,赵良,等.七水合硫酸亚铁热分解及脱水非等温动力学研究[J].河北师范大学学报,1997,21(2):164-167.
[16]Prahan V R,Hu J,Tierney J W,et al.Sulfated and molybdated Iron(Ⅲ)oxide catalysts in coal liquefaction[J].American Chemical Society,Division of Fuel Chemistry,1993,38(2):8-13.
[17]Kotanigama T,Yanamoto M,Sasaki M,et al.Active site of iron-based catalyst in coal liquefaction[J].Energy&Fuels,1997,11(1):190-193.
[18]Liu Z,Yang J,Zondlo J W,et al.In situimpregnated ironbased catalyst for direct coal liquefaction[J].Fuel,1996,75(1):51-57.
[19]张立安,杨建丽,刘振宇,等.硫酸亚铁基催化剂对两种中国烟煤直接液化的催化作用[J].燃料化学学报,1999,27(12):35-36.