N-甲酰吗啉相关体系基础物性和相平衡研究
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摘要
N-甲酰吗啉(NFM)因其良好的选择性和热稳定性,作为抽提溶剂广泛的应用于芳烃抽提工艺。要进行相关的工艺设计或改进,必然需要相应NFM的物性数据和相平衡数据。
密度和黏度数据是化合物的重要基础物性,是液体流动、传热和传质过程研究和工程计算中不可缺少的数据。本论文在常压下利用DA-505 U型振动管密度仪和乌氏毛细管黏度计分别测定了苯-NFM,甲苯-NFM,邻二甲苯-NFM,间二甲苯-NFM及对二甲苯-NFM五个二元体系的密度和黏度数据。计算出了每个体系的超额摩尔体积VE和混合黏度的变化Δη,并用Redlich-Kister型方程分别对VE和Δη进行了回归。
相平衡数据是精馏、吸收、萃取、结晶等分离操作的重要计算或设计的依据,在化工数据中占有重要地位。为了准确地进行分离工艺和设备的设计,需要进行大量的实验测定工作。
本研究用改进的Rose釜测定了101.3 kPa下苯-NFM,甲苯-NFM,邻二甲苯-NFM,间二甲苯-NFM及对二甲苯-NFM五个二元体系的等压汽液平衡数据。并采用Wilson和NRTL活度系数模型方程分别对这五个体系的汽液平衡实验数据进行了关联计算,得到了各个体系的模型参数。
同时在101.3 kPa测定了苯-甲苯-NFM三元物系的等压汽液平衡数据,并采用Wilson模型方程,利用苯-NFM,甲苯-NFM和苯-甲苯三个二元体系汽液平衡数据对苯-甲苯-NFM三元体系平衡数据进行预测,并与实验数据进行比较,误差不大。
N-Formylmorpholine (NFM) is widely used in the recovery of aromatic hydrocarbons as a solvent for its good selectivity and heat stability. In order to design or improve these processes, it is extremely important to determine the physical properties and phase equilibrium data of NFM containing systems.
Experiment liquid densities and viscosities of pure compound and their mixtures are needed for the design of chemical processes in heat and mass transfers or fluid mechanics. Densities and viscosities of the ternary systems of benzene+NFM,toluene +NFM,o-xylene+NFM,m-xylene+NFM and p-xylene+NFM (298.15～353.15) K were determined under atmospheric pressure using a vibrating U-shaped sample tube densimeter (model DA-505U) and a Ubbelohde suspended-level viscometer respectively. Density data were used in determination of excess molar volume and viscosity data were used to calculate deviation of viscosity. The excess molar volume and deviation of viscosity were fitted by the Redlich-Kister equation.
Equilibrium data is the basis for the design and computation of separating processes, such as distillation, absorption, extraction and crystallization. An abundance of experimental data is needed for an accurate design of separation processes and facilities.
Isobaric vapor-liquid equilibrium (VLE) data for benzene+NFM,toluene+NFM,o-xylene+NFM,m-xylene+NFM and p-xylene+NFM were measured at 101.33 kPa with an improved Rose equilibria cell. Wilson and NRTL equations were used to correlate the VLE data through the nonlinear least square method.
Then the VLE data of benzene-toluene-NFM ternary system at 101.33kPa were measured and compared with the data predicted by Wilson model from the VLE data of the binary systems of benzene-NFM, toluene-NFM and benzene-toluene., and the deviations are acceptable.
密度和黏度数据是化合物的重要基础物性,是液体流动、传热和传质过程研究和工程计算中不可缺少的数据。本论文在常压下利用DA-505 U型振动管密度仪和乌氏毛细管黏度计分别测定了苯-NFM,甲苯-NFM,邻二甲苯-NFM,间二甲苯-NFM及对二甲苯-NFM五个二元体系的密度和黏度数据。计算出了每个体系的超额摩尔体积VE和混合黏度的变化Δη,并用Redlich-Kister型方程分别对VE和Δη进行了回归。
相平衡数据是精馏、吸收、萃取、结晶等分离操作的重要计算或设计的依据,在化工数据中占有重要地位。为了准确地进行分离工艺和设备的设计,需要进行大量的实验测定工作。
本研究用改进的Rose釜测定了101.3 kPa下苯-NFM,甲苯-NFM,邻二甲苯-NFM,间二甲苯-NFM及对二甲苯-NFM五个二元体系的等压汽液平衡数据。并采用Wilson和NRTL活度系数模型方程分别对这五个体系的汽液平衡实验数据进行了关联计算,得到了各个体系的模型参数。
同时在101.3 kPa测定了苯-甲苯-NFM三元物系的等压汽液平衡数据,并采用Wilson模型方程,利用苯-NFM,甲苯-NFM和苯-甲苯三个二元体系汽液平衡数据对苯-甲苯-NFM三元体系平衡数据进行预测,并与实验数据进行比较,误差不大。
N-Formylmorpholine (NFM) is widely used in the recovery of aromatic hydrocarbons as a solvent for its good selectivity and heat stability. In order to design or improve these processes, it is extremely important to determine the physical properties and phase equilibrium data of NFM containing systems.
Experiment liquid densities and viscosities of pure compound and their mixtures are needed for the design of chemical processes in heat and mass transfers or fluid mechanics. Densities and viscosities of the ternary systems of benzene+NFM,toluene +NFM,o-xylene+NFM,m-xylene+NFM and p-xylene+NFM (298.15～353.15) K were determined under atmospheric pressure using a vibrating U-shaped sample tube densimeter (model DA-505U) and a Ubbelohde suspended-level viscometer respectively. Density data were used in determination of excess molar volume and viscosity data were used to calculate deviation of viscosity. The excess molar volume and deviation of viscosity were fitted by the Redlich-Kister equation.
Equilibrium data is the basis for the design and computation of separating processes, such as distillation, absorption, extraction and crystallization. An abundance of experimental data is needed for an accurate design of separation processes and facilities.
Isobaric vapor-liquid equilibrium (VLE) data for benzene+NFM,toluene+NFM,o-xylene+NFM,m-xylene+NFM and p-xylene+NFM were measured at 101.33 kPa with an improved Rose equilibria cell. Wilson and NRTL equations were used to correlate the VLE data through the nonlinear least square method.
Then the VLE data of benzene-toluene-NFM ternary system at 101.33kPa were measured and compared with the data predicted by Wilson model from the VLE data of the binary systems of benzene-NFM, toluene-NFM and benzene-toluene., and the deviations are acceptable.
引文
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[3]田龙胜,抽提蒸馏分离苯及溶剂油的研究,石油炼制与化工,2001,32(7):5-8
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[2]段松涛,张吉波,芳烃优良抽提溶剂—N-甲酰吗啉,精细与专用化学品,2002,(14):12-15
[3]田龙胜,抽提蒸馏分离苯及溶剂油的研究,石油炼制与化工,2001,32(7):5-8
[4]周仕颖,张敏,以N-甲酰基吗啉抽提蒸馏回收苯和甲苯,石化技术,1998,5(2):119-121
[5] Dr-Ing.Hans J Vollmer, N-Fomylmorphline the superior solvent for aroungtics recovery,Krupp Koppers Gmbh 10th Chisa Congress Pragne,1990,26-31
[6] Preusser G, Emmrich D G, Recovery of high-purity aromatics: new precess technologies improve economy, Che-mical Age of India, 1987, 38(1): 39-44.
[7] Koppers K,Recovery of high-purity BTX Aromatics from Reformate and/or Pyrolysis Gasoline using the Morphylex Process,1991
[8] Krupp Koppers,Recovery of aromatics by MORPHYLANE and MORPHYLEX Process,1991
[9]邹东雷,隋振英,芳烃萃取剂N-甲酰吗啉的合成,精细化工中间体,2003,(4):26-27
[10] Lee L S, Chung M L, Excess volumes of cyclohexane with 2-propanone, 2-butanont systems, J. Chem. Eng. Data, 1997, 42(5): 850-853
[11] JoséT, Concepcion D, Densities and tefractive indices for 1-hexene + o-xylene + m-xylene + p-xylene and + ethylbenzene, J. Chem. Eng. Data,1995, 40: 96-98
[12] Hatschek E, The Viscosity of liquids, New York: D. Van Nostrand Co, 1963, 406-520
[13] Boon J P,Legros J C,Thomaes G,The Viscosity of liquefied Gases,1967,33(3):547-557
[14]陈惠钊,黏度测量,北京:中国计量出版社, 1994
[15] Alejandro E B, Juan F J, Gustava A, Experimental liquid viscosities of decane and octane + decane from 298.15K to 373.15K and up to 25MPa, J. Chem. Eng.Data, 1998, 43(3): 441-446
[16] Dymond J H, Robertson J, Isdale J D, Transport Properties of nonelectrolyte liquid mixtures, Int. J. Thermophys., 1981, 2(3): 223-236
[17] Harrison D E, Gosser R B, Rolling ball viscometer for use at temperatures to 400℃under pressures to 5 kilobar, Rev. Sci. Instrum., 1965, 36: 1840-1843
[18] Isade J D, Spence C M, A self-centring falling body viscometer for high pressures, National Engineering Report, 1975: No.592
[19] Estrada B A, Alvarado J F, Experimental liquid viscosities of decane and octane + decane from 298.15 to 373.15K and up to 25MPa, J. Chem. Eng. Data, 1998, 43(4): 601-604
[20]张淑云,曹汇川,马沛生,烃类物质液体密度的关联,天然气化工, 1996, 21(4):47-52
[21]陈钟秀,顾飞燕,化工热力学,北京:化学工业出版社,1993,34-36
[22]马沛生,石油化工基础数据手册,北京:化学工业出版社,1993,1-150
[23] Gambill W R, How to estimate mixture viscosities, Chem. Eng., 1959, 66(5): 151-156
[24] Amalendu P, Gurcharan D, Excess Molar Volumes and Viscosities for binary liquid mixtures of 2-propoxgethnol with methanol, 2-propanol, 1-pentanol at 298.15K, J. Chem. Eng. Data, 2000, 45(4): 693-698
[25]马沛生,化工数据,北京:中国石化出版社,2003,276-308
[26] Poling B E, Prausnitz J M, O′Connel J P, The Properties of Gases and liquids, 5th ed, New York: Mc Graw-Hill, 2005, 320-380
[27] Knapp H, Prausnnitz J M, Vapor-Liquid Equilibria for Mixtures of Low Boilling Substances, Dechema Chemistry Data Series, 1982,6: 396-472.
[28] Walas S T, Phase Equilibria in Chemical Engineering, Butterworth Publishers, 1985, 358-374
[29]瓦拉斯(美),化工相平衡(韩世钧),北京:中国石化出版社,1991,448-449
[30]刘光永,化工开发实验技术,天津:天津大学出版社,1994,40-44
[31] Wilson G M, A New Expression for the Excess Free Energy of Mixing, J.Am.Chem.Soc.,1964, 86:127-130
[32] Abrams D S, Prausnjtz J M, Statistical thermodynamics of liquid mixtures: A new expression for the excess Gibbs energy of partly or completely miscible systems, AIChE J., 1975, 21(1):116-128
[33]阿格?弗雷登斯隆德,于根?格麦林,彼特?拉斯穆,UNIFAC功能团法推算汽-液平衡,北京:化学工业出版社,1982,14-22
[34] Fredenslund A, Jones R L, Prausnitz J M,Group contribution estimation of activity coefficients in nonideal liquid mixtures, AIChE J., 1975,21:1086-1099
[35] Abrams D S, Prausnitz J M,Statistical Thermodynamics of Liquid Mixtures: A New Expression for the Excess Gibbs Energy of Partly or Completely Miscible Systems,AIChE J., 1975, 21(1): 116-128
[36] Hansen H K, Vapor-liquid equilibria by UNIFAC group contribution, Ind. Eng. chem. Res., 1991, 30(10):2352 -2355
[37] Fredenslund A, Gmehling J, Rasmussen P, Vapor-Liquid Equilibria Using UNIFAC, Elsevier: Amsterdam, 1977
[38] Gmehling J, Vapor-Liquid Equilibria by UNIFAC Group Contribution. 2. Revision and Extension, Ind. Eng. Chem. Pro. Des. Dev., 1982, 21: 118-127.
[39] Macedo E A, Weidlich U, Gmehling J, Vapor-Liquid Equilibria by UNIFAC Group Contribution.3. Revision and Extension, Ind. Eng. Chem. Pro. Des. Dev., 1983, 22: 676-678.
[40] Tiegs D, Gmehling J, Rasmussen P, A Fredenslund. Vapor-Liquid Equilibria by UNIFAC Group Contribution.4. Revision and Extension, Ind. Eng. Chem. Res., 1987, 26: 159-161.
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