氧化石墨烯作为新型促进剂加速CO_2水合物生成实验  

Experiment on a new accelerant—graphene oxide for accelerating the formation of CO_2 hydrate

作　　者：代文杰[1,2] 王树立[1,2] 饶永超[1,2] 吕晓方[1,2] 刘波[3] 郑亚星 

机构地区：[1]常州大学石油工程学院 [2]江苏省油气储运技术重点实验室 [3]中国石化销售有限公司江苏常州石油分公司

出　　处：《天然气工业》2016年第11期83-88,共6页Natural Gas Industry

基　　金：国家自然科学基金项目"基于螺旋流的天然气管道水合物堵塞风险边界拓展机制研究"(编号:51574045)

摘　　要：为了解决气体水合物生成速率慢、储气密度低、生成条件苛刻等难题，利用高压反应釜生成实验装置，探究了添加质量浓度为0．2g／L的氧化石墨烯对CO2水合物生成的诱导时间、气体消耗量及CO2水合物相平衡压力的影响，揭示了温度和压力的变化规律，与去离子水中CO2水合物生成实验进行了比较并分析了其促进机理。结果表明：①氧化石墨烯具有动力学促进和热力学促进的双重作用，能够加快CO2水合物体系的传热传质效率，促进气体溶解，提高成核速率和气体消耗量，降低相平衡压力；②与去离子水相比，氧化石墨烯体系下CO2水合物生成诱导时间缩短了74％～85％；③温度为6℃时，随着初始压力的不同氧化石墨烯均能提高气体消耗量，在4MPa时气体消耗量增长幅度最大，达17．2％，提高了水合物储气密度；④氧化石墨烯降低CO2水合物相平衡压力的最大降幅为20％。结论认为，该新型促进剂能够提高CO2水合物的生成速率和储气密度。Gas hydrate is faced with the problems of low formation rate, low gas storage density and harsh formation conditions. In view of these problems, the effects of graphene oxide （mass concentration of 0.2 g/L） on the induction time, gas consumption and phase equilibrium pressure for the formation of CO2 hydrate were investigated by using the high-pressure reactor, and the changing laws of temperature and pressure were revealed. Furthermore, it was compared with the formation experiment of CO2 hydrate in deionized water and its accelerating mechanism was analyzed. It is shown that graphene oxide plays a dual role of kinetics and thermodynamics in the formation of CO2 hydrate. It can accelerate the heat and mass transfer efficiency of CO2 hydrate system, promote the gas dissolution, increase the nucleation rate and gas consumption, and decrease the phase equilibrium pressure; that the induction time for the formation of CO2 hydrate in graphene oxide system is 74-85% shorter than that in deionized water; that when graphene oxide is under 6℃, it can increase the gas consumption and hydrate gas storage density even the initial pressure is different. When the initial pressure is 4 MPa, the increasing range of gas consumption is the highest, up to 17.2%; and when graphene oxide is added, the phase equilibrium pressure of CO2 hydrate can be decreased by 20% to the utmost. In conclusion, this new accelerant can enhance the generation rate of CO2 hydrate and its gas storage density.

关 键 词：水合物技术应用 CO2水合物 氧化石墨烯 新型促进剂 传热效率 诱导时间 气体消耗量 相平衡压力 

分 类 号：TQ127.11[化学工程—无机化工] TE89[石油与天然气工程—油气储运工程]