胜利褐煤水蒸气气化制富氢合成气及其固有矿物质的催化作用

doi:10.3969/j.issn.0438-1157.2013.06.027

化工学报 ›› 2013, Vol. 64 ›› Issue (6): 2092-2102.DOI: 10.3969/j.issn.0438-1157.2013.06.027

• 催化、动力学与反应器 • 上一篇下一篇

胜利褐煤水蒸气气化制富氢合成气及其固有矿物质的催化作用

周晨亮, 刘全生, 李阳, 智科端, 滕英跃, 宋银敏

内蒙古工业大学化工学院,内蒙古工业催化重点实验室,内蒙古呼和浩特 010051

收稿日期:2012-09-10 修回日期:2013-01-05 出版日期:2013-06-05 发布日期:2013-06-05
通讯作者: 刘全生
作者简介:周晨亮(1981—),男,博士研究生。
基金资助:
国家自然科学基金项目(21066008,21266017);高等学校博士学科点专项科研基金项目(20111514110001);内蒙古自然科学基金项目(2009ZD01);内蒙古科技计划项目(20101502);内蒙古工业大学"煤化工特色学科"及内蒙古工业大学科学研究项目(ZS201138)。

Production of hydrogen-rich syngas by steam gasification of Shengli lignite and catalytic effect of inherent minerals

ZHOU Chenliang, LIU Quansheng, LI Yang, ZHI Keduan, TENG Yingyue, SONG Yinmin

School of Chemical Engineering, Inner Mongolia University of Technology, Inner Mongolia Key Laboratory of Industrial Catalysis, Huhhot 010051, Inner Mongolia, China

Received:2012-09-10 Revised:2013-01-05 Online:2013-06-05 Published:2013-06-05
Supported by:
supported by the National Natural Science Foundation of China(21066008,21266017),the Research Fund for the Doctoral Program of Higher Education of China(20111514110001),the Natural Science Foundation Project of Inner Mongolia(2009ZD01),the Science and Technology Plan Project of Inner Mongolia(20101502),the Coal-chemical Engineering Characteristic Specialized Subject of IMUT and Science and Research Project of IMUT(ZS201138).

摘要/Abstract

摘要： 利用微型固定床反应装置,研究了内蒙古胜利褐煤水蒸气气化过程中H₂、CO₂、CO和CH₄生成规律及其固有矿物质的催化效应。原煤(SL-raw)、盐酸洗脱(SL-HCl)、氢氟酸洗脱(SL-HF)及盐酸洗脱液回添煤样(SL-HCl-Re)在水蒸气气化反应过程中,H₂、CO₂和CO生成速率存在明显差异,充分说明胜利褐煤中某些固有的矿物质对其水蒸气气化反应具有显著的催化作用,可大幅度提高其气化反应速率,并使其起始气化温度降低96℃,气化反应主体温度降低150℃以上,同时促进了合成气中H₂生成,抑制了CO的生成,使胜利褐煤水蒸气气化反应过程中一直维持着较高的H₂/CO摩尔比,SL-raw、SL-HCl-Re水蒸气气化所得合成气中H₂/CO摩尔比分别为17.3和4.3,而SL-HCl和SL-HF水蒸气气化所得合成气中H₂/CO摩尔比均只有1.22。SL-HCl和SL-HF水蒸气气化生成H₂、CO₂和CO的规律基本相同,说明起催化作用的物质是可溶解在盐酸洗脱液中的矿物质。经过分析,发现矿物质对胜利褐煤水蒸气气化反应的催化作用主要是通过提高水煤气变换反应(WGSR)速度实现的。最后结合文献报道提出了胜利褐煤水蒸气气化反应过程中矿物质的原位催化机理。

关键词: 胜利褐煤, 水蒸气气化, 固有矿物质, 催化, 富氢合成气

Abstract: The temperature programmed steam gasification and isothermal steam gasification (TPSG and ISG) of Shengli lignite were studied on a fixed-bed micro-reactor equipment.The TPSG results suggested that some inherent minerals effectively improved steam gasification of Shengli lignite.The initial reaction temperature and gas-reaction temperature for steam gasification decreased by about 96℃ and 150℃, respectively, when the mineral elements were retained in the lignite.The minerals in the lignite which were assumed to be catalysts aiding the lignite-steam gasification could be separated with hydrochloric acid.The effect of different acid treatments of the lignite on steam gasification was also studied.The H₂/CO molar ratio in the syngas produced from the steam gasification of raw lignite (SL-raw) and the lignite back- added with HCl eluate (SL-HCl-Re) were as high as 17.3 and 4.3, respectively, but it was only 1.22 for the lignite treated with HCl or HF.It was speculated that the enhanced steam gasification of Shengli lignite could be attributed to the promotion effect of inherent minerals on water-gas shift reaction (WGSR).Finally, the possible in-situ catalytic mechanism of inherent minerals in Shengli lignite for steam gasification reaction was suggested.

Key words: Shengli lignite, steam gasification, inherent minerals, catalytic effect, hydrogen-rich syngas

中图分类号:

TQ54

周晨亮, 刘全生, 李阳, 智科端, 滕英跃, 宋银敏. 胜利褐煤水蒸气气化制富氢合成气及其固有矿物质的催化作用[J]. 化工学报, 2013, 64(6): 2092-2102.

ZHOU Chenliang, LIU Quansheng, LI Yang, ZHI Keduan, TENG Yingyue, SONG Yinmin. Production of hydrogen-rich syngas by steam gasification of Shengli lignite and catalytic effect of inherent minerals[J]. CIESC Journal, 2013, 64(6): 2092-2102.

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胜利褐煤水蒸气气化制富氢合成气及其固有矿物质的催化作用

Production of hydrogen-rich syngas by steam gasification of Shengli lignite and catalytic effect of inherent minerals

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