多孔介质储气研究
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摘要
使用清洁、可再生能源是目前世界一项紧迫任务,天然气进而氢气被认为是合适的选择。气体在机动车上的存储是解决车用气体燃料的关键技术之一,而吸附被认为是有望解决这一问题的有效手段。近年来,对碳纳米管储氢的报道很多,结果却大相径庭。本论文测定了不同温度下碳纳米管对氢气的系列吸附等温线,并与活性炭上的储氢量进行比较。结果表明,氢气在碳纳米管上的吸附量很小,常温10MPa下吸附量只有0.2wt%。液氮温度下吸附量有所增加,但还是低于DOE标准。本论文以提高储氢容量为目的进行了多项尝试,其中包括活性炭表面的酸碱改性、SBA-15负载金属钯等。通过对实验数据的分析探讨了吸附储氢的机理,指出:临界温度以上的物理吸附遵循单分子层吸附机制,比表面积和储气温度是吸附量的决定因素,材料的其它特征和性质对储氢容量没有实质性影响。
以提高甲烷的有效存储容量为目的,本论文研究了多孔介质湿储甲烷的方法。结果表明,预吸水的多孔介质对甲烷的吸入量较干燥样品有大幅提高,以BY-1活性炭为例,其对甲烷的吸入量可提高63%。随后进行的充放气研究表明,湿储过程中的热效应远低于吸附天然气温度的波动。对影响甲烷储量的诸多因素,如温度、载水量、填充密度、孔径分布等进行了考察。通过对甲烷湿储机理的分析证实了水存在条件下甲烷储量的提高是由于微孔中甲烷水合物的生成。
考虑到氢氧燃料电池汽车发动机对氧源装置体积的严格限制,本论文研究了氧气在高比表面活性炭上的吸附特性,测定了氧气跨越临界温度的系列吸附等温线。实验温度为118～313K,压力为0～10MPa。并从实验数据计算了吸附热。以Gibbs定义和绝对吸附量模型为基础的过剩吸附量等温线模型很好地描述了氧气在活性炭上跨越临界点的大温度范围吸附平衡数据。实验结果显示了对氧气吸附存储的可行性。
二氧化碳以水合物形式进行深海填埋是解决温室气体过量排放的有效手段之一。本文考察了水存在条件下多孔介质对二氧化碳的固定作用,测定了预吸水的炭材料对二氧化碳的吸入等温线,分析了二氧化碳吸入量的影响因素。实验证实了水存在条件下CO_2吸入量的提高是由于在微孔内生成了水合物。作者还测定了二氧化碳和甲烷的混合气在预吸水活性炭上的平衡等温线,计算了固定态混合气中各组分的含量,为二氧化碳深海填埋及可燃冰开采的实际需要提供了基础数据。
To develop a clean and renewable energy source is an urgent task for the world. Natural gas and hydrogen are thought to be appropriate alternative fuels. Gas storage on board of vehicle is one of the most important technologies in utilizing these alternative fuels. Many works on hydrogen storage using carbon nanotubes as the carrier have been reported. However, the results reported for the hydrogen storage capacity are quite divergent. In this dissertation, adsorption isotherms of hydrogen on multiwalled carbon nanotubes (MWNT) were measured for a wide range of temperature with a volumetric method, which was compared with the results collected on activated carbon AX-21. It is concluded that the amount of hydrogen absorbed on MWNT is very low, only 0.2wt% at room temperature and 10MPa. Although the storage capacity increases at 77K, it is much lower compared to the DOE criterior. In order to enhance the hydrogen uptake, many experiments, such as the modification of activated carbons using acid and alkali, Pd-loading on SBA-15 and so on were tested. These tests indicate that the physical adsorption above the critical temperature follows a monolayer surface coverage mechanism. Specific surface area and temperature are the decisive factors for the amount adsorbed. Other properties of the porous media only have minor effect on hydrogen storage capacity.
Aiming to enhance the storage capacity of methane, methane sorption in porous media in the presence of water was studied. It is shown that 63% more methane was stored pre unit mass of activated carbon BY-1 compared to that of dry sample. The charging/discharging process of methane into/from the wet carbon indicate that the thermal effect is much more less than that with dry carbon. Effects of temperature, water ratio, package density and pore size distribution on the sorption amount of methane are studied. It was proven that the enhanced sorption of methane is due to the formation of methane hydrates in the pore spaces of carbon.
Limitations on the equipment dimension of oxygen supplier promoted the study on oxygen storage in high surface activated carbon. Adsorption isotherms of oxygen on activated carbon AX-21 were collected for a range of 118-313K and 0-10 MPa. The isosteric heat of adsorption were evaluated basing of the isotherms. A model is presented for the experimental isotherms basing on the Gibbs definition of adsorption and the determination of absolute adsorption quantity. The model fits the isotherms very well for the whole range tested. Based of the measurements, the enhancement effect of adsorption for the storage of oxygen is proven.
Carbon dioxide is an important greenhouse gas, however, it can be sequestrated as hydrates deep in the sea. The sorption isotherms of CO_2 in porous media were measured in the presence of water. All effects affecting the sorption amount of CO_2 in wet materials were discussed. The mechanism of enhanced storage capacity of CO_2 is proved to be the formation of hydrates in the pore spaces. The sorption isotherms of a mixture of CO_2 and CH4 in wet activated carbon were collected and the proportions of components in the adsorbed phase were calculated. These data might be useful for CO_2 sequestration and CH4 exploitation.
以提高甲烷的有效存储容量为目的,本论文研究了多孔介质湿储甲烷的方法。结果表明,预吸水的多孔介质对甲烷的吸入量较干燥样品有大幅提高,以BY-1活性炭为例,其对甲烷的吸入量可提高63%。随后进行的充放气研究表明,湿储过程中的热效应远低于吸附天然气温度的波动。对影响甲烷储量的诸多因素,如温度、载水量、填充密度、孔径分布等进行了考察。通过对甲烷湿储机理的分析证实了水存在条件下甲烷储量的提高是由于微孔中甲烷水合物的生成。
考虑到氢氧燃料电池汽车发动机对氧源装置体积的严格限制,本论文研究了氧气在高比表面活性炭上的吸附特性,测定了氧气跨越临界温度的系列吸附等温线。实验温度为118～313K,压力为0～10MPa。并从实验数据计算了吸附热。以Gibbs定义和绝对吸附量模型为基础的过剩吸附量等温线模型很好地描述了氧气在活性炭上跨越临界点的大温度范围吸附平衡数据。实验结果显示了对氧气吸附存储的可行性。
二氧化碳以水合物形式进行深海填埋是解决温室气体过量排放的有效手段之一。本文考察了水存在条件下多孔介质对二氧化碳的固定作用,测定了预吸水的炭材料对二氧化碳的吸入等温线,分析了二氧化碳吸入量的影响因素。实验证实了水存在条件下CO_2吸入量的提高是由于在微孔内生成了水合物。作者还测定了二氧化碳和甲烷的混合气在预吸水活性炭上的平衡等温线,计算了固定态混合气中各组分的含量,为二氧化碳深海填埋及可燃冰开采的实际需要提供了基础数据。
To develop a clean and renewable energy source is an urgent task for the world. Natural gas and hydrogen are thought to be appropriate alternative fuels. Gas storage on board of vehicle is one of the most important technologies in utilizing these alternative fuels. Many works on hydrogen storage using carbon nanotubes as the carrier have been reported. However, the results reported for the hydrogen storage capacity are quite divergent. In this dissertation, adsorption isotherms of hydrogen on multiwalled carbon nanotubes (MWNT) were measured for a wide range of temperature with a volumetric method, which was compared with the results collected on activated carbon AX-21. It is concluded that the amount of hydrogen absorbed on MWNT is very low, only 0.2wt% at room temperature and 10MPa. Although the storage capacity increases at 77K, it is much lower compared to the DOE criterior. In order to enhance the hydrogen uptake, many experiments, such as the modification of activated carbons using acid and alkali, Pd-loading on SBA-15 and so on were tested. These tests indicate that the physical adsorption above the critical temperature follows a monolayer surface coverage mechanism. Specific surface area and temperature are the decisive factors for the amount adsorbed. Other properties of the porous media only have minor effect on hydrogen storage capacity.
Aiming to enhance the storage capacity of methane, methane sorption in porous media in the presence of water was studied. It is shown that 63% more methane was stored pre unit mass of activated carbon BY-1 compared to that of dry sample. The charging/discharging process of methane into/from the wet carbon indicate that the thermal effect is much more less than that with dry carbon. Effects of temperature, water ratio, package density and pore size distribution on the sorption amount of methane are studied. It was proven that the enhanced sorption of methane is due to the formation of methane hydrates in the pore spaces of carbon.
Limitations on the equipment dimension of oxygen supplier promoted the study on oxygen storage in high surface activated carbon. Adsorption isotherms of oxygen on activated carbon AX-21 were collected for a range of 118-313K and 0-10 MPa. The isosteric heat of adsorption were evaluated basing of the isotherms. A model is presented for the experimental isotherms basing on the Gibbs definition of adsorption and the determination of absolute adsorption quantity. The model fits the isotherms very well for the whole range tested. Based of the measurements, the enhancement effect of adsorption for the storage of oxygen is proven.
Carbon dioxide is an important greenhouse gas, however, it can be sequestrated as hydrates deep in the sea. The sorption isotherms of CO_2 in porous media were measured in the presence of water. All effects affecting the sorption amount of CO_2 in wet materials were discussed. The mechanism of enhanced storage capacity of CO_2 is proved to be the formation of hydrates in the pore spaces. The sorption isotherms of a mixture of CO_2 and CH4 in wet activated carbon were collected and the proportions of components in the adsorbed phase were calculated. These data might be useful for CO_2 sequestration and CH4 exploitation.
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