Propane hydrate nucleation: Experimental investigation and correlation

被引:60
作者
Jensen, Lars [1 ]
Thomsen, Kaj [1 ]
von Solms, Nicolas [1 ]
机构
[1] Tech Univ Denmark, Dept Chem & Biochem Engn, Ctr Phase Equilibria & Separat Processes IVC SEP, DK-2800 Lyngby, Denmark
关键词
aqueous solutions; interfacial energy; nucleation; crystallization; gas hydrate; polymers;
D O I
10.1016/j.ces.2008.03.006
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
In this work the nucleation kinetics of propane gas hydrate has been investigated experimentally using a stirred batch reactor. The experiments have been performed isothermally recording the pressure as a function of time. Experiments were conducted at different stirring rates, but in the same supersaturation region. The experiments showed that the gas dissolution rate rather than the induction time of propane hydrate is influenced by a change in agitation. This was especially valid at high stirring rates when the water surface was severely disturbed. Addition of polyvinylpyrrolidone (PVP) to the aqueous phase was found to reduce the gas dissolution rate slightly. However the induction times were prolonged quite substantially upon addition of PVP. The induction time data were correlated using a newly developed induction time model based on crystallization theory also capable of taking into account the presence of additives. In most cases reasonable agreement between the data and the model could be obtained. The results revealed that especially the effective surface energy between propane hydrate and water is likely to change when the stirring rate varies from very high to low. The prolongation of induction times according to the model is likely to be due to a change in the nuclei-substrate contact angle. (C) 2008 Elsevier Ltd. All rights reserved.
引用
收藏
页码:3069 / 3080
页数:12
相关论文
共 29 条
[11]   Induction time in crystallization of gas hydrates [J].
Kashchiev, D ;
Firoozabadi, A .
JOURNAL OF CRYSTAL GROWTH, 2003, 250 (3-4) :499-515
[12]   Nucleation of gas hydrates [J].
Kashchiev, D ;
Firoozabadi, A .
JOURNAL OF CRYSTAL GROWTH, 2002, 243 (3-4) :476-489
[13]  
KELLAND MA, 1995, 30402 SPE, P531
[14]   Effective kinetic inhibitors for natural gas hydrates [J].
Lederhos, JP ;
Long, JP ;
Sum, A ;
Christiansen, RL ;
Sloan, ED .
CHEMICAL ENGINEERING SCIENCE, 1996, 51 (08) :1221-1229
[15]  
MUNCK J, 1988, CHEM ENG SCI, V43, P2662
[16]   INDUCTION PHENOMENA IN GAS HYDRATE NUCLEATION [J].
NATARAJAN, V ;
BISHNOI, PR ;
KALOGERAKIS, N .
CHEMICAL ENGINEERING SCIENCE, 1994, 49 (13) :2075-2087
[17]   MEASUREMENT AND PREDICTION OF HYDRATE FORMATION IN LIQUID HYDROCARBON-WATER SYSTEMS [J].
NG, HJ ;
ROBINSON, DB .
INDUSTRIAL & ENGINEERING CHEMISTRY FUNDAMENTALS, 1976, 15 (04) :293-298
[18]   DISSOCIATION PRESSURES OF GAS HYDRATES FORMED BY GAS-MIXTURES [J].
PARRISH, WR ;
PRAUSNITZ, JM .
INDUSTRIAL & ENGINEERING CHEMISTRY PROCESS DESIGN AND DEVELOPMENT, 1972, 11 (01) :26-+
[19]   DYNAMIC SURFACE-TENSION AND CLASSICAL NUCLEATION THEORY [J].
RASMUSSEN, DH .
JOURNAL OF CHEMICAL PHYSICS, 1986, 85 (04) :2272-2276
[20]   MEASUREMENT OF INDUCTION TIMES FOR THE FORMATION OF METHANE AND ETHANE GAS HYDRATES [J].
SKOVBORG, P ;
NG, HJ ;
RASMUSSEN, P ;
MOHN, U .
CHEMICAL ENGINEERING SCIENCE, 1993, 48 (03) :445-453