煤基近零排放系统建模分析及系统内煤加氢气化机理研究
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摘要
依靠电力运行的载运工具,动力大多来自燃煤电站,对于以气为动力源的载运工具,若能利用煤制合成气,也能够充分适应我国“富煤、贫油、少气”的能源结构特点。因此,研究开发新型高效洁净煤利用与转化技术对我国而言意义重大。本文以一种煤基近零排放发电系统(ZEC:Zero Emission Coal)为研究对象,首先分析了系统的整体运行特性,然后对系统内的煤加氢气化模块进行了深入分析研究。
首先,根据ZEC系统的思想,本文建立了ZEC系统整体模型,并对系统的主要运行单元进行了验证。分析了氢气循环率风,钙碳摩尔比Rctc以及燃料电池的燃料利用率Uf等主要参数对系统能量效率Een、(?)效率Eex、总能量效率Eten和总(?)效率Etex以及CO2捕集效率Rcs的影响,提出所建系统的最优运行参数为Rh=0.75,Rctc=1.5以及Uf=0.8。在该运行参数下,系统的Een为36.2%,Etom为46.8%, Eex为35.7%,Etex为46.2%,Rc,为87.4%。随后,计算分析了系统中各个单元的能量和(?)的平衡关系,对比了系统各单元能量和(?)损失的大小,发现汽轮机中的能量损失最大,而燃料电池中的(?)损失最大,由此指出为了进一步提升系统的运行效率需要降低燃料电池内高品质能量的过大损失。
在对ZEC系统整体性能进行了全面研究后,本文着重对其中的煤加氢气化模块从零维热力学平衡模型、零维化学反应动力学模型、三维数值模拟以及试验研究等方面进行了深入探析。首先,考虑到热力学平衡模型良好的通用性以及采用热力学平衡模型对煤加氢气化的研究仍不充分,本文建立了煤加氢气化热力学平衡模型,验证了模型的可靠性,并利用该模型对煤的加氢气化特性进行了预测。若对气化温度进行控制,则当压力pt为7MPa,反应温度T为1000K时,氢煤质量比Rh/c为0.25左右可以使气化产物中甲烷具有较高的摩尔分数。若不控制气化温度,则当pt为7MPa时,Rh/c为约0.5时,煤中的碳才能够完全转化。
其次,鉴于煤加氢气化过程的动力学计算模型尚不完善,本文建立了煤加氢气化动力学模型,验证了模型的可靠性,并利用该模型对煤加氢气化特性进行了预测分析。当pt为13MPa,反应时间t为10s,其他运行参数保持和基准运行参数一致时,煤粉整体转化率CCR可达90%,合成气中CH4的摩尔分数MMF可达32%,H2摩尔分数HMF约占60%。当其他运行参数保持和基准运行参数一致时,如果T不超过1273K,则增加T可以从整体上促进煤加氢气化反应的进行。如果T高于1273K,增加T会对煤的加氢气化反应起到抑制作用。
由于鲜见国内外对煤的加氢气化炉三维数值模拟结果的报道,本文完善了煤的加氢气化动力学模型,提出了针对气固异相反应的“带有压力修正的联合随机孔隙-未反应碳缩核模型(CRPSC-PC:Combined Random Pore and Shrinking Core Model with Pressure Correction)",在此基础上针对气流床煤加氢气化炉建立了带有化学反应的气固两相流三维数学模型,并借助商业软件Fluent对该模型进行求解,在所用的模拟方法得到验证后,利用该模型对某气化炉的加氢气化特性进行了预测分析。经过综合分析发现,该气化炉的最佳运行工况组合为pt=7MPa,Rh/c,＝0.4,氧氢质量比Ro/h=1.5。在这一运行条件组合下,Rchar为96.78%,MMF为17.42%,冷气效率CGE为76.4%。
最后,考虑到煤加氢热解和气化的动力学基础数据尚不完善,本文对一种褐煤、一种烟煤进行了加压热重分析,研究了不同压力下褐煤、烟煤的失重曲线、失重速率曲线,获得了反应动力学特性的典型参数,确定了反映褐煤、烟煤加氢热解和加氢气化的动力学机理函数并计算了不同压力下褐煤、烟煤的动力学参数,分析了不同压力下褐煤及烟煤加氢热解和加氢气化过程的动力学补偿效应。
For the traveling transportation vehicles drived by electricity, most of the power is generated in the coal-fired power station. For gas driveling vehicles, it would be very suitable for the Chinese situation of "rich coal, meager oil and little gas" if part of the gas could be produced by coal gasification. It is, therefore, very meaningful to study the novel, clean and efficient coal utilization technologies. The present work aims to study the integrated operation property of a zero emission coal (ZEC) system and the coal hydro-gasification (CHG) characteristics in the system.
First, a detailed ZEC system is setup based on the original ZEC concept and the effects of operating parameters including H2recycling ratio (Rh), calcium to carbon ratio (Rctc) and fuel utilization factor (Uf) on the energy efficiency (Een), exergy efficiency (Eex), total energy efficiency (Een), total exergy efficiency (Eex) and carbon dioxide (CO2) sequestration ratio (Rcs) are analyzed for this system. Rh of0.75, Uf of0.8and Rctc of1.5are found the optimum operation parameters. With these parameters, the ZEC system can achieve Een of36.2%, Eten of46.8%, Eex of35.7%, Etex of46.2%, and Rcs of87.4%. The energy and exergy analyses of the system are then implemented and the maximum energy loss is found occuring in the steam turbine (ST) while the maximum exergy loss occuring in the solid oxide fuel cell (SOFC). Thus, to further improve the system efficiency, the exergy efficiency of SOFC should be improved.
After the performance of the ZEC system is evaluated in detail, the CHG component of the system is then focused and studied deeply from the views of chemical equilibrium, chemical kinetics, numerical simulation and experiments. In view of the universality of the chemical equilibrium method and the lack of study on CHG with this method, a chemical equilibrium model (CEM) for CHG is firstly proposed to study the effects of different reaction conditions on the CHG characteristics. The results from the model are then validated against literature available experimental data and the model is proved reliable. When pt is7MPa and T is1,000K, the carbon will be totally converted when Rh/c is about0.25and the maximum methane mole fraction (MMF) will be obtained. If T is not controlled, carbon will be all converted at7MPa when Rh/c is about0.5.
Then, in view of the lack of kinetic models reported for CHG, a hydrogasification kinetic model is established and validated against experimental data available in literatures. The model is then used to predict the effects of different reaction conditions on the CHG properties. When pt is13MPa, the reaction time t is10s and other parameters are kept consistent with those of the baseline case, the coal conversion ratio (CCR) is nearly0.9, CH4mole fraction is about0.32and H2mole fraction is about0.6. Increasing T can promote the hydrogasification process when it is not higher than1273K. When T is higher than1273K, however, increasing T will restrain the gasification process.
After that, the CHG kinetic model is studied further and a Combined Random Pore and Shrinking Core Model with Pressure Correction (CRPSC-PC) is developed for the heterogeneous reactions. Then, considering the muti-dimensional n umerical simulations about entrained flow coal hydrogasifier are still rarely reported, a three-dimensional mathematical model about the gas-solid turbulent flow with chemical reaction is set up and solved with the assistant of Fluent. The simulation methods are validated and are then used to analyze the hydrogasification properties of an entrained flow bed gasifier. After comprehensive analyses, the synthetically optimal combination of the operating condition is found to he pt=7MPa, Rh/c=0.3, and Ro/h=1.5. With this combination, the char conversion ratio (Rchar) can be96.78%, MMF can be17.42%, and the cold gas efficiency (CGE) can reach76.4%.
Finally, in view of the lack of experimental data about the coal hydropyrolysis (CHP) or CHG kinetics, the hydropyrolysis and hydrogasification kinetic characteristics of a lignite coal and a bituminous coal are studied in a pressurized thermo-gravimetric analyzer (P-TGA). The thermo-gravimetric (TG) and derivative thermo-gravimetric (DTG) curves at different reaction pressures are illustrated and compared. The kinetic mechanism function is determined and the kinetic parameters are calculated. In addition, the kinetic compensation effects of the hydropyrolysis and hydrogasification processes of the lignite coal and bituminous coal are analyzed and the corresponding isokinetic points are calculated.
首先,根据ZEC系统的思想,本文建立了ZEC系统整体模型,并对系统的主要运行单元进行了验证。分析了氢气循环率风,钙碳摩尔比Rctc以及燃料电池的燃料利用率Uf等主要参数对系统能量效率Een、(?)效率Eex、总能量效率Eten和总(?)效率Etex以及CO2捕集效率Rcs的影响,提出所建系统的最优运行参数为Rh=0.75,Rctc=1.5以及Uf=0.8。在该运行参数下,系统的Een为36.2%,Etom为46.8%, Eex为35.7%,Etex为46.2%,Rc,为87.4%。随后,计算分析了系统中各个单元的能量和(?)的平衡关系,对比了系统各单元能量和(?)损失的大小,发现汽轮机中的能量损失最大,而燃料电池中的(?)损失最大,由此指出为了进一步提升系统的运行效率需要降低燃料电池内高品质能量的过大损失。
在对ZEC系统整体性能进行了全面研究后,本文着重对其中的煤加氢气化模块从零维热力学平衡模型、零维化学反应动力学模型、三维数值模拟以及试验研究等方面进行了深入探析。首先,考虑到热力学平衡模型良好的通用性以及采用热力学平衡模型对煤加氢气化的研究仍不充分,本文建立了煤加氢气化热力学平衡模型,验证了模型的可靠性,并利用该模型对煤的加氢气化特性进行了预测。若对气化温度进行控制,则当压力pt为7MPa,反应温度T为1000K时,氢煤质量比Rh/c为0.25左右可以使气化产物中甲烷具有较高的摩尔分数。若不控制气化温度,则当pt为7MPa时,Rh/c为约0.5时,煤中的碳才能够完全转化。
其次,鉴于煤加氢气化过程的动力学计算模型尚不完善,本文建立了煤加氢气化动力学模型,验证了模型的可靠性,并利用该模型对煤加氢气化特性进行了预测分析。当pt为13MPa,反应时间t为10s,其他运行参数保持和基准运行参数一致时,煤粉整体转化率CCR可达90%,合成气中CH4的摩尔分数MMF可达32%,H2摩尔分数HMF约占60%。当其他运行参数保持和基准运行参数一致时,如果T不超过1273K,则增加T可以从整体上促进煤加氢气化反应的进行。如果T高于1273K,增加T会对煤的加氢气化反应起到抑制作用。
由于鲜见国内外对煤的加氢气化炉三维数值模拟结果的报道,本文完善了煤的加氢气化动力学模型,提出了针对气固异相反应的“带有压力修正的联合随机孔隙-未反应碳缩核模型(CRPSC-PC:Combined Random Pore and Shrinking Core Model with Pressure Correction)",在此基础上针对气流床煤加氢气化炉建立了带有化学反应的气固两相流三维数学模型,并借助商业软件Fluent对该模型进行求解,在所用的模拟方法得到验证后,利用该模型对某气化炉的加氢气化特性进行了预测分析。经过综合分析发现,该气化炉的最佳运行工况组合为pt=7MPa,Rh/c,＝0.4,氧氢质量比Ro/h=1.5。在这一运行条件组合下,Rchar为96.78%,MMF为17.42%,冷气效率CGE为76.4%。
最后,考虑到煤加氢热解和气化的动力学基础数据尚不完善,本文对一种褐煤、一种烟煤进行了加压热重分析,研究了不同压力下褐煤、烟煤的失重曲线、失重速率曲线,获得了反应动力学特性的典型参数,确定了反映褐煤、烟煤加氢热解和加氢气化的动力学机理函数并计算了不同压力下褐煤、烟煤的动力学参数,分析了不同压力下褐煤及烟煤加氢热解和加氢气化过程的动力学补偿效应。
For the traveling transportation vehicles drived by electricity, most of the power is generated in the coal-fired power station. For gas driveling vehicles, it would be very suitable for the Chinese situation of "rich coal, meager oil and little gas" if part of the gas could be produced by coal gasification. It is, therefore, very meaningful to study the novel, clean and efficient coal utilization technologies. The present work aims to study the integrated operation property of a zero emission coal (ZEC) system and the coal hydro-gasification (CHG) characteristics in the system.
First, a detailed ZEC system is setup based on the original ZEC concept and the effects of operating parameters including H2recycling ratio (Rh), calcium to carbon ratio (Rctc) and fuel utilization factor (Uf) on the energy efficiency (Een), exergy efficiency (Eex), total energy efficiency (Een), total exergy efficiency (Eex) and carbon dioxide (CO2) sequestration ratio (Rcs) are analyzed for this system. Rh of0.75, Uf of0.8and Rctc of1.5are found the optimum operation parameters. With these parameters, the ZEC system can achieve Een of36.2%, Eten of46.8%, Eex of35.7%, Etex of46.2%, and Rcs of87.4%. The energy and exergy analyses of the system are then implemented and the maximum energy loss is found occuring in the steam turbine (ST) while the maximum exergy loss occuring in the solid oxide fuel cell (SOFC). Thus, to further improve the system efficiency, the exergy efficiency of SOFC should be improved.
After the performance of the ZEC system is evaluated in detail, the CHG component of the system is then focused and studied deeply from the views of chemical equilibrium, chemical kinetics, numerical simulation and experiments. In view of the universality of the chemical equilibrium method and the lack of study on CHG with this method, a chemical equilibrium model (CEM) for CHG is firstly proposed to study the effects of different reaction conditions on the CHG characteristics. The results from the model are then validated against literature available experimental data and the model is proved reliable. When pt is7MPa and T is1,000K, the carbon will be totally converted when Rh/c is about0.25and the maximum methane mole fraction (MMF) will be obtained. If T is not controlled, carbon will be all converted at7MPa when Rh/c is about0.5.
Then, in view of the lack of kinetic models reported for CHG, a hydrogasification kinetic model is established and validated against experimental data available in literatures. The model is then used to predict the effects of different reaction conditions on the CHG properties. When pt is13MPa, the reaction time t is10s and other parameters are kept consistent with those of the baseline case, the coal conversion ratio (CCR) is nearly0.9, CH4mole fraction is about0.32and H2mole fraction is about0.6. Increasing T can promote the hydrogasification process when it is not higher than1273K. When T is higher than1273K, however, increasing T will restrain the gasification process.
After that, the CHG kinetic model is studied further and a Combined Random Pore and Shrinking Core Model with Pressure Correction (CRPSC-PC) is developed for the heterogeneous reactions. Then, considering the muti-dimensional n umerical simulations about entrained flow coal hydrogasifier are still rarely reported, a three-dimensional mathematical model about the gas-solid turbulent flow with chemical reaction is set up and solved with the assistant of Fluent. The simulation methods are validated and are then used to analyze the hydrogasification properties of an entrained flow bed gasifier. After comprehensive analyses, the synthetically optimal combination of the operating condition is found to he pt=7MPa, Rh/c=0.3, and Ro/h=1.5. With this combination, the char conversion ratio (Rchar) can be96.78%, MMF can be17.42%, and the cold gas efficiency (CGE) can reach76.4%.
Finally, in view of the lack of experimental data about the coal hydropyrolysis (CHP) or CHG kinetics, the hydropyrolysis and hydrogasification kinetic characteristics of a lignite coal and a bituminous coal are studied in a pressurized thermo-gravimetric analyzer (P-TGA). The thermo-gravimetric (TG) and derivative thermo-gravimetric (DTG) curves at different reaction pressures are illustrated and compared. The kinetic mechanism function is determined and the kinetic parameters are calculated. In addition, the kinetic compensation effects of the hydropyrolysis and hydrogasification processes of the lignite coal and bituminous coal are analyzed and the corresponding isokinetic points are calculated.
引文
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