不同气氛下煤矸石热解特性及热解动力学机理
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摘要
煤矸石是目前排放量最大的工业固体废弃物之一,具有低挥发分、高灰分、低热值和难燃烧等特点,从而限制了煤矸石大规模能源化利用,采用低热值气体与煤矸石混合燃烧可有效提高其燃烧效果。在燃烧过程中,低热值气体组分对煤矸石热解特性有重要影响,合理气氛下煤矸石的热解对提高燃烧效率有重要作用。目前,关于这方面的研究比较少,对煤矸石在不同气氛下的热解特性与机理也未被充分的认识和理解,阻碍了煤矸石能源化技术的进一步应用和发展,因此,研究煤矸石在不同气氛下的热解特性及动力学机理是非常必要的。
于此,本文在深入分析煤矸石和低热值气体利用现状和形势的基础上,对煤矸石特性进行了分析,考察了煤矸石组成成分的特点。采用非等温热重法对4种不同产地的煤矸石进行了热重试验分析。研究了不同煤矸石种类,不同升温速率,不同试样粒径,不同压力和CO2或CH4与N2的混合比例为10%,30%,60%,100%的混合气氛等试验参数对煤矸石热解特性的影响,并在此基础上,进行了煤矸石在不同气氛下热解动力学机理研究,得出以下主要结论:
(1)不同产区的煤矸石成分差别比较大。其中,煤矸石挥发分含量在9.69%～13.26%,固定碳含量在6.35%～30.3%,灰分含量在54.67%～82.4%。煤矸石C元素含量在39%～55%,H元素含量在1.1%～2.3%,氧含量在1.9%～6.5%之间。
(2)煤矸石在热解过程中随温度的升高经历三个阶段:低温失重阶段,主要热分解阶段和二次脱气阶段。热解温度是影响煤矸石热解反应最主要的因素。
(3)煤矸石热解的挥发分初析温度、挥发分析出最大速率及其对应的温度,以及挥发分析出特性指数D随煤矸石种类、样品粒径、热解升温速率、压力和气氛的不同差别较大。
(4)不同气氛对煤矸石的热解影响是分段进行的。不同的温度段有不同影响程度,提出可用N2气氛下与其它气体组分下热解失重百分率之差ΔW =ΔWN 2?ΔW气氛来判定不同气氛对煤矸石热解转化率的影响。
(5)CH4气氛对煤矸石的热解促进作用存在着一个最佳温度段△Topt。CH4在析碳温度之前,对煤矸石的热解均表现为促进作用。
(6)不同气氛下煤矸石热解过程很复杂,均不能用一步反应描述。在煤矸石热解第一阶段,热解反应服从三维球形扩散模型(D4模型);热解第二阶段受液化反应的控制,热解过程服从级数为2的化学反应(F2模型)模型;热解第三阶段根据煤种的不同而不同,含碳量高的煤矸石热解过程服从级数为2的化学反应模型(F2模型),含碳量低的煤矸石(C<10%)服从级数为1的化学反应模型(F1模型)。
(7)不同气氛下,煤矸石活化能均呈现出在热解第一、第三阶段较小,第二阶段最大现象。不同煤矸石在相同的热解阶段的活化能差别较大。
(8)CO2气氛下,煤矸石活化能在热解第一、第二阶段随着CO2浓度的增高而增大,第三阶段随着CO2浓度的增高而降低。而在CH4气氛下,活化能在热解的第一阶段随着CH4浓度的增高而降低,在第二阶段活化能随CH4浓度增加而升高。
本文通过煤矸石在不同气氛下的热解特性的研究,为煤矸石与低热值气体的混合热解技术的发展建立了一定的理论基础,也为今后的深入研究提供了有价值的参考依据。
Coal residue is one of the most quantity industrial solid residues,with the characteristics of lower volatile, high ash, lower heat value and hard-to-burn. So, the large scale utilization of coal residue is limited. Co-combustion of low caloric gas and coal residue could improve the combustion efficiently. In the combustion, the component of low caloric gas influence the characteristics of coal residue pyrolysis greatly. Pyrolysis in the appropriate atmosphere is important to the combustion efficiency. So far, research in this field is limitted and the characteristics and mechanisms of coal residue pyrolysis in different atmosphere are covered and un-recognized, which hindering the further utilization and development. So, it is necessary to study the characteristics and mechanisms of coal residue pyrolysis in different atmosphere.
Based on the deeply analysis of the status of utilization and the situation of coal residue and low caloric gas, the characteristics of coal residue was analyzed. The experiments of coal residue pyrolysis have been investigated on 4 kinds of different coal residues by non-isothermal thermogravimetric method, researching the effects of experiment parameters, such as different heat rate, different sample diameter, different pressure and different gas mixture of CO2 or CH4 with N2 with the concentration of 10%, 30%, 60%, 100%, to the pyrolysis characteristics, then analyzing the kinetic characteristics. The main conclusions are as follow:
(1) The component of different coal residues changed. The content of volatile is 9.69%～13.26%, the content of Fixed Carbon is 6.35%～30.3%, the content of Ash is 54.67%～82.4%. The content of constituent is Carbon 39%～55%,Hydrogen 1.1%～2.3%,Oxygen 1.9%～6.5%.
(2) With the rise of the temperature, coal residues pyrolysis experienced three stages: low temperature weight loss stage; main decomposes stage and second release gas stage. Temperature is the main factor to influence the coal residue pyrolysis.
(3) The primary pyrolysis temperature, (dw/dt)max and its temperature, quality number D vary with different coal residues, sample diameter, heat rate, pressure and atmosphere.
(4) The influence of atmosphere is different at respective pyrolysis phases.ΔW =ΔW N 2 ?ΔWatmosphere is used for judging the degree of percent conversion.
(5) A most optimum pyrolysis temperature phase△Topt exists in the pyrolysis process in the CH4 atmosphere. Before the carbon deposition temperature, CH4 improves the pyrolysis,ΔW CH4could express that.
(6) The coal residue pyrolysis is very complicated in the different atmosphere; the whole process can not be described by one step reaction. The results show that in the first stage, the pyrolysis reaction obeys the mechanism of three-dimensi onal spherical diffusion(D4); In the second stage, the reaction obeys the liquefaction reaction and the progression of chemical reaction is 2(F2);in the third stage, the pyrolysis of high Carbon coal residues still obeyed F2, but the lower Carbon’s(C<10%) obeyed the chemical reaction with the progression of 1(F1).
(7) In the different atmosphere, the activation energy is lower in the fist and third stage, the higher in the second stage. The same stage of different coal residues have the different activation energy.
(8) In CO2 atmosphere, the activation energy is higher and higher with the higher CO2 concentration in the first and second stage, but lower in the third stage. Whereas, in the CH4 atmosphere, the activation energy is lower and lower with the higher CH4 concentration in the first stage and higher in the second stage.
The conclusion from above experiments and analysis of coal residue pyrolysis in the different atmosphere are helpful to the development of co-pyrolysis of coal residue and low caloric gas and supply valuable reference data for more research in this field.
于此,本文在深入分析煤矸石和低热值气体利用现状和形势的基础上,对煤矸石特性进行了分析,考察了煤矸石组成成分的特点。采用非等温热重法对4种不同产地的煤矸石进行了热重试验分析。研究了不同煤矸石种类,不同升温速率,不同试样粒径,不同压力和CO2或CH4与N2的混合比例为10%,30%,60%,100%的混合气氛等试验参数对煤矸石热解特性的影响,并在此基础上,进行了煤矸石在不同气氛下热解动力学机理研究,得出以下主要结论:
(1)不同产区的煤矸石成分差别比较大。其中,煤矸石挥发分含量在9.69%～13.26%,固定碳含量在6.35%～30.3%,灰分含量在54.67%～82.4%。煤矸石C元素含量在39%～55%,H元素含量在1.1%～2.3%,氧含量在1.9%～6.5%之间。
(2)煤矸石在热解过程中随温度的升高经历三个阶段:低温失重阶段,主要热分解阶段和二次脱气阶段。热解温度是影响煤矸石热解反应最主要的因素。
(3)煤矸石热解的挥发分初析温度、挥发分析出最大速率及其对应的温度,以及挥发分析出特性指数D随煤矸石种类、样品粒径、热解升温速率、压力和气氛的不同差别较大。
(4)不同气氛对煤矸石的热解影响是分段进行的。不同的温度段有不同影响程度,提出可用N2气氛下与其它气体组分下热解失重百分率之差ΔW =ΔWN 2?ΔW气氛来判定不同气氛对煤矸石热解转化率的影响。
(5)CH4气氛对煤矸石的热解促进作用存在着一个最佳温度段△Topt。CH4在析碳温度之前,对煤矸石的热解均表现为促进作用。
(6)不同气氛下煤矸石热解过程很复杂,均不能用一步反应描述。在煤矸石热解第一阶段,热解反应服从三维球形扩散模型(D4模型);热解第二阶段受液化反应的控制,热解过程服从级数为2的化学反应(F2模型)模型;热解第三阶段根据煤种的不同而不同,含碳量高的煤矸石热解过程服从级数为2的化学反应模型(F2模型),含碳量低的煤矸石(C<10%)服从级数为1的化学反应模型(F1模型)。
(7)不同气氛下,煤矸石活化能均呈现出在热解第一、第三阶段较小,第二阶段最大现象。不同煤矸石在相同的热解阶段的活化能差别较大。
(8)CO2气氛下,煤矸石活化能在热解第一、第二阶段随着CO2浓度的增高而增大,第三阶段随着CO2浓度的增高而降低。而在CH4气氛下,活化能在热解的第一阶段随着CH4浓度的增高而降低,在第二阶段活化能随CH4浓度增加而升高。
本文通过煤矸石在不同气氛下的热解特性的研究,为煤矸石与低热值气体的混合热解技术的发展建立了一定的理论基础,也为今后的深入研究提供了有价值的参考依据。
Coal residue is one of the most quantity industrial solid residues,with the characteristics of lower volatile, high ash, lower heat value and hard-to-burn. So, the large scale utilization of coal residue is limited. Co-combustion of low caloric gas and coal residue could improve the combustion efficiently. In the combustion, the component of low caloric gas influence the characteristics of coal residue pyrolysis greatly. Pyrolysis in the appropriate atmosphere is important to the combustion efficiency. So far, research in this field is limitted and the characteristics and mechanisms of coal residue pyrolysis in different atmosphere are covered and un-recognized, which hindering the further utilization and development. So, it is necessary to study the characteristics and mechanisms of coal residue pyrolysis in different atmosphere.
Based on the deeply analysis of the status of utilization and the situation of coal residue and low caloric gas, the characteristics of coal residue was analyzed. The experiments of coal residue pyrolysis have been investigated on 4 kinds of different coal residues by non-isothermal thermogravimetric method, researching the effects of experiment parameters, such as different heat rate, different sample diameter, different pressure and different gas mixture of CO2 or CH4 with N2 with the concentration of 10%, 30%, 60%, 100%, to the pyrolysis characteristics, then analyzing the kinetic characteristics. The main conclusions are as follow:
(1) The component of different coal residues changed. The content of volatile is 9.69%～13.26%, the content of Fixed Carbon is 6.35%～30.3%, the content of Ash is 54.67%～82.4%. The content of constituent is Carbon 39%～55%,Hydrogen 1.1%～2.3%,Oxygen 1.9%～6.5%.
(2) With the rise of the temperature, coal residues pyrolysis experienced three stages: low temperature weight loss stage; main decomposes stage and second release gas stage. Temperature is the main factor to influence the coal residue pyrolysis.
(3) The primary pyrolysis temperature, (dw/dt)max and its temperature, quality number D vary with different coal residues, sample diameter, heat rate, pressure and atmosphere.
(4) The influence of atmosphere is different at respective pyrolysis phases.ΔW =ΔW N 2 ?ΔWatmosphere is used for judging the degree of percent conversion.
(5) A most optimum pyrolysis temperature phase△Topt exists in the pyrolysis process in the CH4 atmosphere. Before the carbon deposition temperature, CH4 improves the pyrolysis,ΔW CH4could express that.
(6) The coal residue pyrolysis is very complicated in the different atmosphere; the whole process can not be described by one step reaction. The results show that in the first stage, the pyrolysis reaction obeys the mechanism of three-dimensi onal spherical diffusion(D4); In the second stage, the reaction obeys the liquefaction reaction and the progression of chemical reaction is 2(F2);in the third stage, the pyrolysis of high Carbon coal residues still obeyed F2, but the lower Carbon’s(C<10%) obeyed the chemical reaction with the progression of 1(F1).
(7) In the different atmosphere, the activation energy is lower in the fist and third stage, the higher in the second stage. The same stage of different coal residues have the different activation energy.
(8) In CO2 atmosphere, the activation energy is higher and higher with the higher CO2 concentration in the first and second stage, but lower in the third stage. Whereas, in the CH4 atmosphere, the activation energy is lower and lower with the higher CH4 concentration in the first stage and higher in the second stage.
The conclusion from above experiments and analysis of coal residue pyrolysis in the different atmosphere are helpful to the development of co-pyrolysis of coal residue and low caloric gas and supply valuable reference data for more research in this field.
引文
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