油泥与微藻生物质掺混共热解动力学研究
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摘要
针对油泥与微藻生物质掺混共热解处理工艺,利用热分析仪在N_2气氛下对其进行不同升温速率(β)以及不同掺混比(φ)的实验研究,分析了各自组成及性质,通过分析质量损失(TG)、质量损失变化率(DTG)曲线,对热解过程进行反应阶段划分。此外,采用Doyle积分及Hancock经验公式进行热解动力学参数拟合求解。实验结果表明,油泥与微藻掺混热解过程可划分为5个阶段;其中,掺混共热解过程中阶段Ⅱ、Ⅲ、Ⅳ的反应级数分别为1级、1.5级、0.5级,活化能分别为15.07～42.34 kJ/mol、62.69～76.86 kJ/mol、7.99～15.66 kJ/mol;油泥与微藻掺混共热解,改善了油泥的颗粒形态,提高了传热传质效率,降低了反应阻力,从而降低了热解过程中的活化能。
To investigate co-pyrolysis treatment of oil sludge and microalgae, the composition and properties of oil sludge and microalgae were analyzed, respectively. With utilizing a thermogravimetric analyzer, co-pyrolysis experiments were performed with different heating rates(β) and mixing ratios(φ) under nitrogen atmosphere. The thermogravimetry(TG) curves and derivative thermogravimetric(DTG) curves were analyzed to understand the co-pyrolysis reaction kinetics. Experimental results show that the co-pyrolysis process can be divided into several different stages. In addition, Doyle integral and Hancock empirical formula were applied to obtain kinetic parameters from experimental data. It was found that there are five stages in the sludge and microalgae co-pyrolysis process. Reaction orders of stage Ⅱ, Ⅲ and Ⅳ are 1, 1.5 and 0.5, respectively, and their corresponding activation energies are 15.07-42.34 kJ/mol, 62.69-76.86 kJ/mol, and 7.99-15.66 kJ/mol. Co-pyrolysis of oil sludge and microalgae can lead to preferred particle morphology, improve heat and mass transfer efficiency, reduce the reaction resistance, and thus reduce activation energy in the pyrolysis process.
To investigate co-pyrolysis treatment of oil sludge and microalgae, the composition and properties of oil sludge and microalgae were analyzed, respectively. With utilizing a thermogravimetric analyzer, co-pyrolysis experiments were performed with different heating rates(β) and mixing ratios(φ) under nitrogen atmosphere. The thermogravimetry(TG) curves and derivative thermogravimetric(DTG) curves were analyzed to understand the co-pyrolysis reaction kinetics. Experimental results show that the co-pyrolysis process can be divided into several different stages. In addition, Doyle integral and Hancock empirical formula were applied to obtain kinetic parameters from experimental data. It was found that there are five stages in the sludge and microalgae co-pyrolysis process. Reaction orders of stage Ⅱ, Ⅲ and Ⅳ are 1, 1.5 and 0.5, respectively, and their corresponding activation energies are 15.07-42.34 kJ/mol, 62.69-76.86 kJ/mol, and 7.99-15.66 kJ/mol. Co-pyrolysis of oil sludge and microalgae can lead to preferred particle morphology, improve heat and mass transfer efficiency, reduce the reaction resistance, and thus reduce activation energy in the pyrolysis process.
引文
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[2]JINSHENG Z,MINGHUA Z.Perspectives on recent development in oily sludge treatment[J].Oxidation Communications,2015,38(4):1813-1822.
[3]HU G,LI J,ZENG G.Recent development in the treatment of oily sludge from petroleum industry:A review[J].J Hazard Mater,2013,261(13):470-490.
[4]SCHMIDT H,KAMINSKY W.Pyrolysis of oil sludge in a fluidised bed reactor[J].Chemosphere,2001,45(3):285-290.
[5]SáNCHEZ M,MENéNDEZ J,DOMíNGUEZ A,et al.Effect of pyrolysis temperature on the composition of the oils obtained from sewage sludge[J].Biomass and Bioenergy,2009,33(6):933-940.
[6]全翠,李爱民,高宁博,等.采用热解方法回收油泥中原油[J].石油学报(石油加工),2010,26(5):742-746.(QUAN Cui,LI Aimin,GAO Ningbo,et al.Oil recovery from oily-sludge by pyrolysis method[J].Acta Petrolei Sinica(Petroleum Processing Section),2010,26(5):742-746.)
[7]KARAYILDIRIM T,YANIK J,YUKSEL M,et al.Characterisation of products from pyrolysis of waste sludges[J].Fuel,2006,85(10):1498-1508.
[8]CHENG S,WANG Y,FUMITAKE T,et al.Effect of steam and oil sludge ash additive on the products of oil sludge pyrolysis[J].Applied Energy,2017,185(Part 1):146-157.
[9]CHENG S,WANG Y,GAO N,et al.Pyrolysis of oil sludge with oil sludge ash additive employing a stirred tank reactor[J].Journal of Analytical and Applied Pyrolysis,2016,120:511-520.
[10]HU G,LI J,ZHANG X,et al.Investigation of waste biomass co-pyrolysis with petroleum sludge using a response surface methodology[J].Journal of Environmental Management,2017,192:234-242.
[11]ALVAREZ J,AMUTIO M,LOPEZ G,et al.Fast co-pyrolysis of sewage sludge and lignocellulosic biomass in a conical spouted bed reactor[J].Fuel,2015,159:810-818.
[12]LIU J,JIANG X,ZHOU L,et al.Pyrolysis treatment of oil sludge and model-free kinetics analysis[J].Journal of Hazardous Materials,2009,161(2):1208-1215.
[13]WANG Z,GUO Q,LIU X,et al.Low temperature pyrolysis characteristics of oil sludge under various heating conditions[J].Energy&Fuels,2007,21(2):957-962.
[14]岳勇,刘鹏,王蓉沙,等.油田含油污泥与芦苇共热解实验研究[J].油气田环境保护,2012,22(1):7-9.(YUE Yong,LIU Peng,WANG Rongsha,et al.Study on co-pyrolysis of oily sludge and reeds[J].Environmental Protection of Oil&Gas Fields,2012,22(1):7-9.)
[15]WANG X,ZHAO B,YANG X.Co-pyrolysis of microalgae and sewage sludge:Biocrude assessment and char yield prediction[J].Energy Conversion and Management,2016,117:326-334.
[16]宋薇,刘建国,聂永丰.含油污泥组成及其对热解特性的影响[J].环境科学,2008,29(7):2063-2067.(SONG Wei,LIU Jianguo,NIE Yongfeng.Components of oil sludge and their influence on pyrolysis behaviors[J].Environmental Science,2008,29(7):2063-2067.)
[18]胡荣祖,高胜利,赵凤起,等.热分析动力学[M].北京:科学出版社,2001:31-32.
[19]于伯龄,姜胶东.实用热分析[M].北京:纺织工业出版社,1990:151-156.
[20]RAZMJOO N,SEFIDARI H.Thermal treatment of sludge[M].Sweden:School of Engineering,University of Borás,2011:9-10.
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