不同冷冻润滑油对HFO1234yf溶解吸收特性的研究

doi:10.11949/0438-1157.20190553

摘要/Abstract

摘要：

在原有的溶解度实验台位基础上，研制了一套基于可视等体积饱和法的制冷剂/润滑油溶解实验系统，增加可视窗口的实验本体、调整恒温系统以及改进搅拌系统。采用新研制的实验系统，实验研究了温度范围为283.15~348.15 K制冷剂HFO1234yf与角鲨烷的溶解吸收特性，并采用PR状态方程和HVOS混合规则及活度系数NRTL模型对实验结果进行了关联，计算值和实验值的平均相对误差为1.22 %。此外，温度范围为283.15 ~323.15 K内发现了不互溶分层的现象。

关键词: 溶解性, 状态方程, 测量, 相平衡

Abstract:

On the basis of the original solubility experimental system, a new experimental system using the visual isochoric method was developed to measure the solubility for a refrigerant and a lubricant. In new experimental system, visual experimental cell was added, thermostatic system was adjusted, and magnetic stirring system was modified. Solubilities of HFO1234yf in squalane was measured between 283.15 K and 348.15 K. The experimental data were correlated by PR equation of state with HVOS mixing rule in which the excess Gibbs free energy was represented by the NRTL equation. The absolute average deviation between experimental and calculated data was 1.22 %. Moreover, the immiscibility between HFO134yf and squalane was found from 283.15 K to 323.15 K.

Key words: solubility, equation of state, measurement, phase equilibria

中图分类号:

TK 121

孙艳军, 邸高雷, 夏娟, 王晓坡, 龚娜. 不同冷冻润滑油对HFO1234yf溶解吸收特性的研究[J]. 化工学报, 2019, 70(S2): 25-30.

Yanjun SUN, Gaolei DI, Juan XIA, Xiaopo WANG, Na GONG. Investigation of solubility behavior between HFO1234yf and lubricants[J]. CIESC Journal, 2019, 70(S2): 25-30.

图/表 6

图1 溶解吸收实验系统图

Fig.1 Diagram of solubility measurement

表1 HFO1234yf与角鲨烷的溶解度实验数据

Table 1 Experimental data for solubility of HFO1234zyf in squalene

T/K	x ₁	p/MPa	T/K	x ₁	p/MPa
283.15	0.0211	0.023	333.15	0.0104	0.03
	0.0502	0.065		0.0298	0.083
	0.1382	0.16		0.0755	0.21
	0.2986	0.326		0.1611	0.449
293.15	0.019	0.024		0.2299	0.655
	0.048	0.068		0.3212	0.916
	0.1201	0.171		0.4745	1.352
	0.2557	0.356	343.15	0.0087	0.031
	0.3753	0.5		0.0272	0.086
303.15	0.0173	0.025		0.0697	0.219
	0.0421	0.072		0.1485	0.47
	0.1015	0.183		0.2122	0.687
	0.2202	0.383		0.2966	0.966
	0.3226	0.546		0.4354	1.445
	0.4656	0.734	353.15	0.0078	0.032
313.15	0.014	0.027		0.0261	0.087
	0.0382	0.075		0.0665	0.223
	0.0933	0.191		0.1435	0.479
	0.195	0.407		0.2046	0.702
	0.2829	0.585		0.2864	0.99
	0.3978	0.805		0.421	1.489
323.15	0.0123	0.029
	0.0333	0.079
	0.0832	0.201
	0.1757	0.429
	0.253	0.621
	0.3538	0.863
	0.5365	1.24

图2 303.15 K压力升高时R1234yf与角鲨烷的溶解情况

Fig.2 Solubility of R1234yf in squalane at 350 K with increasing pressure

表2 可调参数

Table 2 Adjustable parameter

体系	$α$	$τ 12,0$	$τ 12,1$	$τ 21,0$	$τ 21,1$
R1234yf + squalane	0.42	2.2853	0.0171	-2.7626	0.0030

表2 可调参数

Table 2 Adjustable parameter

体系	$α$	$τ 12,0$	$τ 12,1$	$τ 21,0$	$τ 21,1$
R1234yf + squalane	0.42	2.2853	0.0171	-2.7626	0.0030

图3 制冷剂HFO1234yf与角鲨烷的溶解度实验结果

Fig.3 Experimental results of solubility of HFO1234yf in squalane ◆—283.15 K；■—293.15 K；●—303.15 K；▲—313.15 K；▼—323.15 K；□—333.15 K；○—343.15 K；△—348.15 K

图4 制冷剂HFO1234yf与角鲨烷的溶解度实验值与计算值的相对偏差

Fig.4 Relative deviation between experimental and calculated values of HFO1234yf in squalane ◆—283.15 K；■—293.15 K；●—303.15 K；▲—313.15 K； ▼—323.15 K；□—333.15 K；○—343.15 K；△—348.15 K

参考文献 30

1	Official Journal of the European Union . Directive 2006/40/EC of the European parliament and of the council of 17 May 2006 relating to emissions from air-conditioning systems in motor vehicles and amending council directive 70/156/EEC [R]. European Union: OJ, 2006.
2	Official Journal of the European Union . Regulation(EU) No. 517/2014 of the European parliament and of the council of 16 April 2014 on fluorinated greenhouse gases and repealing regulation (EC) No 842/2006 [R]. European Union: OJ, 2014.
3	EI-Sayed A R , Morsi M EI , Mahmoud N A . A review of the potential replacements of HCFC/HFCs using environmental friendly refrigerants[J]. International Journal of Air-Conditioning and Refrigeration, 2018, 26: 18300021-183000224.
4	Tashtoush B , Younes M B . Comparative thermodynamic study of refrigerants to select the best environment-friendly refrigerant for use in a solar ejector cooling system[J]. Arab. J. Sci. Eng., 2019, 44: 1165-1184.
5	孟照峰, 张华, 秦延斌, 等 . R1234yf/R134a混合物在汽车空调中替代R134a的实验研究[J]. 化工学报, 2019, 69(6): 2396-2403.
	Meng Z F , Zhang H , Qin Y B , et al . Experimental study on R1234yf/R134a mixture as alternative to R134a in automobile air conditioner[J]. CIESC Journal, 2019, 69(6): 2396-2403.
6	Calm J M . The next generation of refrigerants historical review consideration and outlook[J]. Int. J. Refrig., 2008, 31: 1123-1133.
7	杨富方, 段远源, 杨震 . R1234yf + CO₂和R1234ze(E) + CO₂二元混合物的比容平移Soave-Redlich-Kwong方程[J]. 化工学报, 2016, 67(S2): 14-19.
	Yang F F , Duan Y Y , Yang Z . Volume translation Soave-Redlich-Kwong equation of state for binary mixtures of R1234yf + CO₂ and R1234ze(E) + CO₂ [J]. CIESC Journal, 2016, 67(S2): 14-19.
8	Tanaka K , Higashi Y . Thermodynamic properties of HFO-1234yf (2,3,3,3-tetrafluoropropene)[J]. Int. J. Refrig., 2010, 33: 474-479.
9	邱金友, 张华, 余晓明, 等 . 新型制冷剂R1234ze(E)水平圆管内流动沸腾换热特性[J]. 化工学报, 2016, 67(6): 2255-2262.
	Qiu J Y , Zhang H , Yu X M , et al . Flow boiling heat transfer characteristic of refrigerant R1234ze(E) in horizontal circular tube[J]. CIESC Journal, 2016, 67(6): 2255-2262.
10	Marsh K N , Kandil M E . Review of thermodynamic properties of refrigerants + lubricant oils[J]. Fluid Phase Equilib., 2002, 199: 319-334.
11	金梧凤, 于斌, 高攀, 等 . R32与新型PVE 油的互溶性及其对空调性能的影响[J]. 化工学报, 2018, 69(4): 1631-1637.
	Jin W F , Yu B , Gao P , et al . Effect of solubility between R32 and new PVE oil on performance of air conditioning system[J]. CIESC Journal, 2018, 69(4): 1631-1637.
12	Shen B , Groll E . Review article: a critical review of the influence of lubricants on the heat transfer and pressure drop of refrigerants (Ⅰ): Lubricant influence on pool and flow boiling[J]. HVAC & R Research, 2005, 11:341-359.
13	Chang Y N , Nagashima A . Effect of dissolved lubricating oils on the viscosity of alternative refrigerants [J]. Int. J. Thermophys., 1993, 14: 1007-1019.
14	田田, 杨昭, 吴曦, 等 . RE170、RE170/R227ea 与矿物油的互溶性评价[J]. 化工学报, 2015, 66(6): 2005-2010.
	Tian T , Yang Z , Wu X , et al . Miscibility evaluation of RE170 and RE170/R227ea with a mineral oil[J]. CIESC Journal, 2015, 66(6): 2005-2010.
15	Wang X P , Sun Y J , Gong N . Experimental investigations for the phase equilibrium of R1234yf and R1234ze(E) with two linear chained pentaerythritol esters[J]. Int. J. Thermophys., 2016, 92: 66-71.
16	Bobbo S , Zilio C , Scattolini M , et al . R1234yf as a substitute of R134a in automotive air conditioning. Solubility measurements in two commercial PAG oils [J]. Int. J. Refrig., 2014, 40: 302-308.
17	Marcelino Neto M A , Franca R M , Barbosa J R . Convection-driven absorption of R-1234yf in lubricating oil[J]. Int. J. Refrig., 2014, 44: 151-160.
18	Sun Y J , Wang X P , Gong N , et al . Solubility of trans-1,3,3,3-tetrafluoropropene (R1234ze(E)) in pentaerythritol ester heptanoic aid (PEC7) and in pentaerythritol tetranonanoate (PEC9) between 283.15 K and 353.15 K[J]. Fluid Phase Equilib., 2015, 387: 154-159.
19	Sun Y J , Wang X P , Gong N , et al . Solubility of trans-1,3,3,3-tetrafluoroprop-1-ene in pentaerythritol tetrapentanoate (PEC5) in the temperature from 283.15 to 353.15 K[J]. Int. J. Refrig., 2014, 48: 114-120.
20	Wang X P , Sun Y J , Kang K . Experimental investigation for the solubility of R1234ze(E) in pentaerythritol tetrahexanoate and pentaerythritol tetraoctanoate[J]. Fluid Phase Equilib., 2015, 400: 38-42.
21	Sun, Y J, Wang X P , Gong N , et al . Solubility of dimethyl ether in pentaerythritol tetrahexanoate (PEC6) and in pentaerythritol trtraoctanoate(PEC8) between (283.15 and 353.15) K[J]. J. Chem. Eng. Data, 2014, 59: 3791-3797.
22	Sun Y J , Wang X P , Gong N , et al . Solubility of dimethyl ether in pentaerythritol tetrabutyrate and in pentaerythritol tetrapentanoate. Comparison with other pentaerythritol tetraalkyl esters[J]. Int. J. Thermophys., 2015, 87: 23-28.
23	Fandino O , Pensado A S , Lugo L , et al . Compressed liquid densities of squalane and pentaerythritol tetra-(2-ethylhexanoate) [J]. J. Chem. Eng. Data, 2005, 50: 939-946.
24	Lemmon E W , Huber M L , McLinden, M O . NIST Reference Fluid Thermodynamic and Transport Properties - REFPROP, Version 9.1 [CP]. National Institute of Standards and Technology: Boulder, CO, 2013.
25	Peng D Y , Robinson D B . A new two-constant equation of state[J]. Ind. Eng. Chem., Fundam., 1976, 15: 59-64.
26	VonNiederhausern D M , Wilson G M , Giles N F . Critical point and vapor pressure measurements at high temperatures by means of a new apparatus with ultralow residence times[J]. J. Chem. Eng. Data, 2000, 45: 157-160.
27	Nikitin E D , Popov A P . Vapor-liquid critical properties of squalane measured by the pulse-heating technique[J]. Fluid Phase Equilib., 2005, 237: 16-20.
28	Orbey H , Sandler S I . On the combination of equation of state and excess free energy model[J]. Fluid Phase Equilib., 1995, 111: 53-70.
29	Orbey H , Sandler S I . A comparison of Huron-Vidal type mixing rules of mixtures of compounds with large size differences, and a new mixing rule[J]. Fluid Phase Equilib., 1997, 132: 1-14.
30	Renon H , Prausnitz J M . Local compositions in thermodynamic excess functions for liquid mixtures[J]. AIChE Journal, 1968, 14: 135-144.

[1]	杨百玉, 寇悦, 姜峻韬, 詹亚力, 王庆宏, 陈春茂. 炼化碱渣湿式氧化预处理过程DOM的化学转化特征[J]. 化工学报, 2023, 74(9): 3912-3920.
[2]	仪显亨, 周骛, 蔡小舒, 蔡天意. 光纤后向动态光散射测量纳米颗粒的浓度适用范围研究[J]. 化工学报, 2023, 74(8): 3320-3328.
[3]	于旭东, 李琪, 陈念粗, 杜理, 任思颖, 曾英. 三元体系KCl + CaCl₂ + H₂O 298.2、323.2及348.2 K相平衡研究及计算[J]. 化工学报, 2023, 74(8): 3256-3265.
[4]	闫琳琦, 王振雷. 基于STA-BiLSTM-LightGBM组合模型的多步预测软测量建模[J]. 化工学报, 2023, 74(8): 3407-3418.
[5]	邵伟明, 韩文学, 宋伟, 杨勇, 陈灿, 赵东亚. 基于分布式贝叶斯隐马尔可夫回归的动态软测量建模方法[J]. 化工学报, 2023, 74(6): 2495-2502.
[6]	陈科, 杜理, 曾英, 任思颖, 于旭东. 四元体系LiCl+MgCl₂+CaCl₂+H₂O 323.2 K相平衡研究及计算[J]. 化工学报, 2023, 74(5): 1896-1903.
[7]	陈俊先, 姬忠礼, 赵瑜, 张倩, 周岩, 刘猛, 刘震. 基于微波技术的天然气管道内颗粒物在线检测方法研究[J]. 化工学报, 2023, 74(3): 1042-1053.
[8]	毛元敬, 杨智, 莫松平, 郭浩, 陈颖, 罗向龙, 陈健勇, 梁颖宗. C₆~C₁₀烷醇的SAFT-VR Mie状态方程参数回归及其热物性研究[J]. 化工学报, 2023, 74(3): 1033-1041.
[9]	高靖博, 孙强, 李青, 王逸伟, 郭绪强. 考虑水合物结构转变的含氢气体水合物相平衡模型[J]. 化工学报, 2023, 74(2): 666-673.
[10]	程文婷, 李杰, 徐丽, 程芳琴, 刘国际. AlCl₃·6H₂O在FeCl₃、CaCl₂、KCl及KCl–FeCl₃溶液中溶解度的实验及预测[J]. 化工学报, 2023, 74(2): 642-652.
[11]	蔡进, 王晓辉, 汤涵, 陈光进, 孙长宇. TBAB水溶液体系中半笼型水合物的相平衡预测模型[J]. 化工学报, 2023, 74(1): 408-415.
[12]	周桓, 张梦丽, 郝晴, 吴思, 李杰, 徐存兵. 硫酸镁型光卤石转化钾盐镁矾的过程机制与动态规律[J]. 化工学报, 2022, 73(9): 3841-3850.
[13]	王永倩, 王平, 程康, 毛晨林, 刘文锋, 尹智成, Ferrante Antonio. 氨气/甲烷贫预混旋转湍流火焰稳定性及NO生成[J]. 化工学报, 2022, 73(9): 4087-4094.
[14]	刘潜, 张香兰, 李志平, 李玉龙, 韩梦醒. 油酚分离过程低共熔溶剂的筛选及萃取性能研究[J]. 化工学报, 2022, 73(9): 3915-3928.
[15]	任玉鑫, 徐润峰, 王婉颖, 陈鹏忠, 彭孝军. 彩色光刻胶用蒽醌染料的合成及稳定性研究[J]. 化工学报, 2022, 73(5): 2251-2261.