化工进展 ›› 2016, Vol. 35 ›› Issue (03): 700-705.DOI: 10.16085/j.issn.1000-6613.2016.03.007

• 化工过程与装备 • 上一篇    下一篇

水逸度模型预测THF添加剂体系下气体水合物相平衡

梁海峰1,2, 朱耀剑2, 赵阳升1, 赵建忠1   

  1. 1 太原理工大学采煤工艺研究所, 山西 太原 030024;
    2 太原理工大学化学化工学院, 山西 太原 030024
  • 收稿日期:2015-09-02 修回日期:2015-10-23 出版日期:2016-03-05 发布日期:2016-03-05
  • 通讯作者: 梁海峰(1980-),男,博士,讲师,主要从事多孔介质内传热传质及水合物开采研究。E-mail:lianghaifeng@tyut.edu.cn.
  • 基金资助:

    国家自然科学基金青年基金(51106104)、山西省自然科学基金青年基金(20120210022-5)及国家自然科学基金(51074111)项目。

Phase equilibrium study of gas mixtures hydrate formation with additives THF based on water fugacity model

LIANG Haifeng1,2, ZHU Yaojian2, ZHAO Yangsheng1, ZHAO Jianzhong1   

  1. 1 Mining Technology Institute, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China;
    2 College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
  • Received:2015-09-02 Revised:2015-10-23 Online:2016-03-05 Published:2016-03-05

摘要: 加入添加剂降低水合物生成压力是当前水合物法分离混合气体研究热点。本研究以水的逸度模型为基础, 结合PRSV2 状态方程研究了CH4、O2、N2 及其混合气体水合物在纯水体系下的相平衡条件;通过UNIFAC 基团 贡献法对添加剂四氢呋喃(THF)水溶液进行基团划分,计算该体系下液相各组分的活度,理论研究了添加剂 THF 对气体水合物相平衡条件的影响;结果表明在相应的温度范围内,与其他模型相比,在纯水体系下该模型 预测精度较高,在THF 水溶液体系下该模型对单组分和双组分气体的预测精度平均相对误差在7%左右,随着 THF 浓度增加,气体水合物相平衡压力的降低幅度减小;当THF 摩尔分数达到6%时,对气体水合物相平衡影 响达到最大。相关研究结果为混合气体的大规模工业提纯分离提供了理论基础。

关键词: 模型, 水合物, 相平衡, 活度系数, 四氢呋喃, UNIFAC 基团贡献法

Abstract: Gas hydrates have absorbed more and more attentions as a potential medium for gas separation. The additive promoters can reduce the hydrate equilibrium pressure at a given temperature. In this paper,we had mainly conducted on phase equilibrium of CH4、O2、N2 and corresponding gas mixtures hydrate based on the water fugacity model integrated with the gas state equations of PRSV2. Furthermore , the groups of additive-aqueous solution were divided based on UNIFAC group contribution method to calculate activity of each composition in aqueous phase,and the effects of additives on phase equilibrium pressure of aforementioned gas mixtures hydrate were studied. The results showed that the water fugacity model is more accurate compared with other models in pure water system. Under the condition of tetrahydrofuran (THF) aqueous solution system,the water fugacity model prediction accuracy is about 7% for single or double-component gas hydrate. With the increase of THF concentration,the scale of the equilibrium pressure depression is reduced. When the THF aqueous solution concentration reaches 6% mole fraction,the phase equilibrium pressure of gas hydrate reaches the minimum.

Key words: model, hydrate, phase equilibria, activity coefficient, THF additives, UNIFAC group contribution method

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