基于物化结构特征的生物质与煤共气化特性研究
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摘要
生物质资源丰富,且可再生。将生物质与煤共气化不仅可有效减少SOx、NOx等有害物排放,还可促进碳的完全转化,提高生物质和煤气化效率。开展生物质与煤共气化技术研发对实现煤的高效清洁利用意义重大。由于生物质与煤共气化过程中产生协同作用的机理尚不明确,尤其是关于共气化过程中气相产物的形成释放机理及固体焦样表面物化结构特征的演变规律的研究并不深入,本文在对生物质与煤气化半焦微观形貌及官能团的变化规律进行分析的基础上,从理论和试验两个方面系统的开展褐煤与生物质流化床共气化特性的研究,考察了生物质掺混比、空气当量比等对流化床共气化的影响规律,揭示了生物质与煤共气化的协同作用机制。本文主要从以下几方面开展研究工作：
进行了生物质和煤共气化的热分析实验研究,详细研究了升温速率、反应气氛、掺混比例对共气化特性的影响。采用C-R法及DAEM法对生物质与煤共气化动力学特性进行研究,建立了共气化的反应动力学模型,获得了共气化动力学参数,并分析了关键反应阶段活化能的变化趋势,确定了生物质与煤共气化过程协同效应发生的反应阶段。结果表明,褐煤与生物质共气化过程由干燥、预热、挥发分析出和焦炭气化四个阶段组成,共气化在挥发分析出阶段没有表现出明显的协同作用,而在焦炭气化阶段,协同效应明显,且松木屑掺混比为50%时,协同作用最显著。共气化过程的热解段可用均相反应模型描述,气化段的反应机理符合未反应收缩核模型。焦炭气化段的活化能明显高于热解段。
在热分析实验的基础上,利用TG-FTIR联用技术开展了生物质与煤共气化气相产物析出规律的实验研究,考察了升温速率等因素对气相产物析出的影响,并结合气化半焦的微观形貌(SEM-EDX)及官能团(FTIR)分析,揭示了可燃气组分CO和CH4的析出机理。结果表明,CH4、CO口H20是褐煤气化过程中的主要气相产物,松木屑气化除之外CO、CH4、H2O之外,还还用大量醇类、醛类、酸类和酚类等有机物。共气化过程,CH4的析出归因于褐煤和松木屑的甲基、亚甲基、甲氧基中C-H键的断裂、重组,且贯穿于挥发分析出和焦炭气化的全过程；CO的析出集中于挥发分析出段和焦炭气化段,在挥发分析出段主要归因于羧基、甲氧基、羰基和醚键的断裂,气化段CO的析出主要是由于CO2参与焦炭的气化反应。升温速率对可燃气体析出有一定影响,较低的升温速率有利于CO和CH4的生成。随气化反应的进行,半焦孔隙结构经历了先增多、至逐渐塌陷、后闭合的过程。
在自行设计搭建的流化床反应器上,开展了生物质与煤共气化的试验研究,系统的研究了掺混比例、空气当量比ER、水蒸汽／燃料比S/F等操作条件对共气化特性的影响,优化了生物质与煤流化床共气化的关键参数。结果表明,松木屑的加入,有利于气体产物CO生成,对CH4无明显影响,在掺混比例为50%时,二者的协同效应最显著。气化气热值在空气当量比为0.26时达到最大值。共气化中加入水蒸汽有利于H2的生成,在S/F=0.28时,气化气热值、碳转化率和气化效率均达到最大值。
以生物质与煤流化床共气化试验数据为基础,以化工计算软件Aspen Plus为模拟平台,结合气化过程的反应动力学及流体动力学模型,采用嵌入FORTRAN气化动力学及流体动力学子程序的连续搅拌釜式反应器来表征流化床的气化反应过程,构建了流化床生物质与煤共气化的气化反应模型,模拟了掺混比例、空气当量比、水蒸汽／物料质量比对气化气组分、热值和气化效率等参数的影响,并与试验数据进行了比较,结果表明,所建模型能够准确地模拟生物质和煤的流化床气化过程。
Biomass is an abundant and renewable source of energy. Co-gasification of biomass with coal could not only reduce the harmful gases emissions such as SOx and NOx, but also obtain the complete transformation of carbon and improve the efficiency of co-gasification. Therefore, the study of the co-gasification of biomass with coal process is one of the crucial areas of the clean utilization of coal. However, the mechanism of the synergistic effect in the co-gasification of biomass with coal process remains unclear. Further studies are necessary to understand the formation of gas products, dissociation mechanisms and the evolution of physical and chemical structure characteristics occurd on the surface of coke. In this paper, the physicochemical properties of biomass and coal and the change of microstructure in gasification process were analyzed. Based on these results, co-gasification characteristic of biomass and coal in fluidized bed was systematically studied in both theory and experiment, and from the effects of various factors such as biomass blending ratio and equivalence ratio(ER), the synergistic effect mechanism of co-gasification of biomass and coal was revealed. The following investigations are made in this thesis:
The thermal analysis of co-gasification of biomass with coal was performed. The effects from heating rate, reaction atmosphere, mixing proprotion were studied on in details. The C-R and DAEM method were applied to theatrically analyze the co-gasification kinetics characteristic. A co-gasification reaction kinetics model was established, and parameters were acquired. The trend of activation energy in the critical reaction stage was analyzed. The reaction stage where co-gasification compensation effect happened was confirmed. The results showed that the co-gasification of biomass with coal process included four stages:drying, preheating, volatile precipitation and coke gasification. There was no significant synergistic effect in the volatile precipitation stage. However, a significant synergistic effect was observed in the coke gasification stage.This effect got the maximum, when mixing proprotion was50%. The pyrolysis stage of co-gasification can be described by a homogeneous reaction model. The reaction mechanism of the gasification matched the unreacted shrinking core model. The activation energy of coke gasification stage was significantly higher than that of the volatile precipitation stage.
Based on thermal analysis experiments, a TG-FTIR was employed to study the gas products of co-gasification of biomass with coal. The effects of temperature-rising rate on the gas products were studied. By the analysis of the micro surface morphology/microstructure(SEM, EDX) and functional groups (FTIR) of gasification semicoke, a mechanism of formation of the flammable gas such as CO and CH4was proposed. The results showed the evolution of the surface morphology of semicoke in the gasification. Initially, the porous cannel structure formed. Then the poles collapsed and cannels were closed eventually. The main gas products of pine sawdust gasification were CO, CH4, H2O and organic matters such asalcohols, aldehydes, carboxylic acids, phenols and so on. In the co-gasification process, the formation of CH4was the results of the rupture and reformation of C-H bonds in the methyl, methylene and methoxy groups in lignite and pine sawdust, which throughout the process of volatiles releasing and coke gasification. CO is mostly released in volatile precipitation stage and coke gasification stage, which can be attributed to carboxyl, methoxy, carbonyl, ether bond rupture in volatile precipitation stage and the reduction of CO2in coke gasification. The gasification heating-rate affect the formation of the gas products. A lower gasification heating-rate might lead to more CO and CH4.
The experimental investigation of co-gasification of biomass and coal was carried out on a self-designed fluidized bed reactor. The effects of biomass blending ratio, equivalence ratio(ER) as well as steam-to-fuel ratio(S/F) on co-gasification characteristic of biomass and coal were systematically studied, the above results provide a basis for selection and operation of co-gasification system of biomass and coal. The test results showed that when the blending ratio of pine sawdust increases, the volume concentration of CO incereased, the change of CH4was not notable, the heating value reached a maximum at a blending ratio of50%. The gasification efficiency reached a maximum at an ER of0.26. The results showed that the introduction of steam resulted in more hydrogen production. When the steam-to-fuel ratio(S/F) was0.28, the heating value, the carbon conversion ratio and the gasification efficiency all reached the maximum.
Based on the bed test of the co-gasification of biomass with coal, the ASPEN PLUS was applied to simulate the co-gasification of biomass with coal in a fluidized bed gasifier by considering the hydrodynamic and reaction rate kinetics simultaneously, the external FORTRAN subroutines for hydrodynamics and kinetics nested in ASPEN PLUS simulate the gasification process, the model was developed to study the co-gasification of biomass with coal in fluidized bed gasifier was employed to studied the effects of equivalence ratio(ER), blending ratio as well as steam-to-fuel ratio(S/F) on the gas composition, heating value and gasification efficiency, and the results were compared with the experimental results. Above results show that the co-gasification of biomass with coal in fluidized bed gasifier could be simulated accurately with the model developed in this thesis.
进行了生物质和煤共气化的热分析实验研究,详细研究了升温速率、反应气氛、掺混比例对共气化特性的影响。采用C-R法及DAEM法对生物质与煤共气化动力学特性进行研究,建立了共气化的反应动力学模型,获得了共气化动力学参数,并分析了关键反应阶段活化能的变化趋势,确定了生物质与煤共气化过程协同效应发生的反应阶段。结果表明,褐煤与生物质共气化过程由干燥、预热、挥发分析出和焦炭气化四个阶段组成,共气化在挥发分析出阶段没有表现出明显的协同作用,而在焦炭气化阶段,协同效应明显,且松木屑掺混比为50%时,协同作用最显著。共气化过程的热解段可用均相反应模型描述,气化段的反应机理符合未反应收缩核模型。焦炭气化段的活化能明显高于热解段。
在热分析实验的基础上,利用TG-FTIR联用技术开展了生物质与煤共气化气相产物析出规律的实验研究,考察了升温速率等因素对气相产物析出的影响,并结合气化半焦的微观形貌(SEM-EDX)及官能团(FTIR)分析,揭示了可燃气组分CO和CH4的析出机理。结果表明,CH4、CO口H20是褐煤气化过程中的主要气相产物,松木屑气化除之外CO、CH4、H2O之外,还还用大量醇类、醛类、酸类和酚类等有机物。共气化过程,CH4的析出归因于褐煤和松木屑的甲基、亚甲基、甲氧基中C-H键的断裂、重组,且贯穿于挥发分析出和焦炭气化的全过程；CO的析出集中于挥发分析出段和焦炭气化段,在挥发分析出段主要归因于羧基、甲氧基、羰基和醚键的断裂,气化段CO的析出主要是由于CO2参与焦炭的气化反应。升温速率对可燃气体析出有一定影响,较低的升温速率有利于CO和CH4的生成。随气化反应的进行,半焦孔隙结构经历了先增多、至逐渐塌陷、后闭合的过程。
在自行设计搭建的流化床反应器上,开展了生物质与煤共气化的试验研究,系统的研究了掺混比例、空气当量比ER、水蒸汽／燃料比S/F等操作条件对共气化特性的影响,优化了生物质与煤流化床共气化的关键参数。结果表明,松木屑的加入,有利于气体产物CO生成,对CH4无明显影响,在掺混比例为50%时,二者的协同效应最显著。气化气热值在空气当量比为0.26时达到最大值。共气化中加入水蒸汽有利于H2的生成,在S/F=0.28时,气化气热值、碳转化率和气化效率均达到最大值。
以生物质与煤流化床共气化试验数据为基础,以化工计算软件Aspen Plus为模拟平台,结合气化过程的反应动力学及流体动力学模型,采用嵌入FORTRAN气化动力学及流体动力学子程序的连续搅拌釜式反应器来表征流化床的气化反应过程,构建了流化床生物质与煤共气化的气化反应模型,模拟了掺混比例、空气当量比、水蒸汽／物料质量比对气化气组分、热值和气化效率等参数的影响,并与试验数据进行了比较,结果表明,所建模型能够准确地模拟生物质和煤的流化床气化过程。
Biomass is an abundant and renewable source of energy. Co-gasification of biomass with coal could not only reduce the harmful gases emissions such as SOx and NOx, but also obtain the complete transformation of carbon and improve the efficiency of co-gasification. Therefore, the study of the co-gasification of biomass with coal process is one of the crucial areas of the clean utilization of coal. However, the mechanism of the synergistic effect in the co-gasification of biomass with coal process remains unclear. Further studies are necessary to understand the formation of gas products, dissociation mechanisms and the evolution of physical and chemical structure characteristics occurd on the surface of coke. In this paper, the physicochemical properties of biomass and coal and the change of microstructure in gasification process were analyzed. Based on these results, co-gasification characteristic of biomass and coal in fluidized bed was systematically studied in both theory and experiment, and from the effects of various factors such as biomass blending ratio and equivalence ratio(ER), the synergistic effect mechanism of co-gasification of biomass and coal was revealed. The following investigations are made in this thesis:
The thermal analysis of co-gasification of biomass with coal was performed. The effects from heating rate, reaction atmosphere, mixing proprotion were studied on in details. The C-R and DAEM method were applied to theatrically analyze the co-gasification kinetics characteristic. A co-gasification reaction kinetics model was established, and parameters were acquired. The trend of activation energy in the critical reaction stage was analyzed. The reaction stage where co-gasification compensation effect happened was confirmed. The results showed that the co-gasification of biomass with coal process included four stages:drying, preheating, volatile precipitation and coke gasification. There was no significant synergistic effect in the volatile precipitation stage. However, a significant synergistic effect was observed in the coke gasification stage.This effect got the maximum, when mixing proprotion was50%. The pyrolysis stage of co-gasification can be described by a homogeneous reaction model. The reaction mechanism of the gasification matched the unreacted shrinking core model. The activation energy of coke gasification stage was significantly higher than that of the volatile precipitation stage.
Based on thermal analysis experiments, a TG-FTIR was employed to study the gas products of co-gasification of biomass with coal. The effects of temperature-rising rate on the gas products were studied. By the analysis of the micro surface morphology/microstructure(SEM, EDX) and functional groups (FTIR) of gasification semicoke, a mechanism of formation of the flammable gas such as CO and CH4was proposed. The results showed the evolution of the surface morphology of semicoke in the gasification. Initially, the porous cannel structure formed. Then the poles collapsed and cannels were closed eventually. The main gas products of pine sawdust gasification were CO, CH4, H2O and organic matters such asalcohols, aldehydes, carboxylic acids, phenols and so on. In the co-gasification process, the formation of CH4was the results of the rupture and reformation of C-H bonds in the methyl, methylene and methoxy groups in lignite and pine sawdust, which throughout the process of volatiles releasing and coke gasification. CO is mostly released in volatile precipitation stage and coke gasification stage, which can be attributed to carboxyl, methoxy, carbonyl, ether bond rupture in volatile precipitation stage and the reduction of CO2in coke gasification. The gasification heating-rate affect the formation of the gas products. A lower gasification heating-rate might lead to more CO and CH4.
The experimental investigation of co-gasification of biomass and coal was carried out on a self-designed fluidized bed reactor. The effects of biomass blending ratio, equivalence ratio(ER) as well as steam-to-fuel ratio(S/F) on co-gasification characteristic of biomass and coal were systematically studied, the above results provide a basis for selection and operation of co-gasification system of biomass and coal. The test results showed that when the blending ratio of pine sawdust increases, the volume concentration of CO incereased, the change of CH4was not notable, the heating value reached a maximum at a blending ratio of50%. The gasification efficiency reached a maximum at an ER of0.26. The results showed that the introduction of steam resulted in more hydrogen production. When the steam-to-fuel ratio(S/F) was0.28, the heating value, the carbon conversion ratio and the gasification efficiency all reached the maximum.
Based on the bed test of the co-gasification of biomass with coal, the ASPEN PLUS was applied to simulate the co-gasification of biomass with coal in a fluidized bed gasifier by considering the hydrodynamic and reaction rate kinetics simultaneously, the external FORTRAN subroutines for hydrodynamics and kinetics nested in ASPEN PLUS simulate the gasification process, the model was developed to study the co-gasification of biomass with coal in fluidized bed gasifier was employed to studied the effects of equivalence ratio(ER), blending ratio as well as steam-to-fuel ratio(S/F) on the gas composition, heating value and gasification efficiency, and the results were compared with the experimental results. Above results show that the co-gasification of biomass with coal in fluidized bed gasifier could be simulated accurately with the model developed in this thesis.
引文
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