褐煤提质及其燃烧行为特性的研究
摘要
褐煤的高含水量不仅增加运输成本,而且降低锅炉燃烧效率,增加二氧化碳的排放,因此褐煤提质技术的开发是清洁和有效利用褐煤的关键。本文针对褐煤的提质行为特性及提质处理对褐煤热解和燃烧反应性的影响进行研究。
对一种印度尼西亚褐煤(用YN表示)和两种中国神华褐煤(分别用SH1和SH2表示)的干燥特性进行实验研究,考察温度、粒径等不同因素对干燥速率的影响;采用相关系数判别法对褐煤干燥动力学特性进行解析,确定干燥过程的动力学参数和反应机理函数；借助SEM和FTIR定性分析褐煤十燥过程中物理和化学结构的变化。结果表明：粒径小于10mm的褐煤,干燥速率不受传热限制,干燥过程符合随机成核与随后生长机理。干燥过程中会发生大孔的收缩,干燥过程中有羟基、羰基和羧基官能团的分解而逸出H20和CO2气体。
利用自主设计的双辊成型机制备出高强度的无粘结剂型煤,研究水分含量、压缩比等因素对型煤强度的影响。结果表明：十燥后的褐煤水分含量对于无粘结剂成型是一个关键的因素。增加成型压力、减小粒径、提高成型温度以及采用水蒸气干燥可以改善型煤的冷压强度,同时也会增加设备的磨损,提高产品的成本。YN型煤的表面致密、有光泽,成型特性好,冷压强度最高,能够满足长时间在水中浸泡后强度的要求。
对YN褐煤干燥后的水分再吸收动力学特性进行了实验研究和理论分析。结果表明：由于煤中孔结构在干燥过程中发生了不可逆的崩塌,使得褐煤干燥后吸湿表现出一定的滞后性；干燥后的煤样吸湿速率与粒径无关而与干燥温度有关,提高干燥温度会降低吸湿速率和平衡水分；褐煤干燥后重新吸收水分过程是水蒸气物理吸附在褐煤表面和毛细孔中的过程,没有发现其与煤的表而官能团形成氢键的迹象。
利用高温沉降炉和热重分析仪对提质处理后褐煤的热解及燃烧特性进行了实验研究,其中燃烧特性包括在空气(O2/N2)和富氧(O2/CO2)燃烧条件下的燃烧特性。结果表明：提质后的型煤与原煤相比,挥发份产量降低,可燃性指数、燃尽指数和燃烧综合指数降低。
对制备的YN型煤进行了工业应用研究,包括配煤炼焦实验和工业燃烧实验。结果表明：YN型煤可以用于配煤炼焦。YN褐煤经过提质后,热值显著提高,自燃着火倾向明显降低,具有较好的可磨性和较高的燃尽率,属于中等轻微结渣煤,燃烧后SO2和NOx的生成量相对较低。
The development of upgrading technology is the key to the clean and effective use of lignites because the high moisture content of lignites leads to high transportation cost, the low thermal efficiency of boilers firing lignites and high carbon dioxide emissions. This thesis studies the behavior of lignite during upgrading and the effects on pyrolysis and combustion reactivity by means of various experimental approaches.
The drying experiments focusing on the characteristics of an Indonesian lignite coal (assigned as YN sample) and two Chinese Shenhua lignite coals (assigned as SH1 and SH2 samples) were carried out and the factors influencing the drying rates were carefully investigated, including drying temperature and particle size, et al. The drying kinetic parameters and mechanistic functions in drying process were obtained by correlative judging method. The physical and chemical structure changes during drying process were qualitatively analyzed using SEM and FTIR. The results showed that drying rate was not limited by heat transfer when the coal particle size was smaller than 10mm, and the drying process may be described with random nucleation and growth mechanism function. As water was progressively removed, the macropores tended to collapse and shrinkage took place while hydroxyl, carbonyl and carboxyl groups decomposed to release H2O and CO2.
The high-strength binderless briquettes were produced by a specially designed double-ring roller briquetting machine. Factors influencing the compressive strength were investigated, including briquette moisture content and compression ratio, et al. The results showed that moisture was a critical factor in the binderless briquetting of dried lignites. The compressive strength could be improved by increasing the compressing pressure, reducing particle size and higher drying temperature. The surface of the YN briquettes was visually compact, smooth and lustrous. The YN briquettes had good molding characteristics, and had the highest compressive strength and the strength after water immersion among the three coals.
The kinetics of moisture re-adsorption was studied experimentally and theoretically. The results showed that the moisture desorption and readsorption isotherms of the coal showed irreversibility in the desorption-readsorption cycles, indicative of irreversible coal structure changes during drying, which was dependent on drying temperature and independent of coal particle size. The moisture readsorption rate and equilibrium moisture content decreased with increasing drying temperature. The water vapor was physically adsorbed on the particle surface and capillary pore surfaces. The formation of hydrogen bond between the water molecules and the surface functional groups during the moisture re-adsorption process was not evident.
Pyrolysis and combustion characteristics of YN lignite were studied under air (O2/N2) and oxy-fuel (O2/CO2) conditions using a drop tube furnace and a thermogravimetric analyzer. Raw coal, dried coal and binderless briquette samples of the same coal were used in the experiments and the effects of drying and binderless briquetting on the reactivity of the coal under different conditions were investigated. The results showed that the briquetted coal had a decreased volatile matter yield, flammability index, burnout index and combustion synthesis index.
The industry application potential of YN briquettes was investigated through coking tests and burnout experiments on a pilot scale boiler. The results showed that the YN briquettes could be used for blending for coking. Upgrading of YN lignite has improved its calorific value and achieved favourable results in milling. Laboratory tests for spontaneous combustion indicated that YN briquettes had low to moderate propensity to spontaneous combustion. The burnout was high and the briquetted coal belonged to moderate slight-slaging coal. The emission of SO2 and NOX was low compared to reference coals.
对一种印度尼西亚褐煤(用YN表示)和两种中国神华褐煤(分别用SH1和SH2表示)的干燥特性进行实验研究,考察温度、粒径等不同因素对干燥速率的影响;采用相关系数判别法对褐煤干燥动力学特性进行解析,确定干燥过程的动力学参数和反应机理函数；借助SEM和FTIR定性分析褐煤十燥过程中物理和化学结构的变化。结果表明：粒径小于10mm的褐煤,干燥速率不受传热限制,干燥过程符合随机成核与随后生长机理。干燥过程中会发生大孔的收缩,干燥过程中有羟基、羰基和羧基官能团的分解而逸出H20和CO2气体。
利用自主设计的双辊成型机制备出高强度的无粘结剂型煤,研究水分含量、压缩比等因素对型煤强度的影响。结果表明：十燥后的褐煤水分含量对于无粘结剂成型是一个关键的因素。增加成型压力、减小粒径、提高成型温度以及采用水蒸气干燥可以改善型煤的冷压强度,同时也会增加设备的磨损,提高产品的成本。YN型煤的表面致密、有光泽,成型特性好,冷压强度最高,能够满足长时间在水中浸泡后强度的要求。
对YN褐煤干燥后的水分再吸收动力学特性进行了实验研究和理论分析。结果表明：由于煤中孔结构在干燥过程中发生了不可逆的崩塌,使得褐煤干燥后吸湿表现出一定的滞后性；干燥后的煤样吸湿速率与粒径无关而与干燥温度有关,提高干燥温度会降低吸湿速率和平衡水分；褐煤干燥后重新吸收水分过程是水蒸气物理吸附在褐煤表面和毛细孔中的过程,没有发现其与煤的表而官能团形成氢键的迹象。
利用高温沉降炉和热重分析仪对提质处理后褐煤的热解及燃烧特性进行了实验研究,其中燃烧特性包括在空气(O2/N2)和富氧(O2/CO2)燃烧条件下的燃烧特性。结果表明：提质后的型煤与原煤相比,挥发份产量降低,可燃性指数、燃尽指数和燃烧综合指数降低。
对制备的YN型煤进行了工业应用研究,包括配煤炼焦实验和工业燃烧实验。结果表明：YN型煤可以用于配煤炼焦。YN褐煤经过提质后,热值显著提高,自燃着火倾向明显降低,具有较好的可磨性和较高的燃尽率,属于中等轻微结渣煤,燃烧后SO2和NOx的生成量相对较低。
The development of upgrading technology is the key to the clean and effective use of lignites because the high moisture content of lignites leads to high transportation cost, the low thermal efficiency of boilers firing lignites and high carbon dioxide emissions. This thesis studies the behavior of lignite during upgrading and the effects on pyrolysis and combustion reactivity by means of various experimental approaches.
The drying experiments focusing on the characteristics of an Indonesian lignite coal (assigned as YN sample) and two Chinese Shenhua lignite coals (assigned as SH1 and SH2 samples) were carried out and the factors influencing the drying rates were carefully investigated, including drying temperature and particle size, et al. The drying kinetic parameters and mechanistic functions in drying process were obtained by correlative judging method. The physical and chemical structure changes during drying process were qualitatively analyzed using SEM and FTIR. The results showed that drying rate was not limited by heat transfer when the coal particle size was smaller than 10mm, and the drying process may be described with random nucleation and growth mechanism function. As water was progressively removed, the macropores tended to collapse and shrinkage took place while hydroxyl, carbonyl and carboxyl groups decomposed to release H2O and CO2.
The high-strength binderless briquettes were produced by a specially designed double-ring roller briquetting machine. Factors influencing the compressive strength were investigated, including briquette moisture content and compression ratio, et al. The results showed that moisture was a critical factor in the binderless briquetting of dried lignites. The compressive strength could be improved by increasing the compressing pressure, reducing particle size and higher drying temperature. The surface of the YN briquettes was visually compact, smooth and lustrous. The YN briquettes had good molding characteristics, and had the highest compressive strength and the strength after water immersion among the three coals.
The kinetics of moisture re-adsorption was studied experimentally and theoretically. The results showed that the moisture desorption and readsorption isotherms of the coal showed irreversibility in the desorption-readsorption cycles, indicative of irreversible coal structure changes during drying, which was dependent on drying temperature and independent of coal particle size. The moisture readsorption rate and equilibrium moisture content decreased with increasing drying temperature. The water vapor was physically adsorbed on the particle surface and capillary pore surfaces. The formation of hydrogen bond between the water molecules and the surface functional groups during the moisture re-adsorption process was not evident.
Pyrolysis and combustion characteristics of YN lignite were studied under air (O2/N2) and oxy-fuel (O2/CO2) conditions using a drop tube furnace and a thermogravimetric analyzer. Raw coal, dried coal and binderless briquette samples of the same coal were used in the experiments and the effects of drying and binderless briquetting on the reactivity of the coal under different conditions were investigated. The results showed that the briquetted coal had a decreased volatile matter yield, flammability index, burnout index and combustion synthesis index.
The industry application potential of YN briquettes was investigated through coking tests and burnout experiments on a pilot scale boiler. The results showed that the YN briquettes could be used for blending for coking. Upgrading of YN lignite has improved its calorific value and achieved favourable results in milling. Laboratory tests for spontaneous combustion indicated that YN briquettes had low to moderate propensity to spontaneous combustion. The burnout was high and the briquetted coal belonged to moderate slight-slaging coal. The emission of SO2 and NOX was low compared to reference coals.
引文
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