平朔煤热解过程中PAHs的释放特性

孔娇; 程柱; 董洁; 焦海丽; 李凡

平朔煤热解过程中PAHs的释放特性

太原理工大学煤科学与技术教育部及山西省重点实验室, 山西太原 030024

基金项目: 国家自然科学基金(20876103);山西省自然科学基金(2008011023)。

详细信息

通讯作者:
李凡(1956- ),女,教授,主要从事煤结构特征和有机污染物的控制研究,Tel:0351-6018076;Fax:0351-6010482;E-mail:fanli@tyut.edu.cn。

中图分类号: TQ530.2
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出版历程
- 收稿日期: 2013-03-14
- 修回日期: 2013-05-26
- 刊出日期: 2013-11-30

Release of PAHs during pyrolysis of Pingshuo coal

Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China

摘要

摘要: 利用热解-气质联用仪(PY-GC-MS)研究了平朔煤在不同热解温度下多环芳烃(PHAs)的释放规律,并探讨了该过程中PAHs的生成机理。研究结果表明,16种PAHs的生成总量随着热解温度的升高先增大后减少,在800℃达到最大值。且PAHs环数分布规律对热解温度具有显著的依赖性,不同环数的PAHs,其最大生成量时所对应的热解温度亦不同。随着热解温度的升高,煤结构中的桥键、芳香环上的脂肪侧链以及较难断裂的甲基、酚羟基等依次断裂,使得PAHs的生成量不断增加,当温度升高至1 000、1 200℃时,伴随着缩合反应加剧,大环PAHs的生成量继续增加。由总体趋势看出,平朔煤大分子网络结构的热裂解主要发生在600~800℃,热解缩合反应主要发生在高温下。平朔煤热解过程中的PAHs除小部分来自煤中可萃取的芳烃结构挥发外,主要来自煤中大分子芳香结构裂解以及热解生成自由基碎片的高温聚合。
- 平朔煤 /
- 热解 /
- 多环芳烃 /
- PY-GC-MS
Abstract: A flash pyroprobe combined with GC-MS was used to investigate the effects of temperature on the release property of PAHs (polycyclic aromatic hydrocarbons) during pyrolysis of Pingshuo coal. The formation mechanism of PAHs was also discussed. The results indicate that the total amounts of the 16 PAHs released increase obviously with increasing temperature during pyrolysis, reach the maximum at 800℃, and then decrease. The ring distributions of PAHs have a notable dependence on the pyrolysis temperature. The different species of PAHs reaches the maximum yields at individual temperature. With increase in pyrolysis temperature, the total amount of PAHs increase observably, which is attributed to cracking of the bridge bonds, the fat side chain on aromatic ring, the methyl and phenolic group in the coal macrostructure. With further increase to 1 000 and 1 200℃, the amount of high-ring PAHs increases due to the occurrence of condensation reaction. Thermal cracking of macromolecular compounds concentrated during 600~800℃, and condensation are the main reactions occurred at high temperatures. The PAHs during coal pyrolysis are generated from the volatilization of aromatics structure in coal, the cracking reactions of macromolecular compounds and the condensation reactions of radicals at high temperature; meanwhile, the last one is the major source of high-ring PAHs during coal pyrolysis.
- Pingshuo coal /
- pyrolysis /
- PAHs /
- PY-GC-MS

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参考文献(23)

谢克昌. 煤的结构与反应性[M]. 北京: 科学出版社, 2002. (XIE Ke-chang. Coal structure and its reactivity[M]. Beijing: Science Press, 2002.)

赵文昌, 程金平, 谢海赟, 马英歌, 王文华. 环境中多环芳烃(PAHs)的来源与监测分析方法[J]. 环境科学与技术, 2006, 29(3): 105-107. (ZHAO Wen-chang, CHENG Jin-ping, XIE Hai-yun, MA Ying-ge, WANG Wen-hua. PAHs: sources, pathway and their monitoring and analysis[J]. Environmental Science & Technology, 2006, 29(3): 105-107.)

刘淑琴, 靳志伟, 张尚军. 大尺度煤热解多环芳烃生成及排放规律[J]. 煤炭学报, 2012, 37(6): 1039-1045. (LIU Shu-qin, JIN Zhi-wei, ZHANG Shang-jun. Formation and distribution of polycyclic aromatic hydrocarbons during large size coal pyrolysis[J]. Journal of China Coal Society, 2012, 37(6): 1039-1045.)

王连生. 有机污染化学[M]. 北京: 高等教育出版社, 2004. (WANG Lian-sheng. Chemistry of organic pollution[M]. Beijing: Higher Education Press, 2004.)

戴朝霞, 陈振翔, 王格慧, 王连生. 典型城市大气颗粒物中多环芳烃的污染研究[J]. 环境科学与技术, 2006, 29(2): 29-31. (DAI Zhao-xia, CHEN Zhen-xiang, WANG Ge-hui, WANG Lian-sheng. Study on polycyclic aromatic hydrocarbons in aerosol of representative cities[J]. Environmental Science and Technology, 2006, 29(2): 29-31.)

许士奋, 蒋新, 汪涟生, 全燮, MARTENS D. 长江和辽河沉积物中的多环芳烃类污染物[J]. 中国环境科学, 2000, 20(2): 128-131. (XU Shi-fen, JIANG Xin, WANG Lian-sheng, QUAN Xie, MARTENS D. Polycyclic aromatic hydrecarbons (PAHs) pollutants in sediments of the Yangtse river and the Liaohe river [J]. China Environmental Science, 2000, 20(2): 128-131.)

刘大锰, 刘志华, 李运勇. 煤中有害物质及其对环境的影响研究进展[J]. 地球科学进展, 2002, 17(6): 840-847. (LIU Da-meng, LIU Zhi-hua, LI Yun-yong. Advances in studies of harmful substances in coal and their impact on the environment[J]. Advance In Earth Sciences, 2002, 17(6): 840-847.)

董洁, 李凡, 谢克昌. 煤转化过程中多环芳烃排放的研究现状[J]. 现代化工, 2009, 29(S1): 344-346. (DONG Jie, LI Fan, XIE Ke-chang. Progress in formation of polycyclic aromatic hydrocarbons during coal conversion process[J]. Modern Chemical Industry, 2009, 29(S1): 344-346.)

何选明, 黄鹂, 韩军, 李振东, 李耀拉. 炼焦煤中多环芳烃的分布特性研究[J]. 煤炭转化, 2009, 32(4): 70-73. (HE Xuan-ming, HUANG Li, HAN Jun, LI Zhen-dong, LI Yao-la. Distribution characteristic of polycyclic aromatic hydrocarbons in coking coal[J]. Coal Conversion, 2009, 32(4): 70-73.)

刘淑琴, 庞旭林, 王媛媛, 张尚军, 鲍鹏程, 党金莉. 不同煤种热解多环芳烃的生成分布特征研究[J]. 煤炭转化, 2011, 34(1): 1-6. (LIU Shu-qin, PANG Xu-lin, WANG Yuan-yuan, ZHANG Shang-jun, BAO Peng-cheng, DANG Jin-li. Study on the distribution characteristic of polycyclic aromatic hydrocarbons during pyrolysis of different ranks of coal[J]. Coal Conversion, 2011, 34(1): 1-6.)

孙庆雷, 李文, 陈皓侃, 李保庆. 神木煤显微组分热解和加氢热解的焦油组成[J]. 燃料化学学报, 2005, 33(4): 412-415. (SUN Qing-lei, LI Wen, CHEN Hao-kan, LI Bao-qing. Compositions of coal tar from pyrolysis and hydropyrolysis of Shenmu coalmacerals[J]. Journal of Fuel Chemistry and Technology, 2005, 33(4): 412-415.)

DONG J, LI F, XIE K C. Study on the source of polycyclic aromatic hydrocarbons (PAHs) during coal pyrolysis by PY-GC-MS[J]. J Hazard Mater, 2012, 243: 80-85.

罗孝俊. 珠江三角洲河流、河口和邻近南海海域水体和沉积物中多环芳烃和有机氯农药研究[D]. 广州: 中国科学院广州地球化学研究所, 2004. (LUO Xiao-jun. A study of PAHs and OCPs on water body and sediments of rivers in pearl river delta, pearl river estuary and offshore of south China sea[D]. Guangzhou: Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, 2004.)

DI NOLA G, DE JONG W, SPLIETHOFF H. TG-FTIR characterization of coal and biomass single fuels and blends under slow heating rate conditions: Partitioning of the fuel-bound nitrogen[J]. Fuel Process Technol, 2010, 91(1): 103-115.

焦海丽. 原煤中可抽提多环芳烃(PAHs)及其热解特性[D]. 太原: 太原理工大学, 2010. (JIAO Hai-li. The PAHs in the raw coal extracts and their pyrolysis properties[D]. Taiyuan: Taiyuan University of Technology, 2010.)

高晋生. 煤的热解、炼焦和煤焦油加工[M]. 北京: 化学工业出版社, 2010. (GAO Jin-sheng. Coal pyrolysis,coking and coal tar processing[M]. Beijing: Chemical Industry Press, 2010.)

尤孝方. 燃烧过程中多环芳烃的生成与数值模拟[D]. 浙江: 浙江大学, 2006. (YOU Xiao-fang. The formation of polycyclic aromatic hydrocarbons (PAHs) from combustion processes and its modelling[D]. Zhejiang: Zhejiang University, 2006.)

何选明. 煤化学[M]. 2版. 北京: 冶金工业出版社, 2010. (HE Xuan-ming. Coal chemistry[M]. 2nd ed. Beijing: Metallurgical Industry Press, 2010.)

WISER W H, HILL G R, KERTAMUS N J. Kinetic study of pyrolysis of high volatile bituminous coal[J]. Ind Eng Chem Process Des Dev, 1967, 6(1): 133-138.

RAJ A, PRADA I D C, AMER A A, CHUNG S H. A reaction mechanism for gasoline surrogate fuels for large polycyclic aromatic hydrocarbons[J]. Combust Flame, 2012, 159(2): 500-515.

COMANDINI A, MALEWICKI T, BREZINSKY K. Chemistry of polycyclic aromatic hydrocarbons formation from phenyl radical pyrolysis and reaction of phenyl and acetylene[J]. J Phys Chem A, 2012, 116(10): 2409-2434.

SHUKLA B, KOSHI M. Comparative study on the growth mechanisms of PAHs[J]. Combust Flame, 2012, 158(2): 369-375.

吴爱坪, 潘铁英, 史新梅, 周丽芳, 刘瑞民, 张德祥, 高晋生. 中低阶煤热解过程中自由基的研究[J]. 煤炭转化, 2012, 35(2): 1-5. (WU Ai-ping, PAN Tie-ying, SHI Xin-mei, ZHOU Li-fang, LIU Rui-min, ZHANG De-xiang, GAO Jin-sheng. Study on free radicals in low rank coal pyrolysis process[J]. Coal Conversion, 2012, 35(2): 1-5.)

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