中低阶煤基乙炔多联产系统的研究
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摘要
基于中低阶煤的高效利用,采用中低阶煤基乙炔工艺路线代替石油乙烯工艺路线是缓解石油资源供应紧张的有效解决办法。
本文依托国家重点基础发展计划973项目(2011CB201306),围绕中低阶煤分级转化联产低碳燃料和化学品展开研究,以氧热法煤转化残焦制备电石乙炔的低能耗新工艺为研究对象,开展了中低阶煤基化学品制备系统与动力系统集成、反应过程能量转化、能量耦合、能量损失的热力学机理研究以及工艺路线对比研究。旨在研究氧热法电石炉内部反应体系的热力学机理,提出氧热法煤基电石乙炔新工艺系统,以及开拓中低阶煤基化学品(乙炔、熟石灰、CO、热解气与热解焦油)生产工艺与燃料电池/蒸汽联合循环发电工艺、热解焦油制备乙烯工艺整合后的中低阶煤基化学品/动力多联产新系统,重点研究了氧热法电石炉内部的能量转化机理和化学反应平衡限度。本论文主要内容如下：
首先,针对高温高能耗的关键单元——氧热法电石炉单元开展能量性质分析。建立氧热法电石制备反应过程的能量构型,采用△G-T图和α-H-ε图,分析反应过程能量耦合、能量转化的热力学机理以及高能耗产生的原因。结果显示氧热法电石炉中,部分碳与氧气燃烧生成CO炉气的燃烧反应具有较大的不可逆性,为过程支付了热力学代价。对于电石炉内部的化学反应过程,通过考察温度、压力、进料组成对反应体系的化学平衡限度影响,探讨了CaC2的产率和反应选择性随操作条件的变化规律,同时考虑了Ca蒸汽对化学反应平衡的影响。按反应体系升温过程和过程自发性变化情况,提出四阶段反应机理,获得了氧热法电石炉化学平衡的新认知。此外,还通过△G-T图来预测CaC2反应发生温度以及反应发生顺序。
其次,提出适用于不同基准、多种产出条件下的工艺系统评价指标。从能量、环境以及经济性角度,综合对比了氧热法电石工艺与电热法电石工艺。从中选择最优的电石制备工艺来构建中低阶煤基氧热法乙炔工艺系统,并开展流程模拟研究。同时,借助新型图示火用分析方法——火用流结构Grassman图,开展能量分析与评价,考察了工艺系统的能量利用情况和火用损失分布。全系统的能量分析和火用分析结果表明,电石炉单元火用损失最大,占系统内部火用损失的57.52%。然后,对比评价中低阶煤基氧热法乙炔新工艺和中低阶煤基气化乙烯传统工艺两条煤基化学品路线,证实新工艺路线的节能减排特性。
最后,中低阶煤基氧热法乙炔工艺系统副产大量CO炉气和热解焦油,二者均具有较高的再利用价值。鉴于高温CO炉气既具有化学能又具有热能,可采用融碳酸盐燃料电池／蒸汽联合循环回收电石炉气联产电和热,实现能量的梯级利用。而热解焦油含有多种有机化合物,具有较高的化学能。可以借鉴石油工艺来生产乙烯,探索焦油制乙烯新工艺。通过充分回收利用中低阶煤基氧热法乙炔工艺系统的副产品,最终提出中低阶煤基化学品／动力多联产工艺系统。
Based on high efficient utilization of middle-low-rank-coal, the middle-low-rank-coal-based oxy-thermal acetylene manufacturing process is established to replace the petroleum ethylene manufacturing process route. That is the most effective way to relieve the recent petroleum resource shortage.
Depending on the National Basic Research Program of China (also called973Program, No.2011CB201306), the middle-low-rank-coal cascaded conversion for low-carbon fuel and chemicals cogeneration system is investigated. For further researching novel energy-saving process of coal-based oxy-thermal carbide acetylene manufacturing, the thermodynamic mechanism of system integration, energy conversion, energy coupling and energy loss of middle-low-rank-coal-based chemicals and power manufacturing system as well as some process route comparison are also discussed. With the detailed investigation of oxy-thermal carbide furnace thermodynamic mechanism, the novel coal-based oxy-thermal acetylene manufacturing process system is proposed. Simultaneously, combining middle-low-rank-coal-based chemicals (acetylene, lime hydrates, off-gas and pyrolysis tar) manufacturing process, fuel cell/steam combined cycle power producing process and coal tar phrolysis ethylene manufacturing process, the novel coal-based cogeneration system is also researched and developed. The most significant is energy conversion mechanism investigation and chemical reaction equilibrium exploration of oxy-thermal carbide furnace. The main contents are as follows:
First of all, for high temperature and high energy consumption key unit, i.e. oxy-thermal carbide furnace, the thermodynamic analysis is carried on. The research work includes oxy-thermal carbide reaction process energy configuration establishing with△G-T and α-H-ε diagram analysis for thermodynamic mechanism of energy coupling, energy conversion and high energy consumption reason. The results show that the combustion reaction between partial carbon and oxygen to produce carbon monoxide in the oxy-thermal carbide furnace has great irreversibility and pays most of thermodynamic penalty. For internal reaction process of carbide furnace, by studying the temperature, pressure and feedstock composition affection of chemical reaction equilibrium limit, the yield of CaC2and reaction selectivity change with variation of the operating conditions is investigated. In the meantime, the calcium vapor affection of chemical reaction equilibrium is considered. In addition, by using△G-T diagram, the reaction temperature and reaction order of CaC2is predicted.
Second, system evaluation index, which applies to different basis and multiple output of process system, is proposed. Comparing oxy-thermal carbide process with electro-thermal carbide process in the view of energy, environment and economy, the relatively desirable one is selected to establish the middle-low-rank-coal-based oxy-thermal acetylene manufacturing process system and relevant process simulation is then carried on. Simultaneously, with the novel exergy framework Grassman diagram analysis, the energy utilization and exergy loss distribution of process system are investigated. Energy analysis and exergy analysis results of entire system show that the calcium carbide production unit has the maximum exergy loss, which accounts for57.52%of the total internal exergy loss. Then novel middle-low-rank-coal-based oxy-thermal acetylene manufacturing process is compared with traditional middle-low-rank-coal-based gasification ethylene manufacturing process and these two coal-based chemicals manufacturing process routes are evaluated. The results prove that the new process route has the characteristics of energy-saving and emission-reduction.
Finally, a large number of byproducts, which produced by the middle-low-rank-coal-based oxy-thermal acetylene manufacturing process system, e.g. carbon monoxide off-gas and pyrolysis tar, is highly reusable. Because of chemical and thermal energy of high-temperature CO off-gas, the molten carbonate fuel cell/steam combined cycle can be used to recycle the off-gas for generating electricity and heat and then the entire system can realize the energy cascade utilization. Besides, pyrolysis tar contains a variety of organic compounds, which have higher chemical energy. Referring to petroleum ethylene manufacturing process, those pyrolysis tars can be reused as the the feedstock of novel ethylene manufacturing process. By fully recycling by-products (i.e. carbon monoxide off-gas and pyrolysis tar) of middle-low-rank-coal-based oxy-thermal acetylene manufacturing process system, the middle-low-rank-coal-based chemicals/power cogeneration process system is finally proposed.
本文依托国家重点基础发展计划973项目(2011CB201306),围绕中低阶煤分级转化联产低碳燃料和化学品展开研究,以氧热法煤转化残焦制备电石乙炔的低能耗新工艺为研究对象,开展了中低阶煤基化学品制备系统与动力系统集成、反应过程能量转化、能量耦合、能量损失的热力学机理研究以及工艺路线对比研究。旨在研究氧热法电石炉内部反应体系的热力学机理,提出氧热法煤基电石乙炔新工艺系统,以及开拓中低阶煤基化学品(乙炔、熟石灰、CO、热解气与热解焦油)生产工艺与燃料电池/蒸汽联合循环发电工艺、热解焦油制备乙烯工艺整合后的中低阶煤基化学品/动力多联产新系统,重点研究了氧热法电石炉内部的能量转化机理和化学反应平衡限度。本论文主要内容如下：
首先,针对高温高能耗的关键单元——氧热法电石炉单元开展能量性质分析。建立氧热法电石制备反应过程的能量构型,采用△G-T图和α-H-ε图,分析反应过程能量耦合、能量转化的热力学机理以及高能耗产生的原因。结果显示氧热法电石炉中,部分碳与氧气燃烧生成CO炉气的燃烧反应具有较大的不可逆性,为过程支付了热力学代价。对于电石炉内部的化学反应过程,通过考察温度、压力、进料组成对反应体系的化学平衡限度影响,探讨了CaC2的产率和反应选择性随操作条件的变化规律,同时考虑了Ca蒸汽对化学反应平衡的影响。按反应体系升温过程和过程自发性变化情况,提出四阶段反应机理,获得了氧热法电石炉化学平衡的新认知。此外,还通过△G-T图来预测CaC2反应发生温度以及反应发生顺序。
其次,提出适用于不同基准、多种产出条件下的工艺系统评价指标。从能量、环境以及经济性角度,综合对比了氧热法电石工艺与电热法电石工艺。从中选择最优的电石制备工艺来构建中低阶煤基氧热法乙炔工艺系统,并开展流程模拟研究。同时,借助新型图示火用分析方法——火用流结构Grassman图,开展能量分析与评价,考察了工艺系统的能量利用情况和火用损失分布。全系统的能量分析和火用分析结果表明,电石炉单元火用损失最大,占系统内部火用损失的57.52%。然后,对比评价中低阶煤基氧热法乙炔新工艺和中低阶煤基气化乙烯传统工艺两条煤基化学品路线,证实新工艺路线的节能减排特性。
最后,中低阶煤基氧热法乙炔工艺系统副产大量CO炉气和热解焦油,二者均具有较高的再利用价值。鉴于高温CO炉气既具有化学能又具有热能,可采用融碳酸盐燃料电池／蒸汽联合循环回收电石炉气联产电和热,实现能量的梯级利用。而热解焦油含有多种有机化合物,具有较高的化学能。可以借鉴石油工艺来生产乙烯,探索焦油制乙烯新工艺。通过充分回收利用中低阶煤基氧热法乙炔工艺系统的副产品,最终提出中低阶煤基化学品／动力多联产工艺系统。
Based on high efficient utilization of middle-low-rank-coal, the middle-low-rank-coal-based oxy-thermal acetylene manufacturing process is established to replace the petroleum ethylene manufacturing process route. That is the most effective way to relieve the recent petroleum resource shortage.
Depending on the National Basic Research Program of China (also called973Program, No.2011CB201306), the middle-low-rank-coal cascaded conversion for low-carbon fuel and chemicals cogeneration system is investigated. For further researching novel energy-saving process of coal-based oxy-thermal carbide acetylene manufacturing, the thermodynamic mechanism of system integration, energy conversion, energy coupling and energy loss of middle-low-rank-coal-based chemicals and power manufacturing system as well as some process route comparison are also discussed. With the detailed investigation of oxy-thermal carbide furnace thermodynamic mechanism, the novel coal-based oxy-thermal acetylene manufacturing process system is proposed. Simultaneously, combining middle-low-rank-coal-based chemicals (acetylene, lime hydrates, off-gas and pyrolysis tar) manufacturing process, fuel cell/steam combined cycle power producing process and coal tar phrolysis ethylene manufacturing process, the novel coal-based cogeneration system is also researched and developed. The most significant is energy conversion mechanism investigation and chemical reaction equilibrium exploration of oxy-thermal carbide furnace. The main contents are as follows:
First of all, for high temperature and high energy consumption key unit, i.e. oxy-thermal carbide furnace, the thermodynamic analysis is carried on. The research work includes oxy-thermal carbide reaction process energy configuration establishing with△G-T and α-H-ε diagram analysis for thermodynamic mechanism of energy coupling, energy conversion and high energy consumption reason. The results show that the combustion reaction between partial carbon and oxygen to produce carbon monoxide in the oxy-thermal carbide furnace has great irreversibility and pays most of thermodynamic penalty. For internal reaction process of carbide furnace, by studying the temperature, pressure and feedstock composition affection of chemical reaction equilibrium limit, the yield of CaC2and reaction selectivity change with variation of the operating conditions is investigated. In the meantime, the calcium vapor affection of chemical reaction equilibrium is considered. In addition, by using△G-T diagram, the reaction temperature and reaction order of CaC2is predicted.
Second, system evaluation index, which applies to different basis and multiple output of process system, is proposed. Comparing oxy-thermal carbide process with electro-thermal carbide process in the view of energy, environment and economy, the relatively desirable one is selected to establish the middle-low-rank-coal-based oxy-thermal acetylene manufacturing process system and relevant process simulation is then carried on. Simultaneously, with the novel exergy framework Grassman diagram analysis, the energy utilization and exergy loss distribution of process system are investigated. Energy analysis and exergy analysis results of entire system show that the calcium carbide production unit has the maximum exergy loss, which accounts for57.52%of the total internal exergy loss. Then novel middle-low-rank-coal-based oxy-thermal acetylene manufacturing process is compared with traditional middle-low-rank-coal-based gasification ethylene manufacturing process and these two coal-based chemicals manufacturing process routes are evaluated. The results prove that the new process route has the characteristics of energy-saving and emission-reduction.
Finally, a large number of byproducts, which produced by the middle-low-rank-coal-based oxy-thermal acetylene manufacturing process system, e.g. carbon monoxide off-gas and pyrolysis tar, is highly reusable. Because of chemical and thermal energy of high-temperature CO off-gas, the molten carbonate fuel cell/steam combined cycle can be used to recycle the off-gas for generating electricity and heat and then the entire system can realize the energy cascade utilization. Besides, pyrolysis tar contains a variety of organic compounds, which have higher chemical energy. Referring to petroleum ethylene manufacturing process, those pyrolysis tars can be reused as the the feedstock of novel ethylene manufacturing process. By fully recycling by-products (i.e. carbon monoxide off-gas and pyrolysis tar) of middle-low-rank-coal-based oxy-thermal acetylene manufacturing process system, the middle-low-rank-coal-based chemicals/power cogeneration process system is finally proposed.
引文
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