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Chinese Journal of Chemical Engineering 1997年第3期5卷 12-19页

作者：郑大庆郭天民 high pressure fluid phase behavior & property research laboratory University of Petroleum

The three-parameter Petal-Teja equation of state coupled with a characterization proceduref0r C7+-fraction based on gamma distribution function was employed to predict the phase behaviorof eight gas *** lumping of the subdivided single carbon number（SCN）hydrocarbons inthe plus-fraction and the choice of empirical correlations for calculating the critical properties andacentric factor of SCN hydrocarbons were discussed.

关键词： gas condensates phase behavior equation of state prediction characterization of plus-fraction

R12 hydrate formation kinetics based on laser light scattering technique

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Science China Chemistry 2003年第5期46卷 487-494页

作者：孙长宇陈光进郭天民 high pressure fluid phase behavior & property research laboratory University of Petroleum Beijing 102249 China

A circulating flow system consisting of a transparent U-bend flow loop, a mixing tank and a laser granulometer was set up for studying the kinetics hydrate formation and the pressure is up to 4 MPa. Refrigerant CCl2F2 (R12) hydrate formation experiments were performed using laser light scattering method at 277.1 K and pressures of 0.24 and 0.32 MPa. The liquid flow rates were in the range of 300—1400 L/h. The size distribution and density of R12 hydrate particles in pure water were measured using a laser granulometer. Experimental results show that the size of hydrate particles increases sharply at the initial stage and approaches gradually to a stable size. The hydrate particle concentration in the aqueous phase increases with pressure and circulating liquid flow rate. Based on the material balance, the mathematical model among gas consumption, average hydrate particle size and shading ratio has been established. The calculated results using the mathematical model accord well with the experimental gas consumption data.

关键词： hydrate, kinetics, flow loop, laser light scattering, R12, model.

Study on the recovery of hydrogen from refinery (hydrogen+methane) gas mixtures using hydrate technology

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Science China Chemistry 2008年第2期51卷 171-178页

作者： WANG XiuLin CHEN GuangJin YANG LanYing ZHANG LinWei high pressure fluid phase behavior&property research laboratory University of PetroleumBeijing 102200China

A novel technique for separating hydrogen from (H2 + CH4) gas mixtures through hydrate formation/dissociation was proposed. In this work, a systematic experimental study was performed on the separation of hydrogen from (H2 + CH4) feed mixtures with various hydrogen contents (mole fraction x = 40%–90%). The experimental results showed that the hydrogen content could be enriched to as high as ～94% for various feed mixtures using the proposed hydrate technology under a temperature slightly above 0°C and a pressure below 5.0 MPa. With the addition of a small amount of suitable additives, the rate of hydrate formation could be increased significantly. Anti-agglomeration was used to disperse hydrate particles into the condensate phase. Instead of preventing hydrate growth (as in the kinetic inhibitor tests), hydrates were allowed to form, but only as small dispersed particles. Anti-agglomeration could keep hydrate particles suspended in a range of condensate types at 1°C and 5 MPa in the water-in-oil emulsion.

关键词： hydrate recovery refinery gas

Vapor-hydrate phases equilibrium of (CH_4+C_2H_6) and (CH_4+C_2H_4) systems

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Petroleum Science 2008年第4期5卷 359-366页

作者： Ma Qinglan Chen Guangjin Zhang Lingwei high pressure fluid phase behavior ＆ property research laboratory China University of Petroleum Beijing 102249 China

Separation of the （C1 ＋ C2） hydrocarbon system is of importance in natural gas processing and ethylene production. However it is the bottleneck because of its high refrigeration energy consumption, and needs to be urgently addressed. The technology of separating gas mixtures by forming hydrate could be used to separate （C1 ＋ C2） gas mixtures at around 0℃ and has attracted increasing attention worldwide. In this paper, investigation of vapor-hydrate two-phase equilibrium was carried out for （C1 ＋ C2） systems with and without tetrahydrofuran （THF）. The compositions of vapor and hydrate phases under phase equilibrium were studied with model algorithm when structure Ⅰ and structure Ⅱ hydrates coexisted for the （methane ＋ ethane） system. The average deviation between the modeled and actual mole fractions of ethane in hydrate and vapor phases was 0.55%, and that of ethylene was 5.7% when THF was not added. The average deviation of the mole fraction of ethane in vapor phase was 11.46% and ethylene was 7.38% when THF was added. The test results showed that the proposed algorithm is practicable.

关键词： Chen-Guo model vapor-hydrate equilibrium gas separation

Viscosities of ternary systems Y(NO_3)_3+La(NO_3)_3+H_2O,La(NO_3)_3+Ce(NO_3)_3+H_2O,La(NO_3)_3+Nd(NO_3)_3+H_2O and their binary subsystems at different temperatures

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Journal of Rare Earths 2012年第3期30卷 250-255页

作者：彭效明胡玉峰金传伟王智鑫苗超李哲宇 State Key laboratory of Heavy Oil Processing and high pressure fluid phase behavior&property research laboratory China University of Petroleum

Viscosities were measured for the ternary systems Y（NO3）3＋La（NO3）3＋H2O, La（NO3）3＋Ce（NO3）3＋H2O, and La（NO3）3＋Nd（NO3）3＋ H2O and their binary subsystems Y（NO3）3＋H2O, La（NO3）3＋H2O, Ce（NO3）3＋H2O, and Nd（NO3）3＋H2O at 293.15, 298.15 and 308.15 K. The results were used to test the applicability of simple equations for the viscosity of the mixed solutions. The predictions agreed well with measured values, implying that the viscosities of the examined electrolyte solutions could be related to those of their constituent binary solutions using these simple equations.

关键词： viscosity electrolyte solution semi-ideal solution theory rare earth nitrate

Kinetics of hydrate formation using gas bubble suspended in water

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Science China Chemistry 2002年第2期45卷 208-215页

作者：马昌峰陈光进郭天民 high pressure fluid phase behavior & property research laboratory School of Chemical Engineering University of Petroleum Beijing China

An innovative experimental technique, which was devised to study the effects of temperature and pressure on the rate of hydrate formation at the surface of a gas bubble suspended in a stagnant water phase, was adapted in this work. Under such conditions, the hydrate-growth process is free from dynamic mass transfer factors. The rate of hydrate formation of methane and carbon dioxide has been systematically studied. The measured hydrate-growth data were correlated by using the molar Gibbs free energy as driving force. In the course of the experiments, some interesting surface phenomena were observed.

关键词： hydrate formation, kinetics, suspended gas bubble, methane, carbon dioxide.

The remarkable effect of organic salts on 1,3,5-trioxane synthesis

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Petroleum Science 2016年第4期13卷 770-775页

作者： Liu-Yi Yin Yu-Feng Hu Hai-Yan Wang State Key laboratory of Heavy Oil Processing and high pressure fluid phase behavior and property research laboratory China University of PetroleumBeijing

The effects of organic salts on 1,3,5-trioxane synthesis were investigated through batch reaction and continuous production experiments. The organic salts used include sodium methanesulfonate（CH3NaO3S）, sodium benzenesulfonate（C6H5NaO3S）, sodium 4-methylbenzenesulfonate（C7H7NaO3S）, and sodium 3-nitrobenzene sulfonate（C6H4NNaO5S）. It was shown that the effects of organic salts on the yield of 1,3,5-trioxane in reaction solution and distillate follow the order CH3NaO3S ／C6H5NaO3S／C7H7NaO3S／C6H4NNaO5S, which is inversely related to the charge density of the anions of the organic salts. In comparison with Cl–-based salts such as magnesium chloride, organic salts have the advantages of less formic acid generation and low corrosion. Studies on water activity revealed that the effect of organic salts on the activity of water was quite small at low concentration of organic salts. UV–visible spectroscopy and vapor–liquid equilibrium experiments were performed to uncover the mechanisms that govern such effects. The results showed that the effect of organic salts on the yield of 1,3,5-trioxane relies primarily on their ability to increase the catalytic activity of sulfuric acid and increase the relative volatilities of 1,3,5-trioxane and water and of 1,3,5-trioxane and oligomers.

关键词： 1,3,5-Trioxane Organic salt Salt effect Hammett function Relative volatility

Bronsted-acidic ionic liquids as catalysts for synthesizing trioxane

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Chinese Journal of Chemical Engineering 2016年第10期24卷 1392-1398页

作者： Yamei Zhao Yufeng Hu Jianguang Qi Weiting Ma State Key laboratory of Heavy Oil Processing and High Pressure Fluid Phase Behavior&Property Research LaboratoryChina University of PetroleumBeijing 102249China

The batch reaction experiments have been made for the first time to investigate the effect of ionic structure on the reactivity and selectivity of the trioxane-forming reaction catalyzed by a Br?nsted-acidic ionic liquid(IL).The ILs considered include 1-cyclohexyl-2-pyrrolidinonium trifluoromethanesulfonate([NCy P][TfO ]),1-cyclohexyl-2-pyrrolidinonium benzenesulfonate([NCyP ][BSA]),1-cyclohexyl-2-pyrrolidinonium p-toluenesulfonate([NCyP ][pTSA]),1-octyl-2-pyrrolidinonium 2,4-dinitrobenzenesulfonate([NOP][DNBSA]),1-octyl-2-pyrrolidinonium benzenesulfonate([NOP][BSA]),1-octyl-2-pyrrolidinonium methanesulfonate([NOP][MSA]),and 1-octyl-2-pyrrolidinonium trifluoromethanesulfonate([NOP][Tf O]).It is found that the yield of trioxane in the reaction solution correlates inversely with the Hammett acidity function H0 of the aqueous solution of the corresponding *** of the cation structure from [NCyP ]+to [NOP]+exerts little influence on the yield and the selectivity of trioxane in the reaction *** [TfO ]-or [DNBSA]-in place of [MSA]-or [BSA]-apparently increases the yield of trioxane,but only slightly increases the concentration of formic acid in the reaction *** continuous production experiments have been made to investigate the performance of [NOP][MSA],[NOP][DNBSA],[NCyP ][TfO ],and H2SO4 as an extraction distillation *** effect of [NCyP ][TfO ] considerably overrides that of *** yield and the selectivity of trioxane are both increased when [NCyP ][TfO ] is used instead of H2SO4 at a reaction time 5 h.

关键词： Bronsted-acidic Ionic liquids Trioxane Catalyst Hammett acidity function

Prediction of density and viscosity of ternary systems [C_2q]Br+[C_4q]Br+H_2O, [C_2q]Br+[C_6q]Br +H_2O, and [C_4q]Br+[C_6q]Br+H_2O at different temperatures using their binary subsystems data

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Petroleum Science 2012年第2期9卷 242-250页

作者： Peng Xiaoming Hu Yufeng Chu Hongda Miao Chao Li Zheyu WangZhixin Statc Key laboratory of Heavy Oil Processing and high pressure fluid phase behavior&property research laboratory China University of PetroleumBeijing 102249China

The simple equations for prediction of the density and viscosity of mixed electrolyte solutions were extended to the related properties of mixed ionic liquid solutions. The density and viscosity were measured for ternary solutions [C2q]Br（N-ethylquinolinium bromide）＋[C4q]Br （N-butylquinolinium bromide）＋H2O, [C2q]Br＋[C6q]Br（N-hexylquinolinium bromide）＋H2O, and [C4q]Br＋[C6q]Br＋H2O and their binary subsystems [C2q]Br＋H2O, [C4q]Br＋H2O, and [C6q]Br＋H2O at 15, 20 and 25 °C, respectively. The results were used to test the predictability of the extended equations. The comparison results show that these simple equations can be used to predict the density and viscosity of the mixed ionic liquid solutions from the properties of their binary subsystems of equal ionic strength.

关键词： Density viscosity prediction N-ethylquinolinium bromide N-butylquinolinium bromide N-hexylquinolinium bromide

Dissociation behavior of (CH_4+C_2H_4) hydrate in the presence of sodium dodecyl sulfate

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Petroleum Science 2010年第1期7卷 112-117页

作者： Peng Baozi Sun Changyu Chen Guangjin Tang Xulong Liu Peng Chen Jun Zhang Yanqin State Key laboratory of Heavy Oil Processing China University of Petroleum Beijing 102249 China high pressure fluid phase behavior ＆ property research laboratory China University of Petroleum Beijing 102249 China

Separation of a mixture of CH4＋C2H4 gas by forming hydrate in ethylene production has become of interest, and the dissociation behavior of （CH4＋C2H4） hydrate is of great importance for this process. The hydrate formation rate could be increased by adding a small amount of sodium dodecyl sulfate （SDS） into water. In this work, the kinetic data of CH4（18.5 mol%）＋C2H4（81.5 tool%） hydrate decomposition in the presence of 1000 mg.L-~ SDS at different temperatures and pressures were measured with the depressurizing method using a sapphire cell apparatus. The experimental results show that the dissociation rate of （CH4＋C2H4） mixed gas hydrate was large at high temperature and low pressure, and temperature had great influence on the dissociation rate at high pressure. A kinetic model for hydrate dissociation was proposed and the calculated results from the kinetic model were in good agreement with the experimental data. The activation energy for dissociation of the （CH4＋C2H4） mixed gas hydrate was determined to be 43.9 kJ-mol-~, which is lower than that of methane （81.0 ***-~） and ethane （104.0 kJ＇mol-~） hydrate in water （Clarke and Bishnoi, 2004）. As the similar molecular dimensions between ethane and ethylene, the close activation energy need to be provided for ethylene hydrate dissociation. The obtained activation energy of the （CH4＋C2H4） mixed gas hydrate dissociation indicates that the dissociation of the （CH4＋C2H4） mixed gas hydrate is easier than that of pure CH4 or C2H4 gas hydrate.

关键词： Methane ethylene hydrate dissociation SDS