Citation: HU Jun-hao, LI Yang, YANG Hai-ping, YANG Qing, SHAO Jing-ai, WANG Xian-hua, CHEN Han-ping. Release of nitrogenous products and the catalytic characteristics of metal ions during coal pyrolysis[J]. Journal of Fuel Chemistry and Technology, ;2014, 42(8): 913-921. shu

Release of nitrogenous products and the catalytic characteristics of metal ions during coal pyrolysis

1.
State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China

Corresponding author: YANG Hai-ping,
Received Date: 23 January 2014
Available Online: 24 April 2014
Fund Project: 国家自然科学基金(51276075) (51276075)国家重点基础研究发展规划(973计划,2010CB227003-02) (973计划,2010CB227003-02)公益性行业(农业)科研专项(201303095)。 (农业)科研专项(201303095)

The influence of metal ions on the release characteristics of nitrogenous pollutants from pyrolysis of 3 typical coals with different ranks were studied by demineralization and adding metal salts of Fe, Ca and Na. The interactions of coal type and temperature during coal pyrolysis were explored. The results show that yields of HCN and NH₃ from the demineralized coals are lower than that from the raw coals. The yield of HCN increases gradually with the increase of temperature, while the yield of NH₃ increases first and then decreases, with a maximum value at 800 ℃. Catalytic effects of metal ions on nitrogenous pollutants release from different ranks of coals are different. Fe and Na restrain HCN release from medium rank coals, but promote that from low rank coals, while Ca facilitates the HCN release from all coals to some extent. Three metal ions all inhibit the release of NH₃ from medium rank coals, but promote that for low rank coals. Catalysis of each metal ion on yield of HCN and NH₃ has its own range of effectiveness. Release of nitrogenous pollutants during coal pyrolysis is influenced by the interactions of many kinds of inherent metal ions in coals.
- coal,
- pyrolysis,
- catalytic effect,
- metal ions,
- HCN,
- NH₃
1. [1]
  [1] 刘海峰, 刘银河, 刘艳华, 车得福. 煤热解过程中含氮气相产物转化规律的实验研究[J]. 燃料化学学报, 2008, 36(2): 134-138. (LIU H F, LIU Y H, LIU Y H, CHE D F. Experimental investigation on the conversion of nitrogenous gas products during coal pyrolysis[J]. Journal of Fuel Chemistry and Technology, 2008, 36(2): 134-138.)
2. [2]
  [2] FRIEBEL J, KÖPSEL R F W. The fate of nitrogen during pyrolysis of German low rank coals-A parameter study[J]. Fuel, 1999, 78(8): 923-932.
3. [3]
  [3] DENG L, JIN X, ZHANG Y, CHE D F. Release of nitrogen species during rapid pyrolysis of model coals[J]. Energy Fuels, 2013, 27(1): 430-439.
4. [4]
  [4] 赵炜, 常丽萍, 冯志华, 谢克昌. 煤热解过程中生成氮化物的研究[J]. 燃料化学学报, 2002, 30(5): 408-412. (ZHAO Wei, CHANG Li-ping, FENG Zhi-hua, XIE Ke-chang. Formation of nitrogenous species during coal pyrolysis[J]. Journal of Fuel Chemisty and Technology, 2002, 30(5): 408-412.)
5. [5]
  [5] YUAN S, ZHOU Z J, LI J, CHEN X L, WANG F C. HCN and NH₃ (NO_x precursors) released under rapid pyrolysis of biomass/coal blends[J]. J Anal Appl Pyrolysis, 2011, 92(2): 463-469.
6. [6]
  [6] 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[J]. 燃料化学学报, 2007, 35(1): 5-9. (XU M Y, CUI Y P, QIN L L, CHANG L P, XIE K C. Key factors influencing the release and formation of HCN during pyrolysis of iron-containing coal[J]. Journal of Fuel Chemisty and Technology, 2007, 35(1): 5-9.)
7. [7]
  [7] TIAN Y, ZHANG J, ZUO W, CHEN L, CUI Y N, TAN T. Nitrogen conversion in relation to NH₃ and HCN during microwave pyrolysis of sewage sludge[J]. Environ Sci Technol, 2013, 47(7): 3498-3505.
8. [8]
  [8] LIU Z G, QUEK A, PARSHETTI G, JAIN A, SRINIVASAN M P, HOEKMAN S K, BALASUBRAMANIAN R. A study of nitrogen conversion and polycyclic aromatic hydrocarbon (PAH) emissions during hydrochar-lignite co-pyrolysis[J]. Appl Energy, 2013, 108: 74-81.
9. [9]
  [9] AHMAD T, AWAN I A, NISAR J, AHMAD I. Influence of inherent minerals and pyrolysis temperature on the yield of pyrolysates of some Pakistani coals[J]. Energy Convers Manage, 2009, 50(5): 1163-1171.
10. [10]
  [10] REN Q Q, ZHAO C S, WU X, LIANG C, CHEN X P, SHEN J Z, TANG G Y, WANG Z. Effect of mineral matter on the formation of NO_x precursors during biomass pyrolysis[J]. J Anal Appl Pyrolysis, 2009, 85(1/2): 447-453.
11. [11]
  [11] 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.)
12. [12]
  [12] 鞠付栋, 陈汉平, 杨海平, 王贤华, 杜奇, 张世红. 不同变质煤热解和气化中燃料氮的转化规律[J]. 煤炭转化, 2011, 34(3): 21-26. (JU Fu-dong, CHEN Han-ping, YANG Hai-ping, WANG Xian-hua, DU Qi, ZHANG Shi-hong. Fuel nitrogen evolution of different rank coal during pyrolysis and gasification[J]. Coal Conversion, 2011, 34(3): 21-26.)
13. [13]
  [13] LI C Z. Some recent advances in the understanding of the pyrolysis and gasification behaviour of Victorian brown coal[J]. Fuel, 2007, 86(12/13): 1664-1683.
14. [14]
  [14] WU Z H, OHTSUKA Y. Nitrogen distribution in a fixed bed pyrolysis of coals with different ranks: Formation and source of N₂[J]. Energy Fuels, 1997, 11(2): 477-482.
15. [15]
  [15] WU Z H, SUGIMOTO Y, KAWASHIMA 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.
16. [16]
  [16] WU Z H, 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.
17. [17]
  [17] TSUBOUCHI 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.
18. [18]
  [18] TSUBOUCHI N, OHTSUKA Y. Formation of N₂ during pyrolysis of Ca-loaded coals[J]. Fuel, 2002, 81(11/12): 1423-1431.
19. [19]
  [19] TSUBOUCHI N, XU C, OHTSUKA Y. Effect of alkaline earth metals on N₂ formation during fixed bed pyrolysis of a low rank coal[J]. Fuel Process Technol, 2004, 85(8/10): 1039-1052.
20. [20]
  [20] TSUBOUCHI N, OHTSUKA Y. Nitrogen chemistry in coal pyrolysis: Catalytic roles of metal cations in secondary reactions of volatile nitrogen and char nitrogen[J]. Fuel Process Technol, 2008, 89(4): 379-390.
21. [21]
  [21] YAN M, CHE D F, XU T M. Effect of rank, temperatures and inherent minerals on nitrogen emissions during coal pyrolysis in a fixed bed reactor[J]. Fuel Process Technol, 2005, 86(7): 739-756.
22. [22]
  [22] 秦玲丽. 金属化合物对煤热解过程中氮、硫转化的影响. 太原: 太原理工大学, 2007. (QIN Ling-li. Effect of metal compound on the transformation of coal-N and coal-S during coal pyrolysis. Taiyuan: Taiyuan University of Technology, 2007.)
23. [23]
  [23] 刘海峰, 刘银河, 刘艳华, 车得福. 煤热解过程中含氮气相产物转化规律的实验研究[J]. 燃料化学学报, 2008, 36(2): 134-138. (LIU Hai-feng, LIU Yin-he, LIU Yan-hua, CHE De-fu. Experimental investigation on the conversion of nitrogenous gas products during coal pyrolysis[J]. Journal of Fuel Chemistry and Technology, 2008, 36(2): 134-138.)
24. [24]
  [24] 李军, 袁帅, 梁钦锋, 周志杰, 王辅臣. 煤及其模型化合物快速热解过程中HCN和NH3逸出规律的研究[J]. 高校化学工程学报, 2011, 25(1): 55-60. (LI Jun, YUAN Shuai, LIANG Qin-feng, ZHOU Zhi-jie, WANG Fu-chen. Formation of HCN and NH₃ during the rapid pyrolysis of coal and model compounds[J]. Journal of Chemical Engineering of Chinese Universities, 2011, 25(1): 55-60.)
25. [25]
  [25] 刘海明, 张军营, 郑楚光, 孟韵. 煤中吡咯型和吡啶型氮热解稳定性研究[J]. 华中科技大学学报(自然科学版), 2004, 32(11): 13-15. (LIU Hai-ming, ZHANG Jun-ying, ZHENG Chu-guang, MENG Yun. Quantum chemical study of the pyrolysis stability of pyrrolic nitrogen and pyridinic nitrogen in coal[J]. Journal of Huazhong University of Science and Technology(Nature science edition), 2004, 32(11): 13-15.)
26. [26]
  [26] KELEMEN S R, GORBATY M L, KWIATEK P J, FLETCHER T H, WATT M, SOLUM M S, PUGMIRE R J. Nitrogen transformations in coal during pyrolysis[J]. Energy Fuels, 1998, 12(1): 159-173.
27. [27]
  [27] 袁帅, 李军, 周志杰, 王辅臣. 吡啶型氮快速热解中HCN和NH₃生成机理研究[J]. 燃料化学学报, 2011, 39(6): 413-418. (YUAN Shuai, LI Jun, ZHOU Zhi-jie, WANG Fu-chen. Mechanisms of HCN and NH₃ formation during rapid pyrolysis of pyridinic nitrogen containing substances[J]. Journal of Fuel Chemisty and Technology, 2011, 39(6): 413-418.)
28. [28]
  [28] LI C Z, PETER N. Interactions of quartz, zircon sand and stainless steel with ammonia: Implications for the measurement of ammonia at high temperatures[J]. Fuel, 1996, 75(4): 525-526.
29. [29]
  [29] 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, 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.)
30. [30]
  [30] OHTSUKA Y, WU Z H. Effects of metal cations present naturally in coal on the fate of coal-bound nitrogen in the fixed-bed pyrolysis of 25 Coals with different ranks: Correlation between inherent Fe cations and N₂ formation from low-rank coals[J]. Energy Fuels, 2009, 23(10): 4774-4781.
31. [31]
  [31] 袁帅. 煤、生物质及其混合物的快速热解及过程中氮的迁移[D]. 上海: 华东理工大学, 2012. (YUAN Shuai. Rapid pyrolysis of coal, biomass, and coal/biomass blends, and nitrogen evolution during rapid pyrolysis[D]. Shanghai: East China University of Science and Technology, 2012.)
32. [32]
  [32] LI C Z, TAN L L. Formation of NO_x and SO_x 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.
33. [33]
  [33] 杨海平, 陈汉平, 鞠付栋, 王静, 王贤华, 张世红. 热解温度对神府煤热解与气化特性的影响[J]. 中国电机工程学报, 2008, 28(08): 40-45. (YANG Hai-ping, CHEN Han-ping, JU Fu-dong, WANG Jing, WANG Xian-hua, ZHANG Shi-hong. Influence of temperature on coal pyrolysis and char gasification[J]. Proceedings of the CSEE, 2008, 28(08): 40-45.)
34. [34]
  [34] CHANG L P, FENG Z H, XIE K C. Effect of coal properties on HCN and NH₃ release during coal pyrolysis[J]. Energ Source, 2005, 27(15): 1399-1407.
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