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

酸洗脱矿对胜利褐煤热解过程中N迁移转化的影响

王永刚,  郑盼盼,  杨萨莎,  张书,  白艳萍,  贾晓路

downloadPDF
文章导航 > 燃料化学学报（中英文）  > 2014 >  42(05): 519-526
王永刚, 郑盼盼, 杨萨莎, 张书, 白艳萍, 贾晓路. 酸洗脱矿对胜利褐煤热解过程中N迁移转化的影响[J]. 燃料化学学报（中英文）, 2014, 42(05): 519-526.
引用本文: 王永刚, 郑盼盼, 杨萨莎, 张书, 白艳萍, 贾晓路. 酸洗脱矿对胜利褐煤热解过程中N迁移转化的影响[J]. 燃料化学学报（中英文）, 2014, 42(05): 519-526.
shu
WANG Yong-gang, ZHENG Pan-pan, YANG Sa-sha, ZHANG Shu, BAI Yan-ping, JIA Xiao-lu. Influence of demineralization using acid wash on N migration and transformation during pyrolysis of Shengli brown coal[J]. Journal of Fuel Chemistry and Technology, 2014, 42(05): 519-526.
Citation: WANG Yong-gang, ZHENG Pan-pan, YANG Sa-sha, ZHANG Shu, BAI Yan-ping, JIA Xiao-lu. Influence of demineralization using acid wash on N migration and transformation during pyrolysis of Shengli brown coal[J]. Journal of Fuel Chemistry and Technology, 2014, 42(05): 519-526.
shu

酸洗脱矿对胜利褐煤热解过程中N迁移转化的影响

  • 中国矿业大学(北京) 化学与环境工程学院, 北京 100083

基金项目: 国家科技支撑计划 （2012BAA04B02）。
详细信息
    通讯作者:

    王永刚，Tel：010-62339882，E-mail：wyg1960@126.com; 张书，Tel：010-62331048，E-mail：zhangshuwo@hotmail.com。

  • 中图分类号: TQ541

Influence of demineralization using acid wash on N migration and transformation during pyrolysis of Shengli brown coal

  • School of Chemical and Environmental Engineering, China University of Mining and Technology (Beijing), Beijing 100083, China

    摘要
  • 摘要: 在石英管流化床反应器中对胜利褐煤进行快速热解实验，考察了773~1 173 K下酸洗脱矿对胜利褐煤热解过程中N迁移转化规律的影响。通过比较原煤和酸洗后煤中N的不同逸出规律可以得出，影响酸洗前后胜利褐煤热解过程中N迁移转化规律的主要是碱金属Na及碱土金属Ca；热解过程中，煤中的Na和Ca促使煤中的N向NH3转化并有效抑制了HCN的生成，金属离子的存在对催化焦油N转化为NH3的作用较为明显；原煤中的碱金属和碱土金属的赋存使半焦裂解反应加剧，降低了固体半焦的产率，半焦N的产率也随之减少；与原煤相比，酸洗煤热解半焦中的吡啶型N（N-6）含量较多，而吡咯型N（N-5）和季N（N-Q）相对较少。
    Abstract: This paper is to examine effects of inherent minerals in coal on N migration and transformation during the fast pyrolysis of Shengli brown coal at the temperatures of 773~1 173 K in a bench-scale fluidized-bed quartz reactor. Based on the comparison between raw coal and acid-washed coal, we can find that the alkali Na and alkaline Ca were the key reasons for the difference in N evolutions from raw coal and demineralized coal during the pyrolysis. The Na and Ca could efficiently facilitate the formation of NH3 and inhibit the production of HCN. The metallic species had obvious catalytic effects for the conversion from tar-N to NH3. Meantime, the existence of alkali and alkaline metals has enhanced the cracking reactions of coal char, thus reducing the yields of char and char-N. In addition, the relative amount of pyridinic(N-6) in demineralized coal char was higher than that in raw coal, while less quternary type nitrogen (N-Q) and pyrrolic nitrogen(N-5) were found in the demineralized coal char.
    • HTML全文
    • 参考文献(38)
  • 刘振宇. 煤炭能源中的化学问题[J]. 化学进展, 2000, 12(4): 458-462. (LIU Zhen-yu. Chemistry in coal energy[J]. Progress in Chemistry, 2000, 12(4): 458-462.)
    尤先锋, 刘生玉, 吴争鸣, 任军, 谢克昌. 煤热解过程中氮和硫化合物分配及生成机理[J]. 煤炭转化, 2001, 24(3): 1-5. (YOU Xian-feng, LIU Sheng-yu, WU Zheng-ming, REN Jun, XIE Ke-chang. Study of nitrogen and sulfur distribution and functional forms during coal pyrolysis[J]. Coal Conversion, 2001, 24(3): 1-5.)
    冯志华, 常丽萍, 任军, 谢克昌. 煤热解过程中氮的分配及存在状态的研究进展[J]. 煤炭转化, 2000, 23(3): 6-12. (FENG Zhi-hua, CHANG Li-ping, REN Jun, XIE Ke-chang. Study of nitrogen distribution and functional forms during coal pyrolysis[J]. Coal Conversion, 2000, 23(3): 6-12.)
    WU Z, SUGIMOTO Y, KAWASHIMA H. Effect of demineralization and catalyst addition on N2 formation during coal pyrolysis and on char gasification[J]. Fuel, 2003, 82(15/17): 2057-2064.
    TSUBOUCHI N, OHTSUKA Y. Formation of N2 during pyrolysis of Ca-loaded coals[J]. Fuel, 2002, 81(11/12): 1423-1431.
    OHTSUKA Y, WU Z, EDWARD F. Effect of alkali and alkaline metals on nitrogen release during temperature programmed pyrolysis of coal[J]. Fuel, 1997, 76(14/15): 1361-1367.
    TSHBOUCHI N, OHTSUKA Y. Nitrogen release during high temperature pyrolysis of coals and catalytic role of calcium in N2 formation[J]. Fuel, 2002, 81(18): 2335-2342.
    WU Z H. The influence of mineral matter and catalyst on nitrogen release during slow pyrolysis of coal and related material: A comparative study[J]. Energy Fuels, 2002, 16(2): 451-456.
    FRIEBEL J, KOPSEL R F. The fate of nitrogen during pyrolysis of German low rank coals-A parameter study[J]. Fuel, 1999, 78(8): 923-932.
    赵娅鸿, 常丽萍, 谢克昌, 李灵芝. 矿物质对煤转化过程中含氮物迁移的影响[J]. 现代化工, 2004, 24(1): 11-15. (ZHAO Ya-hong, CHANG Li-ping, XIE Ke-chang, LI Ling-zhi. Effect of mineral matter on transformation of nitrogen during coal conversion[J]. Modern Chemical Industry, 2004, 24(1): 11-15.)
    常丽萍, 赵娅鸿. 煤中固有矿物质在热解过程中对氮释放的影响[J]. 煤炭转化, 2005, 28(2): 36-38. (CHANG Li-ping, ZHAO Ya-hong. Influence of inherent minerals on nitrogen release during coal pyrolysis[J]. Coal Conversion, 2005, 28(2): 36-38.)
    赵娅鸿, 林建英, 常丽萍, 赵炜, 谢克昌. 矿物质对煤热解气化过程中NH3形成的影响[J]. 环境化学, 2004, 23(1): 26-30. (ZHAO Ya-hong, LIN Jian-ying, CHANG Li-ping, ZHAO Wei, XIE Ke-chang. The effect of mineral matter on the NH3 formation during coal pyrolysis and gasification[J]. Environmental Chemistry, 2004, 23(1): 26-30.)
    赵娅鸿. 矿物质对煤热解/气化过程中氮迁移的影响[D]. 太原: 太原理工大学, 2003. (ZHAO Ya-hong. Effect of minerals on transformation of nitrogen during coal pyrolysis/gasification[D]. Taiyuan: Taiyuan University of Technology, 2003.)
    徐明艳, 崔银萍, 秦玲丽, 常丽萍, 谢克昌. 含铁煤热解过程中HCN形成的主要影响因素分析[J]. 燃料化学学报, 2007, 35(1): 5-9. (XU Ming-yan, CUI Yin-ping, QIN Ling-li, CHANG Li-ping, XIE Ke-chang. Key factors influencing the release and formation of HCN during iron-containing coal pyrolysis[J]. Journal of Fuel Chemistry and Technology, 2007, 35(1): 5-9.)
    徐秀峰, 顾永达, 陈诵英. 铁催化剂对煤热解过程中氮元素迁移的影响[J]. 燃料化学学报, 1998, 26(1): 18-23. (XU Xiu-feng, GU Yong-da, CHEN Song-ying. Effect of iron addition on transformation of nitrogen during coal pyrolysis[J]. Journal of Fuel Chemistry and Technology, 1998, 26(1): 18-23.)
    LI C Z. Some recent advances in the understanding of the pyrolysis and gasification behavior of Victorian brown coal[J]. Fuel, 2007, 86(12): 1664-1683.
    WOOD B J, SANCIER K M. The mechanism of the catalytic gasification of coal char: A critical review[J]. Catal Rev Sci Eng, 1984, 26(2): 233-279.
    VERNAGLIA B A, WORNAT M J, LI C Z, NELSON P F. The effects of pyrolysis temperature and ion-exchanged metals on the composition of brown coal tars produced in a fluidized-bed reactor[C]//Symposium (International) on Combustion. Amsterdam: Elsevier Press, 1996, 26(2): 3287-3294.
    LI C Z. Advances in the science of Victorian brown coal[M]. Access Online via Elsevier, 2004: 286-350.
    赵明举, 谢克昌, 凌大琦. 煤中矿物质在煤气化中的应用[J]. 煤炭转化, 1989, 1: 23-29. (ZHAO Ming-ju, XIE Ke-chang, LING Da-qi. The application of the minerals in coal during coal gasification[J]. Coal Conversion, 1989, 1: 23-29.)
    王磊, 余江, 尹丰魁, 王冬梅. 钙元素对褐煤热解和气化特性的影响[J]. 煤化工, 2012, (1): 27-30. (WANG Lei, YU Jiang, YIN Feng-kui, WANG Dong-mei. Impact of calcium on pyrolysis and gasification characteristics of brown coal[J]. Coal Chemical Industry, 2012, (1): 27-30.)
    ZHANG S, LI C Z. Volatilization and catalytic effects of alkali and alkaline earth metallic species during the cytolysis and gasification of Victorian brown coal. Part IX. Effects of volatile-char interactions on char-H2O and char-O2 reactivates[J]. Fuel, 2011, 90(4): 1655-1661.
    张书, 白艳萍, 郑盼盼, 陈绪军, 许德平, 王永刚. 升温速率对胜利褐煤热解过程中N迁移转化的影响[J]. 燃料化学学报, 2013, 41(10): 1153-1159. (ZHANG Shu, BAI Yan-ping, ZHENG Pan-pan, CHEN Xu-jun, XU De-ping, WANG Yong-gang. Effect of heating rate on the migration and transformation of N during pyrolysis of Shengli brown coal[J]. Journal of Fuel Chemistry and Technology, 2013, 41(10): 1153-1159.)
    秦玲丽, 崔银萍, 徐明艳, 常丽萍. 煤氮催化转化研究中的主要影响因素分析[J]. 现代化工, 2006, 26(2): 382-385. (QIN Ling-li, CUI Yin-ping, XU Ming-yan, CHANG Li-ping. Main influencing factors in the research on catalytic conversion of coal-nitrogen[J]. Modern Chemical Industry, 2006, 26(2): 382-385.)
    LI C Z, LI L T. Formation of NOx and SOx precursors during the cytolysis of coal and biomass. Part Ⅲ. Further discussion on the formation of HCN and NH3 during cytolysis[J]. Fuel, 2002, 79(15): 1899-1906.
    朱廷钰, 汤忠, 黄戒介, 张建民, 王洋. 煤温和气化特性的热重研究[J]. 燃料化学学报, 1999, 27(5): 420-423. (ZHU Ting-yu, TANG Zhong, HUANG Jie-jie, ZHANG Jian-min, WANG Yang. Thermo-gravimetric study of coal mild gasification[J]. Journal of Fuel Chemistry and Technology, 1999, 27(5): 420-423.)
    QUYN D M, WU H, HAYASHI J, LI C Z. Volatilisation and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal. Part IV. Catalytic effects of NaCl and ion-exchangeable Na in coal on char reactivity[J]. Fuel, 2003, 82(5): 587-593.
    TSUBOUCHI N, OHTSUKA Y. Nitrogen chemistry in coal cytolysis: Catalytic roles of metal captions in secondary reactions of volatile nitrogen and char nitrogen[J]. Fuel Process Technol, 2008, 89(4): 379-390.
    SATHE C, PANG Y, LI C Z. Effects of heating rate and ion-exchangeable captions on the pyrolysis yields from a Victorian brown coal[J]. Energy Fuels, 1999, 13(3): 748-755.
    QUYN D M, WU H, LI C Z. Volatilization and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal. Part I. Volatilization of Na and Cl from a set of NaCl-loaded samples[J]. Fuel, 2002, 81(2): 143-149.
    赵新法, 杨黎燕, 石振海. 煤中矿物质在气化反应中的催化作用分析[J]. 煤炭技术, 2005, 24(1): 103-105. (ZHAO Xin-fa, YANG Li-yan, SHI Zhen-hai. Analysis on catalysis of mineral in coal gasification[J]. Coal Technology, 2005, 24(1): 103-105.)
    XIE J J, YANG X M, LV X S, DING T L, YAO J Z, LIN W G. Progress on transformation behavior of sulfur and nitrogen during coal pyrolysis[J]. Chem Ind Eng Prog, 2004, 23(11): 1214-1218.
    闫晓, 车得福, 徐通模. 煤热解过程中焦炭氮变化规律的实验研究[J]. 西安交通大学学报, 2004, 38(9): 980-984. (YAN Xiao, CHE De-fu, XU Tong-mo. Experimental investigation on char nitrogen conversion during coal pyrolysis[J]. Journal of Xi'an Jiaotong University, 2004, 38(9): 980-984.)
    WU Z, SUGIMOTO Y, KAWASHIMA H. The influence of mineral matter and catalyst on nitrogen release during slow cytolysis of coal and related material: A comparative study[J]. Energy Fuels, 2002, 16(2): 451-456.
    KAPTEIGIN F, MOULIGIN J A, MATZNER S, BOEHMB H P. The development of nitrogen functionality in model chars during gasification in CO2 and O2[J]. Carbon, 1999, 37(7): 1143-1150.
    SCHMIERS H, FRIEBEL J, STREUBEL P, HESSEB R, KÖPSELA R. Change of chemical bonding of nitrogen of polymeric N-heterocyclic compounds during pyrolysis[J]. Carbon, 1999, 37(12): 1965-1978.
    FRIEBEL J, KOPSEL R F W. The fate of nitrogen during pyrolysis of German low rank coals-A parameter study[J]. Fuel, 1999, 78(8): 923-932.
    常丽萍. 煤热解、气化过程中含氮化合物的生成与释放研究[D]. 太原: 太原理工大学, 2004. (CHANG Li-ping. The study of generation and release of nitrogen compounds during coal pyrolysis/gasification[D]. Taiyuan: Taiyuan University of Technology, 2004.)
    • 相关文章
    • 施引文献
  • 资源附件(0)
  • 加载中
WeChat 点击查看大图
计量
  • 文章访问数:  863
  • HTML全文浏览量:  19
  • PDF下载量:  720
  • 被引次数: 0
出版历程
  • 收稿日期:  2013-10-09
  • 修回日期:  2013-12-24
  • 刊出日期:  2014-05-30

目录

    /

    返回文章
    返回
    友情链接： 新型炭材料 中国科学院 中国知网 万方论文查重系统

    主办单位：中国科学院山西煤炭化学研究所 中国化学会主编：房倚天

    电子邮件：rlhx@sxicc.ac.cn

    版权所有 © 《燃料化学学报（中英文）》编辑部 本系统由 北京仁和汇智信息技术有限公司 开发    百度统计

    x 关闭 永久关闭

    2023年《燃料化学学报（中英文）》评优结果公布！