不同水合物环境下恒压 CO2 置换 CH4：结构和形态,Energy & Fuels

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不同水合物环境下恒压 CO2 置换 CH4：结构和形态
Energy & Fuels ( IF 5.2 ) Pub Date : 2023-11-15 , DOI: 10.1021/acs.energyfuels.3c02991
Andrea Rossi ₁ , Michele Ciulla ₂ , Valentino Canale ₂ , Marco Zannotti ₁ , Marco Minicucci ₃ , Pietro Di Profio ₂ , Rita Giovannetti ₁

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气体水合物 (GH) 是由水分子组成的固体冰状化合物，形成容纳气体分子的晶格结构，在高压和低温下产生。水合物结构受到周围环境的影响，在此背景下，提出了在不同环境、超纯水、海水、合成砂、天然砂和十二烷基硫酸钠中制备的GH的结构表征。特别地，拉曼光谱已被用于研究水笼的结构变化、水合物结构中的气体吸收、CH ₄笼占有率、水合数以及恒压下二氧化碳置换的产率。为了进行比较，在上述五种不同的实验条件下制备CH ₄水合物、CO ₂水合物和CH ₄ /CO _{2水合物（通过实施的置换过程获得）并进行结构表征。}根据拉曼研究，纯CH ₄水合物在大笼中几乎完全占据(>95%)，并且在小笼占据中与不同测试介质相关的显着变化。_{CO 2} /CH ₄水合物的笼占有率计算表明，UP水中可以获得较高的置换率，并且CH ₄水合物在最能代表自然环境的天然砂和海水中表现出良好的效果。用CO ₂替代CH ₄。此外，通过扫描电子显微镜 (SEM) 对 GH 进行异位形态表征可以突出显示所研究样品之间的形态差异。

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Constant Pressure CO2 Replacement of CH4 in Different Hydrate Environments: Structure and Morphology

Gas hydrates (GHs) are solid, ice-like compounds composed of water molecules forming a lattice structure that hosts gas molecules, produced under high pressure and low temperature. The structure of the hydrate structure is affected by the surrounding environment, and in this context, a structural characterization of GHs prepared in different environments, ultrapure (UP) water, seawater, synthetic sand, natural sand, and sodium dodecyl sulfate, has been proposed. In particular, the Raman spectroscopy has been used to investigate the structural changes in the water cages, the gas uptake in the hydrate structure, the CH₄ cage occupancies, the hydration number, and the yield of carbon dioxide replacement at constant pressure. For this comparison, CH₄-hydrates, CO₂-hydrates, and CH₄/CO₂-hydrates (obtained from an implemented replacement process) were prepared in five different experimental conditions mentioned above and structurally characterized. From Raman investigation, pure CH₄-hydrates displayed almost full (>95%) occupation in the large cage and a significant change in the small cage occupation related to the different tested media. The cage occupancy calculation of CO₂/CH₄-hydrates showed that a higher yield of replacement can be obtained in UP water and that CH₄-hydrates in natural sand and in seawater, which are the most representing of natural environments, displayed a good replacement of CH₄ with CO₂. Additionally, the ex situ morphological characterization of the GHs by scanning electron microscopy (SEM) allowed the highlighting of morphological differences among the investigated samples.

更新日期：2023-11-15

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