【摘要】 通过使用表面活性剂来提升水合物的生成速度和转化率是提高水合物技术经济价值的主要方法。因为泡沫过多不利于生产,低起泡性的聚苯乙烯磺酸钠(PSS)在水合物技术领域具有很好应用的潜力。本文根据对含PSS体系的水合物生成热力学研究,提出了乙烯-PSS溶液体系的热力学模型以定量描述PSS对水合物的热力学影响,该模型可较为准确地预测水合物的热力学临界生成压力:平均相对误差为1.1%,最大相对误差为3.8%。在上述研究基础上,本文研究了在PSS存在的情况下,PSS初始浓度和热力学推动力对Ⅰ型水合物的生成速度、最终转化率(水合物生成结束时的转化率)等参数的影响。结果表明,PSS对Ⅰ型水合物的热力学负面影响很小。PSS使水合物的最终转化率由59.6%±1.9%提升到80%以上,并使水合物的生成速度显著提升。当PSS初始浓度或压力低于特定值时,提高PSS初始浓度或压力可有效提升水合物的生成速度和最终转化率;但PSS初始浓度或压力高于特定值时,提高PSS初始浓度或压力对水合物生成速度和最终转化率的提升效果不再明显。更多还原

【Abstract】 Increasing the hydrate formation rate（rH） and the conversion rate of the water into hydrate（RWH） by using surfactants is the main method to increase the economic value of hydrate-based technologies（HBTs）. Sine foams are detrimental to the industrial application of HBTs, poly（sodium 4-styrenesulfonate）（PSS）, which is a surfactant with low foaming ability, has good potential in the fields of HBTs. Based on the investigation on the thermodynamics of the hydrate formation in presence of PSS in this paper, this paper proposed a thermodynamic model of ethylene-PSS solution system to quantitatively describe the thermodynamic effect of PSS on the formation of structure Ⅰ hydrate. The above model can predict the thermodynamic equilibrium hydrate formation pressure accurately: the average related deviation is 1.1% and the maximum related deviation is 3.8%. Based on the above investigations, this paper investigated the effects of the initial concentration of the PSS in liquid phase（wp,0） and thermodynamic driving force on the rH, the final R_WHand other parameters. The experimental results show that, PSS had little negative thermodynamic effect on the formation of structure Ⅰ hydrate. The presence of PSS not only increased the final RWHfrom 59.6%±1.9% to higher than 80% but also significantly increased the rH. When pressure/wp,0 was lower than a specific value, both the final R_WH and the rHcan be significantly increased by increasing pressure/wp,0. When pressure/w_p,0 was lower than the specific value,neither the final RWHnor the rHcan be significantly increased by increasing pressure/w_p,0.更多还原