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In situ Raman spectroscopic investigation of flux-controlled crystal growth under high pressure: A case study of carbon dioxide hydrate growth in aqueous solution
Ou, Wenjia1; Lu, Wanjun1,2; Qu, Kang2; Geng, Lantao1; Chou, I-Ming3; Wanjun Lu
2016-10-01
Source PublicationINTERNATIONAL JOURNAL OF HEAT AND MASS TRANSFER
Volume101Issue:834Pages:834-843
AbstractWe developed a high-pressure in-situ non-invasive technique to measure the solute concentration distribution in the solution around a growing crystal, in order to study the effect of increasing flux to the crystal surface on the growth process. Growth rates of carbon dioxide hydrate in pure water in a capillary high-pressure optical cell were determined at 20 and 40 MPa and 275.15, 278.15, 280.15, and 283.15 K. During the growth of the hydrate, CO2 was supplied through diffusion in the aqueous phase from the liquid CO2-aqueous solution interface, and the dissolved CO2 concentrations along the diffusion path were monitored by Raman spectroscopy. We demonstrated that the hydrate growth rates could change a lot under constant driving force, such as under the same degrees of super-saturation, supercooling or over-pressurization of the system, and that the growth rates depend on the mass transfer flux to the surface of the hydrate crystal; with the increasing flux to the crystal surface, the rate-dominant process changes from "diffusion controlled" to "interfacial reaction controlled" after the diffusion flux reaches a critical (maximum) value. The interfacial reaction coefficient k(r) is estimated to be 1.31 x 10(-6) m/s at 20 MPa and 280.15 K, and the molar volume and hydration number of CO2 hydrate vary from 21.7 to 22.0 cm(3)/mol and 7.09 to 7.67, respectively. These observations and measurements could be useful for the design of crystal growth. (C) 2016 Elsevier Ltd. All rights reserved.
SubtypeArticle
KeywordCarbon Dioxide Hydrate Kinetics Concentration Gradient Mass Transfer Raman Spectroscopy
WOS HeadingsScience & Technology ; Physical Sciences ; Technology
DOI10.1016/j.ijheatmasstransfer.2016.05.082
Indexed BySCI
Language英语
WOS KeywordCO2 HYDRATE ; METHANE HYDRATE ; KINETICS ; WATER ; DISSOCIATION ; SOLUBILITY ; PHASE ; MPA ; EQUILIBRIUM ; PREDICTION
WOS SubjectThermodynamics ; Engineering, Mechanical ; Mechanics
WOS IDWOS:000380417300083
Citation statistics
Cited Times:7[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Version预印本
Identifierhttp://ir.idsse.ac.cn/handle/183446/1610
Collection深海科学研究部_深海极端环境模拟研究实验室
Corresponding AuthorWanjun Lu
Affiliation1.China Univ Geosci, Fac Earth Resources, Minist Educ, Key Lab Tecton & Petr Resources, Wuhan 430074, Peoples R China
2.China Univ Geosci, State Key Lab Geol Proc & Mineral Resources, Wuhan 430074, Peoples R China
3.Chinese Acad Sci, Sanya Inst Deep Sea Sci & Engn, Sanya 572000, Hainan, Peoples R China
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GB/T 7714
Ou, Wenjia,Lu, Wanjun,Qu, Kang,et al. In situ Raman spectroscopic investigation of flux-controlled crystal growth under high pressure: A case study of carbon dioxide hydrate growth in aqueous solution[J]. INTERNATIONAL JOURNAL OF HEAT AND MASS TRANSFER,2016,101(834):834-843.
APA Ou, Wenjia,Lu, Wanjun,Qu, Kang,Geng, Lantao,Chou, I-Ming,&Wanjun Lu.(2016).In situ Raman spectroscopic investigation of flux-controlled crystal growth under high pressure: A case study of carbon dioxide hydrate growth in aqueous solution.INTERNATIONAL JOURNAL OF HEAT AND MASS TRANSFER,101(834),834-843.
MLA Ou, Wenjia,et al."In situ Raman spectroscopic investigation of flux-controlled crystal growth under high pressure: A case study of carbon dioxide hydrate growth in aqueous solution".INTERNATIONAL JOURNAL OF HEAT AND MASS TRANSFER 101.834(2016):834-843.
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