甲烷在甲醇和烃类混合溶剂中高压溶解度的研究
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摘要
随着环保意识的加强和汽车工业的发展，相对清洁、经济的天然气汽车成为现今研究的重点，如何实现天然气经济、高效地贮存则成为发展天然气汽车的当务之急，而将天然气溶解于适当的溶剂是一条有效的解决途经。本文为选择理想的天然气溶剂进行了相关的基础研究。
本文结合天然气汽车、甲醇汽车、乙醇汽车的发展要求，选择甲醇与正己烷、正庚烷、环己烷、苯、甲苯等烃类物质的二元混合溶液及甲醇-汽油和乙醇-汽油混合溶液作为溶剂，利用一套常温、高压下气体溶解度的实验装置准确测定了甲烷在各种混合溶剂中的溶解度数据。
选择PRSV状态方程的不同混合规则对甲烷-甲醇-烃极性物系的三元GLE数据进行了拟合计算。同时，还分别使用改进的活度系数法和缔合理论对实验数据进行了计算。结果表明：对于极性较强的体系，活度系数法虽然也能计算高压下的GLE，但计算效果不如状态方程法；当将缔合理论引入状态方程法时，计算精度得到了明显提高。
此外，本文测定了甲烷在汽油、苯-环己烷、苯-正庚烷、环己烷-正庚烷非极性混合溶剂中的高压溶解度数据，并用状态方程法对实验数据进行了计算，结果表明，对于非极性体系，用二元的GLE数据可以估算三元GLE数据，估算结果与实验结果能很好的吻合。
使用PR状态方程和A-K经验模型计算了各种实验体系的高压液相摩尔体积（密度）。并对A-K经验模型进行了修正，用于估算含醇物系的高压液相摩尔体积，修正后的A-K模型精度有较大的提高。结果表明用溶剂贮存天然气，可以降低燃料罐的储存压力并提高燃料贮存密度。
综上所述，本论文测定了甲烷常温下在各种混合溶剂中的高压溶解度，提供了实际应用的必需数据，提出了各种计算方法，可供设计含溶剂的天然气汽车燃料配方使用，也促进了气液相平衡理论及计算方法的进展。
With the improvement of environment consciousness and development of vehicles, relatively clean and economical natural gas vehicles become the emphasis of research. The very urgent problem of natural gas vehicle is how to store natural gas economically and efficiently. Dissolving natural gas in appropriate solvents maybe an effective way for putting natural gas vehicle in wide use. Some fundamental researches were done to select the ideal solvents for natural gas in the paper.
In order to tie in with the development of methanol vehicles, ethanol vehicles and natural gas vehicles, methanol mixing with n-hexane, n-heptane, benzene, toluene, cyclehexane, gasoline and ethanol-gasoline were selected as solvents separately. The solubilities of methane in these different kinds of mixed solvents at high pressures were measured by a set of experiment apparatus for measuring gas solubility under high pressures systematically.
The PRSV EOS coupled with different mixing rules were adopted to calculate the ternary GLE data of methane-methanol-hydrocarbon polar systems under high pressures by correlation. And the modified method based on activity coefficient and the EOS combined with associated theory were used to calculate the experimental data. It shows that the calculation result of the modified method based on activity coefficient is not as good as that of the PRSV EOS. And when the associated theory was used to EOS, the precision of calculation was improved greatly.
In addition, the solubilities of methane under high pressures in benzene -cyclehexane, benzene-n-heptane, cyclehexane-n-heptane and gasoline were determinated and the experimental data were calculated by PR EOS. It indicates that the ternary GLE data can be well estimated by the method using binary GLE data.
PR EOS and A-K model were both used to calculate the molar volumes
of liquid phase under high pressures for experimental systems. Besides, the A-K model was modified in order to estimate data of the systems containing alcohols more accurately. It shows that it is feasible to dissolve NG in solvents because by this means the energy storage density can be increased and the storage pressure can be decreased.
In a word, the methane solubilities in different mixed solvents under high pressures were determinated. It provided the necessary data for practical application. Some calculation methods were put forward; it can be used to design the natural gas vehicle fuels containing solvents. At the same time, the theory of phase equilibria and the calculation methods were advanced.
本文结合天然气汽车、甲醇汽车、乙醇汽车的发展要求，选择甲醇与正己烷、正庚烷、环己烷、苯、甲苯等烃类物质的二元混合溶液及甲醇-汽油和乙醇-汽油混合溶液作为溶剂，利用一套常温、高压下气体溶解度的实验装置准确测定了甲烷在各种混合溶剂中的溶解度数据。
选择PRSV状态方程的不同混合规则对甲烷-甲醇-烃极性物系的三元GLE数据进行了拟合计算。同时，还分别使用改进的活度系数法和缔合理论对实验数据进行了计算。结果表明：对于极性较强的体系，活度系数法虽然也能计算高压下的GLE，但计算效果不如状态方程法；当将缔合理论引入状态方程法时，计算精度得到了明显提高。
此外，本文测定了甲烷在汽油、苯-环己烷、苯-正庚烷、环己烷-正庚烷非极性混合溶剂中的高压溶解度数据，并用状态方程法对实验数据进行了计算，结果表明，对于非极性体系，用二元的GLE数据可以估算三元GLE数据，估算结果与实验结果能很好的吻合。
使用PR状态方程和A-K经验模型计算了各种实验体系的高压液相摩尔体积（密度）。并对A-K经验模型进行了修正，用于估算含醇物系的高压液相摩尔体积，修正后的A-K模型精度有较大的提高。结果表明用溶剂贮存天然气，可以降低燃料罐的储存压力并提高燃料贮存密度。
综上所述，本论文测定了甲烷常温下在各种混合溶剂中的高压溶解度，提供了实际应用的必需数据，提出了各种计算方法，可供设计含溶剂的天然气汽车燃料配方使用，也促进了气液相平衡理论及计算方法的进展。
With the improvement of environment consciousness and development of vehicles, relatively clean and economical natural gas vehicles become the emphasis of research. The very urgent problem of natural gas vehicle is how to store natural gas economically and efficiently. Dissolving natural gas in appropriate solvents maybe an effective way for putting natural gas vehicle in wide use. Some fundamental researches were done to select the ideal solvents for natural gas in the paper.
In order to tie in with the development of methanol vehicles, ethanol vehicles and natural gas vehicles, methanol mixing with n-hexane, n-heptane, benzene, toluene, cyclehexane, gasoline and ethanol-gasoline were selected as solvents separately. The solubilities of methane in these different kinds of mixed solvents at high pressures were measured by a set of experiment apparatus for measuring gas solubility under high pressures systematically.
The PRSV EOS coupled with different mixing rules were adopted to calculate the ternary GLE data of methane-methanol-hydrocarbon polar systems under high pressures by correlation. And the modified method based on activity coefficient and the EOS combined with associated theory were used to calculate the experimental data. It shows that the calculation result of the modified method based on activity coefficient is not as good as that of the PRSV EOS. And when the associated theory was used to EOS, the precision of calculation was improved greatly.
In addition, the solubilities of methane under high pressures in benzene -cyclehexane, benzene-n-heptane, cyclehexane-n-heptane and gasoline were determinated and the experimental data were calculated by PR EOS. It indicates that the ternary GLE data can be well estimated by the method using binary GLE data.
PR EOS and A-K model were both used to calculate the molar volumes
of liquid phase under high pressures for experimental systems. Besides, the A-K model was modified in order to estimate data of the systems containing alcohols more accurately. It shows that it is feasible to dissolve NG in solvents because by this means the energy storage density can be increased and the storage pressure can be decreased.
In a word, the methane solubilities in different mixed solvents under high pressures were determinated. It provided the necessary data for practical application. Some calculation methods were put forward; it can be used to design the natural gas vehicle fuels containing solvents. At the same time, the theory of phase equilibria and the calculation methods were advanced.
引文
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郭志东， 迎接普及天然气汽车的浪潮, 北京汽车，2001, (2): 17-26.
[2]
孙志军，候树荣，天然气作业汽车燃料的应用及发展, 汽车技术，1997,(10): 9-14.
[3]
Stefano D P, Femia A, Luzzati T，Natural gas, cars and the environment，A (relatively) ‘clean’ and cheap fuel looking for users, Ecological Economics, 2001, 38: 179-189.
[4]
唐晓东,白剑，增湿天然气用作天然气汽车燃料的探讨, 天然气工业，1999, 19(4): 84-87.
[5]
孙济美主编, 天然气和液化石油气汽车, 北京: 北京理工大学出版社,1999.
[6]
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