强非共沸工质R1234yf/R170/R14系气液相平衡的模拟
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摘要
超额吉布斯自由能-状态方程法(G~E-EoS)是继传统的状态方程法和活度系数法之后预测气液相平衡的一个新思路。本文采用PRWS-UNIFAC-PSRK模型对R161/R1234yf、R32/R125/R134a及强非共沸工质R1234yf/R170/R14系的气液相平衡数据进行计算。结果表明:R161/R1234yf系压力和气相组分质量分数的计算值与实验值的偏差在±1.5%和±0.02以内,优于REFPROP9.0软件的计算结果,而R32/R125/R134a系的偏差分别在±4%和±0.02以内。根据计算结果及三维相平衡图发现,R1234yf/R170/R14在质量分数比为0.4/0.2/0.4附近时体系的温度滑移现象最为明显,最大的滑移温度达到72.5 K;且R1234yf组分的质量分数越大,泡点温度与露点温度越高。
The excess Gibbs free energy-equation of state(G~E-EoS) is a new method for predicting the vapor liquid equilibrium(VLE)with respect to the equation of state(EoS) and activity coefficient method.In this study,the Peng Robinson(PR) equation of state was employed in combination with the Wong-Sandler(WS) mixing rule to predict binary and ternary systems coupled with the activity coefficient model:the modified universal quasichemical functional group activity coefficient(UNIFAC) used in the predictive Soave-RedlichKwong(PSRK).So a gas-liquid equilibrium prediction model of the mixture(PRWS-UNIFAC-PSRK) was constructed to calculated VLE data of R161/R1234yf,R32/R125/R134 a,and the strong zeotropic ternary system of R1234yf/R170/R14 were calculated.The results indicated that for R161/R1234yf,the relative deviation of the pressures and the absolute deviation of the vapor phase mass fraction between the experimental and calculated data were within ± 1.5% and ± 0.02,respectively,which were better than those found using the REFPROP9.0 software,while the deviations for R32/R125/R134 a were within ± 4% and ± 0.02,respectively.The calculated VLE data and three-dimensional phase equilibrium diagrams showed that the temperature glide phenomenon of R1234yf/R170/R14 was the most obvious at the mass fraction ratio of 0.4/0.2/0.4,and the maximum sliding temperature reached 72.5 K.The dew-point and bubblepoint temperatures increased with the increase in the mass fraction of R1234yf.
The excess Gibbs free energy-equation of state(G~E-EoS) is a new method for predicting the vapor liquid equilibrium(VLE)with respect to the equation of state(EoS) and activity coefficient method.In this study,the Peng Robinson(PR) equation of state was employed in combination with the Wong-Sandler(WS) mixing rule to predict binary and ternary systems coupled with the activity coefficient model:the modified universal quasichemical functional group activity coefficient(UNIFAC) used in the predictive Soave-RedlichKwong(PSRK).So a gas-liquid equilibrium prediction model of the mixture(PRWS-UNIFAC-PSRK) was constructed to calculated VLE data of R161/R1234yf,R32/R125/R134 a,and the strong zeotropic ternary system of R1234yf/R170/R14 were calculated.The results indicated that for R161/R1234yf,the relative deviation of the pressures and the absolute deviation of the vapor phase mass fraction between the experimental and calculated data were within ± 1.5% and ± 0.02,respectively,which were better than those found using the REFPROP9.0 software,while the deviations for R32/R125/R134 a were within ± 4% and ± 0.02,respectively.The calculated VLE data and three-dimensional phase equilibrium diagrams showed that the temperature glide phenomenon of R1234yf/R170/R14 was the most obvious at the mass fraction ratio of 0.4/0.2/0.4,and the maximum sliding temperature reached 72.5 K.The dew-point and bubblepoint temperatures increased with the increase in the mass fraction of R1234yf.
引文
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[35]公茂琼,吴剑锋,罗二仓.深冷混合工质节流制冷原理及应用[M].北京:中国科学技术出版社,2014.(GONG Maoqiong,WU Jianfeng,LUO Ercang.The principle and application of throttling refrigeration for cryogenic mixtures[M].Beijing:China Science and Technology Press,2014.)
[36]PENG D Y,ROBINSON D B.A new two-constant equation of state[J].Industrial&Engineering Chemistry Fundamentals,1976,15(1):59-64.
[37]WONG D S H,SANDLER S.A theoretically correct mixing rule for cubic equations of state[J].Aiche Journal,1992,38(5):671-680.
[38]ORBEY H,SANDLER S I.Modelling vapour-liquid equilibria:cubic equation of state and their mixing rules[J].Cambridge:Cambridge University Press,1998.
[39]ZHANG Haiyang,GONG Maoqiong,LI Huiya,et al.A simple model for temperature-independent kij of the PRvd W model for mixtures containing HCs,HFCs,PFCs,HFOs,CO2,RE170 and R13I1[J].Fluid Phase Equilibria,2016,425:374-384.
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[2]RUHEMANN M.The separation of gases[M].2nd ed.London:Oxford University Press,1949.
[3]KLEEMENKO A P.One-flow cascade cycle[C]//Proceedings of 10th International Congress of Refrigeration.Copenhagen,1959.
[4]FUDERER A.Compression process for refrigeration:US3203194[P].1965-08-31.
[5]LITTLE W A,SAPOZHNIKOV I.Low cost cryocoolers for cryoelectronics[J].Cryocooler,1997,9:509-513.
[6]NAYAK H G,VENKATARATHNAM G.Performance of an auto refrigerant cascade refrigerator operating in gas refrigerant supply(GRS)mode with nitrogen hydrocarbon and argon-hydrocarbon refrigerants[J].Cryogenics,2009,49(7):350-359.
[7]NARASIMHAN N L,VENKATARATHNAM G.Effect of mixture composition and hardware on the performance of a single stage JT refrigerator[J].Cryogenics,2011,51(8):446-451.
[8]REDDY K R,MURTHY S S,VENKATARATHNAM G.Relationship between the cool down characteristics of J-T refrigerators and mixture composition[J].Cryogenics,2010,50(6/7):421-425.
[9]李文林.混合制冷剂的研究与发展[J].流体工程,1986,15(4):60-64.(LI Wenlin.Research and development of mixed refrigerants[J].Fluid Machinery,1986,15(4):60-64.)
[10]李文林,华小龙.混合工质制冷循环的试验研究[J].流体工程,1987,9(5):49-54.(LI Wenlin,HUA Xiaolong.Experimental study on refrigeration cycle of mixed refrigerant[J].Fluid Machinery,1987,9(5):49-54.)
[11]LUO Ercang,GONG Maoqiong,ZHOU Yuan,et al.Experimental investigation of a mixed refrigerant T-T cryocooler operating from 30 to 60 K[J].Advanced in Cryogenic Engineering,2000,45:315-322.
[12]WU J F,GONG M Q,LIU J L,et al.A new type mixture refrigeration auto-cascade cycle with partial condensation and separation reflux exchanger and its preliminary experimental test[J].Advances in Cryogenic Engineering,2002,47:887-892.
[13]GONG Maoqiong,WU Jianfeng,LUO Ercang,et al.Further development of the mixture refrigeration cycle with a dephlegmation separator[J].Cryocoolers,2003,12:603-608.
[14]GONG Maoqiong,WU Jianfeng,LUO Ercang,et al.Study of the single-stage mixed-gases refrigeration cycle for cooling temperature-distributed heat loads[J].International Journal of Thermal Sciences,2004,43(1):31-41.
[15]王国栋.非共沸制冷剂自复叠制冷系统特性及应用研究[D].上海:上海理工大学,2004.(WANG Guodong.Study on the characteristics and application of non azeotropic refrigerant auto cascade refrigeration system[D].Shanghai:University of Shanghai for Science and Technology,2002.)
[16]陆向阳.三级自动复叠制冷循环的实验研究[D].上海:上海理工大学,2002.(LU Xiangyang.Experimental study on three stage auto cascade refrigeration cycle[D].Shanghai:University of Shanghai for Science and Technology,2004.)
[17]荆磊.R600a/R23自动复叠制冷系统及其应用[D].上海:上海理工大学,2006.(JING Lei.Auto cascade refrigeration system and application of R600a/R23[D].Shanghai:University of Shanghai for Science and Technology,2006.)
[18]刘红绍.单级自动复叠制冷系统的实验研究[D].上海:上海理工大学,2008.(LIU Hongshao.Experimental study on single stage auto cascade refrigeration system[D].Shanghai:University of Shanghai for Science and Technology,2008.)
[19]朱军韬,张华.混合工质Linde-Hampson制冷系统的实验研究[J].制冷学报,2012,33(2):18-23.(ZHU Juntao,ZHANG Hua.The experimental research on refrigerant mixtures of a Linde-Hampson refrigeration system[J].Journal of Refrigeration,2012,33(2):18-23.)
[20]HU Peng,CHEN Longxiang,ZHU Wanbao,et al.Isothermal VLE measurements for the binary mixture of 2,3,3,3-tetrafluoroprop-1-ene(HFO-1234yf)+1,1-difluoroethane(HFC-152a)[J].Fluid Phase Equilibria,2014,373:80-83.
[21]HU Peng,CHEN Longxiang,CHEN Zeshao.Vapor-liquid equilibria for binary system of 2,3,3,3-tetrafluoroprop-1-ene(HFO-1234yf)+isobutane(HC-600a)[J].Fluid Phase Equilibria,2014,365:1-4.
[22]CHEN Longxiang,HU Peng,ZHU Wanbao,et al.Vaporliquid equilibria of fluoroethane(HFC-161)+2,3,3,3-tetrafluoroprop-1-ene(HFO-1234yf)[J].Fluid Phase Equilibria,2015,392:19-23.
[23]HU Peng,ZHU Wanbao,CHEN Longxiang,et al.Vaporliquid equilibria measurements of 1,1,1,2-tetrafluoroethane(HFC-134a)+2,3,3,3-tetrafluoroprop-1-ene(HFO-1234yf)+isobutane(HC-600a)ternary system[J].Fluid Phase Equilibria,2016,414:111-116.
[24]HU Peng,CHEN Longxiang,CHEN Zeshao.Vapor-liquid equilibria for the 1,1,1,2-tetrafluoroethane(HFC-134a)+1,1,1,2,3,3,3-heptafluoropropane(HFC-227ea)and1,1,1-trifluoroethane(HFC-143a)+2,3,3,3-tetrafluoroprop-1-ene(HFO-1234yf)systems[J].Fluid Phase Equilibria,2013,360:293-297.
[25]胡芃,高敬轩,陈龙祥,等.PR方程结合vd W混合法则推算二元及三元HFC/HC混合工质汽液相平衡性质[J].化工学报,2012,63(2):350-355.(HU Peng,GAO Jingxuan,CHEN Longxiang,et al.Prediction of vapor-liquid equilibria for binary and ternary HFC/HC mixtures using PR equation of state and vd W mixing rule[J].CIESC Journal,2012,63(2):350-355.)
[26]LIA J,TILLNER-ROTHB R,SATOA H,et al.Equation of state for hydrofluorocarbon refrigerant mixtures of HFC-125/143a,HFC-125/134a,HFC-134a/143a and HFC-125/134a/143a[J].Fluid Phase Equilibria,1999,161(2):225-239.
[27]GONG Maoqiong,ZHAO Yanxing,DONG Xueqiang.Measurements of isothermal(vapor+liquid)equilibria for the(propane+cis-1,3,3,3-tetrafluoropropene)system at temperatures from(253.150 to 293.150)K[J].The Journal of Chemical Thermodynamics,2016,98:319-323.
[28]GONG Maoqiong,GUO Hao,DONG Xueqiang.(Vapor+liquid)phase equilibria measurements for{trifluoroiodomethane(R13I1)+propane(R290)}from T=(258.150 to 283.150)K[J].The Journal of Chemical Thermodynamics,2014,79:167-170.
[29]LIM J S,PARK J Y,KANG J W,et al.Measurement of vapor-liquid equilibria for the binary systems of propane+1,1,1,2-tetrafluoroethane and 1,1,1-trifluoroethane+propane at various temperatures[J].Fluid Phase Equilibria,2006,243(1/2):57-63.
[30]JU M,YUN Y,SHINM S,et al.(Vapour+liquid)equilibria of the{trifluoromethane(HFC-23)+propane}and{trifluoromethane(HFC-23)+n-butane}systems[J].The Journal of Chemical Thermodynamics,2009,41(12):1339-1342.
[31]陈秀萍,祁影霞,赵胜喜,等.新型二元混合制冷剂(R290+R227ea)气液相平衡研究[J].制冷学报,2014,35(5):94-100.(CHEN Xiuping,QI Yingxia,ZHAO Shengxi,et al.Vapor-liquid equilibrium properties of new binary mixture refrigerant(R290+R227ea)[J].Journal of Refrigeration,2014,35(5):94-100.)
[32]BUDINSKY R,VACEK V,LISAL M.Vapor-liquid equilibria of alternative refrigerants and their binaries by molecular simulations employing the reaction Gibbs ensemble Monte Carlo method[J].Fluid Phase Equilibria,2004,(222/223):213-220.
[33]HO Q N,YOO K S,LEE B G.Measurement of vapor-liquid equilibria for the binary mixture of propylene(R1270)+propane(R290)[J].Fluid Phase Equilibria,2006,245(1):63-70.
[34]HO Q N,LEE B G,PARK J Y,et al.Measurement of vapor-liquid equilibria for the binary mixture of propylene(R-1270)+1,1,1,2-tetrafluoroethane(HFC-134a)[J].Fluid Phase Equilibria,2004,225:125-132.
[35]公茂琼,吴剑锋,罗二仓.深冷混合工质节流制冷原理及应用[M].北京:中国科学技术出版社,2014.(GONG Maoqiong,WU Jianfeng,LUO Ercang.The principle and application of throttling refrigeration for cryogenic mixtures[M].Beijing:China Science and Technology Press,2014.)
[36]PENG D Y,ROBINSON D B.A new two-constant equation of state[J].Industrial&Engineering Chemistry Fundamentals,1976,15(1):59-64.
[37]WONG D S H,SANDLER S.A theoretically correct mixing rule for cubic equations of state[J].Aiche Journal,1992,38(5):671-680.
[38]ORBEY H,SANDLER S I.Modelling vapour-liquid equilibria:cubic equation of state and their mixing rules[J].Cambridge:Cambridge University Press,1998.
[39]ZHANG Haiyang,GONG Maoqiong,LI Huiya,et al.A simple model for temperature-independent kij of the PRvd W model for mixtures containing HCs,HFCs,PFCs,HFOs,CO2,RE170 and R13I1[J].Fluid Phase Equilibria,2016,425:374-384.
[40]ZHAO Yanxing,GONG Maoqiong,DONG Xueqiang,et al.Prediction of ternary azeotropic refrigerants with a simple method[J].Fluid Phase Equilibria,2016,425:72-83.
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