高压CO_(2)水合物的生成机理实验和模拟  

Experiment and Simulation of Carbon Dioxide Hydrate Formation Mechanism under High Pressure

作　　者：曹学文[1] 杨凯然 杨健 唐国祥 边江[1] CAO Xuewen;YANG Kairan;YANG Jian;TANG Guoxiang;BIAN Jiang(College of Pipeline and Civil Engineering,China University of Petroleum,Qingdao 266580,Shandong,China)

机构地区：[1]中国石油大学(华东)储运与建筑工程学院,山东青岛266580

出　　处：《高压物理学报》2021年第3期171-178,共8页Chinese Journal of High Pressure Physics

基　　金：国家自然科学基金(52074341,51274232)。

摘　　要：温室气体CO_(2)的捕捉和储存对减缓温室效应具有重大意义。CO_(2)水合物法储存CO_(2)具有效率高、储量大、易运输等优点。为了更高效制备CO_(2)水合物,对其生成机理进行实验和模拟研究。通过建立水合物生成的热力学模型,对水合物生成条件进行预测,利用高压静态釜式反应容器开展水合物生成实验,通过温度压力数据验证模型的准确性。在选取化学势能差作为水合物生成驱动力的基础上建立气体消耗速率模型,并与实验结果对比,结果表明:模型的预测值与实验值相对吻合。在低于水合物相平衡温度的条件下,升高容器的内反应压力可以促进气-液质量交换过程,提高生成效率。在生成过程中测得不同位置的电阻率变化数据,发现容器内的电阻率随固态水合物的生成而升高,并且首先在容器上部靠近壁面处结晶、团聚。The capturing and storage of green-house gas carbon dioxide are greatly significant to alleviation of green-house effect.The storage method producing carbon dioxide hydrate has advantages of high efficiency,large amount of storage,and easily transporting,etc.In order to provide suggestions for producing CO_(2) hydrate,experimental and modelling study of CO_(2) hydrate formation mechanism were initiated in this study.Hydrate formation thermodynamic model was established to give a prediction of temperature and pressure conditions for CO_(2) hydrate formation and made verification through the experimental data obtained by high-pressure constant reactor system.Hydrate formation kinetic model was built on the assumption that the chemical potential difference serves as the formation drive force.Compared with the experimental results,the model predicted results are agreed in tolerant discrepancy.Moreover,the pressure influence of reactor on CO_(2) hydrate formation rate was also analyzed.It is indicated that the escalation of pressure can stimulate the formation drive force under lower equilibrium temperature,prompting the gas-liquid mass transferring and production efficiency.Based on the change of electrical resistance ratio obtained from experimental record,CO_(2) hydrates firstly nucleate and agglomerate at top area of the reactor,additionally close to the wall.

关 键 词：CO_(2)水合物 高压反应容器 生成动力学 气体消耗速率 电阻率分布 

分 类 号：TE642[石油与天然气工程—油气加工工程] O521.9[理学—高压高温物理]