低变质煤热解—气化耦合工艺模拟优化研究
摘要
煤炭是我国的主要一次能源，其中低变质的褐煤、长焰煤、不粘煤、弱粘煤等资源丰富且质量较好，近年来开采比重日益增大。针对低变质煤挥发份含量高的特点而提出的煤炭分级转化技术，根据煤在不同阶段反应特性不同的特点，实施煤热解、气化和燃烧分级转化，可提高煤炭利用率，简化煤炭气化技术，减小投资降低成本，并能有效解决煤中污染物的脱除问题。
本文借鉴“联合热转化技术”思想，在对国内外主要热解和部分气化工艺研究分析的基础上，提出低变质煤热解-部分气化耦合工艺，并对该工艺进行了模拟研究与分析，为进一步的具体技术开发和操作控制提供了参考和指导。
通过对煤热解反应动力学分析，并基于分布活化能模型DAEM，建立了集总反应动力学模型来表示煤炭热解过程，确定了可以预测热解产物组成、分布与热解终温和升温速率关系的动力学方程。研究表明，随热解温度升高，各种挥发份产物析出率越接近最大产率，半焦C含量增加，但产率下降，H、O、N和S等元素降低。因此，升温有利于提高半焦脱硫、脱氮率。600℃左右，除H2外的大部分挥发份基本析出，半焦元素变化幅度减小。热解终温较低且一定时，较慢的升温速率有利于各热解挥发份最大限度的析出。分析结果显示，将热解终温控制在550℃，升温速率10℃/min左右有利于热解挥发份完全析出。
运用Aspen Plus化工流程模拟软件，建立了将煤干馏热解和半焦部分气化相结合的两段气化模拟模型。结果表明，建立的气化炉模型能对本文提出的两段工艺进行较准确地模拟。热解段得焦油12.23%，半焦收率为65.11%，基本符合煤炭热解结果。调节分割器分割率为0.53:0.47时，可使热解段湿煤预热至指定温度110℃。通过对气化段做灵敏度分析可得，当氧气煤比（O2/C）为0.33，蒸汽煤比（H2O/C）为0.20，或者氧气煤比0.356，蒸汽煤比0.25时，气化炉温度可维持在900℃左右，且冷煤气效率最高。
Coal is the primary energy source of China, in which low metamorphic coal includinglignite, long flame coal, non-caking coal and light sticky coal are abundant and have highquality, and the proportion of mining are increaseing improved. Coal staged conversion whichwas proposed considering that low metamorphic coal had the character of high volatile matter,according to the different reaction features of different coal in different conversion period,implement classification conversion about pyrolysis, gasification and combustion. Thistechnology can raise coal utilization, simplify gasification, reduce the investment and cost,and effectively solve the problem of removal of contaminants of coal.
Reference to the“combined thermal-conversion technologies”, based on the analysis andstudy on pyrolysis and partial gasification technology of domestic and oversea, the thesis putforward the low metamorphic coal pyroglysis-partial gasification coupling technology, andthis process was simulated and analyzed to provide reference and guidance for the furtherdevelopment of specific method and operational control.
Through the analysis of coal pyrolysis reaction dynamics, based on distribution activationenergy model (DAEM), the lumped reaction kinetics model was established to represent thepyrolysis process, and kinetics equations which can estimate the relation among thecomposition and distribution of pyrolytic products and final pyrolysis temperature and heatingrate were determined. The research showed that the emission rate of volatile matterapproached the ultimate production rate with the rising of final pyrolysis temperature, whilesemi-coke yield reduced, of which C content increased and the others including H, N, O and Scontent decreased. Therefore, the rising of final temperature favored the desulfurization anddenitrification of semi-coke. The most volatile except H2 basically released and elementschange range of semi-coke decreased at 600℃. When pyrolysis temperature remained constant, slow heating was beneficial to the full emission of volatile matter. Analysis resultsshowed that controlling the temperature at 550℃and heating rate of 10℃/min volatile mattercan wholly release.
Based on ASPEN PLUS, the simulation method of the two-stage gasification technologyintegrated with pyrolysis model of coal and partial gasification of semi-coke was presented.The results showed that the established gasifier model can accurately simulate the two-stagetechnology which the thesis put forward. Tar yield of the pyrolysis-stage was 12.23%, andsemi-coke yield was 65.11%. By regulating the segmentation rate of splitter at 0.53:0.47, thewet coal can be preheated to the specified temperature at 110℃. Finally, the gasification-stagewas optimized based on performance parameters adjustment and sensitivity analysis. Whenratio of oxygen to coal (O2/C) was 0.33 and ratio of steam to coal (H2O/C) was 0.2, or O2/Cand H2O/C were 0.356 and 0.25 respectively, the temperature of gasifier can maintain at 900℃and the cold gas efficiency was highest.
本文借鉴“联合热转化技术”思想，在对国内外主要热解和部分气化工艺研究分析的基础上，提出低变质煤热解-部分气化耦合工艺，并对该工艺进行了模拟研究与分析，为进一步的具体技术开发和操作控制提供了参考和指导。
通过对煤热解反应动力学分析，并基于分布活化能模型DAEM，建立了集总反应动力学模型来表示煤炭热解过程，确定了可以预测热解产物组成、分布与热解终温和升温速率关系的动力学方程。研究表明，随热解温度升高，各种挥发份产物析出率越接近最大产率，半焦C含量增加，但产率下降，H、O、N和S等元素降低。因此，升温有利于提高半焦脱硫、脱氮率。600℃左右，除H2外的大部分挥发份基本析出，半焦元素变化幅度减小。热解终温较低且一定时，较慢的升温速率有利于各热解挥发份最大限度的析出。分析结果显示，将热解终温控制在550℃，升温速率10℃/min左右有利于热解挥发份完全析出。
运用Aspen Plus化工流程模拟软件，建立了将煤干馏热解和半焦部分气化相结合的两段气化模拟模型。结果表明，建立的气化炉模型能对本文提出的两段工艺进行较准确地模拟。热解段得焦油12.23%，半焦收率为65.11%，基本符合煤炭热解结果。调节分割器分割率为0.53:0.47时，可使热解段湿煤预热至指定温度110℃。通过对气化段做灵敏度分析可得，当氧气煤比（O2/C）为0.33，蒸汽煤比（H2O/C）为0.20，或者氧气煤比0.356，蒸汽煤比0.25时，气化炉温度可维持在900℃左右，且冷煤气效率最高。
Coal is the primary energy source of China, in which low metamorphic coal includinglignite, long flame coal, non-caking coal and light sticky coal are abundant and have highquality, and the proportion of mining are increaseing improved. Coal staged conversion whichwas proposed considering that low metamorphic coal had the character of high volatile matter,according to the different reaction features of different coal in different conversion period,implement classification conversion about pyrolysis, gasification and combustion. Thistechnology can raise coal utilization, simplify gasification, reduce the investment and cost,and effectively solve the problem of removal of contaminants of coal.
Reference to the“combined thermal-conversion technologies”, based on the analysis andstudy on pyrolysis and partial gasification technology of domestic and oversea, the thesis putforward the low metamorphic coal pyroglysis-partial gasification coupling technology, andthis process was simulated and analyzed to provide reference and guidance for the furtherdevelopment of specific method and operational control.
Through the analysis of coal pyrolysis reaction dynamics, based on distribution activationenergy model (DAEM), the lumped reaction kinetics model was established to represent thepyrolysis process, and kinetics equations which can estimate the relation among thecomposition and distribution of pyrolytic products and final pyrolysis temperature and heatingrate were determined. The research showed that the emission rate of volatile matterapproached the ultimate production rate with the rising of final pyrolysis temperature, whilesemi-coke yield reduced, of which C content increased and the others including H, N, O and Scontent decreased. Therefore, the rising of final temperature favored the desulfurization anddenitrification of semi-coke. The most volatile except H2 basically released and elementschange range of semi-coke decreased at 600℃. When pyrolysis temperature remained constant, slow heating was beneficial to the full emission of volatile matter. Analysis resultsshowed that controlling the temperature at 550℃and heating rate of 10℃/min volatile mattercan wholly release.
Based on ASPEN PLUS, the simulation method of the two-stage gasification technologyintegrated with pyrolysis model of coal and partial gasification of semi-coke was presented.The results showed that the established gasifier model can accurately simulate the two-stagetechnology which the thesis put forward. Tar yield of the pyrolysis-stage was 12.23%, andsemi-coke yield was 65.11%. By regulating the segmentation rate of splitter at 0.53:0.47, thewet coal can be preheated to the specified temperature at 110℃. Finally, the gasification-stagewas optimized based on performance parameters adjustment and sensitivity analysis. Whenratio of oxygen to coal (O2/C) was 0.33 and ratio of steam to coal (H2O/C) was 0.2, or O2/Cand H2O/C were 0.356 and 0.25 respectively, the temperature of gasifier can maintain at 900℃and the cold gas efficiency was highest.
引文
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