Microscopic Experimental Study on the Crystallization of TBAB-CO2 Hydrate

doi:10.3964/j.issn.1000-0593(2019)09-2889-05

GIEC OpenIR

	Microscopic Experimental Study on the Crystallization of TBAB-CO2 Hydrate
	Chen Yu-feng 1; Zhou Xue-bing 2,3,4; Liang De-qing2,3,4 ; Wu Neng-you5
	2019-09-01
发表期刊	SPECTROSCOPY AND SPECTRAL ANALYSIS
ISSN	1000-0593
卷号	39 期号:9 页码:2889-2893
通讯作者	Liang De-qing(liangdq@ms.giec.ac.cn)
摘要	TBAB semi-clathrate hydrate has a huge potential for effective application of carbon dioxide (CO2) capture. Because of the complexity of the crystal structure, the kinetics of TBAB hydrate remains poorly understood. In this work, the spectral characteristics of nCO(2)center dot TBAB center dot 26H(2)O and nCO(2)center dot TBAB center dot 38H(2)O were analyzed by Raman and powder X-ray diffraction (PXRD). To understand the gas storage characteristics of TBAB hydrate, the processes of CO2 molecules entering 2 kinds of crystal structures were measured using in situ Raman spectroscopy. Results showed that the Raman spectra of 2 crystal structures had high similarity. The Raman peaks at 1 309.5 and 1 326.9 cm(-1) were assigned to be the C-C deformation vibration mode of TBA(+) cations in nCO(2)center dot TBAB center dot 26H(2)O hydrate. They did not shift in nCO(2)center dot TBAB center dot 38H(2)O hydrate, but became detached and narrow in half-peak width. Meanwhile, the peaks at 1 446.6 and 1 458 cm(-1) were assigned to be the C-H shear vibration mode of TBA(+) cations in nCO(2)center dot TBAB center dot 26H(2)O hydrate. They shifted away from each other and had lower less overlap region in nCO(2)center dot TBAB center dot 38H(2)O hydrate. Those features in Raman spectra were helpful to distinguish the 2 kinds of structures. The PXRD patterns of the 2 TBAB hydrates showed large difference from each other. nCO(2)center dot TBAB center dot 26H(2)O hydrate was tetragonal which had the space group of (P4/m), while nCO(2)center dot TBAB center dot 38H(2)O hydrate was orthorhombic which had the space group of (Pmma). In the PXRD patterns, the peaks at 2 theta=8.406 degrees and 10.941 degrees were (200) and (220) planes of nCO(2)center dot TBAB center dot 38H(2)O hydrate respectively. The structure of nCO(2)center dot TBAB center dot 26H(2)O hydrate was characterized by the (012) and (003) planes at 2 theta=5.976 degrees and 6.969 degrees respectively. During the in situ Raman measurements, nCO(2)center dot TBAB center dot 26H(2)O and nCO(2)center dot TBAB center dot 38H(2)O hydrates grew directly from the prepared TBAB center dot 26H(2)O and TBAB center dot 38H(2)O hydrates at 276 K, 2 MPa. The CO2 molecules were captured by the 5(12) hydrate cages in the 2 kinds of hydrates, formed the characteristic peaks of CO2 at 1 275.4 and 1 379.3 cm(-1) and increased continuously. The Raman peaks at 1 110.3 cm(-1) were chosen as reference peak to compare the CO2 concentration growth in the 2 kinds of hydrates. In the initial 75 minutes of in situ Raman measurements, the content of CO2 in hydrate phase grew linearly with generally the same growth rates in 2 kinds of crystals. As the measuring spots were on the hydrate surface where the gas diffusion resistance in hydrate phase could be neglected and the cage structures used for gas storage were all 5(12) cage, the similar gas storage rates were obtained. The microcosmic experimental study provides a theoretical basis for CO2 capture technology by forming TBAB semi-clathrate hydrate.
关键词	Natural gas hydrate Kinetics Carbon dioxide Raman X-ray diffraction
DOI	10.3964/j.issn.1000-0593(2019)09-2889-05
关键词[WOS]	TETRABUTYLAMMONIUM BROMIDE ; GAS
收录类别	SCI
语种	英语
WOS研究方向	Spectroscopy
WOS类目	Spectroscopy
WOS记录号	WOS:000487766700039
出版者	OFFICE SPECTROSCOPY & SPECTRAL ANALYSIS
引用统计	被引频次：3[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.giec.ac.cn/handle/344007/25659
专题	中国科学院广州能源研究所
通讯作者	Liang De-qing
作者单位	1.Wuzhou Univ, Dept Chem Engn & Resource Recycling, Wuzhou 543000, Peoples R China 2.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangzhou 510640, Guangdong, Peoples R China 3.Chinese Acad Sci, Guangzhou Ctr Gas Hydrate Res, Key Lab Gas Hydrate, Guangzhou 510640, Guangdong, Peoples R China 4.Guangdong Prov Key Lab New & Renewable Energy Res, Guangzhou 510640, Guangdong, Peoples R China 5.China Geol Survey, Key Lab Nat Gas Hydrate, Qingdao Inst Marine Geol, Minist Land & Resources, Qingdao 266071, Shandong, Peoples R China
推荐引用方式 GB/T 7714	Chen Yu-feng,Zhou Xue-bing,Liang De-qing,et al. Microscopic Experimental Study on the Crystallization of TBAB-CO2 Hydrate[J]. SPECTROSCOPY AND SPECTRAL ANALYSIS,2019,39(9):2889-2893.
APA	Chen Yu-feng,Zhou Xue-bing,Liang De-qing,&Wu Neng-you.(2019).Microscopic Experimental Study on the Crystallization of TBAB-CO2 Hydrate.SPECTROSCOPY AND SPECTRAL ANALYSIS,39(9),2889-2893.
MLA	Chen Yu-feng,et al."Microscopic Experimental Study on the Crystallization of TBAB-CO2 Hydrate".SPECTROSCOPY AND SPECTRAL ANALYSIS 39.9(2019):2889-2893.