基于褐煤的生物质型煤成型机理及其特性研究
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摘要
褐煤,是世界上丰富而广泛存在的化石资源,但它却受到自身高水分、高灰分、低热值、低灰熔点、热稳定性差和容易风化自燃等特点的影响,限制了其使用范围和利用途径。而传统粗放的褐煤利用(发电)方式最终会威胁到它的有限的资源属性,也会恶化环境。因此,褐煤在利用前必须对其进行提质,同时混合生物质可直接减少依靠燃烧化石燃料而产生的二氧化碳、硫氧化物和氮氧化物的排放量,最终实现褐煤和生物质的高效洁净利用。本论文针对褐煤和生物质利用的研究现状,采用机械热压脱水方法对我国褐煤和生物质混合成型工艺展开了研究,探讨了生物质和褐煤在机械和加热的共同作用下物料颗粒间的成型粘结机理,并对加工的生物质型煤的热解特性进行了初步研究。
首先,进行了生物质型煤热压工艺条件的研究和成型工艺的优化。以小龙潭褐煤、先锋褐煤与生物质(水稻秸杆、小麦秸杆、云杉锯末)为试验物料,选择成型压力、成型温度、保压时间、生物质配比、颗粒粒径等因素,以生物质型煤机械强度(抗压强度、抗破碎强度、跌落强度)为指标对生物质型煤成型工艺展开研究,探讨了成型工艺条件与生物质型煤强度的关系。在选择的因素水平中,影响生物质型煤机械强度主次因素依次为:成型压力>生物质配比>成型温度>保压时间,且成型压力和生物质配比的交互作用对抗压强度和抗冲击强度影响显著,成型温度和保压时间的交互作用对于抗压强度的影响不显著。
其次,对生物质型煤的成型粘结机理进行了研究。通过显微结构观察分析,生物质不同长度的纤维相互连接,互相缠绕交联,形成网络,褐煤颗粒包裹于纤维网络中;在热压作用下生物质出现了玻璃化转变,和水以及褐煤的部分熔融物质一起形成了颗粒间的液体桥,在生物质型煤出模后该液体桥转变为固体桥,增加了生物质型煤的抗压强度。另外热压的作用也会增加生物质型煤的塑性,减弱生物质型煤出模后的松弛性(弹性),避免型煤产品开裂,有助于提高生物质型煤的跌落强度。而将生物质采用稀碱液处理后作为型煤的粘结剂可以提高型煤的机械强度和防水性能。从电势和颗粒特性分析知,褐煤和生物质表面Zeta电位均为负值,而且它们亲水性均较高,热压作用虽然可以增加其接触角,但从防水性试验来看热压效果不显著;另外,热压作用可降低褐煤孔容、比表面积和孔隙率。生物质型煤具有较好的机械强度是多种机制共同作用的结果,综合生物质型煤颗粒间的结合力,颗粒间桥接为主要机制,而机械结合力和物理化学结合力(化学键、静电力、范德华力等)起到的作用比较小。
再次,对生物质型煤成型工艺条件进行了小试研究,得到了跌落强度试验指标与各组分之间的回归方程,并求出了优化成型条件:稻壳配比为27-31%,保压时间为20~21min,温度为146-153℃。而小龙潭褐煤/小麦秸秆混合燃料最佳的成型条件为:秸秆粒度为0.16-0.38mm,温度为140℃,压力为15MPa,保压时间为20min。
最后,对生物质型煤的热解特性展开了初步研究。试验物料的热解过程可以分为四个阶段,其中第三阶段为物料发生热解的主要阶段,物料失重最多,达40 %-50 %。褐煤和水稻秸杆混合后,热重曲线分阶段出现褐煤和秸杆的热解特性,近似为二者的叠加。随后采用Coats-Redfern法对热解曲线进行了拟合,建立了分阶段的拟合动力学方程。
该论文有图65幅,表25个,参考文献146篇。
Lignite is abundant and widely distributed solid fossil resource in the world. However, its current industrial utilization (i.e. lignite fired power generation) is inefficient and has been causing environmental pollution, due to the lignite disadvantages of high moisture content, high ash content, low calorific heating value, low ash fusion temperature, easy weathering, self-ignition and high elemental contents of sulfur and nitrogen. Therefore, it is nessessary to upgrade liginte quality before utilization. One potential technology is to blend lignite with carbon-neutral biomass resouce for combution, which can reduce not only fossil-based CO_2 emission but also the emissions of other pollutants such as SOx and NOx. In this dissertation research, a process based on Mechnical and Thermal dewatering system was developed and studied to produce fuel briquettes from lignite-biomass blends. The binding mechanisms between lignite and biomass and the co-pyrolysis of lignite and biomass were investigated and discussed, respectively. Specifically, this dissertation research was divided into 4 sections as follows.
Firstly, the briquetting processing conditions and the optimization of processing parameters for bio-briquette were studied. Two Chinese lignite (Xianfeng & Xiaolongtan) were blended with the biomass samples of rice stalk, wheat straw and spruce sawdust, respectively. The effects of briquetting pressures, briquetting temperatures, pressure holding times, the mass ratios of biomass to lignite and particle sizes on the strength of the bio-briquettes were studied. The mechanical strength of obtained briquettes was evaluated with respect to compressive strength, impact strength and drop strength. The relation between processing conditions and mechanical strength of bio-briquette was further studied. The order of these factors in terms of importance was briquetting pressure, biomass/lignite mass ratio, treatment temperature and treatment time. The interaction effects between briquetting pressure, biomass/lignite mass ratio and compressive strength and impact strength were significant. But, the interaction effects between temperature, treatment time and compressive strength was not statistically significant.
Secondly, the binding mechanisms between lignite and biomass were investigated. With micro-structural analysis, it was found that biomass fibers with different lengths interconnected and interlocked each other. As a result, lignite particles well connected together, forming complicated network structure. Under the conditions of high pressures and temperatures, a glass transition was observed during the formation of biomass particle. Liquid bridges were formed between glass transitional materials, water and melted light materials. Then the liquid bridges in the briquette changed to be in the form of solid, after cooled and moved out of the mold. These solid bridges increased the strength of bio-briquettes. Also, the plastic properties of briquettes was improved and the relax properties (elasticities) decreased, due to the high pressure and temperature treatments. The presence of the mechanical interlocking bonds resisted the disruptive forces caused by elastic recovery from compression. These above positive changes improved the drop strength of bio-briquette and avoided cracking. Moreover, the mechanical strength and water resistance of bio-briquettes further improved with the biomass being pretreated with weak alkaline solutions, which acted as a binder between lignite and biomass particles. On the other hand, the particle characteristics and electrical potential characteristics were also investigated. The Zeta potential of lignite and biomass surfaces was always negatively charged, which helped prevent particle agglomeration. Though the mechnical and thermal process increased the contact angles of bio-briquette surface, the water resistance was not improved significantly. The pore volume, specific surface area and porosity were reduced by the process too.
High mechanical strength of bio-briquette was the result of several binding mechanisms. Among different mechanisms, the form of structural bridges connecting particles was the dominant one. By comparison, the mechanical bond force and physical/chemical bond forces (i.e. chemical bonds, electrostatic, Van der Waals’forces et al) were negligible.
Thirdly, a pilot scale test of bio-briquette was examined. A regression equation of the relation between biomass/lignite mass ratio, treatment time, briquetting temperature and drop strength was established. The optimal pilot-scale processing condition was rice husk mass ratio of 27-31 %, treatment time of 21-22min, briquetting temperetue of 146-153℃. The optimal conditions for xiaolongtan lignite/wheat straw were adjusted to be wheat straw size of 0.16-0.38 mm, briquetting temperetue of 140℃, treatment time of 20 min and briquetting pressure of 15 MPa.
Finally, the co-pyrolysis characteristic of lignite with biomass was preliminarily investigated. It revealed that the co-pyrolysis process consisted of 4 stages. The third stage was considered the most important phase, causing 40%-50% mass loss during pyrolysis. Furthermore, based on the analysis of TG curves, it was noted that the co-pyrolysis of lignite/rice stalk blends could be the overall result of pyrolysing lignite and rice stalk independently. In addition, by the method of Coats-Redfern, reaction kinetic model for each stage of the pyrolysis was developed in this dissertation research .
The dissertation has 65 figures, 25 tables and 146 references.
首先,进行了生物质型煤热压工艺条件的研究和成型工艺的优化。以小龙潭褐煤、先锋褐煤与生物质(水稻秸杆、小麦秸杆、云杉锯末)为试验物料,选择成型压力、成型温度、保压时间、生物质配比、颗粒粒径等因素,以生物质型煤机械强度(抗压强度、抗破碎强度、跌落强度)为指标对生物质型煤成型工艺展开研究,探讨了成型工艺条件与生物质型煤强度的关系。在选择的因素水平中,影响生物质型煤机械强度主次因素依次为:成型压力>生物质配比>成型温度>保压时间,且成型压力和生物质配比的交互作用对抗压强度和抗冲击强度影响显著,成型温度和保压时间的交互作用对于抗压强度的影响不显著。
其次,对生物质型煤的成型粘结机理进行了研究。通过显微结构观察分析,生物质不同长度的纤维相互连接,互相缠绕交联,形成网络,褐煤颗粒包裹于纤维网络中;在热压作用下生物质出现了玻璃化转变,和水以及褐煤的部分熔融物质一起形成了颗粒间的液体桥,在生物质型煤出模后该液体桥转变为固体桥,增加了生物质型煤的抗压强度。另外热压的作用也会增加生物质型煤的塑性,减弱生物质型煤出模后的松弛性(弹性),避免型煤产品开裂,有助于提高生物质型煤的跌落强度。而将生物质采用稀碱液处理后作为型煤的粘结剂可以提高型煤的机械强度和防水性能。从电势和颗粒特性分析知,褐煤和生物质表面Zeta电位均为负值,而且它们亲水性均较高,热压作用虽然可以增加其接触角,但从防水性试验来看热压效果不显著;另外,热压作用可降低褐煤孔容、比表面积和孔隙率。生物质型煤具有较好的机械强度是多种机制共同作用的结果,综合生物质型煤颗粒间的结合力,颗粒间桥接为主要机制,而机械结合力和物理化学结合力(化学键、静电力、范德华力等)起到的作用比较小。
再次,对生物质型煤成型工艺条件进行了小试研究,得到了跌落强度试验指标与各组分之间的回归方程,并求出了优化成型条件:稻壳配比为27-31%,保压时间为20~21min,温度为146-153℃。而小龙潭褐煤/小麦秸秆混合燃料最佳的成型条件为:秸秆粒度为0.16-0.38mm,温度为140℃,压力为15MPa,保压时间为20min。
最后,对生物质型煤的热解特性展开了初步研究。试验物料的热解过程可以分为四个阶段,其中第三阶段为物料发生热解的主要阶段,物料失重最多,达40 %-50 %。褐煤和水稻秸杆混合后,热重曲线分阶段出现褐煤和秸杆的热解特性,近似为二者的叠加。随后采用Coats-Redfern法对热解曲线进行了拟合,建立了分阶段的拟合动力学方程。
该论文有图65幅,表25个,参考文献146篇。
Lignite is abundant and widely distributed solid fossil resource in the world. However, its current industrial utilization (i.e. lignite fired power generation) is inefficient and has been causing environmental pollution, due to the lignite disadvantages of high moisture content, high ash content, low calorific heating value, low ash fusion temperature, easy weathering, self-ignition and high elemental contents of sulfur and nitrogen. Therefore, it is nessessary to upgrade liginte quality before utilization. One potential technology is to blend lignite with carbon-neutral biomass resouce for combution, which can reduce not only fossil-based CO_2 emission but also the emissions of other pollutants such as SOx and NOx. In this dissertation research, a process based on Mechnical and Thermal dewatering system was developed and studied to produce fuel briquettes from lignite-biomass blends. The binding mechanisms between lignite and biomass and the co-pyrolysis of lignite and biomass were investigated and discussed, respectively. Specifically, this dissertation research was divided into 4 sections as follows.
Firstly, the briquetting processing conditions and the optimization of processing parameters for bio-briquette were studied. Two Chinese lignite (Xianfeng & Xiaolongtan) were blended with the biomass samples of rice stalk, wheat straw and spruce sawdust, respectively. The effects of briquetting pressures, briquetting temperatures, pressure holding times, the mass ratios of biomass to lignite and particle sizes on the strength of the bio-briquettes were studied. The mechanical strength of obtained briquettes was evaluated with respect to compressive strength, impact strength and drop strength. The relation between processing conditions and mechanical strength of bio-briquette was further studied. The order of these factors in terms of importance was briquetting pressure, biomass/lignite mass ratio, treatment temperature and treatment time. The interaction effects between briquetting pressure, biomass/lignite mass ratio and compressive strength and impact strength were significant. But, the interaction effects between temperature, treatment time and compressive strength was not statistically significant.
Secondly, the binding mechanisms between lignite and biomass were investigated. With micro-structural analysis, it was found that biomass fibers with different lengths interconnected and interlocked each other. As a result, lignite particles well connected together, forming complicated network structure. Under the conditions of high pressures and temperatures, a glass transition was observed during the formation of biomass particle. Liquid bridges were formed between glass transitional materials, water and melted light materials. Then the liquid bridges in the briquette changed to be in the form of solid, after cooled and moved out of the mold. These solid bridges increased the strength of bio-briquettes. Also, the plastic properties of briquettes was improved and the relax properties (elasticities) decreased, due to the high pressure and temperature treatments. The presence of the mechanical interlocking bonds resisted the disruptive forces caused by elastic recovery from compression. These above positive changes improved the drop strength of bio-briquette and avoided cracking. Moreover, the mechanical strength and water resistance of bio-briquettes further improved with the biomass being pretreated with weak alkaline solutions, which acted as a binder between lignite and biomass particles. On the other hand, the particle characteristics and electrical potential characteristics were also investigated. The Zeta potential of lignite and biomass surfaces was always negatively charged, which helped prevent particle agglomeration. Though the mechnical and thermal process increased the contact angles of bio-briquette surface, the water resistance was not improved significantly. The pore volume, specific surface area and porosity were reduced by the process too.
High mechanical strength of bio-briquette was the result of several binding mechanisms. Among different mechanisms, the form of structural bridges connecting particles was the dominant one. By comparison, the mechanical bond force and physical/chemical bond forces (i.e. chemical bonds, electrostatic, Van der Waals’forces et al) were negligible.
Thirdly, a pilot scale test of bio-briquette was examined. A regression equation of the relation between biomass/lignite mass ratio, treatment time, briquetting temperature and drop strength was established. The optimal pilot-scale processing condition was rice husk mass ratio of 27-31 %, treatment time of 21-22min, briquetting temperetue of 146-153℃. The optimal conditions for xiaolongtan lignite/wheat straw were adjusted to be wheat straw size of 0.16-0.38 mm, briquetting temperetue of 140℃, treatment time of 20 min and briquetting pressure of 15 MPa.
Finally, the co-pyrolysis characteristic of lignite with biomass was preliminarily investigated. It revealed that the co-pyrolysis process consisted of 4 stages. The third stage was considered the most important phase, causing 40%-50% mass loss during pyrolysis. Furthermore, based on the analysis of TG curves, it was noted that the co-pyrolysis of lignite/rice stalk blends could be the overall result of pyrolysing lignite and rice stalk independently. In addition, by the method of Coats-Redfern, reaction kinetic model for each stage of the pyrolysis was developed in this dissertation research .
The dissertation has 65 figures, 25 tables and 146 references.
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