留言板

尊敬的读者、作者、审稿人, 关于本刊的投稿、审稿、编辑和出版的任何问题, 您可以本页添加留言。我们将尽快给您答复。谢谢您的支持!

姓名
邮箱
手机号码
标题
留言内容
验证码

褐煤半焦直接加氢制甲烷反应特性及其孔结构和表面形态变化

张天开 张永发 王琪 张静 丁晓阔

张天开, 张永发, 王琪, 张静, 丁晓阔. 褐煤半焦直接加氢制甲烷反应特性及其孔结构和表面形态变化[J]. 燃料化学学报(中英文), 2015, 43(03): 289-301.
引用本文: 张天开, 张永发, 王琪, 张静, 丁晓阔. 褐煤半焦直接加氢制甲烷反应特性及其孔结构和表面形态变化[J]. 燃料化学学报(中英文), 2015, 43(03): 289-301.
ZHANG Tian-kai, ZHANG Yong-fa, WANG Qi, ZHANG Jing, DING Xiao-kuo. Hydrogasification of lignite semicoke to produce methane and the textural properties of coke residues[J]. Journal of Fuel Chemistry and Technology, 2015, 43(03): 289-301.
Citation: ZHANG Tian-kai, ZHANG Yong-fa, WANG Qi, ZHANG Jing, DING Xiao-kuo. Hydrogasification of lignite semicoke to produce methane and the textural properties of coke residues[J]. Journal of Fuel Chemistry and Technology, 2015, 43(03): 289-301.

褐煤半焦直接加氢制甲烷反应特性及其孔结构和表面形态变化

基金项目: 国家重点基础研究发展规划(973计划, 2012CB723105)。
详细信息
    通讯作者:

    张永发,教授,Tel/Fax:0351-6018676,E-mail:yongfaz@tyut.edu.cn。

  • 中图分类号: TQ541

Hydrogasification of lignite semicoke to produce methane and the textural properties of coke residues

  • 摘要: 在高温高压(1 000 ℃、12 MPa)固定床反应器上对内蒙古褐煤半焦的加氢甲烷化反应特性进行了研究,采用氮吸附和扫描电镜(SEM)对甲烷化残渣比表面积、孔结构和表面形态进行了表征。结果表明,半焦加氢甲烷化可分为加氢热解、快速加氢和慢速加氢等三个反应阶段,每阶段分别发生含氧官能团和烷基侧链加氢反应、芳环结构加氢反应以及贫氢骨架碳结构加氢反应。半焦加氢甲烷化最优反应温度为800 ℃,反应压力为3.0~4.0 MPa;提高升温速率可以缩短前段(碳转化率低于46%)反应过程时间,对后段(碳转化率高于46%)反应过程影响较小。半焦甲烷化残渣的吸附-脱附等温线呈反S型,滞后环呈H3回线形状;在甲烷化反应过程中,半焦平均孔径先减小后增大,总孔容积和介孔容积逐渐增大,微孔容积和比表面积先增大后减小。
  • 杨允明, 沙兴中, 任德庆. 煤的加氢气化研究[J]. 煤炭转化, 1992, 15(1): 60-67.(YANG Yun-ming, SHA Xing-zhong, REN De-qing. Study of hydrogasification of coal[J]. Coal Convers, 1992, 15(1): 60-67.)
    杨允明, 沙兴中, 任德庆. 煤和煤焦在压力下加氢气化的动力学研究I. 温度的影响[J]. 华东化工学院学报, 1988, 14(4): 500-504.(YANG Yun-ming, SHA Xing-zhong, REN De-qing. Kinetics of hydrogasification of coal and char at pressure I. Influence of temperature[J]. J East Chin Inst Chem Technol, 1988, 14(4): 500-504.)
    马智华, 王欣荣, 朱子彬, 唐黎华, 倪燕慧, 张成芳. 烟煤快速加氢热解的研究Ⅱ. 温度和压力影响的考察[J]. 燃料化学学报, 1996, 24(5): 40-44.(MA Zhi-hua, WANG Xin-rong, ZHU Zi-bin, TANG Li-hua, NI Yan-hui, ZHANG Cheng-fang. Study on flash hydropyrolysis of bituminous coal Ⅱ. Effect of temperature and pressure[J]. J Fuel Chem Technol, 1996, 24(5): 40-44.)
    刘保林, 崔彦亭, 何伯述. 加氢气化炉内化学反应的热力学研究[J]. 洁净煤技术, 2006, 12(2): 67-71.(LIU Bao-lin, CUI Yan-ting, HE Bo-shu. Thermodynamic based analysis of the chemical reactions in a hydrogasifier[J]. Clean Coal Technol, 2006, 12(2): 67-71.)
    WANG S C, BAEK H I, JANG H T. Hydrogasification of various carbonaceous sources using pressure change properties[J]. Korean J Chem Eng, 2007, 24(3): 532-536.
    战书鹏, 王兴军, 洪冰清, 于广锁, 王辅臣. 褐煤催化加氢气化实验研究[J]. 燃料化学学报, 2012, 40(1): 8-14.(ZHAN Shu-peng, WANG Xing-jun, HONG Bing-qing, YU Guang-suo, WANG Fu-chen. Experimental study on catalytic hydrogasification of lignite[J]. J Fuel Chem Technol, 2012, 40(1): 8-14.)
    LEE S H, LEE J G, KIM J H, CHOI Y C. Hydrogasification characteristics of bituminous coals in an entrained-flow hydrogasifier[J]. Fuel, 2006, 85(5): 803-806.
    YASUDA H, YAMADA O, ZHANG A, NAKANO K, KAIHO M. Hydrogasification of coal and polyethylene mixture[J]. Fuel, 2004, 83(17): 2251-2254.
    GONZLEZ J F, RAMIRO A, SABIO E, ENCINAR J M, GONZALEZ C M. Hydrogasification of almond shell chars. Influence of operating variables and kinetic study[J]. Ind Eng Chem Res, 2002, 41(15): 3557-3565.
    YASUDA H, YAMADA O, KAIHO M, NAKAGOME H. Effect of polyethylene addition to coal on hydrogasification enhancement[J]. J Mater Cycles Waste Manage, 2014, 16(1): 151-155.
    ZHOU Y, ZHENG Y, WANG W X, ZHENG C G. An experimental investigation on hydrogasification of coal chars in a fixed bed reactor under high pressure[J]. Adv Mater Res, 2012, 524: 863-870.
    JEON S K, PARK C S, HACKETT C E, NORBECK J M. Characteristics of steam hydrogasification of wood using a micro-batch reactor[J]. Fuel, 2007, 86(17): 2817-2823.
    TOMITA A, MAHAJAN O P, WALKER P L. Reactivity of heat-treated coals in hydrogen[J]. Fuel, 1977, 56(2): 137-144.
    ZHANG J, DING H R, WANG J. Methane production by hydrogenation of low-rank coal in a fixed-bed reactor[J]. Pittsburgh, 2013, 30(2): 1186-1191.
    杨景标, 郑炯. 微观结构对煤焦气化反应性的影响[J]. 化学工程与装备, 2009, 5: 33-37.(YANG Jing-biao, ZHENG Jiong. Effect of microstructure on coke gasification reactivity[J]. Chem Eng Equipm, 2009, 5: 33-37.)
    TAKARADA T, TAMAI Y, TOMITA A. Reactivities of 34 coals under steam gasification[J]. Fuel, 1985, 64(10): 1438-1442.
    BLACKWOOD J D. The reaction of carbon with hydrogen at high pressure[J]. Aust J Chem, 1959, 12(1): 14-28.
    KARCZ A, PORADA S. The influence of coal rank on formation of gaseous hydrocarbons in hydrogasification of coal[J]. Fuel, 1996, 75(5): 641-645.
    SCHRADER L, 杨继涛. 煤的加氢气化[J]. 煤炭转化, 1981, 4: 64-74.(SCHRADER L, YANG Ji-tao. Coal hydrogasification[J]. Coal Convers, 1981, 4: 64-74.)
    张永发, 张天开, 丁晓阔, 徐英, 陈磊, 李香兰. 一种低阶煤制甲烷工艺: 中国, 102911756A[P]. 2013-02-06.(ZHANG Yong-fa, ZHANG Tian-kai, DING Xiao-kuo, XU Ying, CHEN Lei, LI Xiang-lan. Process for producing methane from low-rank coal: CN, 102911756A[P]. 2013-02-06.)
    张永发, 陈磊, 武云霞, 唐健, 丁晓阔, 张天开, 孙亚玲. 一种载热气体用于煤的热解装置: 中国, 102911677A[P]. 2013-02-06.(ZHANG Yong-fa, CHEN Lei, WU Yun-xia, TANG Jian, DING Xiao-kuo, ZHANG Tian-kai, SUN Ya-ling. A gas heating apparatus for the pyrolysis of coal: CN, 102911677A[P]. 2013-02-06.)
    张永发, 王影, 丁晓阔, 张国杰, 孙亚玲. 一种制备甲烷化炭材料的方法: 中国, 102676190A[P]. 2012-09-19.(ZHANG Yong-fa, WANG Ying, DING Xiao-kuo, ZHANG Guo-jie, SUN Ya-ling. A method for the preparation of methane carbon material: CN, 102676190A[P]. 2012-09-19.)
    董跃, 张丙模, 赵文军, 王莉萍, 张国杰, 张永发. 煤制甲烷小型高温高压反应器的研究和开发[J]. 煤炭转化, 2010, 33(2): 64-67+71.(DONG Yue, ZHANG Bing-mu, ZHAO Wen-jun, WANG Li-ping, ZHANG Guo-jie, ZHANG Yong-fa. Research and development of a small-scale high-temperature and high-pressure reactor for coal methanation[J]. Coal Convers, 2010, 33(2): 64-67+71.)
    DING X K, ZHANG Y F, ZHANG T K, TANG J, XU Y, ZHANG J. Effect of operational variables on the hydrogasification of Inner Mongolian lignite semicoke[J]. Energy Fuels, 2013, 27(8): 4589-4597.
    孙庆雷, 王晓, 刘建华, 程传格, 李文, 李保庆. 煤加氢气化过程热力学研究[J]. 山东科技大学学报(自然科学版), 2004, 23(4): 27-29+38.(SUN Qing-lei, WANG Xiao, LIU Jian-hua, CHENG Chuan-ge, LI Wen, LI Bao-qing. The thermodynamic study on hydrogasification process of coal[J]. J Shandong Univ Sci Technol (Nat Sci), 2004, 23(4): 27-29+38.)
    李保庆. 煤加氢热解研究: I 宁夏灵武煤加氢热解的研究[J]. 燃料化学学报, 1995, 23(1): 57-61.(LI Bao-qing. Hydropyrolysis of Chinese coals: I Hydropyrolysis of Lingwu bituminous coal[J]. J Fuel Chem Technol, 1995, 23(1): 57-61.)
    徐泽夕, 吴晋沪, 王洋, 张东柯. 甲烷在褐煤煤焦上的裂解反应研究[J]. 燃料化学学报, 2009, 37(3): 277-281.(XU Ze-xi, WU Jin-hu, WANG Yang, ZHANG Dong-ke. Methane cracking over lignite char[J]. J Fuel Chem Technol, 2009, 37(3): 277-281.)
    CYPRES R, BETTENS B. La formation de la plupart des composes aromatiques produits lors de la pyrolyse du phenol, ne fait pas intervenir le carbone porteur de la function hydroxyle[J]. Tetrahedron, 1975, 31(4): 359-365.
    李保庆. 我国煤加氢热解研究II. 先锋褐煤加氢及催化加氢热解的热重研究[J]. 燃料化学学报, 1995, 23(2): 186-191.(LI Bao-qing. Hydropyrolysis of Chinese coals II. Thermogravimetric study on catalytic and non-catalytic hydropyrolysis of xianfeng lignite[J]. J Fuel Chem Technol, 1995, 23(2): 186-191.)
    步学明, 于涌年, 逄进. 煤炭加氢气化的研究[J]. 煤气与热力, 1989, 5: 4-11+2.(BU Xue-ming, YU Yong-nian, PANG Jin. The study of coal hydrogasification[J]. Gas Heat, 1989, 5: 4-11+2.)
    杨允明, 沙兴中, 任德庆. 煤和煤焦压力下加氢气化动力学的研究[J]. 煤气与热力, 1989, 4: 4-10+2.(YANG Yun-ming, SHA Xing-zhong, REN De-qing. Research hydrogenation of coal and coal char gasification kinetics under pressure[J]. Gas Heat, 1989, 4: 4-10+2.)
    MISIRLIOGLU Z, CANEL M, SINAG A. Hydrogasification of chars under high pressures[J]. Energy Convers Manage, 2007, 48(1): 52-58.
    徐英, 张永发, 张国杰, 陈磊, 李香兰. 褐煤低温热解气生成特性的研究[J]. 太原理工大学学报, 2013, 44(4): 414-416+421.(XU Ying, ZHANG Yong-fa, ZHANG Guo-jie, CHEN Lei, LI Xiang-lan. The pyrolysis gas properties from lignite[J]. J Taiyuan Univ Technol, 2013, 44(4): 414-416+421.)
    BAKER D C. Lignite hydrogasification kinetics[D]. Lubbock: Texas Tech University, 1984.
    GAN H, NANDI S P, WALKER P L Jr. Nature of the porosity in American coals[J]. Fuel, 1972, 51(4): 272-277.
  • 加载中
计量
  • 文章访问数:  400
  • HTML全文浏览量:  14
  • PDF下载量:  488
  • 被引次数: 0
出版历程
  • 收稿日期:  2014-08-07
  • 刊出日期:  2015-03-30

目录

    /

    返回文章
    返回