大型煤制甲醇工艺技术研究
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摘要
以煤为原料生产甲醇的工艺过程包括空气分离、煤气化、一氧化碳变换、合成气净化、甲醇合成、甲醇精馏等工艺单元。本文以年产180万吨煤制甲醇装置为背景,主要围绕水煤浆制甲醇工艺过程中的CO变换、合成气净化和甲醇合成三个工序,建立数学模型,通过模拟计算,研究分析了流程配置、热回收方案、工艺参数和主要设备大小,并进行了优化分析。
通过热力学和动力学模拟,研究了变换工序的流程设置、工艺参数、催化剂装填量和催化剂在初、中、末期时调节CO总变换量的手段,认为煤制甲醇装置可以通过改变变换气气量有效调节CO总变换量,变换反应器的催化剂装填量可相对较少。利用流程模拟和夹点技术对水煤浆制甲醇装置变换工序的余热利用进行了模拟计算与分析,结果显示,在高温位区域传热温差较大,在低温位区域传热温差较小；提高变换反应器入口气体温度,使出变换反应器内的反应温度达到485℃左右,可副产11.OMPaG等级的高压蒸汽和0.5MPaG等级的低压蒸汽,此时高温区域的传热温差变小,但仍远远大于全网络的最小传热温差；反应器内的热点温度在几种主要耐硫变换催化剂的最高使用温度之下；副产高压蒸汽时增加的主要投资是变换炉的造价增加以及后续余热回收的换热设备投资增加,可在1.5年内回收。
低温甲醇洗和NHD(Selexol)脱硫脱碳两种技术都可用于煤制甲醇装置,低温甲醇洗脱硫、脱碳的投资高于NHD法,但水、电、汽等公用工程消耗低于NHD法。Linde公司的低温甲醇洗技术比Lurgi公司的低温甲醇洗技术投资略高一些,但冷量、低压氮气、电等公用工程的消耗减小。低温甲醇洗系统含高压气体和强极性物质,由于缺少适合该体系的热力学方法,通用的流程模拟软件无法模拟该工艺过程,本文采用Soave-Redlich-Kwong (SRKH)立方型状态方程,结合Huron-Vidal昆合规则和非随机双流体Non-Random-Two-Liquid活度系数模型建立热力学模型,从已有的气体溶解度和气液平衡数据拟合获得了45对活度系数模型参数,可用于低温甲醇洗脱碳工艺的过程模拟,低压和高压系统的模拟结果和实际工业数据符合很好。应用该热力学模型对低温甲醇洗洗涤系统进行了模拟计算,结果表明可以通过改变贫液和半贫液的量来调节净化气中的CO2浓度,使甲醇合成反应在最佳条件下进行。
以甲醇和CO2为关键组分,以CO和CO2加氢生产甲醇的2个反应为平行的独立反应,建立了气冷一水冷串联式甲醇合成反应器的一维拟均相数学模型；对气冷—水冷串联式甲醇反应器进行了模拟计算,得到了各反应器内的温度分布和浓度分布,考察了温度,操作压力以及入塔气中CO2浓度对串联式反应器中甲醇合成反应的影响。结果表明,水冷式反应器入口气体温度以及饱和沸腾水温度对甲醇产量影响很小,水冷式反应器入口气体温度对各反应器中的温度分布影响较大；随着操作压力的升高,水冷式反应器中甲醇产量增加,气冷式反应器中甲醇产量降低,串联式反应器中总甲醇产量增加；随着入塔气中CO2浓度的增加,气冷式反应器出口温度及水冷式反应器入口温度均增加,甲醇产量降低,新鲜气中CO2浓度不宜太高。对不同负荷(50%～110%)下年产180万吨甲醇的气冷—水冷串联式反应器进行了模拟计算,结果表明气冷—水冷串联式反应器对不同生产负荷都具有较好的适应性。
The process for producing methanol taking coal as feedstock is composed of such units as air separation, coal gasification, CO-shift, syn-gas purification, methanol synthesis and methanol rectification. This article, by taking a coal-to-methanol plant in the capacity of1,800,000t/a as a background, has set up a mathematical model centering on CO-shift, syn-gas purification and methanol synthesis units included in methanol production process taking coal-slurry as feedstock and with the simulation calculations the process configuration, scheme for heat recovery, process parameters and the size of main equipment have been studied and optimized analysis conducted.
With both the thermo-dynamic and dynamic simulations the process configuration, process parameters, catalyst charges and the means for regulating the total shifted CO respectively at initial, intermediate and last phase in the shift-conversion unit have been studied and it takes that a coal-to-methanol plant can effectively regulate the total shifted CO by changing the volume of shifted gas and the quantity of loaded catalyst into the shift-conversion reactor may comparatively be less. Also calculations and analysis for the surplus-heat utilization of the CO-shift unit in the methanol plant from coal-slurry are carried out by taking process simulations and pinch technology:there is a bigger heat-transfer temperature difference in high-temperature region whereas a smaller difference in low-temperature region, by increasing the gas temperature in the shifted reactor the temperature of the reactor may reach around485℃and this may by-produce HP-steam of11.0MPaG and LP-steam of0.5MPaG; the heat-transfer temperature difference becomes smaller, but still far bigger than the minimum heat-transfer temperature difference over the full network:the hot-point temperature inside the reactor is still below the maximum service temperature for several typical S-resistant shift-conversion catalysts and the increased major investment for the by-produced HP-steam is the addition of reformer cost of manufacture and the investment increase of heat-exchanging equipment for follow-up surplus-heat recovery, the increased investment can be recovered in1.3years.
Both the Rectisol and NHD(Selexol) de-sulfuration and de-carbonization technologies may be applied to coal-to-methanol plant with higher investment of the former than tie latter and lower utility consumptions of water, power and steam:the investment for Rectisol technology of Linde is a little bit higher than that of Lurgi but the consumptions of refrigeration. LP-steam and electricity lower. Since the Rectisol system involves HP-gas and material of strong polarity and there is short of thermo-dynamic method suitable for the system, the process can not be simulated with universal software for process simulation, this article has employed a cubic state equation of Soave-Redlich-Kwong and a thermo-dynamic model set up by combining with Huron-Vida mixed rule and Non-Random-Two-Liquid activity coefficient model has obtained45pairs of parameters of activity coefficient model through a data fit from the existing gas solubility and gas-liquid balance data that can be used in the simulation of Rectisol de-carbonization process and there is a good coincidence between the simulation results of both high and low pressure systems and actual industrial data. Also simulation calculations taking this thermo-dynamic model has been conducted for Rectisol scrubbing system and the results show that the CO2concentration in the purified gas can be regulated by changing the volume of barren and semi-barren liquor to make the methanol synthesis reaction proceed under best condition.
A mathematical model of one-dimensional plan homogenous phase to implement a simulation calculation of methanol synthesis reactor of serial air cool-water cool type has been set up by taking methanol and CO2as key component and the hydrogenation reaction of CO and CO2as independent reaction; both the temperature and concentration distribution in each reactor have been obtained from such simulation calculation and the effect on the methanol synthesis in reactors of such type by temperature, pressure and CO2concentration in the introduced gas has been investigated. The results show that the inlet gas temperature at water-cooled reactor and the temperature of saturated boiling water have a little effect on the methanol yield, but the inlet gas temperature has a bigger effect on the temperature distribution in each reactor; with the rise of operating pressure the methanol output in water-cooled reactor increases whereas the output of methanol in air-cooled reactor reduces with the increase of total methanol output in serial reactors; with the increase of CO2concentration in the introduced gas both the outlet temperature at air-cooled reactor and the inlet temperature at water-cooled reactor increase and methanol output reduces. CO2concentration in virgin gas should not be too high. A simulation calculation is also carried out for reactors of a serial air cool-water cool type in a1,800.000t/a methanol plant at different load (50%～110%)and the results show that the reactor of such type has a better adaptability at different production load.
通过热力学和动力学模拟,研究了变换工序的流程设置、工艺参数、催化剂装填量和催化剂在初、中、末期时调节CO总变换量的手段,认为煤制甲醇装置可以通过改变变换气气量有效调节CO总变换量,变换反应器的催化剂装填量可相对较少。利用流程模拟和夹点技术对水煤浆制甲醇装置变换工序的余热利用进行了模拟计算与分析,结果显示,在高温位区域传热温差较大,在低温位区域传热温差较小；提高变换反应器入口气体温度,使出变换反应器内的反应温度达到485℃左右,可副产11.OMPaG等级的高压蒸汽和0.5MPaG等级的低压蒸汽,此时高温区域的传热温差变小,但仍远远大于全网络的最小传热温差；反应器内的热点温度在几种主要耐硫变换催化剂的最高使用温度之下；副产高压蒸汽时增加的主要投资是变换炉的造价增加以及后续余热回收的换热设备投资增加,可在1.5年内回收。
低温甲醇洗和NHD(Selexol)脱硫脱碳两种技术都可用于煤制甲醇装置,低温甲醇洗脱硫、脱碳的投资高于NHD法,但水、电、汽等公用工程消耗低于NHD法。Linde公司的低温甲醇洗技术比Lurgi公司的低温甲醇洗技术投资略高一些,但冷量、低压氮气、电等公用工程的消耗减小。低温甲醇洗系统含高压气体和强极性物质,由于缺少适合该体系的热力学方法,通用的流程模拟软件无法模拟该工艺过程,本文采用Soave-Redlich-Kwong (SRKH)立方型状态方程,结合Huron-Vidal昆合规则和非随机双流体Non-Random-Two-Liquid活度系数模型建立热力学模型,从已有的气体溶解度和气液平衡数据拟合获得了45对活度系数模型参数,可用于低温甲醇洗脱碳工艺的过程模拟,低压和高压系统的模拟结果和实际工业数据符合很好。应用该热力学模型对低温甲醇洗洗涤系统进行了模拟计算,结果表明可以通过改变贫液和半贫液的量来调节净化气中的CO2浓度,使甲醇合成反应在最佳条件下进行。
以甲醇和CO2为关键组分,以CO和CO2加氢生产甲醇的2个反应为平行的独立反应,建立了气冷一水冷串联式甲醇合成反应器的一维拟均相数学模型；对气冷—水冷串联式甲醇反应器进行了模拟计算,得到了各反应器内的温度分布和浓度分布,考察了温度,操作压力以及入塔气中CO2浓度对串联式反应器中甲醇合成反应的影响。结果表明,水冷式反应器入口气体温度以及饱和沸腾水温度对甲醇产量影响很小,水冷式反应器入口气体温度对各反应器中的温度分布影响较大；随着操作压力的升高,水冷式反应器中甲醇产量增加,气冷式反应器中甲醇产量降低,串联式反应器中总甲醇产量增加；随着入塔气中CO2浓度的增加,气冷式反应器出口温度及水冷式反应器入口温度均增加,甲醇产量降低,新鲜气中CO2浓度不宜太高。对不同负荷(50%～110%)下年产180万吨甲醇的气冷—水冷串联式反应器进行了模拟计算,结果表明气冷—水冷串联式反应器对不同生产负荷都具有较好的适应性。
The process for producing methanol taking coal as feedstock is composed of such units as air separation, coal gasification, CO-shift, syn-gas purification, methanol synthesis and methanol rectification. This article, by taking a coal-to-methanol plant in the capacity of1,800,000t/a as a background, has set up a mathematical model centering on CO-shift, syn-gas purification and methanol synthesis units included in methanol production process taking coal-slurry as feedstock and with the simulation calculations the process configuration, scheme for heat recovery, process parameters and the size of main equipment have been studied and optimized analysis conducted.
With both the thermo-dynamic and dynamic simulations the process configuration, process parameters, catalyst charges and the means for regulating the total shifted CO respectively at initial, intermediate and last phase in the shift-conversion unit have been studied and it takes that a coal-to-methanol plant can effectively regulate the total shifted CO by changing the volume of shifted gas and the quantity of loaded catalyst into the shift-conversion reactor may comparatively be less. Also calculations and analysis for the surplus-heat utilization of the CO-shift unit in the methanol plant from coal-slurry are carried out by taking process simulations and pinch technology:there is a bigger heat-transfer temperature difference in high-temperature region whereas a smaller difference in low-temperature region, by increasing the gas temperature in the shifted reactor the temperature of the reactor may reach around485℃and this may by-produce HP-steam of11.0MPaG and LP-steam of0.5MPaG; the heat-transfer temperature difference becomes smaller, but still far bigger than the minimum heat-transfer temperature difference over the full network:the hot-point temperature inside the reactor is still below the maximum service temperature for several typical S-resistant shift-conversion catalysts and the increased major investment for the by-produced HP-steam is the addition of reformer cost of manufacture and the investment increase of heat-exchanging equipment for follow-up surplus-heat recovery, the increased investment can be recovered in1.3years.
Both the Rectisol and NHD(Selexol) de-sulfuration and de-carbonization technologies may be applied to coal-to-methanol plant with higher investment of the former than tie latter and lower utility consumptions of water, power and steam:the investment for Rectisol technology of Linde is a little bit higher than that of Lurgi but the consumptions of refrigeration. LP-steam and electricity lower. Since the Rectisol system involves HP-gas and material of strong polarity and there is short of thermo-dynamic method suitable for the system, the process can not be simulated with universal software for process simulation, this article has employed a cubic state equation of Soave-Redlich-Kwong and a thermo-dynamic model set up by combining with Huron-Vida mixed rule and Non-Random-Two-Liquid activity coefficient model has obtained45pairs of parameters of activity coefficient model through a data fit from the existing gas solubility and gas-liquid balance data that can be used in the simulation of Rectisol de-carbonization process and there is a good coincidence between the simulation results of both high and low pressure systems and actual industrial data. Also simulation calculations taking this thermo-dynamic model has been conducted for Rectisol scrubbing system and the results show that the CO2concentration in the purified gas can be regulated by changing the volume of barren and semi-barren liquor to make the methanol synthesis reaction proceed under best condition.
A mathematical model of one-dimensional plan homogenous phase to implement a simulation calculation of methanol synthesis reactor of serial air cool-water cool type has been set up by taking methanol and CO2as key component and the hydrogenation reaction of CO and CO2as independent reaction; both the temperature and concentration distribution in each reactor have been obtained from such simulation calculation and the effect on the methanol synthesis in reactors of such type by temperature, pressure and CO2concentration in the introduced gas has been investigated. The results show that the inlet gas temperature at water-cooled reactor and the temperature of saturated boiling water have a little effect on the methanol yield, but the inlet gas temperature has a bigger effect on the temperature distribution in each reactor; with the rise of operating pressure the methanol output in water-cooled reactor increases whereas the output of methanol in air-cooled reactor reduces with the increase of total methanol output in serial reactors; with the increase of CO2concentration in the introduced gas both the outlet temperature at air-cooled reactor and the inlet temperature at water-cooled reactor increase and methanol output reduces. CO2concentration in virgin gas should not be too high. A simulation calculation is also carried out for reactors of a serial air cool-water cool type in a1,800.000t/a methanol plant at different load (50%～110%)and the results show that the reactor of such type has a better adaptability at different production load.
引文
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