沸石13XAPG吸附分离CO_2-N_2混合气过程研究及其应用
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摘要
大气中CO2浓度的不断提升导致全球变暖己成为学术界共识,各种碳减排技术的开发和改进已得到国际社会的普遍关注。二氧化碳的捕集与封存技术是目前碳减排最直接有效的手段之一。吸附法以其设备简单、能耗低、腐蚀问题易处理和易实现自动化操作等优点受到越来越多的关注。本文基于新型高效CO2吸附材料沸石13XAPG,通过基础实验、理论模拟和中试实验,对其吸附捕集燃煤电厂烟道气中CO2的性能进行评估。
首先,采用磁悬浮天平分别测定了CO2和N2在沸石13XAPG上的吸附平衡等温线,以Multi-site Langmuir等温线模型拟合,并计算吸附热。根据纯组分气体模型参数预测CO2/N2双组分的竞争吸附平衡,并进行实验验证,为吸附过程的设计提供基础数据。
其次,测量CO2/N2混合气在沸石13XAPG上的吸附突破解吸曲线,结合双分散二级孔线性推动力扩散模型,计算扩散系数和传递参数,研究CO2/N2在沸石13XAPG上的吸附动力学。此外,实验发现H2O对沸石13XAPG吸附CO2的容量有显著影响,所以在实际烟道气吸附捕集过程中,需要预处理脱水单元。
之后,采用沸石13XAPG填充吸附柱,通过实验和模拟研究几种循环吸附/解吸分离C02/N2的工艺,包括真空变压吸附工艺VPSA、变温吸附工艺TSA和真空变压变温耦合吸附工艺VTSA。研究发现真空变压变温耦合吸附工艺较为有效,具有一定应用前景,但是该工艺涉及变温过程,循环时间较长。在后续的中试实验中,采用快速的真空变压吸附(VPSA)技术来捕集燃煤电厂中二氧化碳。
最后采用沸石13XAPG吸附捕集上海申能星火热电厂烟道气中的CO2,实验考察了中试规模单级和两级VPSA工艺的捕集效率和能耗。脱硫后烟道气经过氧化铝脱湿单元除去水蒸汽,再经过吸附单元捕集CO2。单级VPSA单元填充261kg沸石13XAPG,采用三柱八步流程,对于37.0Nm3/h的干烟气,经过单级VPSA单元能够将C02提浓到75.7%,回收率达到90.3%,能耗为2.08MJ/kgCO2。可见单级捕集得到的C02纯度未达到封存要求(>95%),因此进一步设计和运行两级真空变压吸附工艺,第一级VPSA单元即为上述单级VPSA单元,第二级VPSA单元填充68.6kg活性炭小球并运行两柱六步流程,且将第二级废气回流到第一级入口处。实验结果表明,处理35.5Nm3/h的干燥后烟道气,经过第一级VPSA单元CO2能够提浓到74.5%,然后通过第二级VPSA单元浓缩到95.6%,回收率达到90.2%,需要能耗为2.44MJ/kgCO2,能耗较低,且随着高吸附吸附剂的开发以及吸附工艺的优化,吸附法将成为比较有前景的燃烧后CO2捕集方法。
Academic concerns have been raised with respect to the impact of the increasing concentration of carbon dioxide in the atmosphere on the environment as global warming. This global recognition has attracted great attention in relation to the creation, development and improvement upon technologies and strategies for the reduction of CO? emissions. Carbon capture and storage (CCS) is one of the most effective CO2emission abatement strategies in the world. Among all the post combustion capture technologies, adsorption process relying on well-engineered solid adsorbents is suggested as a promising option due to simple equipment, low energy requirement, less corrosion problems, easiness to achieve automatic operation and operating flexibility. In this work, a novel adsorbent zeolite13XAPG was employed as the selective adsorbent for CO2/N2separation. The feasibility and efficiency of adsorption technology for post-combustion CO2capture from Hue gas using zeolite13XAPG were evaluated by fundamental experiments, simulation and pilot-scale experiments in an existed coal-fired power plant.
Firstly, the adsorption equilibrium isotherms of CO2and N2on zeolite13XAPG were measured by a magnetic suspension balance. The adsorption heat was caculated from adsorption equilibrium data. Then Multi-site Langmuir model was employed to fit the experimental data with good agreement, and the fitted parameters were adopted in the prediction of binary competitive adsorption equilibrium, providing basic data for the design of adsorption process.
Secondly, adsorption kinetics of CO2/N2on zeolite13XAPG was investigated by the experimental data of breakthrough and desorption curves. A mathematical model based on the bi-LDF approximation was derived from mass, energy and momentum balances. Diffusion coefficient and transfer parameters were calculated through the comparison of experimental and simulated results. Moreover, it was found from experiments that the adsorption capacity of H2O was much larger than CO2, and the adsorption of H2O had a significant impact on the CO2adsorption capacity on zeolite13XAPG. so a dehumidified unit was usually required before the adsorption unit in the capture process.
thirdly, several adsorption processes by fixed bed packed with zeolite13XAPG were explored for CO2/N2separation by experiments and simulation, including vacuum pressure swing adsorption (VPSA) process (single bed. multibed and two-stage VPSA unit). temperature swing adsorption (TSA) process and hybrid vacuum pressure swing adsorption (VTSA) process. It was found that VTSA process was the most effective and promising process. However, the cycle time of VTSA process was too long due to the temperature swing process. Therefore, the VPSA process was adopted in the pilot-scale experiments for CO2capture from flue gas in an existing coal-fired power plant.
At last, an experimental evaluation combined with simulation was performed for CO2capture from flue gas using a pilot-scale single and two-stage VPSA unit in Shanghai Shengneng XingHuo thermo-power plant. The desulfurized flue gas passed through the dehumidifying unit to remove moisture and then was supplied to the carbon capture plant. With a single3-bed8-step VPSA unit packed with261kg zeolite13XAPG, CO2can be concentrated to75.7%with a CO2recovery of90.3%from flue gas at feed flowrate of37.0Nm3/h, and the power consumption was measured onsite as2.08MJ/kgCO2. The purity was lower than the demand for storage (>95%), therefore a two-stage VPSA unit with the effluent from the second unit recycled to the inlet was designed and tested. The first unit was the same as the single VPSA unit before and the second VPSA unit packed with68.6kg pitch-based ACBs was operated as2-bed6-step cycle. With this process, a CO2purity of95.6%was obtained with recovery of90.2%at the feed flowrate of35.5Nm3/h, and the power consumption was2.44MJ/kgCO2(lower than absorption). With the development of the adsorbent and further optimization of the processes, the adsorption technology can be a promising CO2capture technology.
首先,采用磁悬浮天平分别测定了CO2和N2在沸石13XAPG上的吸附平衡等温线,以Multi-site Langmuir等温线模型拟合,并计算吸附热。根据纯组分气体模型参数预测CO2/N2双组分的竞争吸附平衡,并进行实验验证,为吸附过程的设计提供基础数据。
其次,测量CO2/N2混合气在沸石13XAPG上的吸附突破解吸曲线,结合双分散二级孔线性推动力扩散模型,计算扩散系数和传递参数,研究CO2/N2在沸石13XAPG上的吸附动力学。此外,实验发现H2O对沸石13XAPG吸附CO2的容量有显著影响,所以在实际烟道气吸附捕集过程中,需要预处理脱水单元。
之后,采用沸石13XAPG填充吸附柱,通过实验和模拟研究几种循环吸附/解吸分离C02/N2的工艺,包括真空变压吸附工艺VPSA、变温吸附工艺TSA和真空变压变温耦合吸附工艺VTSA。研究发现真空变压变温耦合吸附工艺较为有效,具有一定应用前景,但是该工艺涉及变温过程,循环时间较长。在后续的中试实验中,采用快速的真空变压吸附(VPSA)技术来捕集燃煤电厂中二氧化碳。
最后采用沸石13XAPG吸附捕集上海申能星火热电厂烟道气中的CO2,实验考察了中试规模单级和两级VPSA工艺的捕集效率和能耗。脱硫后烟道气经过氧化铝脱湿单元除去水蒸汽,再经过吸附单元捕集CO2。单级VPSA单元填充261kg沸石13XAPG,采用三柱八步流程,对于37.0Nm3/h的干烟气,经过单级VPSA单元能够将C02提浓到75.7%,回收率达到90.3%,能耗为2.08MJ/kgCO2。可见单级捕集得到的C02纯度未达到封存要求(>95%),因此进一步设计和运行两级真空变压吸附工艺,第一级VPSA单元即为上述单级VPSA单元,第二级VPSA单元填充68.6kg活性炭小球并运行两柱六步流程,且将第二级废气回流到第一级入口处。实验结果表明,处理35.5Nm3/h的干燥后烟道气,经过第一级VPSA单元CO2能够提浓到74.5%,然后通过第二级VPSA单元浓缩到95.6%,回收率达到90.2%,需要能耗为2.44MJ/kgCO2,能耗较低,且随着高吸附吸附剂的开发以及吸附工艺的优化,吸附法将成为比较有前景的燃烧后CO2捕集方法。
Academic concerns have been raised with respect to the impact of the increasing concentration of carbon dioxide in the atmosphere on the environment as global warming. This global recognition has attracted great attention in relation to the creation, development and improvement upon technologies and strategies for the reduction of CO? emissions. Carbon capture and storage (CCS) is one of the most effective CO2emission abatement strategies in the world. Among all the post combustion capture technologies, adsorption process relying on well-engineered solid adsorbents is suggested as a promising option due to simple equipment, low energy requirement, less corrosion problems, easiness to achieve automatic operation and operating flexibility. In this work, a novel adsorbent zeolite13XAPG was employed as the selective adsorbent for CO2/N2separation. The feasibility and efficiency of adsorption technology for post-combustion CO2capture from Hue gas using zeolite13XAPG were evaluated by fundamental experiments, simulation and pilot-scale experiments in an existed coal-fired power plant.
Firstly, the adsorption equilibrium isotherms of CO2and N2on zeolite13XAPG were measured by a magnetic suspension balance. The adsorption heat was caculated from adsorption equilibrium data. Then Multi-site Langmuir model was employed to fit the experimental data with good agreement, and the fitted parameters were adopted in the prediction of binary competitive adsorption equilibrium, providing basic data for the design of adsorption process.
Secondly, adsorption kinetics of CO2/N2on zeolite13XAPG was investigated by the experimental data of breakthrough and desorption curves. A mathematical model based on the bi-LDF approximation was derived from mass, energy and momentum balances. Diffusion coefficient and transfer parameters were calculated through the comparison of experimental and simulated results. Moreover, it was found from experiments that the adsorption capacity of H2O was much larger than CO2, and the adsorption of H2O had a significant impact on the CO2adsorption capacity on zeolite13XAPG. so a dehumidified unit was usually required before the adsorption unit in the capture process.
thirdly, several adsorption processes by fixed bed packed with zeolite13XAPG were explored for CO2/N2separation by experiments and simulation, including vacuum pressure swing adsorption (VPSA) process (single bed. multibed and two-stage VPSA unit). temperature swing adsorption (TSA) process and hybrid vacuum pressure swing adsorption (VTSA) process. It was found that VTSA process was the most effective and promising process. However, the cycle time of VTSA process was too long due to the temperature swing process. Therefore, the VPSA process was adopted in the pilot-scale experiments for CO2capture from flue gas in an existing coal-fired power plant.
At last, an experimental evaluation combined with simulation was performed for CO2capture from flue gas using a pilot-scale single and two-stage VPSA unit in Shanghai Shengneng XingHuo thermo-power plant. The desulfurized flue gas passed through the dehumidifying unit to remove moisture and then was supplied to the carbon capture plant. With a single3-bed8-step VPSA unit packed with261kg zeolite13XAPG, CO2can be concentrated to75.7%with a CO2recovery of90.3%from flue gas at feed flowrate of37.0Nm3/h, and the power consumption was measured onsite as2.08MJ/kgCO2. The purity was lower than the demand for storage (>95%), therefore a two-stage VPSA unit with the effluent from the second unit recycled to the inlet was designed and tested. The first unit was the same as the single VPSA unit before and the second VPSA unit packed with68.6kg pitch-based ACBs was operated as2-bed6-step cycle. With this process, a CO2purity of95.6%was obtained with recovery of90.2%at the feed flowrate of35.5Nm3/h, and the power consumption was2.44MJ/kgCO2(lower than absorption). With the development of the adsorbent and further optimization of the processes, the adsorption technology can be a promising CO2capture technology.
引文
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