Ni-Mn基相变型纳米流体对瓦斯水合分离动力学影响实验研究

The heat production of hydrate has the inhibitory effect on the process of gas hydration separation. With the thermal storage effect of martensitic transformation alloy, it is proposed that the process of gas hydration separation is strengthened by the Ni-Mn-based phase transition nanofluids, to explore the effect of the factors such as phase transition medium particle properties on gas hydration separation kinetics process. Therefore, the phase transition condition and experimental scheme are determined firstly based on Chen-Guo model, to prepare Ni-Mn-based phase transition nanofluids with the appropriate martensitic transformation temperature and phase transition latent heat. Secondly, the kinetics parameters of hydration separation are measured by gas hydration separation experimental system in different nanofluids. According to the Clapeyron equation, the hydrate formation heat is calculated. Combining the PR equation, the gas storage capacity of hydrate and separation rate is calculated. And then, the interactional relationship is determined between the induction time, gas storage capacity, separation rate, separation concentration, formation heat of the hydration separation and the factor of nano particle composition, particle size, concentration and phase transition latent heat. Finally, with the heat and mass balance equations, the kinetics model of gas hydration separation is developed, which the hydrate formation heat associated with the separation rate. And the mechanism of action that the phase transition nanofluids influence different gas composite hydration separation kinetics process is explored. This study has significant scientific implications and engineering value in promoting gas separation techniques based on hydrate.

水合物生成热对瓦斯水合分离进程具有抑制作用，利用马氏体相变合金的蓄热作用，提出由Ni-Mn基相变型纳米流体强化瓦斯水合分离进程，探索相变型介质特性变化对瓦斯水合分离动力学影响。为此，首先，基于Chen-Guo模型确定相变条件与瓦斯水合分离实验方案，制备具有适当马氏体相变温度和相变潜热的Ni-Mn基相变型纳米流体；其次，利用瓦斯水合分离实验系统测定不同相变型纳米流体中水合分离动力学参数，根据Clapeyron方程计算水合物生成热，结合PR方程计算水合物储气量与分离速率；进而，确定水合分离过程诱导时间、储气量、分离速率、分离产物浓度及生成热与纳米颗粒成分、粒径、浓度、相变潜热等因素相互影响关系；最后，依据热量与质量衡算方程，建立水合物生成热与分离速率相关联的瓦斯水合分离动力学模型，探寻Ni-Mn基相变型纳米流体对瓦斯水合分离动力学影响机理。该研究对推动瓦斯水合分离技术发展具有重要科学意义。

水合物生成多项界面与生成热对瓦斯水合分离进程具有抑制作用，利用相变型微纳米流体的高传质传热与相变蓄热特性，提出由Ni-Mn基相变型微纳米流体强化瓦斯水合分离进程，探索相变型介质特性变化对瓦斯水合分离动力学影响。依据多元瓦斯水合物相平衡理论模型获得相同温度下4种瓦斯气样水合分离相平衡条件，确定Ni-Mn基相变型纳米颗粒的成分含量，制备三种纳米合金及不同颗粒粒径，并制备出4种浓度纳米流体。同时，采用差示扫描量热法测定不同微纳米颗粒的相变潜热，利用扫描电镜进行表征，利用激光粒度分析仪测定颗粒粒度分布。在相同温度不同驱动力条件下，分别利用动态旋转磁场瓦斯水合过程实验装置与可视化静态瓦斯水合过程实验装置两套动静态实验系统，在不同Ni-Mn基相变型微纳米流体中开展了多轮次瓦斯水合分离动力学实验，获取了微纳米流体中瓦斯水合反应过程温度压力变化特征及水合物相分离产物浓度。依据PR方程计算水合物储气量与分离速率，根据Clapeyron方程计算水合物生成热，阐明了不同气体组分、颗粒浓度、驱动力、流体组成及动静态体系等因素对水合物诱导时间、储气量、分离速率、分离产物浓度及水合物生成热的影响规律。同时，基于上述不同影响因素及动静态复杂体系，对强化瓦斯水合分离动力学进程最佳工艺参数进行了优选，发现动态磁场结合氨基酸促进剂体系强化工艺效果最佳。结合热量与质量衡算方程，并依据微纳米颗粒等相关参数与储气量、分离速率、水合物生成热间相互关系，建立了Ni-Mn基相变型微纳米流体中瓦斯水合分离动力学模型，阐明了Ni-Mn基相变型微纳米流体对瓦斯水合分离动力学影响机理。该研究对推动瓦斯水合分离技术发展具有重要科学意义。