甲烷水合物的固体核磁共振碳谱与激光拉曼光谱研究

发布时间：2018-03-21 05:14

本文选题：固体~()C　切入点：NMR　出处：《波谱学杂志》2017年02期 　论文类型：期刊论文

【摘要】：甲烷水合物(CH_4·n H_2O)是主要由甲烷和水分子构成的冰状笼型化合物,在自然界储量巨大.固体核磁共振(NMR)波谱和激光拉曼光谱是在分子水平分析甲烷水合物的重要手段.该文利用低温固体核磁共振碳谱(~(13)C NMR)对合成的甲烷水合物结构进行了研究,分别使用~(13)C交叉极化(~(13)C CP)和高功率质子去偶(1H HPDEC)2种脉冲程序采集甲烷水合物的~(13)C NMR谱图,结合实验结果分析及理论推导可知,使用1H HPDEC方法得到的~(13)C NMR谱图信号更强,更利于定量分析;甲烷气体与冰粉合成的甲烷水合物为I型,其大笼和小笼占有率分别为0.988和0.824,水合数为6.07;甲烷气体与SH2站位沉积物和冰粉合成的甲烷水合物也为I型,其大笼和小笼占有率分别为0.987和0.887,水合数为5.98;SH2站位沉积物使合成的甲烷水合物的小笼占有率提高、水合数降低、水合物饱和度提高.激光拉曼光谱结果证实了上述结果的准确性.该文为甲烷水合物测试提供了重要的方法参考.
[Abstract]:Methane hydrate CH4 路n H _ 2O) is an ice-cage compound composed mainly of methane and water molecules. There are huge reserves in nature. Solid nuclear magnetic resonance spectroscopy and laser Raman spectroscopy are important means to analyze methane hydrate at molecular level. The structure of synthesized methane hydrates has been studied by using low temperature solid nuclear magnetic resonance carbon spectroscopy (NMRs). The 1H HPDEC)2 pulse program of high power proton decoupling was used to collect the C NMR spectra of methane hydrate. Combined with the analysis of the experimental results and the theoretical derivation, it can be seen that the 1H HPDEC method is more powerful than that obtained by using the 1H HPDEC method. The methane hydrates synthesized from methane gas and ice powder are of type I, with large cage and small cage occupancy of 0.988 and 0.824, respectively, and the hydration number is 6.07. The methane hydrate synthesized by methane gas with sediment and ice powder at SH2 station is also of type I. The ratio of large cage and small cage is 0.987 and 0.887 respectively, the hydration number is 5.98 / h _ 2, the small cage occupation of methane hydrate is increased, and the hydration number is decreased. The results of laser Raman spectroscopy confirm the accuracy of the above results. This paper provides an important method reference for methane hydrate measurement.
【作者单位】：中国科学院广州地球化学研究所;中国科学院天然气水合物重点实验室中国科学院广州能源研究所;中国科学院大学;国土资源部天然气水合物重点实验室青岛海洋地质研究所;青岛海洋科学与技术国家实验室海洋矿产资源评价与探测技术功能实验室;
【基金】：国家自然科学基金资助项目(41273022) 中国石油-中科院科技合作项目(2015A-4813) 中国科学院广州能源研究所所长创新基金培育专项(y307p51001)
【分类号】：TE642

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