低阶烟煤中低温热解及热解产物研究
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摘要
“中低温热解一热解产品深度加工”多联产是目前低阶烟煤转化利用的有效途径之一。论文选取我国典型低阶烟煤集贤煤和东荣煤为样品,应用多种近现代分析表征方法进行了煤质深度评价,分别利用热重仪、管式炉和程控升温马弗炉进行了逐级放大的中低温热解实验,系统研究了热解工艺条件对热解产物分布、组成及工艺性质的影响,探寻准确、定量地表征低阶烟煤热解过程和特性、煤(焦)热解反应性和气化反应活性的方法,在此基础上以热解产物深度加工利用对原料组成、性质的要求为导向,研究、关联了热解产物组成及特异性工艺指标与热解工艺条件间的关系。
结果表明：集贤煤和东荣煤的挥发分、镜质组、壳质组和含氧官能团含量高、弱粘结性、低灰低硫等特点决定了它们是中低温热解的优质原料；在煤样中低温热解过程中,加热终温对热解产品的分布和组成的影响最大,升温速度基本不对产品分布和组成产生影响,保温时间超过90min后对产品分布和组成的影响很小；两种煤在450℃下制备的半焦的可磨性和预测成浆性均最好；半焦的燃烧、气化反应活性和比电阻均随加热终温的提高而降低；集贤煤和东荣煤分别在4500C和400℃下制取的焦油含轻质组分最多,两种煤均在500℃下含重质组分最多,分别在550℃和500℃下含低阶酚最多；煤气热值大体随加热终温的提高而增加；研究提出的热解特征指数尸和气化活性指数He分别可以简单、准确、定量的表征低阶烟煤的热解反应活性和煤(焦)的气化反应活性。论文通过关联利用方向所涉及的特异性指标与热解条件的关系,确定了适合热解产物深加工的热解工艺方案。
Integrated utilization by medium-low temperature pyrolysis is one of efficient and economic ways of low rank bituminous coal (LRC) conversion and utilization. Jixian coal and Dongrong coal, typical LRCs in China, were characterized and evaluated with aids of modern analysis instruments, and then they were pyrolyzed at medium-low temperature using thermogravimetry, electric tube furnace and muffle furnace, respectively. The effects of pyrolysis parameters on products'distribution, composition and properties were studied, and the new indices which could be used to quantitatively and accurately evaluate low-rank bituminous coal's pyrolysis reactivity and char's gasification reactivity were proposed. In accordance with the requirements for feedstocks of pyrolysis products'utilization, the composition and properties of products and pyrolysis parameters were related.
The results show that because of its high contents of volatility, vitrinite, exinite and oxygen functional groups, and low contents of cohesiveness, ash and sulfur, Jixian coal and Dongrong coal are suitable for medium-low temperature pyrolysis. The pyrolysis temperature is the most influential factor among pyrolysis process parameters. The yield and composition of products almost do not change with the variation of heating rate. When the pyrolysis time is more than90min, there is little change in the yield and composition of products. The grindability and forecasting slurry ability of Jixian and Dongrong semicokes pyrolyzed at450℃are best. The gasification reactivity, combustion reactivity and resistivity of semicokes decrease with pyrolysis temperature increasing. The light fractions in tars derived from Jixian coal pyrolysis at450℃and Dongrong coal pyrolysis at400℃is highest, the heavy fractions in tars derived from coal pyrolysis at500℃is highest, and the content of low-rank phenol in tars derived from Jixian coal pyrolysis at450℃and Dongrong coal pyrolysis at400℃is highest. The caloric value of gas increases with pyrolysis temperature increasing. The Pyrolysis Characteristic Index P and Gasification Reactivity Index HG can be used to evaluate low-rank bituminous coal's pyrolysis reactivity and char's gasification reactivity quantitatively and accurately. The pyrolysis parameters suitable for products'utilization are optimized based on the relationship between property and pyrolysis parameter.
结果表明：集贤煤和东荣煤的挥发分、镜质组、壳质组和含氧官能团含量高、弱粘结性、低灰低硫等特点决定了它们是中低温热解的优质原料；在煤样中低温热解过程中,加热终温对热解产品的分布和组成的影响最大,升温速度基本不对产品分布和组成产生影响,保温时间超过90min后对产品分布和组成的影响很小；两种煤在450℃下制备的半焦的可磨性和预测成浆性均最好；半焦的燃烧、气化反应活性和比电阻均随加热终温的提高而降低；集贤煤和东荣煤分别在4500C和400℃下制取的焦油含轻质组分最多,两种煤均在500℃下含重质组分最多,分别在550℃和500℃下含低阶酚最多；煤气热值大体随加热终温的提高而增加；研究提出的热解特征指数尸和气化活性指数He分别可以简单、准确、定量的表征低阶烟煤的热解反应活性和煤(焦)的气化反应活性。论文通过关联利用方向所涉及的特异性指标与热解条件的关系,确定了适合热解产物深加工的热解工艺方案。
Integrated utilization by medium-low temperature pyrolysis is one of efficient and economic ways of low rank bituminous coal (LRC) conversion and utilization. Jixian coal and Dongrong coal, typical LRCs in China, were characterized and evaluated with aids of modern analysis instruments, and then they were pyrolyzed at medium-low temperature using thermogravimetry, electric tube furnace and muffle furnace, respectively. The effects of pyrolysis parameters on products'distribution, composition and properties were studied, and the new indices which could be used to quantitatively and accurately evaluate low-rank bituminous coal's pyrolysis reactivity and char's gasification reactivity were proposed. In accordance with the requirements for feedstocks of pyrolysis products'utilization, the composition and properties of products and pyrolysis parameters were related.
The results show that because of its high contents of volatility, vitrinite, exinite and oxygen functional groups, and low contents of cohesiveness, ash and sulfur, Jixian coal and Dongrong coal are suitable for medium-low temperature pyrolysis. The pyrolysis temperature is the most influential factor among pyrolysis process parameters. The yield and composition of products almost do not change with the variation of heating rate. When the pyrolysis time is more than90min, there is little change in the yield and composition of products. The grindability and forecasting slurry ability of Jixian and Dongrong semicokes pyrolyzed at450℃are best. The gasification reactivity, combustion reactivity and resistivity of semicokes decrease with pyrolysis temperature increasing. The light fractions in tars derived from Jixian coal pyrolysis at450℃and Dongrong coal pyrolysis at400℃is highest, the heavy fractions in tars derived from coal pyrolysis at500℃is highest, and the content of low-rank phenol in tars derived from Jixian coal pyrolysis at450℃and Dongrong coal pyrolysis at400℃is highest. The caloric value of gas increases with pyrolysis temperature increasing. The Pyrolysis Characteristic Index P and Gasification Reactivity Index HG can be used to evaluate low-rank bituminous coal's pyrolysis reactivity and char's gasification reactivity quantitatively and accurately. The pyrolysis parameters suitable for products'utilization are optimized based on the relationship between property and pyrolysis parameter.
引文
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