Kumar Asheesh, Kumar Rajnish, Linga Praveen
Department of Chemical and Biomolecular Engineering, National University of Singapore, Singapore 117 585, Singapore.
Department of Chemical Engineering, Indian Institute of Technology Madras, Chennai, India.
iScience. 2019 Apr 26;14:136-146. doi: 10.1016/j.isci.2019.03.020. Epub 2019 Mar 25.
Methane storage in mixed hydrates is advantageous due to faster kinetics and added stability. However, capacity needs to be improved. Here we study mixed hydrates of methane (CH) and tetrahydrofuran (THF), in the presence of sodium dodecyl sulfate (SDS) as a kinetic promoter for hydrate formation. We report the co-existence of pure methane (sI) and mixed CH-THF hydrates (sII) in the presence of SDS; however, in the absence of SDS, co-existence of pure THF (sII) and mixed CH-THF hydrates (sII) was observed. Thus the presence of SDS preferentially promotes the enclathration of methane over that of THF. Furthermore, through in situ Raman spectrometry, complemented by high-pressure differential scanning calorimeter, we present temperature-dependent methane occupancy in small and large cages of sI and sII hydrates. Our findings offer new insights for enhancing the methane storage capacity in more stable sII hydrate configuration for large-scale methane storage via solidified natural gas technology.
由于动力学更快且稳定性增强,甲烷在混合水合物中的储存具有优势。然而,其储存容量仍有待提高。在此,我们研究了甲烷(CH)与四氢呋喃(THF)的混合水合物,其中十二烷基硫酸钠(SDS)作为水合物形成的动力学促进剂。我们报告了在SDS存在下纯甲烷(sI)和CH-THF混合水合物(sII)的共存情况;然而,在没有SDS的情况下,观察到了纯THF(sII)和CH-THF混合水合物(sII)的共存。因此,SDS的存在优先促进了甲烷而非THF的笼形包合。此外,通过原位拉曼光谱法,并辅以高压差示扫描量热法,我们呈现了sI和sII水合物的小笼和大笼中随温度变化的甲烷占有率。我们的研究结果为通过固化天然气技术在更稳定的sII水合物构型中提高大规模甲烷储存的甲烷储存容量提供了新的见解。