Prediction of solid-liquid equilibrium of binary mixtures containing methane

doi:10.11949/0438-1157.20201905

Abstract

Abstract:

Superconducting energy pipeline is a forward-looking energy transmission technology that cools superconducting cables with liquefied natural gas (LNG) and realizes the simultaneous transmission of two energy sources. The economic operating temperature of superconducting energy pipelines is generally 77—100 K, and LNG has a risk of solidification in this temperature range, so it is necessary to study the solid-liquid equilibrium characteristics of the main components of LNG. This article focuses on five binary mixtures of methane+ethylene, methane+ethane, methane+propane, methane+n-butane, and methane+n-pentane, using the equation of state represented by the Peng–Robinson (PR) equation of state with the simple van der Waals (vdW) mixing rule. The activity coefficient method represented by models such as NRTL (non-random two liquids), WILSON and UNIQUAC (universal quasi–chemical). Based on the binary data of vapor-liquid equilibrium for the studied system and the regressed binary interaction parameters, the solid-liquid equilibrium of five binary mixtures was predicted, and the results were compared with the literature data. The results show that the PR-vdW equation has the best prediction results for the solid-liquid equilibrium of the five binary mixtures containing methane. Furthermore, the effects of the binary interaction parameters in the PR-vdW equation on the calculation results of the vapor or solid-liquid equilibria of the five binary mixtures were studied, and the dependence of the model on temperature was analyzed.

Key words: superconducting energy pipeline, natural gas, vapor-liquid equilibrium, solid-liquid equilibrium, Peng-Robinson equation

摘要：

超导能源管道是以液化天然气（LNG）冷却超导电缆，实现两种能源同时输送的前瞻性能源输送技术。超导能源管道的经济运行温度一般在77~100 K，而在此温区LNG有凝固风险，因此必须研究LNG主要成分的固液相平衡特性。为此，针对甲烷+乙烯、甲烷+乙烷、甲烷+丙烷、甲烷+正丁烷、甲烷+正戊烷5种二元混合物，借助以PR-vdW为代表的状态方程法，以NRTL、WILSON、UNIQUAC等模型为代表的活度系数法，基于所研究体系的二元汽液相平衡数据，回归二元相互作用参数，预测其二元固液相平衡，预测结果与文献数据进行了比较。结果表明，PR-vdW方程对5种甲烷二元体系的固液平衡预测结果最好。进而研究了PR-vdW方程中二元相互作用参数对甲烷二元体系汽液平衡及固液平衡计算结果的影响，分析了模型对温度的依赖关系。

关键词: 超导能源管道, 天然气, 汽液相平衡, 固液相平衡, Peng-Robinson方程

CLC Number:

TK 123

Xian WANG, Yanxing ZHAO, Xueqiang DONG, Xiaogang CHEN, Maoqiong GONG. Prediction of solid-liquid equilibrium of binary mixtures containing methane[J]. CIESC Journal, 2021, 72(8): 4009-4018.

王宪, 赵延兴, 董学强, 陈晓刚, 公茂琼. 甲烷二元体系的固液相平衡预测[J]. 化工学报, 2021, 72(8): 4009-4018.

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