二氧化碳的吸附分离
摘要
随着全球经济的发展和人口的激增，人类活动所排放的大量二氧化碳已引起全球气候变暖，其中绝大部分的二氧化碳是由化石燃料燃烧所产生。由于未来几十年内化石燃料将会继续主导生产，因此从烟道气中捕集和回收利用二氧化碳对降低温室气体的排放具有重要意义。除此之外，在其它的化工工艺或特定场合中（发酵厂、天然气净化、沼气净化、无菌病房、密闭空间），二氧化碳的脱除或分离也具有很重要的现实意义。因此研究如何有效的捕集和回收二氧化碳具有重要的现实意义。
烟道气的主要成分为氮气和二氧化碳，因此二氧化碳和氮气的有效分离是捕集和回收烟道气中二氧化碳的关键。烟道气中的二氧化碳含量较低（8%～15%），采用物理吸收法（选择性低）、化学吸收法（高腐蚀、胺损耗）、低温法（投资多、占地广、能耗高）、膜分离法（产品气浓度低）来捕集烟道气中二氧化碳或多或少存在一些缺点，而吸附法因设备简单、能耗低、温度压力操作范围宽而成为捕集二氧化碳最为优势的方法。
吸附剂的吸附性能是变压吸附分离效果的关键和决定因素。因此，本文首先详细地考察了12种吸附剂对CO_2/N_2的分离性能，分析了温度、吸附剂表面极性、比表面积及孔径大小对分离性能的影响，从而为高效专有吸附剂的研发奠定了理论基础。
其次，由于常温下二氧化碳可以在吸附剂上发生多分子层吸附甚至毛细孔凝聚，而氮气只能发生单分子吸附，因此首次考察了二氧化碳吸附机理的改变对CO_2/N_2分离效果的具体影响。
为了进一步增强吸附剂对CO_2/N_2的分离性能，本文采用不同胺（TEA、MDEA、DEA）改性吸附剂，研究了温度、胺负载率对吸附剂吸附分离CO_2/N_2的影响，并考察了胺改性后吸附剂的再生性和稳定性。结果表明，微孔吸附剂不适宜负载改性，而胺改性后的介孔吸附剂对CO_2/N_2具有较好的分离效果。其中当TEA、MDEA、DEA负载率分别为0.951、0.886、0.699时分离因子最大，分别为3.86、9.83、20.08。虽然DEA改性吸附剂的分离效果最好，但吸附剂在常温下难以再生。
最后，由于烟道气中含有一定量的水蒸气，因此考察了水含量对胺改性吸附剂吸附分离CO_2/N_2的影响。结果表明，分离因子随水负载率的增大而增大，水的存在有利于CO_2/N_2的分离。其中RTEA=0.713的改性吸附剂在RW=0.349时的分离因子最大为24.50。RMDEA=0.644的改性吸附剂在RW=0.397时的分离因子高达29.69。RDEA=0.699的吸附剂在RW=0.347时分离因子高达40.09。而且无论有无水存在，TEA、MDEA改性吸附剂在常温下都具有很好的再生性和稳定性。
With the development of economy, enrichment of atmospheric greenhouse gases,mainly carbon dioxide, resulted from human activities has increased global meantemperature. Because most of the carbon dioxide is emitted from coal-fired power plantsand about80%of global energy supply will still rely on fossil fuels in the future, the studieson CO_2capture from the flue gas are very important.
The main components in the flue gas are CO_2and N_2, so the separation between CO_2and N_2is the key. The methods so far presented for the capture of flue gas CO_2includesbsoption, adsorption, membrane separation and the separation at low temperature. Thechemical absorption of CO_2with aqueous solutions of amines is presently the mosteconomical one, but there are some problems with equipment corrosion, amine lost andhigh-energy cost. The adsorption method bearing advantange in simple equipment,low-energy cost, wide range of pressure and temperature has been the most potentialmethod for the CO_2capture.
The adsorbent is the core of adsorption, which determines the separation performance.So the paper studied the separation coefficients of twelve adsorbents, and the influences oftemperature, surface polarity, specific surface area and pore size on the separationperformance are presented, firstly.
Because CO_2could be adsorbed with the occurrence of multi-layer adsorption andcapillary condensation, while N_2adsorbed with the single molecular adsorption undernormal temperature, so the researches on whether the change of adsorption mechanismcould enhance the separation performance of CO_2and N_2under high pressures areobservated.
Secondly, in order to enhance the separation performances of adsorbent, adsorbentsSG-A and SG-B are modified with different amines. The effects of amine-loading andtemperature on the separation between CO_2and N_2are investigated, and the regenerationand stability are also researched at normal temperature. The results show thatamine-modified adsorbents could enhance the separation performances. And the modifiedadsorbents with TEA or MDEA have a good regeneration at normal temperature, but withDEA couldn’t.
At last, the effects of water on the separation coefficient between CO_2and N_2withloading different amines are presented. The results show that the presence of water could enhance the separation of CO2and N_2, and the modified adorbents with TEA or MDEA alsocould be regenerated in the presence of water.
烟道气的主要成分为氮气和二氧化碳，因此二氧化碳和氮气的有效分离是捕集和回收烟道气中二氧化碳的关键。烟道气中的二氧化碳含量较低（8%～15%），采用物理吸收法（选择性低）、化学吸收法（高腐蚀、胺损耗）、低温法（投资多、占地广、能耗高）、膜分离法（产品气浓度低）来捕集烟道气中二氧化碳或多或少存在一些缺点，而吸附法因设备简单、能耗低、温度压力操作范围宽而成为捕集二氧化碳最为优势的方法。
吸附剂的吸附性能是变压吸附分离效果的关键和决定因素。因此，本文首先详细地考察了12种吸附剂对CO_2/N_2的分离性能，分析了温度、吸附剂表面极性、比表面积及孔径大小对分离性能的影响，从而为高效专有吸附剂的研发奠定了理论基础。
其次，由于常温下二氧化碳可以在吸附剂上发生多分子层吸附甚至毛细孔凝聚，而氮气只能发生单分子吸附，因此首次考察了二氧化碳吸附机理的改变对CO_2/N_2分离效果的具体影响。
为了进一步增强吸附剂对CO_2/N_2的分离性能，本文采用不同胺（TEA、MDEA、DEA）改性吸附剂，研究了温度、胺负载率对吸附剂吸附分离CO_2/N_2的影响，并考察了胺改性后吸附剂的再生性和稳定性。结果表明，微孔吸附剂不适宜负载改性，而胺改性后的介孔吸附剂对CO_2/N_2具有较好的分离效果。其中当TEA、MDEA、DEA负载率分别为0.951、0.886、0.699时分离因子最大，分别为3.86、9.83、20.08。虽然DEA改性吸附剂的分离效果最好，但吸附剂在常温下难以再生。
最后，由于烟道气中含有一定量的水蒸气，因此考察了水含量对胺改性吸附剂吸附分离CO_2/N_2的影响。结果表明，分离因子随水负载率的增大而增大，水的存在有利于CO_2/N_2的分离。其中RTEA=0.713的改性吸附剂在RW=0.349时的分离因子最大为24.50。RMDEA=0.644的改性吸附剂在RW=0.397时的分离因子高达29.69。RDEA=0.699的吸附剂在RW=0.347时分离因子高达40.09。而且无论有无水存在，TEA、MDEA改性吸附剂在常温下都具有很好的再生性和稳定性。
With the development of economy, enrichment of atmospheric greenhouse gases,mainly carbon dioxide, resulted from human activities has increased global meantemperature. Because most of the carbon dioxide is emitted from coal-fired power plantsand about80%of global energy supply will still rely on fossil fuels in the future, the studieson CO_2capture from the flue gas are very important.
The main components in the flue gas are CO_2and N_2, so the separation between CO_2and N_2is the key. The methods so far presented for the capture of flue gas CO_2includesbsoption, adsorption, membrane separation and the separation at low temperature. Thechemical absorption of CO_2with aqueous solutions of amines is presently the mosteconomical one, but there are some problems with equipment corrosion, amine lost andhigh-energy cost. The adsorption method bearing advantange in simple equipment,low-energy cost, wide range of pressure and temperature has been the most potentialmethod for the CO_2capture.
The adsorbent is the core of adsorption, which determines the separation performance.So the paper studied the separation coefficients of twelve adsorbents, and the influences oftemperature, surface polarity, specific surface area and pore size on the separationperformance are presented, firstly.
Because CO_2could be adsorbed with the occurrence of multi-layer adsorption andcapillary condensation, while N_2adsorbed with the single molecular adsorption undernormal temperature, so the researches on whether the change of adsorption mechanismcould enhance the separation performance of CO_2and N_2under high pressures areobservated.
Secondly, in order to enhance the separation performances of adsorbent, adsorbentsSG-A and SG-B are modified with different amines. The effects of amine-loading andtemperature on the separation between CO_2and N_2are investigated, and the regenerationand stability are also researched at normal temperature. The results show thatamine-modified adsorbents could enhance the separation performances. And the modifiedadsorbents with TEA or MDEA have a good regeneration at normal temperature, but withDEA couldn’t.
At last, the effects of water on the separation coefficient between CO_2and N_2withloading different amines are presented. The results show that the presence of water could enhance the separation of CO2and N_2, and the modified adorbents with TEA or MDEA alsocould be regenerated in the presence of water.
引文
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