硅基介孔材料改性吸附/捕集CO_2研究
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摘要
诸多科学研究结果表明，人类活动造成了全球变暖和气候变化，这引起了全世界的极大关切。政府间气候变化委员会（IPCC）在其报告中特别指出，CO_2对全球变暖和气候变化的影响最大，是最为重要的温室气体。CO_2的捕集与封存（CCS）是减少温室气体CO_2排放的最有效手段之一。
本文旨在利用吸附的方法，通过对硅基介孔材料表面改性来捕集分离CO_2。经过X射线光电子能谱（XPS）、X射线衍射（XRD）、能谱仪（EDS）、透射电镜（TEM）及扫描电镜（SEM）等多种方法分析表明乙酸铅浸渍于硅基介孔材料表面后经过焙烧变为PbO。本文分别研究了无水和水存在的条件下PbO/SilicaGel、PbO/SBA-15及PbO/MCM-41等硅基介孔材料改性吸附剂对CO_2的吸附效果，同时研究了这些材料对混合气中CO_2的吸附分离效果。结果表明，这些改性材料在水存在的条件下之所以能吸附CO_2的原因在于其表面的PbO与CO_2发生了化学反应，其对CO_2的吸附量与所负载PbO的量成正比。实验中PbO/SilicaGel、PbO/SBA-15和PbO/MCM-41三种吸附剂对CO_2的吸附量分别达到了240.86mg·g~(-1)、229.89mg·g~(-1)和273.93mg·g~(-1)，并且，随着PbO负载量的增加，硅基改性吸附剂会吸附更多的CO_2，但此时需要更长的时间达到吸附平衡，这便失去了快速捕集CO_2的意义。实验发现，硅基改性吸附剂在PbO单层分散时捕集CO_2的速度最快，此时PbO/Silica Gel、PbO/SBA-15和PbO/MCM-41三种吸附剂的CO_2平衡吸附量分别为116.38mg·g~(-1)、163.54mg·g~(-1)和184.79mg·g~(-1)。
密闭空间中CO_2的浓度高于2%时人便不再适于置留其间，本文中以CO_2含量13.03%的原料气在所制备的硅基改性吸附剂上测试穿透实验，结果显示PbO/Silica gel、PbO/SBA-15和PbO/MCM-41三种吸附剂在水汽存在条件下均能让穿过其间的原料气中CO_2的浓度长时间保持在2%以下，三种吸附剂在PbO单层分散时对原料气中CO_2的吸附量分别达到58.4mg·g~(-1)、80.6mg·g~(-1)和102.2mg·g~(-1)。这表明，本文中所制备的吸附剂不仅能够快速吸附纯CO_2气体，还能捕集碳含量较低的混合气中的CO_2，是一种适用于密闭空间中CO_2捕集的新型改性吸附剂。
化学吸附剂的再生往往较为困难，本文中通过将吸附饱和的硅基改性吸附剂在氮气保护条件下于380℃焙烧3个小时即可再生，经过循环测试，发现再生后的吸附剂吸附捕集CO_2的效果依然良好，因此，用PbO改性硅基介孔材料后所得的吸附剂是一种比较理想的CO_2捕集和分离材料。
Many scientific reports show that human intervention has caused Earth’s currenttemperature and climate changes, and this is a matter of immense concern. TheReports by Intergovernmental Panel on Climate Change (IPCC) suggest that CO_2isthe most important greenhouse gas due to its greatest effect on global warming andclimate changes. CO_2Capture and Storage is one of the most effective measures forgreenhouse carbon oxide emission reduction.
The mean body of this paper aims to research capture and separation CO_2usingmodified silicon-based mesoporous materials through adsorption method. By way ofX ray photoelectron spectroscopy (XPS), X ray diffraction (XRD), energy dispersivespectrometer (EDS), transmission electron microscope (TEM) and scanning electronmicroscope (SEM), the analysis result of experiments indicated that acetic acid leadimpregnated on a silicon surface into PbO by roasting. In this study, CO_2adsorption inthe presence and absence of H2O was investigated on different modified silicon-basedmesoporous materials including lead oxide modified silica gel (PbO/Silica gel), leadoxide modified SBA-15(PbO/SBA-15), as well as lead oxide modified MCM-41(PbO/MCM-41). It is shown that the reason these modified silicon-based mesoporousmaterials adsorb CO_2is that there is a chemical reaction tetween CO_2and PbO scattedon the silica-based mesoporous materials at the existence of water, and the CO_2adsorption quantity is proportional to the amount of and PbO. In the experiments themaximum CO_2adsorption amount of three adsorbents inculuding PbO/Silica gel,PbO/SBA-15and PbO/MCM-41reached to240.86mg·g~(-1),229.89mg·g~(-1)and273.93mg·g~(-1)respectively. The results show that, with the increasing of PbO loaded.Modified silicon-based adsorbents can adsorb more CO_2, but at the longer timerequired to reach adsorption equilibrium, which will be meanless for caputre CO_2rapidly. The study shows that lead oxide modified silicon-based porous materialscapture CO_2fastest when PbO dispersed as a monolayer, meanwhile, the equilibriumCO_2adsorption capacity of PbO/Silica gel, PbO/SBA-15and PbO/MCM-41is116.38mg·g~(-1),163.54mg·g~(-1)and184.79mg·g~(-1)respectively.
The CO_2concentration that is over2%in enclosed chamber will be unsuitablefor healthy.13.03%of the CO_2content of the raw gas is uesd to test penetration experiment in modified silicon adsorbents. The result shows these three kinds ofadsorbents, PbO/Silica gel, PbO/SBA-15and PbO/MCM-41, can make CO_2concentration of gas mixture under2%for a long time in the water vapor condition,and the CO_2adsorption capacity of gas mixture by these three adsorbents is58.4mg·g~(-1),80.6mg·g~(-1)and102.2mg·g~(-1)respectively, which indicates the adsorbentsprepared by this method can not only rapidly adsorb pure CO_2gas, but also cancapture CO_2from low carbon content of mixture and they are new adsorbents beingapplied to capture CO_2in enclosed chamber.
Chemical adsorbent is always much harder to be regenerated. In this paper, thesilica-based-functionalized adsorbents that adsorbed maximumly can be regeneratedat380℃for3hours under the protection of nitrogen. It is found that regeneratedabsorbents have a good effect of adsorption for capture and store carbon dioxide afterseveral cyclings. So lead oxide modified silicon-based porous materials are ideal CO_2capture and separation adsorbents.
本文旨在利用吸附的方法，通过对硅基介孔材料表面改性来捕集分离CO_2。经过X射线光电子能谱（XPS）、X射线衍射（XRD）、能谱仪（EDS）、透射电镜（TEM）及扫描电镜（SEM）等多种方法分析表明乙酸铅浸渍于硅基介孔材料表面后经过焙烧变为PbO。本文分别研究了无水和水存在的条件下PbO/SilicaGel、PbO/SBA-15及PbO/MCM-41等硅基介孔材料改性吸附剂对CO_2的吸附效果，同时研究了这些材料对混合气中CO_2的吸附分离效果。结果表明，这些改性材料在水存在的条件下之所以能吸附CO_2的原因在于其表面的PbO与CO_2发生了化学反应，其对CO_2的吸附量与所负载PbO的量成正比。实验中PbO/SilicaGel、PbO/SBA-15和PbO/MCM-41三种吸附剂对CO_2的吸附量分别达到了240.86mg·g~(-1)、229.89mg·g~(-1)和273.93mg·g~(-1)，并且，随着PbO负载量的增加，硅基改性吸附剂会吸附更多的CO_2，但此时需要更长的时间达到吸附平衡，这便失去了快速捕集CO_2的意义。实验发现，硅基改性吸附剂在PbO单层分散时捕集CO_2的速度最快，此时PbO/Silica Gel、PbO/SBA-15和PbO/MCM-41三种吸附剂的CO_2平衡吸附量分别为116.38mg·g~(-1)、163.54mg·g~(-1)和184.79mg·g~(-1)。
密闭空间中CO_2的浓度高于2%时人便不再适于置留其间，本文中以CO_2含量13.03%的原料气在所制备的硅基改性吸附剂上测试穿透实验，结果显示PbO/Silica gel、PbO/SBA-15和PbO/MCM-41三种吸附剂在水汽存在条件下均能让穿过其间的原料气中CO_2的浓度长时间保持在2%以下，三种吸附剂在PbO单层分散时对原料气中CO_2的吸附量分别达到58.4mg·g~(-1)、80.6mg·g~(-1)和102.2mg·g~(-1)。这表明，本文中所制备的吸附剂不仅能够快速吸附纯CO_2气体，还能捕集碳含量较低的混合气中的CO_2，是一种适用于密闭空间中CO_2捕集的新型改性吸附剂。
化学吸附剂的再生往往较为困难，本文中通过将吸附饱和的硅基改性吸附剂在氮气保护条件下于380℃焙烧3个小时即可再生，经过循环测试，发现再生后的吸附剂吸附捕集CO_2的效果依然良好，因此，用PbO改性硅基介孔材料后所得的吸附剂是一种比较理想的CO_2捕集和分离材料。
Many scientific reports show that human intervention has caused Earth’s currenttemperature and climate changes, and this is a matter of immense concern. TheReports by Intergovernmental Panel on Climate Change (IPCC) suggest that CO_2isthe most important greenhouse gas due to its greatest effect on global warming andclimate changes. CO_2Capture and Storage is one of the most effective measures forgreenhouse carbon oxide emission reduction.
The mean body of this paper aims to research capture and separation CO_2usingmodified silicon-based mesoporous materials through adsorption method. By way ofX ray photoelectron spectroscopy (XPS), X ray diffraction (XRD), energy dispersivespectrometer (EDS), transmission electron microscope (TEM) and scanning electronmicroscope (SEM), the analysis result of experiments indicated that acetic acid leadimpregnated on a silicon surface into PbO by roasting. In this study, CO_2adsorption inthe presence and absence of H2O was investigated on different modified silicon-basedmesoporous materials including lead oxide modified silica gel (PbO/Silica gel), leadoxide modified SBA-15(PbO/SBA-15), as well as lead oxide modified MCM-41(PbO/MCM-41). It is shown that the reason these modified silicon-based mesoporousmaterials adsorb CO_2is that there is a chemical reaction tetween CO_2and PbO scattedon the silica-based mesoporous materials at the existence of water, and the CO_2adsorption quantity is proportional to the amount of and PbO. In the experiments themaximum CO_2adsorption amount of three adsorbents inculuding PbO/Silica gel,PbO/SBA-15and PbO/MCM-41reached to240.86mg·g~(-1),229.89mg·g~(-1)and273.93mg·g~(-1)respectively. The results show that, with the increasing of PbO loaded.Modified silicon-based adsorbents can adsorb more CO_2, but at the longer timerequired to reach adsorption equilibrium, which will be meanless for caputre CO_2rapidly. The study shows that lead oxide modified silicon-based porous materialscapture CO_2fastest when PbO dispersed as a monolayer, meanwhile, the equilibriumCO_2adsorption capacity of PbO/Silica gel, PbO/SBA-15and PbO/MCM-41is116.38mg·g~(-1),163.54mg·g~(-1)and184.79mg·g~(-1)respectively.
The CO_2concentration that is over2%in enclosed chamber will be unsuitablefor healthy.13.03%of the CO_2content of the raw gas is uesd to test penetration experiment in modified silicon adsorbents. The result shows these three kinds ofadsorbents, PbO/Silica gel, PbO/SBA-15and PbO/MCM-41, can make CO_2concentration of gas mixture under2%for a long time in the water vapor condition,and the CO_2adsorption capacity of gas mixture by these three adsorbents is58.4mg·g~(-1),80.6mg·g~(-1)and102.2mg·g~(-1)respectively, which indicates the adsorbentsprepared by this method can not only rapidly adsorb pure CO_2gas, but also cancapture CO_2from low carbon content of mixture and they are new adsorbents beingapplied to capture CO_2in enclosed chamber.
Chemical adsorbent is always much harder to be regenerated. In this paper, thesilica-based-functionalized adsorbents that adsorbed maximumly can be regeneratedat380℃for3hours under the protection of nitrogen. It is found that regeneratedabsorbents have a good effect of adsorption for capture and store carbon dioxide afterseveral cyclings. So lead oxide modified silicon-based porous materials are ideal CO_2capture and separation adsorbents.
引文
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