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. shu

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

  • Corresponding author: ZHANG Shu,  WANG Yong-gang, 
  • Received Date: 28 January 2013
    Available Online: 26 April 2013

    Fund Project: 国家科技支撑计划 (2012BAA04B02)。 (2012BAA04B02)

  • The effects of heating rate on migration, transformation and occurring forms of nitrogen during pyrolysis of Shengli brown coals were studied in a fixed-bed/fluidised-bed quartz reactor. The results indicate that the yields of NH3 and HCN from the fast pyrolysis were much higher than those from the slow pyrolysis. The difference in the yields of NH3 and HCN between the fast and slow heating rates increases with the increasing pyrolysis temperature. The maximum productions of NH3 and HCN mostly occur at 973K, which is attributed to the enhanced condensation and secondary reactions with the increasing pyrolysis temperature. The release rate of char-N is faster than the weight loss rate of char itself at fast heating rate. The results from X-ray photoelectron spectroscopy (XPS) analysis imply that the pyrolysis process has facilitated the transformation of pyrrolic (N-5) to quaternary type nitrogen (N-Q) and pyridinic (N-6). It seems that the fast heating rate favors the formation of N-6 while the content of N-Q in char is relatively high at the slow heating rate.
  • 加载中
    1. [1]

      [1] 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.

    2. [2]

      [2] 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.

    3. [3]

      (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.)

    4. [4]

      [3] 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.

    5. [5]

      [4] 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.

    6. [6]

      [5] XU W C, KUMAGAI M. Nitrogen evolution during rapid hydropyrolysis of coal[J]. Fuel, 2002, 81(18): 2325-2334.

    7. [7]

      [6] 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.

    8. [8]

      [7] 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.

    9. [9]

      [8] 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.

    10. [10]

      [9] 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.

    11. [11]

      [10] 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.

    12. [12]

      [11] 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.

    13. [13]

      [12] 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.

    14. [14]

      [13] 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.

    15. [15]

      [14] 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.

    16. [16]

      [15] 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.

    17. [17]

      [16] 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.

    18. [18]

      [17] 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.

    19. [19]

      [18] 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.

    20. [20]

      [19] 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.

    21. [21]

      [20] 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.

    22. [22]

      [21] 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.

    23. [23]

      [22] 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.

    24. [24]

      [23] 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.

    25. [25]

      (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.)

    26. [26]

      [24] JOHNSSON J E. Formation and reducion of nitrogen oxides in fluidized-bed combution[J]. Fuel, 1994, 73(9): 1398-1415.

    27. [27]

      [25] 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.

    28. [28]

      (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.)

    29. [29]

      [26] 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.

    30. [30]

      ( ZHAO Ya-hong. Effect of m inerals on transformation of nitrogen during coal pyrolysis/gasification[D]. Taiyuan: Taiyuan university of technology, 2003.)

    31. [31]

      [27] 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.

    32. [32]

      [28] 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.

    33. [33]

      (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.)

    34. [34]

      [29] 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.

    35. [35]

      [30] 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.

    36. [36]

      [31] 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.

    37. [37]

      (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.)

    38. [38]

      [32] KELEMEN S R, GORBATY M L, KWIATEK P J. Nirtogen transformations in coal during pyrolysis[J]. Energy Fuel, 1998, 12(l): 159-173.

  • 加载中
    1. [1]

      Shuying Zhu Shuting Wu Ou Zheng . Improvement and Expansion of the Experiment for Determining the Rate Constant of the Saponification Reaction of Ethyl Acetate. University Chemistry, 2024, 39(4): 107-113. doi: 10.3866/PKU.DXHX202310117

    2. [2]

      Heng Zhang . Determination of All Rate Constants in the Enzyme Catalyzed Reactions Based on Michaelis-Menten Mechanism. University Chemistry, 2024, 39(4): 395-400. doi: 10.3866/PKU.DXHX202310047

    3. [3]

      Kexin YanZhaoqi YeLingtao KongHe LiXue YangYahong ZhangHongbin ZhangYi Tang . Seed-Induced Synthesis of Disc-Cluster Zeolite L Mesocrystals with Ultrashort c-Axis: Morphology Control, Decoupled Mechanism, and Enhanced Adsorption. Acta Physico-Chimica Sinica, 2024, 40(9): 2308019-0. doi: 10.3866/PKU.WHXB202308019

    4. [4]

      Zhuo WANGJunshan ZHANGShaoyan YANGLingyan ZHOUYedi LIYuanpei LAN . Preparation and photocatalytic performance of CeO2-reduced graphene oxide by thermal decomposition. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1708-1718. doi: 10.11862/CJIC.20240067

    5. [5]

      Dongqi Cai Fuping Tian Zerui Zhao Yanjuan Zhang Yue Dai Feifei Huang Yu Wang . Exploration of Factors Influencing the Determination of Ion Migration Number by Hittorf Method. University Chemistry, 2024, 39(4): 94-99. doi: 10.3866/PKU.DXHX202310031

    6. [6]

      Jiayu Tang Jichuan Pang Shaohua Xiao Xinhua Xu Meifen Wu . Improvement for Measuring Transference Numbers of Ions by Moving-Boundary Method. University Chemistry, 2024, 39(5): 193-200. doi: 10.3866/PKU.DXHX202311021

    7. [7]

      Yang Lv Yingping Jia Yanhua Li Hexiang Zhong Xinping Wang . Integrating the Ideological Elements with the “Chemical Reaction Heat” Teaching. University Chemistry, 2024, 39(11): 44-51. doi: 10.12461/PKU.DXHX202402059

    8. [8]

      Rui LiHuan LiuYinan JiaoShengjian QinJie MengJiayu SongRongrong YanHang SuHengbin ChenZixuan ShangJinjin Zhao . Emerging Irreversible and Reversible Ion Migrations in Perovskites. Acta Physico-Chimica Sinica, 2024, 40(11): 2311011-0. doi: 10.3866/PKU.WHXB202311011

    9. [9]

      Yang ZHOULili YANWenjuan ZHANGPinhua RAO . Thermal regeneration of biogas residue biochar and the ammonia nitrogen adsorption properties. Chinese Journal of Inorganic Chemistry, 2025, 41(8): 1574-1588. doi: 10.11862/CJIC.20250032

    10. [10]

      Yichang Liu Li An Dan Qu Zaicheng Sun . “双碳”背景下的综合设计实验——以PbCrO4催化甲基蓝的光降解速率常数测定为例. University Chemistry, 2025, 40(6): 222-229. doi: 10.12461/PKU.DXHX202407105

    11. [11]

      Limei CHENMengfei ZHAOLin CHENDing LIWei LIWeiye HANHongbin WANG . Preparation and performance of paraffin/alkali modified diatomite/expanded graphite composite phase change thermal storage material. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 533-543. doi: 10.11862/CJIC.20230312

    12. [12]

      Yuting BaiCenqi YanZhen LiJiaqiang QinPei Cheng . Preparation of High-Strength Polyimide Porous Films with Thermally Closed Pore Property by In Situ Pore Formation Method. Acta Physico-Chimica Sinica, 2024, 40(9): 2306010-0. doi: 10.3866/PKU.WHXB202306010

    13. [13]

      Ronghao Zhao Yifan Liang Mengyao Shi Rongxiu Zhu Dongju Zhang . Investigation into the Mechanism and Migratory Aptitude of Typical Pinacol Rearrangement Reactions: A Research-Oriented Computational Chemistry Experiment. University Chemistry, 2024, 39(4): 305-313. doi: 10.3866/PKU.DXHX202309101

    14. [14]

      Shanghua LiMalin LiXiwen ChiXin YinZhaodi LuoJihong Yu . High-Stable Aqueous Zinc Metal Anodes Enabled by an Oriented ZnQ Zeolite Protective Layer with Facile Ion Migration Kinetics. Acta Physico-Chimica Sinica, 2025, 41(1): 100003-0. doi: 10.3866/PKU.WHXB202309003

    15. [15]

      Yongqing XuYuyao YangMengna WuXiaoxiao YangXuan BieShiyu ZhangQinghai LiYanguo ZhangChenwei ZhangRobert E. PrzekopBogna SztorchDariusz BrzakalskiHui Zhou . Review on Using Molybdenum Carbides for the Thermal Catalysis of CO2 Hydrogenation to Produce High-Value-Added Chemicals and Fuels. Acta Physico-Chimica Sinica, 2024, 40(4): 2304003-0. doi: 10.3866/PKU.WHXB202304003

    16. [16]

      Zhanhui Yang Jiaxi Xu . (m+n+…) or [m+n+…]cycloaddition?. University Chemistry, 2025, 40(3): 387-389. doi: 10.12461/PKU.DXHX202406032

    17. [17]

      Yahui HANJinjin ZHAONing RENJianjun ZHANG . Synthesis, crystal structure, thermal decomposition mechanism, and fluorescence properties of benzoic acid and 4-hydroxy-2, 2′: 6′, 2″-terpyridine lanthanide complexes. Chinese Journal of Inorganic Chemistry, 2025, 41(5): 969-982. doi: 10.11862/CJIC.20240395

    18. [18]

      Le Ye Wei-Xiong Zhang . Structural phase transition in a new organic-inorganic hybrid post-perovskite: (N,N-dimethylpyrrolidinium)[Mn(N(CN)2)3]. Chinese Journal of Structural Chemistry, 2024, 43(6): 100257-100257. doi: 10.1016/j.cjsc.2024.100257

    19. [19]

      Xingfen HuangJiefeng ZhuChuan He . Catalytic enantioselective N-silylation of sulfoximine. Chinese Chemical Letters, 2024, 35(4): 108783-. doi: 10.1016/j.cclet.2023.108783

    20. [20]

      Sanmei WangYong ZhouHengxin FangChunyang NieChang Q SunBiao Wang . Constant-potential simulation of electrocatalytic N2 reduction over atomic metal-N-graphene catalysts. Chinese Chemical Letters, 2025, 36(3): 110476-. doi: 10.1016/j.cclet.2024.110476

Metrics
  • PDF Downloads(0)
  • Abstract views(865)
  • HTML views(70)

通讯作者: 陈斌, bchen63@163.com
  • 1. 

    沈阳化工大学材料科学与工程学院 沈阳 110142

  1. 本站搜索
  2. 百度学术搜索
  3. 万方数据库搜索
  4. CNKI搜索
Address:Zhongguancun North First Street 2,100190 Beijing, PR China Tel: +86-010-82449177-888
Powered By info@rhhz.net

/

DownLoad:  Full-Size Img  PowerPoint
Return