中文摘要：

利用恒压预冷法研究了不同反应物量（30．0，100．0g）、不同压力（2．50，3．50，4．50MPa）、温度为6℃时无搅拌甲烷-叔丁胺-水体系中水合物的生成过程．实验结果表明，水合物在此体系中的生成形态为浆状；CH4水合反应速率随压力升高而增大；当初始反应物量较少（30．0g）时，甲烷储气量（标准状态下水合物中甲烷与初始反应物的体积比）随压力升高而增大不明显（3．50MPa时为3．0mL／mL，4．50MPa时为3．1mL／mL），当初始反应物量较多（100．0g）时，甲烷储气量随压力升高反而降低（由2．50MPa时的5．4mL／mL变为4．50MPa时的0．9mL／mL）；反应过程中可能同时生成了纯叔丁胺结构的Ⅵ型和甲烷／叔丁胺结构的Ⅱ型两种水合物，且Ⅵ型与Ⅱ型量比在反应后期比前期大；甲烷与浓度为9．3％（mol）的叔丁胺溶液生成的水合物中甲烷储气量较低（最高5．4mL／mL）．通过分析甲烷-叔丁胺-水体系中水合物的生成过程，认为其可能包括反应分子接触聚集、水合物骨架形成和水合物晶体增长等3个步骤．

英文摘要：

The formation of hydrate in a methane-tBuNH2 （tert-butylamine）-water system without stirring was studied at 6 ℃ at different pressures （2.50, 3.50 and 4.50 MPa） and at different initialization reaction quantities （30.0 and 100.0 g）. The results showed that the hydrate in this system was pasty, and the reaction rate with CH4 increased when the reaction pressure increased. There is no clear relationship between the reaction pressure and the final CH4 storage capacity （the ratio of volume of CH4 in hydrate to that of initialization reactant at standard condition, mL/mL） while 30.0 g sample was loaded in the reactor, and the final CH4 storage capacity decreased when the reaction pressure increased while 100.0 g sample was loaded in the reactor （5.4 mL/mL at 2.50 MPa, 0.9 mL/mL at 4.50 MPa）. Two hydrate structures, Structure Ⅵ and Structure Ⅱ, may form simultaneously in the reaction, and the ratio of the amount of tBuNH2 Structure Ⅵ hydrate to that of CH4/tBuNH2 Structure Ⅱ hydrate may increase in the end of the reaction time, and the methane-tBuNH2-water system at xtBuNH2=9.3% is not suitable to store the CH4 by formation of the hydrate as the maximal CH4 storage capacity is only 5.4 mL/mL. It is considered that hydrate formation mechanism may undergo three steps： contacting and gathering of reactants molecules, forming of hydrate framework, and growing of hydrate.