褐煤气化半焦对地下水有机污染的模拟脱除
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摘要
通过自制的煤炭地下气化模拟系统,采用富氧空气/水蒸气两阶段气化工艺,完成内蒙褐煤的地下气化模拟实验。利用傅里叶红外光谱、低温氮气物理吸附仪和扫描电镜对气化残留半焦的表面官能团、孔结构及表面形貌进行表征,进而考察了半焦对苯酚模拟废水中苯酚及煤气洗涤水中总有机碳(TOC)的脱除效果。实验结果表明:半焦孔径主要分布在1~4nm之间,表面有较丰富的含氧官能团及较多的孔洞和裂隙,其孔结构、含氧官能团及孔洞裂隙均有利于污染物在半焦内的迁移和吸附;气化半焦对苯酚的吸附符合Langmuir等温吸附模型,为单分子层吸附;实验条件下最大吸附率为97.95%,吸附量为2.44mg/g;气化半焦对煤气洗涤水中TOC的脱除随吸附时间的变化具有阶段性,脱除率可达88.1%。
Through self-designed underground coal gasification(UCG)model test system,the UCG test of Inner Mongolian lignite was carried out by applying oxygen-enriched air/steam two-stage gasification method. The functional groups,porous characteristics and surface morphology of the semi-coke were characterized by applying Fourier transform infrared spectroscopy(FTIR),automatic specific surface and porosity analyzer and scanning electron microscope(SEM). The uptake of phenol in simulated wastewater and TOC in gas washing water by UCG semi-coke were further investigated. Oxygen enriched functional groups,cracks and pores in range of 1—4 nm were found in semi-coke samples,which may be favorable for the migration and adsorption of pollutants. The results showed that adsorption data of phenol by UCG semi-coke can be well fitted by Langmuir adsorption isotherm. The maximum removal rate of phenol and adsorption capacity could be 97.95% and 2.44mg/g,respectively. The removal rate of TOC in gas washing water varied with the increase of time,and the maximum of 88.1% can be reached.
Through self-designed underground coal gasification(UCG)model test system,the UCG test of Inner Mongolian lignite was carried out by applying oxygen-enriched air/steam two-stage gasification method. The functional groups,porous characteristics and surface morphology of the semi-coke were characterized by applying Fourier transform infrared spectroscopy(FTIR),automatic specific surface and porosity analyzer and scanning electron microscope(SEM). The uptake of phenol in simulated wastewater and TOC in gas washing water by UCG semi-coke were further investigated. Oxygen enriched functional groups,cracks and pores in range of 1—4 nm were found in semi-coke samples,which may be favorable for the migration and adsorption of pollutants. The results showed that adsorption data of phenol by UCG semi-coke can be well fitted by Langmuir adsorption isotherm. The maximum removal rate of phenol and adsorption capacity could be 97.95% and 2.44mg/g,respectively. The removal rate of TOC in gas washing water varied with the increase of time,and the maximum of 88.1% can be reached.
引文
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[21]曾昭琼.有机化学[M].3版.北京:高等教育出版社,1993.
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[23]国家环境保护总局.污水排放标准:GB 8978—1996[S].北京:中国标准出版社,1998.
[2]LIANG Jie.Underground coal gasification technology[J].Scientific Chinese,2006,4:82-83.
[3]KAPUSTA K,STA?CZYK K.Pollution of water during underground coal gasification of hard coal and lignite[J].Fuel,2011,90(5):1927-1934.
[4]刘淑琴,周蓉,潘佳,等.煤炭地下气化选址决策及地下水污染防控[J].煤炭科学技术,2013,41(5):23-27.
[5]IMRAN Muhammad,KUMAR Dileep,KUMAR Naresh,et al.Environmental concerns of underground coal gasification[J].Renewable and Sustainable Energy Reviews,2014,31:600-610.
[6]KAPUSTA Krzysztof,STANCZYK Krzysztof,WIATOWSKI Marian,et al.Environmental aspects of afield-scale underground coal gasification trial in a shallow coal seam at the Experimental Mine Barbara in Poland[J].Fuel,2013,(113):196-208.
[7]LIU Shuqin,LI Jingang,MEI Mei,et al.Groundwater pollution from underground coal gasification[J].Journal of China University of Mining&Technology,2007,17(4):467-472.
[8]KAPUSTA Krzysztof,STANCZYK Krzysztof.Pollution of water during underground coal gasification of hard coal and lignite[J].Fuel,2011,90(5):1927-1934.
[9]梁杰,娄元娥.褐煤地下气化过程中铅和砷的迁移规律的研究[J].环境科学学报,2007,27(11):1858-1862
[10]吴仕生,曾玺,任明威,等.含氧/蒸汽气氛中煤高温分解产物分布及反应性[J].燃料化学学报,2012,40(6):660-665.
[11]刘淑琴,董贵明,杨国勇,等.煤炭地下气化酚污染迁移数值模拟[J].煤炭学报,2011,36(5):796-801.
[12]中华人民共和国卫生部,建设部,水利部,国土资源部,国家环境保护总局,等.生活饮用水卫生标准:GB 5749—2006[S].北京:中国标准出版社,2007。
[13]王媛媛,刘洪涛,李金刚,等.煤炭地下气化“三带”痕量元素析出规律模拟试验研究[J].煤炭学报,2012,37(12):2092-2096.
[14]XU Bing,CHEN Lunjian,XING Baolin,et al.Experimental study on the environmental behaviors of poisonous trace elements in post-gasified residues[J].Advanced Materials Research,2013,805/806:1478-1483.
[15]段钰锋,周毅,陈晓平,等.煤气化半焦的孔隙结构[J].东南大学学报,2005,35(1):135-139.
[16]MATSUOKA Koichi,AKIHO Hiroyuki,XU Weichun.The physical character of coal char formed during rapid pyrolysis at high pressure[J].Fuel,2005,84(1):63-69.
[17]张秋香,华志明,赵培,等.活性炭吸附法处理对氨基苯酚生产的废水[J].华东理工大学学报(自然科学版),2004,30(3):245-249.
[18]范延臻,王宝贞,王琳,等.改性活性炭对有机物的吸附性能[J].环境化学,2001,20(5):444-448.
[19]徐冰,谌伦建,邢宝林.鹤壁烟煤地下气化模拟试验研究[J].化学工程,2014,12(12):63-66,78.
[20]张乐,谌伦建,邢宝林,等.烟煤地下气化半焦对模拟废水中苯酚的脱除[J].化工进展,2015,12(9):3790-3794.
[21]曾昭琼.有机化学[M].3版.北京:高等教育出版社,1993.
[22]LUTYNSKI Marcin,SUPONIK Tomasz.Hydrocarbons removal from underground coal gasification water by organic adsorbents[J].Physicochem Probl Miner Process,2014,50(1):289-298.
[23]国家环境保护总局.污水排放标准:GB 8978—1996[S].北京:中国标准出版社,1998.