甲烷水合物的固體核磁共振碳譜與激光拉曼光譜研究
發(fā)布時間:2018-03-21 05:14
本文選題:固體~()C 切入點:NMR 出處:《波譜學雜志》2017年02期 論文類型:期刊論文
【摘要】:甲烷水合物(CH_4·n H_2O)是主要由甲烷和水分子構成的冰狀籠型化合物,在自然界儲量巨大.固體核磁共振(NMR)波譜和激光拉曼光譜是在分子水平分析甲烷水合物的重要手段.該文利用低溫固體核磁共振碳譜(~(13)C NMR)對合成的甲烷水合物結(jié)構進行了研究,分別使用~(13)C交叉極化(~(13)C CP)和高功率質(zhì)子去偶(1H HPDEC)2種脈沖程序采集甲烷水合物的~(13)C NMR譜圖,結(jié)合實驗結(jié)果分析及理論推導可知,使用1H HPDEC方法得到的~(13)C NMR譜圖信號更強,更利于定量分析;甲烷氣體與冰粉合成的甲烷水合物為I型,其大籠和小籠占有率分別為0.988和0.824,水合數(shù)為6.07;甲烷氣體與SH2站位沉積物和冰粉合成的甲烷水合物也為I型,其大籠和小籠占有率分別為0.987和0.887,水合數(shù)為5.98;SH2站位沉積物使合成的甲烷水合物的小籠占有率提高、水合數(shù)降低、水合物飽和度提高.激光拉曼光譜結(jié)果證實了上述結(jié)果的準確性.該文為甲烷水合物測試提供了重要的方法參考.
[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.
【作者單位】: 中國科學院廣州地球化學研究所;中國科學院天然氣水合物重點實驗室中國科學院廣州能源研究所;中國科學院大學;國土資源部天然氣水合物重點實驗室青島海洋地質(zhì)研究所;青島海洋科學與技術國家實驗室海洋礦產(chǎn)資源評價與探測技術功能實驗室;
【基金】:國家自然科學基金資助項目(41273022) 中國石油-中科院科技合作項目(2015A-4813) 中國科學院廣州能源研究所所長創(chuàng)新基金培育專項(y307p51001)
【分類號】:TE642
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