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为探究瓦斯水合物相平衡条件及其分解热特征,利用瓦斯水合物相平衡实验装置结合图形法研究了CH_4—N_2—O_2瓦斯混合气在纯水体系及TBAB(四丁基溴化铵,0.2mol/L)添加剂体系的水合物相平衡条件,将纯水体系下瓦斯水合物相平衡压强实验值与Chen-Guo模型计算值进行对比,基于Clausius-Clapeyron方程计算了瓦斯水合物分解热.结果表明:瓦斯水合物相平衡条件随着CH_4浓度的升高变得更加温和,TBAB可显著改善瓦斯水合物相平衡条件,使水合物相-气相边界向高温低压区域转移;相同温度下,2种瓦斯混合气在纯水体系生成水合物的相平衡压强实验值均低于Chen-Guo模型计算值,相对误差分别为0.18,0.23;水合物分解热随着瓦斯中CH_4浓度的升高而增大,TBAB体系瓦斯水合物分解热远大于纯水体系.
In order to explore the gas hydrate phase equilibrium condition and its decomposition heat characteristics, the gas hydrate phase equilibrium experiment device and the graph method were used to study the effect of CH4-N2-O2 gas mixture on pure water system and TBAB (tetrabutylammonium bromide, 0.2 mol / L) additive system, the equilibrium pressure of gas hydrate phase in pure water system is compared with the calculated value of Chen-Guo model, and the heat of decomposition of methane hydrate is calculated based on the Clausius-Clapeyron equation. The results show that the phase equilibrium of gas hydrate becomes more moderate with the increase of CH 4 concentration. TBAB can significantly improve the gas hydrate phase equilibrium conditions and shift the hydrate phase to gas phase boundary to high temperature and low pressure region. Under the same temperature, The experimental values of gas phase equilibrium pressure of gas mixture generated in pure water system are lower than those calculated by Chen-Guo model, the relative errors are 0.18 and 0.23, respectively. The heat of decomposition of hydrates increases with the CH 4 concentration in gas , TBAB system gas hydrate decomposition heat far greater than pure water system.