CO_2/N_2气氛下煤粉热解气化特性研究及动力学分析
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摘要
采用热重分析仪在CO_2/N_2气氛下对煤粉进行了非等温热解气化实验研究,分析了程序升温速率和CO2浓度对煤粉热解、气化特性的影响,并采用Coats-Redfern法、FWO法和KAS法对煤粉热解、气化过程进行了动力学分析。实验结果表明:在CO_2/N_2气氛下,随着程序升温速率的升高,热解和气化反应速率均增大,表观活化能均减小。在CO_2/N_2气氛下,CO2不会影响煤粉的热解过程,而对气化过程有决定性影响,CO2浓度越高,气化反应速率越大,表观活化能越大。在CO_2/N_2气氛中煤粉气化反应的表观活化能E和表观指前因子A之间具有动力学补偿效应。在相同气氛下,煤粉气化反应的表观活化能随转化率的增大而减小。
The non-isothermal pyrolysis and gasification of pulverized coal in CO_2/N_2 atmosphere were performed by thermogravimetric analyzer in order to study the effects of heating rate and CO_2 concentration on pyrolysis and gasification characteristics.CoatsRedfern method,FWO method and KAS method were adopted to analyze the kinetics of pulverized coal pyrolysis and gasification.The experimental results indicated that the reaction rate of pyrolysis and gasification increased and the apparent activation energy decreased with the increase in heating rate under CO_2/N_2 atmosphere.CO_2 didn't affect the pyrolysis process of pulverized coal in CO_2/N_2 atmosphere,but it had a decisive influence on the gasification process.The gasification rate and the apparent activation energy increased with the increase in CO_2 concentration.There existed a kinetic compensation effect between the activation energy E and the pre-exponential factor A of the pulverized coal gasification in CO_2/N_2 atmosphere.Under the same atmosphere,the apparent activation energy of pulverized coal gasification decreased with the increase of conversion.
The non-isothermal pyrolysis and gasification of pulverized coal in CO_2/N_2 atmosphere were performed by thermogravimetric analyzer in order to study the effects of heating rate and CO_2 concentration on pyrolysis and gasification characteristics.CoatsRedfern method,FWO method and KAS method were adopted to analyze the kinetics of pulverized coal pyrolysis and gasification.The experimental results indicated that the reaction rate of pyrolysis and gasification increased and the apparent activation energy decreased with the increase in heating rate under CO_2/N_2 atmosphere.CO_2 didn't affect the pyrolysis process of pulverized coal in CO_2/N_2 atmosphere,but it had a decisive influence on the gasification process.The gasification rate and the apparent activation energy increased with the increase in CO_2 concentration.There existed a kinetic compensation effect between the activation energy E and the pre-exponential factor A of the pulverized coal gasification in CO_2/N_2 atmosphere.Under the same atmosphere,the apparent activation energy of pulverized coal gasification decreased with the increase of conversion.
引文
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[2]岑建孟,方梦祥,王勤辉,等.煤分级利用多联产技术及其发展前景[J].化工进展,2011,30(1):88-94.
[3]陆小泉.我国煤炭清洁开发利用现状及发展建议[J].煤炭工程,2016,48(3):8-10.
[4]WALL T,LIU Y,SPERO C,et al.An overview on oxyfuel coal combustion-State of the art research and technology development[J].Chemical Engineering Research&Design,2009,87(8):1003-1016.
[5]RATHNAM R K,ELLIOTT L K,WALL T F,et al.Differences in reactivity of pulverised coal in air(O2/N2)and oxy-fuel(O2/CO2)conditions[J].Fuel Processing Technology,2009,90(6):797-802.
[6]熊伯春,杨卫娟,王智化,等.煤的超高温热解与气化特性的热重实验研究[J].煤炭转化,2016,39(4):15-20.
[7]王琳俊,马阳,刘加勋,等.超细煤粉热解特性及热解反应动力学研究[J].锅炉技术,2015,46(6):73-78.
[8]齐永锋,章明川,张健,等.超细煤粉快速热解动力学特性实验研究[J].化学工程,2009,37(3):62-65.
[9]王俊琪,方梦祥,骆仲泱,等.煤的快速热解动力学研究[J].中国电机工程学报,2007,27(17):18-22.
[10]STARINK M J.The determination of activation energy from linear heating rate experiments:a comparison of the accuracy of isoconversion methods[J].Thermochimica Acta,2003,404(1-2):163-176.
[11]WANG C,LIU Y,ZHANG X,et al.A study on coal properties and combustion characteristics of blended coals in northwestern china[J].Energy&Fuels,2011,25(8):3634-3645.
[12]闵凡飞,张明旭.热分析在煤燃烧和热解及气化动力学研究中的应用[J].煤炭转化,2004,27(1):9-12.
[13]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.
[14]徐迪,王波,袁益超,等.混煤燃烧特性的试验研究及反应动力学分析[J].锅炉技术,2013,44(6):40-43.
[15]YORULMAZ S Y,ATIMTAY A T.Investigation of combustion kinetics of treated and untreated waste wood samples with thermogravimetric analysis[J].Fuel Processing Technology,2009,90(7):939-946.
[16]傅旭峰,仲兆平,肖刚,等.不同生物质热解特性及动力学的对比研究[J].锅炉技术,2011,42(5):60-64.
[17]SHU P Z,YU L W,MING D Y,et al.Pyrolysis characteristics and kinetics of the marine microalgae Dunaliella tertiolecta using thermogravimetric analyzer[J].Bioresource Technology,2010,101(1):359-365.
[18]BOONCHOM B,PUTTAWONG S.Thermodynamics and kinetics of the dehydration reaction of FePO4·2H2O[J].Physica B Condensed Matter,2010,405(9):2350-2355.
[19]王俊琪,方梦祥,骆仲泱,等.煤在CO2气氛中的热解气化动力学研究[J].热力发电,2010,39(5):46-49.
[20]吴国光,张荣光.煤炭气化工艺学[M].徐州:中国矿业大学出版社,2015.
[21]谢克昌.煤的结构与反应性[M].北京:科学出版社,2002.
[22]尹瑞丽,陈利平,陈网桦,等.两种量热模式下物质热分解的动力学补偿效应[J].物理化学学报,2016(2):391-398.
[23]张力,彭锦,杨仲卿.CO2气氛下劣质煤气化及动力学特性实验研究[J].热能动力工程,2012,27(3):336-341.
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