基于气体水合物法的分离技术可用于天然气储运、二氧化碳封存和海水淡化 等多个领域，但工业应用的瓶颈在于水合物成核诱导时间长且生长速率缓慢，原因 在于气-液传质效率低以及反应产生的热量无法及时移除。本文以环糊精及其衍生 物作为环境友好型化学促进剂，采用多孔碳化硅泡沫陶瓷(SFC)填料对甲烷水合 物形成过程中的传质与传热进行强化，通过优化反应体系中的多种影响因素来达 到促进水合物生长的目的。首先，采用四种环糊精及其衍生物开展甲烷水合物生长动力学实验，研究环糊 精的结构与浓度对甲烷水合物成核与生长的影响。结果表明，当四种环糊精单独使 用时，均抑制甲烷水合物生成的气体消耗量，但能够在一定条件下缩短诱导时间并 加快反应速率。当环糊精与十二烷基硫酸钠(SDS)联用时，a-环糊精和 b-环糊精 能够显著促进甲烷水合物生长并降低大约 66.7%的 SDS 用量，但 2-羟丙基-b-环 糊与甲基-b-环糊精仍表现出抑制作用。a-环糊精或 b-环糊精与 SDS 联用对甲烷 水合物的促进作用归因于环糊精-SDS 复合物之间形成的亲水通道有利于气液传质。其次，采用 SFC 填料强化甲烷水合物生长，计算反应体系内甲烷水合物形成 过程中的热阻变化，建立传热模型来预测填料质量、孔隙率、导热系数及摆放方式 对反应体系整体及局部热阻的影响规律，并对传热模型进行验证。结果表明，SFC 填料的加入能够显著改善反应体系传热性能，通过优化填料的摆放方式能够进一 步提高体系传热性能。最后，采用前文得到的化学促进剂配方(a-环糊精与 SDS 混合液)，研究 SFC 填料的分层间距以及填料与气-液界面的相对位置变化对甲烷水合物生长动力学的 影响。结果表明，SFC 填料露出液面或完全放置于气相中时，能够在静态条件下有 效提高甲烷水合物形成的气体消耗量、增加反应速率并显著缩短成核诱导时间。其 中，填料完全放置在气相中时对水合物形成的促进效果最为显著，主要归因于两种 驱动力(气相中多孔填料对水分子的毛细力以及水合物簇对水分子的吸附力)促使 填料孔隙内形成有利于水合物成核的低水饱和度区域。

Hydrate-based separation technology has a wide range of applications such as natural gas storage, CO2 capture and water desalination. The bottleneck of the commercialization of gas hydrate technology is the long induction time of nucleation and slow growth kinetics, which is attributed to the hindered gas-water mass transfer and the difficulty to remove hydration heat. In this paper, cyclodextrins and their derivatives were used as environmentally friendly non-toxic substances to promote the formation of methane hydrate. The mass transfer and heat transfer during the methane hydrate growth process in the reactor were improved by using silicon carbide foam ceramic (SFC) packing. The impact factors in the reaction system were optimized to enhance gas hydrate formation.Firstly, four cyclodextrins and their derivatives were used to study the effect of structure and concentration of cyclodextrins on methane hydrate formation. The results showed that the four cyclodextrins decreased the gas consumption during methane hydrate formation when they were used alone, but they could shorten the induction time and accelerate the formation rate under some conditions. When cyclodextrins were used in combination with Sodium dodecyl sulfate (SDS), a-cyclodextrin (aCD) and b- cyclodextrin (bCD) could significantly promote methane hydrate formation and reduce the amount of SDS usage by about 66.7%. But hydroxypropyl-bCD (HPCD) and methyl- bCD (MCD) still exhibited inhibitory effects. The promotion effect on the growth of methane hydrate was closely related to the hydrophilic channel formed by neighbouring cyclodextrin-SDS complex through hydrogen bonds which facilitated mass transfer.Secondly, SFC packings were used to enhance methane hydrate formation. Thermal resistance during methane hydrate growth process were calculated in the silicon carbide foam ceramic packing reactor. A heat transfer model was established and used to predict the effect of packing’s quantity, porosity, thermal conductivity, and stacking pattern on the overall and local thermal resistance. The thermal resistance calculated by the heat transfer model was verified according to the experimental results. Results showed that the addition of SFC packings significantly improved the heat transfer performance of the hydrate formation system. The results also emphasized that the heat transfer could be further improved by optimizing the stacking pattern of SFC packings.Finally, the mixture of aCD and SDS was used as the chemical solution, and the SFC packings were placed at different locations in the reactor to study the effect of the distance between two SFC packings and the relative position of SFC packing and gas- water interface on the growth of methane hydrate. Results showed that when the SFC packings were located above the liquid surface or completely exposed in the gas phase, it could effectively increase the gas consumption, accelerate the formation rate and shorten the induction time of methane hydrate under static conditions. The promotion effect was most significant when the packings were located at the gas phase near the water-gas interface. This was attributed to the synergistic effects between the capillary wicking driven by the porous packings and the water suction driven by the initial hydrate clusters, which made the gas phase pores unsaturated environment falicitating methane hydrate formation.