生物质气化过程中燃料固有氮演变行为研究
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摘要
生物质是一种非常重要的可再生清洁能源。随着能源与环境危机的日渐恶化,废弃生物质资源的综合利用已经成为亟待解决的课题,也是我国目前可再生能源领域的重要研究方向之一。在生物质高温气化过程中,生物质中固有氮(简称燃料氮)通常可以转变为多种形式,如氮气、气相污染物或者污染物前体(包括NH3、HCN和NOX等)是影响生物质气化应用系统的优化设计与污染物控制等方面的重要因素之一,也是目前学术研究领域的焦点课题之一。
本文针对生物质气化过程中燃料氮的迁移演化行为进行了实验和理论研究。建立了一个小型流化床生物质气化装置,提出了氮平衡方法来研究定量化N2含量。在进行元素分析、工业分析和色谱分析等测试的基础上,总结获得了不同生物质燃料氮的存在形式。结合大量实验数据,重点分析了不同当量比、反应温度、生物质种类等条件下,各种气化产物的质量百分比分布情况与变化规律,由此归纳分析出燃料氮的主要迁移演化途径,尤其是揭示了NH3与N2之间的转换反应对于整个燃料氮演化进程的决定性作用。
建立了一个小型生物质热解气化装置。通过大量的热解实验,测试了生物质热解产物中挥发分组成以及含氮组分浓度,获得了不同热解条件(气化温度、生物质种类)对生物质热解过程中燃料氮迁移演化的影响规律。就生物质化学组成结构对热解产物的影响进行了深入分析,并与煤炭热解进行了对比,揭示了以氨基酸形式赋存的生物质燃料氮(弱C-N键)迁移演化的重要机理,同时还初步分析了HCN、HCNO等成分的产生形成对燃料氮演化过程中的各种贡献。在上述研究结果基础上,首次提出了生物质气化过程中燃料氮较为完整的迁移演化路径图,具有比较重要的理论指导意义。
初步建立了流化床生物质气化反应器中燃料氮迁移演变过程的动力学模型,其中考虑了6个总体化学反应、31种组分以及70个单元化学反应,并采用4阶自适应变步长Runge-Kutta方法进行方程离散和数值求解,有效地改善了计算过程的收敛性。在典型气化参数条件下,对模拟计算结果和实验数据之间进行了对比分析。在此基础上,通过动力学模型计算分析了气化过程中主要构成组分含量与反应温度、当量比等影响参数之间的相互依赖关系,同时还对空气气化过程中燃料氮迁移演化区别进行了深入分析,分析了相关含氮气体浓度的变化差异以及内在机理,包括反应物浓度降低而引起的化学反应速率减慢、炭表面活性降低、滞留时间延长等诸多因素,这对于进一步理解生物质燃料氮迁移演化机理奠定了良好基础。
Biomass is a kind of very important renewable clean energy. With the worse and worse situation of energy and environmental crisis, the effective utilization of waste biomass has become a key issue for the research and application of present renewable energy development in China. Fuel bound nitrogen (FBN) in biomass can be converted to molecular nitrogen or gas phase pollutants and pollutant precursors such as ammonia (NH3), hydrogen cyanide (HCN), and oxides of nitrogen (NOx) during the high temperature gasification, which have complex influences on the optimal design of biomass gasification systems and their pollution control. Therefore, the evolution behavior of FBN during gasification is becoming a hot topic that merits academic attention.
In the present work, an extensive investigation on the evolution behavior of FBN during gasification is performed experimentally and theoretically. Firstly, a small-scale experimental equipment for fluidized biomass gasification is built, where·N2 content is analyzed based on the principle of nitrogen balance method. Based on elementary analysis, industrial analysis and GC analysis, the patterns of FBN existed in different biomass are obtained. Further, the experiment of biomass gasification under different operation parameters including gasification temperature, equivalence ratio, and biomass types is performed. The concentration of nitrogenous contents in gasification gas is obtained, based on which the main approach to the evolution behavior of FBN during gasification is summarized. Especially, the contribution of the conversion reaction between NH3 and N2 to the final process of the evolution of FBN is revealed.
Secondly, a small-scale pyrolysis experiment of biomass is built. Based on an extensive pyrolysis experiment, the variations of the major nitrogenous volatilizezing contents are obtained under different operation conditions including the reaction temperature and biomass types. Further, the effect of the difference on the chemical structure of FBN in biomass is analyzed and compared with the results of the conventional coal pyrolysis. An important mechanism of the effect of the fact that the nitrogenous contents in biomass come mainly from the amino acid (the weaker C-N bound) on the evolution of FBN is revealed. In addition, the contribution of the formation of HCN and HCNO on the evolution of FBN is discussed. Considering the results mentioned above, a complete mechanism of the evolution of FBN during the gasification and pyrolysis is presented for the first time, which is of great significance to the application of biomass gasification systems.
Finally, a preliminary reaction dynamic model on the evolution of FBN during the gasification and pyrolysis is presented, where 6 total chemical reactions including 31 kinds of components based on 70 elementary chemical reactions are considered. In order to improve the convergence of the whole calculation process, a self-adaptive fourth order variable-step-length Runge-Kutta method is introduced to make a numerical solution. A comparative analysis between simulated and experimental results is made aiming at some typical operation conditions and parameters. Then, the relationship between the nitrogenous contents, reaction temperature and equlivant ratio during the gasification and pyrolysis is analyzed. Further, a comparison of the evolution of FBN between oxygen and air is performed, and its differences in the nitrogenous contents as well as influencing mechanisms, such as the reduction of chemical reaction velocity caused by the decrease of concentrations of the component contents, the reduction of the surface activity of coal, and the prolong of the lagging time in O2, are discussed in detail. This is helpful to further understand the ultimate evolution behavior of FBN during the gasification and pyrolysis.
本文针对生物质气化过程中燃料氮的迁移演化行为进行了实验和理论研究。建立了一个小型流化床生物质气化装置,提出了氮平衡方法来研究定量化N2含量。在进行元素分析、工业分析和色谱分析等测试的基础上,总结获得了不同生物质燃料氮的存在形式。结合大量实验数据,重点分析了不同当量比、反应温度、生物质种类等条件下,各种气化产物的质量百分比分布情况与变化规律,由此归纳分析出燃料氮的主要迁移演化途径,尤其是揭示了NH3与N2之间的转换反应对于整个燃料氮演化进程的决定性作用。
建立了一个小型生物质热解气化装置。通过大量的热解实验,测试了生物质热解产物中挥发分组成以及含氮组分浓度,获得了不同热解条件(气化温度、生物质种类)对生物质热解过程中燃料氮迁移演化的影响规律。就生物质化学组成结构对热解产物的影响进行了深入分析,并与煤炭热解进行了对比,揭示了以氨基酸形式赋存的生物质燃料氮(弱C-N键)迁移演化的重要机理,同时还初步分析了HCN、HCNO等成分的产生形成对燃料氮演化过程中的各种贡献。在上述研究结果基础上,首次提出了生物质气化过程中燃料氮较为完整的迁移演化路径图,具有比较重要的理论指导意义。
初步建立了流化床生物质气化反应器中燃料氮迁移演变过程的动力学模型,其中考虑了6个总体化学反应、31种组分以及70个单元化学反应,并采用4阶自适应变步长Runge-Kutta方法进行方程离散和数值求解,有效地改善了计算过程的收敛性。在典型气化参数条件下,对模拟计算结果和实验数据之间进行了对比分析。在此基础上,通过动力学模型计算分析了气化过程中主要构成组分含量与反应温度、当量比等影响参数之间的相互依赖关系,同时还对空气气化过程中燃料氮迁移演化区别进行了深入分析,分析了相关含氮气体浓度的变化差异以及内在机理,包括反应物浓度降低而引起的化学反应速率减慢、炭表面活性降低、滞留时间延长等诸多因素,这对于进一步理解生物质燃料氮迁移演化机理奠定了良好基础。
Biomass is a kind of very important renewable clean energy. With the worse and worse situation of energy and environmental crisis, the effective utilization of waste biomass has become a key issue for the research and application of present renewable energy development in China. Fuel bound nitrogen (FBN) in biomass can be converted to molecular nitrogen or gas phase pollutants and pollutant precursors such as ammonia (NH3), hydrogen cyanide (HCN), and oxides of nitrogen (NOx) during the high temperature gasification, which have complex influences on the optimal design of biomass gasification systems and their pollution control. Therefore, the evolution behavior of FBN during gasification is becoming a hot topic that merits academic attention.
In the present work, an extensive investigation on the evolution behavior of FBN during gasification is performed experimentally and theoretically. Firstly, a small-scale experimental equipment for fluidized biomass gasification is built, where·N2 content is analyzed based on the principle of nitrogen balance method. Based on elementary analysis, industrial analysis and GC analysis, the patterns of FBN existed in different biomass are obtained. Further, the experiment of biomass gasification under different operation parameters including gasification temperature, equivalence ratio, and biomass types is performed. The concentration of nitrogenous contents in gasification gas is obtained, based on which the main approach to the evolution behavior of FBN during gasification is summarized. Especially, the contribution of the conversion reaction between NH3 and N2 to the final process of the evolution of FBN is revealed.
Secondly, a small-scale pyrolysis experiment of biomass is built. Based on an extensive pyrolysis experiment, the variations of the major nitrogenous volatilizezing contents are obtained under different operation conditions including the reaction temperature and biomass types. Further, the effect of the difference on the chemical structure of FBN in biomass is analyzed and compared with the results of the conventional coal pyrolysis. An important mechanism of the effect of the fact that the nitrogenous contents in biomass come mainly from the amino acid (the weaker C-N bound) on the evolution of FBN is revealed. In addition, the contribution of the formation of HCN and HCNO on the evolution of FBN is discussed. Considering the results mentioned above, a complete mechanism of the evolution of FBN during the gasification and pyrolysis is presented for the first time, which is of great significance to the application of biomass gasification systems.
Finally, a preliminary reaction dynamic model on the evolution of FBN during the gasification and pyrolysis is presented, where 6 total chemical reactions including 31 kinds of components based on 70 elementary chemical reactions are considered. In order to improve the convergence of the whole calculation process, a self-adaptive fourth order variable-step-length Runge-Kutta method is introduced to make a numerical solution. A comparative analysis between simulated and experimental results is made aiming at some typical operation conditions and parameters. Then, the relationship between the nitrogenous contents, reaction temperature and equlivant ratio during the gasification and pyrolysis is analyzed. Further, a comparison of the evolution of FBN between oxygen and air is performed, and its differences in the nitrogenous contents as well as influencing mechanisms, such as the reduction of chemical reaction velocity caused by the decrease of concentrations of the component contents, the reduction of the surface activity of coal, and the prolong of the lagging time in O2, are discussed in detail. This is helpful to further understand the ultimate evolution behavior of FBN during the gasification and pyrolysis.
引文
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