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升温速率对胜利褐煤热解过程中N迁移转化的影响

张书 白艳萍 米亮 郑盼盼 陈绪军 许德平 王永刚

张书, 白艳萍, 米亮, 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(中英文), 2013, 41(10): 1153-1159.
引用本文: 张书, 白艳萍, 米亮, 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(中英文), 2013, 41(10): 1153-1159.
ZHANG Shu, BAI Yan-ping, MI Liang, ZHENG Pan-pan, CHEN Xu-jun, XU De-ping, WANG Yong-gang. Effect of heating rate on migration and transformation of N during pyrolysis of Shengli brown coal[J]. Journal of Fuel Chemistry and Technology, 2013, 41(10): 1153-1159.
Citation: ZHANG Shu, BAI Yan-ping, MI Liang, ZHENG Pan-pan, CHEN Xu-jun, XU De-ping, WANG Yong-gang. Effect of heating rate on migration and transformation of N during pyrolysis of Shengli brown coal[J]. Journal of Fuel Chemistry and Technology, 2013, 41(10): 1153-1159.

升温速率对胜利褐煤热解过程中N迁移转化的影响

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

Effect of heating rate on migration and transformation of N during pyrolysis of Shengli brown coal

  • 摘要: 在固定床/流化床管式石英反应器中进行了胜利褐煤的快速热解和慢速热解实验,考察了升温速率对N迁移转化及对半焦内部N化学形态变化的影响。研究结果表明,快速升温热解气相N(NH3和HCN)生成量明显高于慢速热解时的生成量,且随着温度的升高,两者差值均逐渐增大。在多数情况下,NH3或HCN的产率在973 K左右并不随温度的升高而增加,这与高温下的半焦热缩聚反应以及挥发分的二次反应有关。快速热解条件下,半焦N的释放速率要快于半焦炭本身失重速率。X射线光电子能谱(XPS)分析认为,热解使得吡咯型N(N-5)部分转化为吡啶型N(N-6)和季氮型N(N-Q),快速热解有利于生成N-6,而慢速热解下半焦中N-Q含量较高。
  • CHEN Z, YUAN S, LIANG Q F, WANG F C,YU Z H. Distribution of HCN, NH3, NO and N2 in an entrained flow gasifier[J]. Chem Eng J, 2009, 148(2): 312-318.
    赵伟, 冯杰, 常丽萍, 谢克昌, 刘美蓉. 煤气化过程中生成氮化物的研究[J]. 燃料化学学报, 2002, 30(6): 519-522.

    (ZHAO Wei, FENG Jie, CHANG Li-ping, XIE Ke-cang, LIU Mei-rong. Release of nitrogenous species during coal gasification[J]. Journal of Fuel Chemistry and Technology, 2002, 30(6): 519-522.)
    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.
    CAI H Y, GUELL A J, DUGWELL D R, KANDIYOTI R. Heteroatom distribution in pyrolysis products as a function of heating rate and pressure[J]. Fuel, 1993, 72(3): 321-327.
    XU W C, KUMAGAI M. Nitrogen evolution during rapid hydropyrolysis of coal[J]. Fuel, 2002, 81(18): 2325-2334.
    NELSON P F, KELLY M D, WORNET M J. Conversion of fuel nitrogen in coal volatiles to NOx precursors under rapid heating conditions[J]. Fuel, 1991, 70(3): 403-407.
    NELSON P F, BUCKLEY A N, KELLY M D. Functional forms of nitrogen in coals and the release of coal nitrogen as NOx precursors (HCN and NH3)[J]. Symp (Int) Combust 1992, 24(1): 1259-1267.
    LI C Z, BUCKLEY A N, NELSON P F. Effects of temperature and molecular mass on the nitrogen functionality of tars produced under high heating rate conditions[J]. Fuel, 1998, 77(3): 157-164.
    TAN L L, LI C Z. Formation of NOx and SOx precursors during the pyrolysis of coal and biomass. Part I. Effects of reactor configuration on the determined yields of HCN and NH3 during pyrolysis[J]. Fuel, 2000, 79(15): 1883-1889.
    TAN L L, LI C Z. Formation of NOx and SOx precursors during the pyrolysis of coal and biomass. Part II. Effects of experimental conditions on the yields of NOx and SOx precursors from the pyrolysis of a Victorian brown coal[J]. Fuel, 2000, 79(15): 1891-1897.
    LI C Z, TAN L L. Formation of NOx and SOx precursors during the pyrolysis of coal and biomass. Part III. Further discussion on the formation of HCN and NH3 during pyrolysis[J]. Fuel, 2000, 79(15): 1899-1906.
    XIE Z L, FENG J, ZHAO W, XIE K C, PRATT K C, LI C Z. Formation of NOx and SOx precursors during the pyrolysis of coal and biomass. Part IV. Pyrolysis of a set of Australian and Chinese coals[J]. Fuel, 2001, 80(15): 2131-2138.
    CHANG L P, XIE Z L, XIE K C, PRATT K C, HAYASHID J I, CHIBA T, LI C Z. Formation of NOx precursors during the pyrolysis of coal and biomass. Part VI. Effects of gas atmosphere on the formation of NH3 and HCN[J]. Fuel, 2003, 82(10): 1159-1166.
    TIAN F J, WU H W, YU J L, MCKENZIE L J, KONSTANTINIDIS S, HAYASHID J I, CHIBA T, LI C Z. Formation of NOx precursors during the pyrolysis of coal and biomass. Part VIII. Effects of pressure on the formation of NH3 and HCN during the pyrolysis and gasification of Victorian brown coal in steam[J]. Fuel, 2005, 84(16): 2102-2108.
    BASSILAKIS R, ZHAO Y, SOLOMON P R, SERIO M A. Sulfur and nitrogen evolution in the Aigolme coals-experiment and modeling[J]. Energy Fuels, 1993, 7(6): 710-720.
    LEPPALAHTI J. Formation of NH3 and HCN in slow-heating-rate inert pyrolysis of peat, coal and bark[J]. Fuel, 1995, 74(9): 1363-1368.
    ZHANG S, LI C Z.Volatilisation and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal. Part IX. Effects of volatile-char interactions on char-H2O and char-O2 reactivities[J]. Fuel, 2011, 90(4): 1655-1661.
    DIMPLE M Q, WU H W, HAYASHID J I, 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.
    TAN L L, LI C Z. Formation of NOx and SOx precursors during the pyrolysis of coal and biomass. Part II. Effects of experimental conditions on the yields of NOx and SOx precursors from the pyrolysis of a Victorian brown coal[J]. Fuel, 2000, 79(15): 1891-1897.
    NAOTO T, YASUO O. Nitrogen chemistry in coal cytolysis: Catalytic roles of metal cations in secondary reactions of volatile nitrogen and char nitrogen[J]. Fuel Process Technol, 2008, 89(4): 379-390.
    QUYN D M, WU H, BHATTACHARYA S, LI C Z. Volatilisation and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal. Part II. Effects of chemical form and valence[J]. Fuel, 2002, 81(2): 151-158.
    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.
    谢建军, 杨学民, 朱文魁, 丁同利, 宋文立, 林伟刚. 煤炭解耦燃烧过程N迁移与转化Ⅰ: 热解阶段煤N 的释放规律[J]. 燃料化学学报, 2012, 40(8): 919-926.

    (XIE Jian-jun, YANG Xue-min, ZHU Wen-kui, DING Tong-li, SONG Wen-li, LIN Wei-gang. Nitrogen transformation during coal decoulpig combustion I: Release behavior of coal-nitrogen during pyrolysis stage[J]. Journal of Fuel Chemistry and Tecchnology, 2012, 40(8): 919-926.)
    JOHNSSON J E. Formation and reducion of nitrogen oxides in fluidized-bed combution[J]. Fuel, 1994, 73(9): 1398-1415.
    范晓雷, 杨帆, 周志杰, 王辅臣. 热解过程中煤焦微晶结构变化及其对煤焦气化反应活性的影响[J]. 燃料化学学报, 2006, 34(4): 396-399.

    (FAN Xiao-lei, YANG Fan, ZHOU Zi-jie, WANG Fu-chen. Variation of the crystalline structure of coal char during pyrolysis and its effect on gasification reactivity[J]. Journal of Fuel Chemistry and Technology, 2006, 34(4): 396-399.)
    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 m inerals on transformation of nitrogen during coal pyrolysis/gasification[D]. Taiyuan: Taiyuan university of technology, 2003.)
    VALENTIM B, GUEDS A, BOAVIDA D. Nitrogen functionality in "oil window"rank range vitrinte rich coals and chars[J]. Org Geochem, 2011, 8(42): 502-509.
    姚明宇, 刘艳华, 车得福. 宜宾煤中氮的形态及其变迁规律研究[J]. 西安交通大学学报, 2003, 37(7): 759-763.

    (YAO Ming-yu, LIU Yan-hua, CHE De-fu. Investigation of nitrogen functionality in Yibin coal and its char[J]. Journal of Xi'an jiaotong university, 2003, 37(7): 759-763.)
    KELEMEN S R, AFEW O, GORBATY M L, KW IATEK P J, SOLUM M S, HU J Z, PUGMIRE R J. XPS and15N NMR study of nitrogen forms in carbonaceous solids[J]. Energy Fuels, 2002, 16(6): 1507-1515.
    PELS J R, KAPTEIJN J A, MOULIJN J A, ZHU Q, THOMAS K M. Evolution of nitrogen functionalities in carbonaceous materials during pyrolysis[J]. Carbon, 1995, 33(11): 1641-1653.
    顾庆超, 楼书聪, 戴庆平, 黄炳荣, 李乔钧, 黄剑朎. 化学用表一有机物[M]. 南京, 江苏科学技术出版社, 1979: 95.

    (GU Qing-chao, LOU Shu-cong, DAI Qing-ping, HUANG Bing-rong, LI Qiao-jun, HUANG Jian-ling. Chemical tables-organic matter[M]. Nanjing: Jiangsu Science and Technology Press, 1979: 95.)
    KELEMEN S R, GORBATY M L, KWIATEK P J. Nirtogen transformations in coal during pyrolysis[J]. Energy Fuel, 1998, 12(l): 159-173.
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出版历程
  • 收稿日期:  2013-01-28
  • 修回日期:  2013-04-26
  • 刊出日期:  2013-10-30

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