The phase equilibrium conditions of gas hydrate systems play a fundamental and essential role in establishing the feasibility of the various hydrate based technological applications. Although the classical isochoric and isothermal pressure search methods can provide accurate and reliable gas hydrate phase equilibrium data, these methods require researchers to devote tremendous time towards achieving each data point. Herein, we extend the phase boundary (PB) method for bulk hydrate systems and demonstrate it to be robust and highly efficient. The PB method involves a controlled pressure drop of the hydrate system to initiate the automatic trace of the pressure and temperature region upon dissociation of the hydrates. Three-phase equilibrium data for four different gas hydrate systems, namely pure methane (CH₄), mixed CH₄/1,3-dioxolane (DIOX), mixed hydrogen (H₂)/DIOX, and mixed carbon dioxide (CO₂)/DIOX, have been obtained using the PB method. Independent measurements made using the isochoric pressure search method have been obtained to validate the accuracy and reliability of the data obtained using the PB method.

天然气水合物系统的相平衡条件在建立各种基于水合物的技术应用的可行性中起着基本和至关重要的作用。尽管经典的等压和等温压力搜索方法可以提供准确而可靠的天然气水合物相平衡数据，但是这些方法需要研究人员花费大量时间来实现每个数据点。在本文中，我们扩展了相量边界（PB）方法用于大量水合物系统，并证明了它的鲁棒性和高效性。PB方法涉及水合物系统的受控压降，以在水合物解离时启动压力和温度区域的自动跟踪。四种不同的天然气水合物系统的三相平衡数据，即纯甲烷（CH ₄），已使用PB方法获得了混合的CH ₄ / 1,3-二氧戊环（DIOX），混合的氢（H ₂）/ DIOX和混合的二氧化碳（CO ₂）/ DIOX。已获得使用等容压力搜索方法进行的独立测量，以验证使用PB方法获得的数据的准确性和可靠性。