煤炭分级利用与富氧燃烧技术机理及应用研究
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摘要
我国能源结构在未来较长的一段时期内仍将以煤炭为主。因此开发煤炭资源的高效清洁利用技术是关系我国能源安全与发展的关键课题之一。煤炭资源的分级利用结合富氧燃烧的多联产技术是一种新型的煤炭清洁利用技术,同时煤的富氧燃烧技术也是实现CO2减排的重要可能途径之一。
本文根据煤的分级利用结合富氧燃烧的多联产系统对煤粉的利用方式,按照“煤粉富氧燃烧热重实验—煤粉热解挥发分析出特性—半焦燃烧及综合应用—煤粉富氧燃烧水平管式炉试验—煤粉富氧燃烧沉降炉试验—热态卧式炉石油焦粉富氧燃烧器着火试验”的研究思路探究了煤粉的富氧燃烧特性,煤粉热解过程的挥发分析出特性以及煤部分热解后半焦的富氧燃烧特性和吸附性变化,最后在2MW实验台上以石油焦粉模拟半焦进行富氧燃烧器的着火特性试验,得到了石油焦粉不同氧气配比下的火焰温度分布。
在热重试验台上进行了煤粉的富氧燃烧特性及反应动力学研究,发现富氧燃烧气氛中的CO2对煤粉燃烧的抑制作用对煤阶低的煤种更为明显。在氧浓度低于60%的范围内,氧浓度对煤粉的燃烧特性参数的影响更为明显,氧浓度由21%提高至100%可以使无烟煤的最大燃烧速率提高至原速率的8.1倍,褐煤和烟煤也可提高5.5倍以上,从而大幅缩短煤粉富氧燃烧过程的反应时间,降低煤粉热重曲线的燃尽温度。通过不同的反应动力学参数计算方法发现高氧浓度的富氧燃烧过程多重扫描速率法计算过程的线性拟合度较差。通过改进单一扫描速率法提高了动力学参数的线性拟合度。计算结果发现,气氛中CO2以及氧浓度对动力学参数的影响主要体现在指前因子中。使用动力学补偿效应对改进的动力学参数计算方法的结果进行了验算,计算结果可靠。
使用快速裂解仪对煤种在超过5000℃/s可控升温速率下对煤粉的热裂解过程进行研究,发现H2在裂解温度高于800℃后产量明显增加；煤阶更高的煤种CH4的产量更大。此外,延长热裂解反应时间对CO2的产量影响较小。煤阶更高的烟煤相对于褐煤热裂解过程释放的大分子产物种类更多,产量也更大,但轻质挥发分如H2,CO和CO2等则小于煤阶较低的褐煤等煤种。
半焦的富氧燃烧试验发现提高氧浓度至40%时半焦的燃烧特性参数已经接近该煤种的空气燃烧工况,燃尽温度和最大失重速率等均优于煤粉空气燃烧工况。但氧浓度对着火温度的影响较小。对半焦吸附性的初步试验发现试验褐煤800℃半焦孔容积达到椰壳活性炭的76.3%,比表面积为椰壳活性炭的66.7%,与垃圾焚烧电站使用的吸附剂相比,吸附特性参数差异不大,鉴于褐煤与吸附剂价格之间的巨大价格差异,褐煤半焦作为吸附剂原料具有极其广阔的市场前景。
通过煤粉水平管式炉富氧燃烧发现氧浓度对于高阶煤种焦炭燃尽过程的影响更为明显,提高反应速率,缩短燃尽时间。而在900℃反应温度下,CO的产量随氧浓度的升高而下降,在5%～10%的氧浓度范围内CO产量下降最快,10%～60%的过程中下降趋势减缓,氧浓度达到60%以上时CO产量的下降速度进一步减缓。
在沉降炉上模拟了煤粉的富氧燃烧过程。在较低氧浓度下发现富氧气氛中的CO2加剧了无烟煤的难燃性,与O2在CO2中的扩散速率降低有关。过量氧气系数从1.05提高至1.3,无烟煤30%氧浓度富氧燃烧烟气中CO的浓度由3.63%下降至0.97%。将燃烧工况的氧浓度由21%提高至50%使试验无烟煤着火位置由距离喷口30mm处提前至10mm处,由于烟气量的下降,50%工况下尾部烟气CO2浓度降至70%左右。反应温度由900℃提高至1300℃的过程中,烟气CO的生成由于气化反应的影响由0.08%升高至0.81%。
最后在2MW卧式炉上使用低挥发分的石油焦粉模拟半焦进行了富氧燃烧器的着火试验,得到不同氧气配比工况下石油焦火焰的温度分布,燃烧组织最好的工况火焰核心高温区温度达到1474℃,而燃烧组织较差的工况火焰核心高温区温度为1320℃左右。根据试验结果对煤粉及半焦的燃烧器设计建议如下：在未进行氧气预热的情况下,大量低温氧气与燃料一同喷入炉膛虽然增加了燃料周围的氧浓度,但会降低燃料与气体混合物的温度,并不利于着火。其他氧气喷口应尽量平均布置于送粉气流周围,喷口流量过高虽然会提高反应区域氧浓度,但低温氧气流速的增加会导致燃料着火位置后移,不利于燃烧器的稳燃。
The energy structure of China will still be coal-based in a long period of time. Therefore the technical development of coal clean efficient utilization is a key issue related with our country's energy security and development. The staged utilization of coal combined with oxy-fuel combustion is a novel coal clean utilization technology, and is one of the possible ways to achieve CO2emission reduction.
This thesis based on the coal staged utilization combined with oxy-fuel combustion system, investigated the combustion characteristics of pulverized coal, the devolatilization characteristics of coal pyrolysis, and semi-coke oxy-fuel combustion characteristics, in according with research ideas of "thermogravimetric analyse of pulverzied coal oxy-fuel combustion—pulverized coal devolatilization characteristics of pyrolysis—semi-coke oxy-fuel combustion characteristics and comprehensive application—pulverized coal oxy-fuel combustion in horizontal tube furnace—pulverized coal oxy-fuel combustion in drop tube furnace—petroleum coke powder oxy-fuel burner test with2MW horizontal furnace."
Investigated the pulverized coal oxy-fuel combustion characteristics by the thermogravimetric experiments. It is found that CO2in oxy-fuel combustion atmosphere has more apparent inhibition to low rank coal. When the oxygen concentration is lower than60%, the effection of oxygen concentration to the combustion characteristics is more obvious. The maximum reaction rate of anthracite increased to8.1times faster, and the maximum reaction rates of lignite and bituminous coal are also5.5times faster, when the oxygen concentration is increased from21%to100%. It will significantly reduce the reaction time of the pulverized coal oxy-fuel combustion, and will decrease the burnout temperature. Investigated three different ways of kinetics calculation, and found that the model-free methods are not suitable for the oxy-fuel combustion. Then retrofit a model-fitting method and improve the linear fit of the kinetic calculation for oxy-fuel combustion. The kinetic analysis found that the CO2and oxygen concentration effection is mainly reflected in the pre-exponential factor. Using the kinetic compensation effect calculation method to check the kinetic calculation results, and the calculation results showed that the retrofitting model-fitting method calculation result were reliable.
Investigated the pulverized coal pyrolysis process with the fast pyrolyzer under a controllable heating rate over5000℃/s. Discovered that the H2production increased significantly when the pyrolysis temperature is higher than800℃. And High rank coal pyrolysis will produce more CH4. In addition, the extension of pyrolysis time has less effection on CO2production. The pyrolysis macromolecular product of high coal rank bituminous has more types and larger production than the low coal rank lignite. But the lightweight volatiles products such as H2, CO and CO2is less than the low coal rank lignite.
According to the semi-coke oxy-fuel combustion thermogravimetric experiment results, the semi-coke combustion characteristics is close to the air combustion condition when the oxygen concentration in the combustion atmosphere is over40%and the burnout temperature and the maximum reaction rate are better than the air combustion condition. It is also found that the ignition temperature was less affected by the oxygen concentration. The absorption experiments of semi-coke results showed that the pore volume of test lignite semi-coke in800℃is76.3%of the coconut shell activated carbon, and the specific surface area is66.7%of the coconut shell activated carbon. Compared with the absorbent using by the garbage power plants, the adsorption characteristic parameters is nearly the same. Based on the huge price difference between lignite and the adsorbent, using the lignite semi-coke as the adsorbent raw material has a very broad market prospects.
According to the pulverized coal oxy-fuel combustion in horizontal tube furnace experiment results, it is found that the oxygen concentration effection to high coal rank char burnout process is more obvious. The high oxygen concentration will increase the reaction rate, and reduce the reaction time. When the furnace temperature is900℃, and the oxygen concentration increased from5%to10%, the amount of CO in flue reduced quickly. And when the oxygen concentration increased from10%to60%, the CO amount decreasing speed slow down. When O2concentration is over60%, the CO amount decreasing speed slowed down further.
Simulate oxy-fuel combustion process of pulverized coal on drop tube furnace. The CO2in oxy-fuel combustion atmosphere increase the flame resistance of anthracite with low oxygen concentration conditions. This is because the diffusion rate of O2in CO2is slower than in N2. When the excess oxygen coefficient increased from1.05to1.3, the CO concentration of anthracite oxy-fuel combustion flue gas is decreased from3.63%to0.97%. When oxygen concentration increased from21%to50%, the ignition distance from the burner decreased from30mm to10mm. The CO concentration of flue gas increased from0.08%to0.81%, when the furnace temperature rised from900℃to1300℃
At last, a burner ignition test of petroleum coke powder was carried out on the2MW horizontal furnace. The flame temperature distribution of the petroleum coke powder was obtained in different oxygen ratio conditions. The maximum temperature of the best organized burning condition was1474℃, and the normal combustion condition highest temperature of the flame is around1320℃. According to the burner test results, some suggestions for oxy-fuel combustion burner design of pulverized coal and semi-coke were obtained:When the oxygen is not preheated, injecting fuel with large amount of cold oxygen will decrease the flow temperature, and obstruct the ignition process. Other oxygen nozzles should be arranged homogenized around the powder delivery flow nozzle. If the oxygen flow rate is too high or too low will delay the ignition postion and not conducive to the combustion stability.
本文根据煤的分级利用结合富氧燃烧的多联产系统对煤粉的利用方式,按照“煤粉富氧燃烧热重实验—煤粉热解挥发分析出特性—半焦燃烧及综合应用—煤粉富氧燃烧水平管式炉试验—煤粉富氧燃烧沉降炉试验—热态卧式炉石油焦粉富氧燃烧器着火试验”的研究思路探究了煤粉的富氧燃烧特性,煤粉热解过程的挥发分析出特性以及煤部分热解后半焦的富氧燃烧特性和吸附性变化,最后在2MW实验台上以石油焦粉模拟半焦进行富氧燃烧器的着火特性试验,得到了石油焦粉不同氧气配比下的火焰温度分布。
在热重试验台上进行了煤粉的富氧燃烧特性及反应动力学研究,发现富氧燃烧气氛中的CO2对煤粉燃烧的抑制作用对煤阶低的煤种更为明显。在氧浓度低于60%的范围内,氧浓度对煤粉的燃烧特性参数的影响更为明显,氧浓度由21%提高至100%可以使无烟煤的最大燃烧速率提高至原速率的8.1倍,褐煤和烟煤也可提高5.5倍以上,从而大幅缩短煤粉富氧燃烧过程的反应时间,降低煤粉热重曲线的燃尽温度。通过不同的反应动力学参数计算方法发现高氧浓度的富氧燃烧过程多重扫描速率法计算过程的线性拟合度较差。通过改进单一扫描速率法提高了动力学参数的线性拟合度。计算结果发现,气氛中CO2以及氧浓度对动力学参数的影响主要体现在指前因子中。使用动力学补偿效应对改进的动力学参数计算方法的结果进行了验算,计算结果可靠。
使用快速裂解仪对煤种在超过5000℃/s可控升温速率下对煤粉的热裂解过程进行研究,发现H2在裂解温度高于800℃后产量明显增加；煤阶更高的煤种CH4的产量更大。此外,延长热裂解反应时间对CO2的产量影响较小。煤阶更高的烟煤相对于褐煤热裂解过程释放的大分子产物种类更多,产量也更大,但轻质挥发分如H2,CO和CO2等则小于煤阶较低的褐煤等煤种。
半焦的富氧燃烧试验发现提高氧浓度至40%时半焦的燃烧特性参数已经接近该煤种的空气燃烧工况,燃尽温度和最大失重速率等均优于煤粉空气燃烧工况。但氧浓度对着火温度的影响较小。对半焦吸附性的初步试验发现试验褐煤800℃半焦孔容积达到椰壳活性炭的76.3%,比表面积为椰壳活性炭的66.7%,与垃圾焚烧电站使用的吸附剂相比,吸附特性参数差异不大,鉴于褐煤与吸附剂价格之间的巨大价格差异,褐煤半焦作为吸附剂原料具有极其广阔的市场前景。
通过煤粉水平管式炉富氧燃烧发现氧浓度对于高阶煤种焦炭燃尽过程的影响更为明显,提高反应速率,缩短燃尽时间。而在900℃反应温度下,CO的产量随氧浓度的升高而下降,在5%～10%的氧浓度范围内CO产量下降最快,10%～60%的过程中下降趋势减缓,氧浓度达到60%以上时CO产量的下降速度进一步减缓。
在沉降炉上模拟了煤粉的富氧燃烧过程。在较低氧浓度下发现富氧气氛中的CO2加剧了无烟煤的难燃性,与O2在CO2中的扩散速率降低有关。过量氧气系数从1.05提高至1.3,无烟煤30%氧浓度富氧燃烧烟气中CO的浓度由3.63%下降至0.97%。将燃烧工况的氧浓度由21%提高至50%使试验无烟煤着火位置由距离喷口30mm处提前至10mm处,由于烟气量的下降,50%工况下尾部烟气CO2浓度降至70%左右。反应温度由900℃提高至1300℃的过程中,烟气CO的生成由于气化反应的影响由0.08%升高至0.81%。
最后在2MW卧式炉上使用低挥发分的石油焦粉模拟半焦进行了富氧燃烧器的着火试验,得到不同氧气配比工况下石油焦火焰的温度分布,燃烧组织最好的工况火焰核心高温区温度达到1474℃,而燃烧组织较差的工况火焰核心高温区温度为1320℃左右。根据试验结果对煤粉及半焦的燃烧器设计建议如下：在未进行氧气预热的情况下,大量低温氧气与燃料一同喷入炉膛虽然增加了燃料周围的氧浓度,但会降低燃料与气体混合物的温度,并不利于着火。其他氧气喷口应尽量平均布置于送粉气流周围,喷口流量过高虽然会提高反应区域氧浓度,但低温氧气流速的增加会导致燃料着火位置后移,不利于燃烧器的稳燃。
The energy structure of China will still be coal-based in a long period of time. Therefore the technical development of coal clean efficient utilization is a key issue related with our country's energy security and development. The staged utilization of coal combined with oxy-fuel combustion is a novel coal clean utilization technology, and is one of the possible ways to achieve CO2emission reduction.
This thesis based on the coal staged utilization combined with oxy-fuel combustion system, investigated the combustion characteristics of pulverized coal, the devolatilization characteristics of coal pyrolysis, and semi-coke oxy-fuel combustion characteristics, in according with research ideas of "thermogravimetric analyse of pulverzied coal oxy-fuel combustion—pulverized coal devolatilization characteristics of pyrolysis—semi-coke oxy-fuel combustion characteristics and comprehensive application—pulverized coal oxy-fuel combustion in horizontal tube furnace—pulverized coal oxy-fuel combustion in drop tube furnace—petroleum coke powder oxy-fuel burner test with2MW horizontal furnace."
Investigated the pulverized coal oxy-fuel combustion characteristics by the thermogravimetric experiments. It is found that CO2in oxy-fuel combustion atmosphere has more apparent inhibition to low rank coal. When the oxygen concentration is lower than60%, the effection of oxygen concentration to the combustion characteristics is more obvious. The maximum reaction rate of anthracite increased to8.1times faster, and the maximum reaction rates of lignite and bituminous coal are also5.5times faster, when the oxygen concentration is increased from21%to100%. It will significantly reduce the reaction time of the pulverized coal oxy-fuel combustion, and will decrease the burnout temperature. Investigated three different ways of kinetics calculation, and found that the model-free methods are not suitable for the oxy-fuel combustion. Then retrofit a model-fitting method and improve the linear fit of the kinetic calculation for oxy-fuel combustion. The kinetic analysis found that the CO2and oxygen concentration effection is mainly reflected in the pre-exponential factor. Using the kinetic compensation effect calculation method to check the kinetic calculation results, and the calculation results showed that the retrofitting model-fitting method calculation result were reliable.
Investigated the pulverized coal pyrolysis process with the fast pyrolyzer under a controllable heating rate over5000℃/s. Discovered that the H2production increased significantly when the pyrolysis temperature is higher than800℃. And High rank coal pyrolysis will produce more CH4. In addition, the extension of pyrolysis time has less effection on CO2production. The pyrolysis macromolecular product of high coal rank bituminous has more types and larger production than the low coal rank lignite. But the lightweight volatiles products such as H2, CO and CO2is less than the low coal rank lignite.
According to the semi-coke oxy-fuel combustion thermogravimetric experiment results, the semi-coke combustion characteristics is close to the air combustion condition when the oxygen concentration in the combustion atmosphere is over40%and the burnout temperature and the maximum reaction rate are better than the air combustion condition. It is also found that the ignition temperature was less affected by the oxygen concentration. The absorption experiments of semi-coke results showed that the pore volume of test lignite semi-coke in800℃is76.3%of the coconut shell activated carbon, and the specific surface area is66.7%of the coconut shell activated carbon. Compared with the absorbent using by the garbage power plants, the adsorption characteristic parameters is nearly the same. Based on the huge price difference between lignite and the adsorbent, using the lignite semi-coke as the adsorbent raw material has a very broad market prospects.
According to the pulverized coal oxy-fuel combustion in horizontal tube furnace experiment results, it is found that the oxygen concentration effection to high coal rank char burnout process is more obvious. The high oxygen concentration will increase the reaction rate, and reduce the reaction time. When the furnace temperature is900℃, and the oxygen concentration increased from5%to10%, the amount of CO in flue reduced quickly. And when the oxygen concentration increased from10%to60%, the CO amount decreasing speed slow down. When O2concentration is over60%, the CO amount decreasing speed slowed down further.
Simulate oxy-fuel combustion process of pulverized coal on drop tube furnace. The CO2in oxy-fuel combustion atmosphere increase the flame resistance of anthracite with low oxygen concentration conditions. This is because the diffusion rate of O2in CO2is slower than in N2. When the excess oxygen coefficient increased from1.05to1.3, the CO concentration of anthracite oxy-fuel combustion flue gas is decreased from3.63%to0.97%. When oxygen concentration increased from21%to50%, the ignition distance from the burner decreased from30mm to10mm. The CO concentration of flue gas increased from0.08%to0.81%, when the furnace temperature rised from900℃to1300℃
At last, a burner ignition test of petroleum coke powder was carried out on the2MW horizontal furnace. The flame temperature distribution of the petroleum coke powder was obtained in different oxygen ratio conditions. The maximum temperature of the best organized burning condition was1474℃, and the normal combustion condition highest temperature of the flame is around1320℃. According to the burner test results, some suggestions for oxy-fuel combustion burner design of pulverized coal and semi-coke were obtained:When the oxygen is not preheated, injecting fuel with large amount of cold oxygen will decrease the flow temperature, and obstruct the ignition process. Other oxygen nozzles should be arranged homogenized around the powder delivery flow nozzle. If the oxygen flow rate is too high or too low will delay the ignition postion and not conducive to the combustion stability.
引文
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