Measurements of Surface Tension of R1234yf and R1234ze(E

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Measurements of Surface Tension of R1234yf and R1234ze(E) Xiaoming Zhao,* Wenhao Duan, Xiaoyang Zeng, and Yu Liu MOE Key Laboratory of Thermo-Fluid Science and Engineering, Xi’an Jiaotong University, Xi’an, Shaanxi 710049, China ABSTRACT: An experimental apparatus based on the differential capillary rise method for measuring the surface tension was built up and verified. The surface tensions of R1234yf and R1234ze(E) were measured from 242 to 365 K and 242 to 380 K, respectively. The surface tension data were correlated as a function of temperature, and the average absolute deviations between the experimental and calculated values were 0.002 mN·m−1 for R1234yf, and 0.009 mN·m−1 for R1234ze(E). The surface tension data at temperature lower than 273 K was first reported.

ethyl fluoride (R161) in our laboratory.4,5 Its principle stems from the observation of capillary phenomenon. In the present work, the apparatus was rebuilt and is shown in Figure 1. Capillaries with different inner radii and a scale were vertically placed in a pressure vessel made of stainless steel with two silica glass windows. Four capillaries were prepared and their radii were precisely measured (r1 = 0.1543 ± 0.0006 mm, r2 = 0.3879 ± 0.0006 mm, r3 = 0.4983 ± 0.0006 mm, r4 = 0.7185 ± 0.0006 mm) by an optical image measurement instrument in Xi’an Institute Metrology. During the experiment, the capillary rise difference Δh was measured, and then the surface tension was determined by the following relation

1. INTRODUCTION Now the low Global Warming Potential (GWP) refrigerants have attracted a great attention due to the application of F-gas regulations in European Union and schemes in various countries, which aim to phase out high GWP fluids. 2,3,3,3Tetrafluoroprop-1-ene (HFO-1234yf) and trans-1,3,3,3-tetrafluoroprop-1-ene (HFO-1234ze(E)) are synthetic fluids that contain a carbon−carbon double bond with zero ODP, low GWP, shorter atmosphere life, and low-toxicity. They are expected as the most promising alternatives for HFCs currently used. R1234yf can be used as a drop-in substitute for R134a in mobile air conditioners and R1234ze(E) has been proposed in heat pump and water-cooled chillers. Surface tension is a useful thermodynamic property with clear significance for optimum design of refrigeration systems, especially influencing the heat transfer, flow, and phase change characteristics. For R1234yf and R1234ze(E), Tanaka et al.1,2 and Zhao et al.3 have reported the surface tension data and recommended correlations. But accurate experimental data below 273 K are not yet available in the open literature. Thus, the surface tension measurements of R1234yf and R1234ze(E) were conducted in the temperature range between 242 and 365 K and between 242 and 380 K, respectively, in the present work.

σ=

(

1

2

)

(1)

where σ is the surface tension, g is the local gravitational acceleration (in this work, g = 9.79666 m·s−2), and ρl and ρg are the densities of saturated liquid and vapor, respectively. In this work, the densities of refrigerants were all calculated by the literature.6 Δh is the height difference of the meniscus bottom in two capillaries. r1 and r2 are the radii of capillaries. Equation 1 is based on the assumption that the contact angle between test liquid and glass wall was zero. From direct observation, the capillary wall was completely wetted by refrigerants and this assumption is reasonable. The detailed information about the principle was reported by Ghatee et al. in literatures.6,7 The pressure vessel was installed in the thermostatic bath whose temperature was stable within 10 mK for at least 2 h. Ethyl alcohol, water, and silicone oil were used as the thermostatic fluids in the temperature range of 240−280 K,

2. EXPERIMENTAL SECTION 2.1. Materials. R1234yf and R1234ze(E) used in this work were purchased from Zhejiang Sinoloong Refrigerant Co., Ltd. with mass-fraction purities better than 99.95%. R600a was provided by Zhejiang Lantian Environmental Protection Hitech Co., Ltd. The mass purity was also better than 99.95%. No further purification was done on the samples before use. The sample description was shown in Table 1. 2.2. Apparatus and Method. The differential capillary rise method, well-known as one of the most accurate methods, was used to measure the surface tension of 2,2-dimethylbutane and © XXXX American Chemical Society

(ρl − ρg )g ⎛ r1 r ⎞ ⎜Δh + − 2⎟ 1 1 ⎝ 3 3⎠ 2 r − r

Received: June 14, 2017 Accepted: October 31, 2017

A

DOI: 10.1021/acs.jced.7b00543 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

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Table 1. Sample Used in This Paper chemical name isobutane R1234yf(2,3,3,3-tetrafluoropropene) R1234ze (E) (trans-1,3,3,3tetrafluoropropene)

CAS number 75-28-5 754-12-1 29118-24-9

source Zhejiang Lantian Environment Protection Hi-Tech Co.Ltd. Zhejiang Sinoloong refrigerant Co.Ltd. Zhejiang Sinoloong refrigerant Co.Ltd.

initial mass fraction purity

purification method

0.9995

none

0.9995 0.9995

none none

Figure 1. Schematic diagram of the surface tension experimental system (1) camera; (2) thermostatic bath; (3) pressure vessel; (4) platinum resistance thermometer (25 Ω); (5) heat exchanger; (6) platinum resistance thermometer (100ω); (7) stirrer; (8) heater; (9) temperature control system; (10) circulating pump; (11) Keithley 2701 digital multimeter; (12) data acquisition system; and (13) refrigeration system.

280−365 K, and 370−450 K, respectively. The temperature was measured with a 100 Ω standard platinum resistance thermometer, which was located in the measuring chamber. The standard uncertainty in the temperature was within 12 mK. The height difference in two capillary was determined by a special designed camera and image processing technique with an uncertainty of 0.012 mm. The image acquired from the camera monitor panel is shown in Figure 2, which can be used to analyze the difference rise height. At least five pictures were taken and analyzed. Figure 3 shows the way to determine the length of a pixel as confusing. The measurement uncertainties of the apparatus are listed in Table 2 and the experimental uncertainty of the surface tension measurement was estimated to be within 0.2 mN·m−1 with a coverage factor k = 2. Figure 3. Enlarged pictures of scale line and meniscus. (a) Red line, the two end points when the millimeter scale of the ruler is selected; yellow line, the distance between two end points. Note that the distance between two red lines is 1 mm. (b) Red line: the baseline of the lowest point of the selected concave surface.

Table 2. Measurement Uncertainties measure parameter

standard uncertainty

temperature capillary rise difference inner radii of capillary

12 mK 0.012 mm 0.0006 mm

3. RESULTS AND DISCUSSIONS 3.1. R600a. In order to check the accuracy and reliability of the surface tension experimental system, the surface tension of R600a was measured from 280 to 350 K. We found a principle that the radii of capillary used in our experiment should not be

Figure 2. Image for determination of differential height B

DOI: 10.1021/acs.jced.7b00543 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

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Table 3. Saturated Liquid Density ρl, Saturated Vapor Density ρg, the Height Difference of the Meniscus Bottom in Two Capillaries Δh, the Surface Tension σ of R600a, the Absolute Deviation between the Experimental Result and the Literature Value AD, and the Relative Deviation from the Literature Value RDa,b σ /mN·m−1 T/K 280.34 283.22 285.45 288.02 290.14 293.53 296.42 299.37 302.08 305.41 307.43 310.75 313.15 315.62 318.22 320.46 323.41 325.44 327.83 329.85 330.18 332.56 335.58 338.10 340.42 342.74 345.39 347.26 350.12

ρl/kg·m

−3

572.24 568.84 566.19 563.10 560.54 556.39 552.81 549.12 545.68 541.40 538.77 534.40 531.19 527.84 524.28 521.16 517.00 514.09 510.63 507.65 507.16 503.60 499.00 495.08 491.40 487.66 483.30 480.16 475.26

ρg/kg·m

−3

5.374 5.880 6.296 6.804 7.247 8.001 8.691 9.443 10.178 11.142 11.761 12.839 13.666 14.562 15.556 16.457 17.709 18.615 19.732 20.720 20.886 22.112 23.758 25.212 26.621 28.100 29.880 31.199 33.322

Δh/mm

this work

refs 8, 9

AD/mN·m−1

RD/%

16.928 16.758 16.420 16.081 15.912 15.472 15.066 14.589 14.354 13.937 13.731 13.227 12.878 12.494 12.112 12.050 11.523 11.355 11.003 10.777 10.689 10.361 10.012 9.720 9.470 9.128 8.815 8.680 8.238

11.988 11.785 11.483 11.173 10.995 10.595 10.235 9.829 9.595 9.223 9.030 8.607 8.314 7.999 7.683 7.584 7.172 7.013 6.731 6.538 6.476 6.214 5.925 5.686 5.479 5.220 4.972 4.847 4.526

11.964 11.635 11.381 11.090 10.851 10.471 10.149 9.821 9.523 9.159 8.939 8.579 8.321 8.057 7.780 7.544 7.234 7.022 6.774 6.566 6.532 6.289 5.982 5.729 5.497 5.266 5.006 4.824 4.547

0.024 0.150 0.102 0.083 0.144 0.124 0.086 0.008 0.072 0.064 0.091 0.028 −0.007 −0.058 −0.097 0.040 −0.062 −0.009 −0.043 −0.028 −0.056 −0.075 −0.057 −0.043 −0.018 −0.046 −0.034 0.023 −0.021

0.20 1.29 0.90 0.75 1.33 1.18 0.85 0.07 0.75 0.71 1.03 0.32 1.48 −0.72 −2.07 0.53 −0.86 −0.14 −1.55 −0.42 −1.80 −1.19 −0.96 −0.74 −0.33 −0.89 −0.68 0.48 −0.47

a AD/mN·m−1 = σexp − σref; RD/% = 100*(σexp − σref)/σref. bStandard uncertainties u are u(T) = 12 mK, u(h) = 0.012 mm, u(r) = 0.0006 mm and the expanded uncertainty U is U(σ) = 0.2 mN·m−1 (0.95 level of confidence, k = 2). Note that ρl and ρg are the literature values.8

too large and radii difference should be a little bigger. The result measured by capillaries with radii of 0.1543 and 0.3879 mm was the most accurate. The experimental surface tensions of R600a and deviations from reference data11 were listed in Table 3. The maximum and average absolute deviation between experimental data in this work and reference values were 0.150 and 0.058 mN·m−1, respectively. The relative deviation range from −2.07% to 1.48% and the average relative deviation was 0.85%. Figure 4 shows the deviations. All the results show the experimental system of surface tension was accurate and reliable. 3.2. R1234yf and R1234ze(E). The surface tension of R1234yf was measured from 242 to 365 K and 44 data points are given in Table 4. The surface tension of R1234ze(E) was measured from 242 to 380 K, and 33 data points are listed in Table 5. Universal scaling law and the renormalizations group theory for the surface tension critical exponent were used to correlate the surface tension data12,13 σ = σ0(1 − Tr)1.26 [1 + σ1(1 − Tr)0.5 + σ2(1 − Tr)]

Figure 4. Deviations of experimental surface tension data of R600a compared with literature.8,9

Figure 5 compares the experimental surface tension of R1234yf, fitted data by literature data.1,3 The absolute deviations of the present experimental data of R1234yf to fitted data and literatures were found. The average and maximum absolute deviations from the correlated values to our experimental data are 0.002 and 0.010 mN·m −1 ,

(2)

where σ0, σ1, and σ2 are the fitting parameters, Tr (= T /Tc) is the reduced temperature, where Tc is the critial temperature. Table 6 lists the correlated parameters of R1234yf and R1234ze(E), include Tc. C

DOI: 10.1021/acs.jced.7b00543 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

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Table 4. Saturated Liquid Density ρl, Saturated Vapor Density ρg, the Height Difference of the Meniscus Bottom in Two Capillaries Δh, the Surface Tension σ of R1234yf from 242 to 365 Ka

Table 5. Saturated Liquid Density ρl, Saturated Vapor Density ρg, the Height Difference of the Meniscus Bottom in Two Capillaries Δh, the Surface Tension σ of R1234ze(E) from 242 to 380 Ka

T/K

ρl/kg·m−3

ρg/kg·m−3

Δh/mm

σ/mN·m−1

T/K

ρl/kg·m−3

ρg/kg·m−3

Δh/mm

σ/mN·m−1

242.21 244.21 245.22 248.08 250.10 252.25 255.34 258.24 260.34 263.12 265.13 268.11 270.15 275.55 278.58 280.24 283.24 285.32 288.00 290.08 296.04 300.01 305.09 310.09 312.28 315.20 317.48 320.48 322.47 325.10 327.30 330.27 332.21 335.26 337.53 340.11 342.54 345.13 347.36 350.21 355.63 360.23 362.34 365.00

1267.10 1261.60 1258.80 1250.70 1245.00 1238.90 1230.00 1221.50 1215.30 1207.00 1201.00 1191.90 1185.60 1168.70 1159.00 1153.60 1143.70 1136.80 1127.70 1120.60 1099.60 1085.10 1065.90 1046.20 1037.40 1025.20 1015.50 1002.40 993.48 981.34 970.86 956.20 946.27 930.00 917.30 902.17 887.14 870.15 854.59 833.21 786.32 736.04 706.96 658.52

5.631 6.117 6.375 7.151 7.743 8.415 9.460 10.530 11.364 12.546 13.460 14.911 15.974 19.083 21.030 22.162 24.335 25.941 28.138 29.948 35.683 40.000 46.182 53.081 56.387 61.093 65.023 70.564 74.492 80.021 84.966 92.155 97.201 105.760 112.690 121.230 130.000 140.270 150.000 163.880 196.440 234.650 258.280 299.980

8.446 8.313 8.246 8.057 7.923 7.781 7.576 7.385 7.245 7.061 6.928 6.731 6.596 6.239 6.038 5.928 5.730 5.592 5.414 5.277 4.882 4.619 4.283 3.952 3.807 3.614 3.463 3.264 3.132 2.959 2.813 2.616 2.488 2.286 2.135 1.965 1.804 1.633 1.485 1.296 0.938 0.633 0.493 0.317

13.248 12.976 12.839 12.453 12.182 11.896 11.486 11.106 10.830 10.468 10.210 9.828 9.568 8.889 8.512 8.307 7.940 7.688 7.364 7.117 6.415 5.956 5.382 4.829 4.591 4.279 4.038 3.726 3.523 3.259 3.041 2.752 2.568 2.284 2.077 1.850 1.640 1.425 1.244 1.023 0.637 0.349 0.234 0.108

242.01 245.14 248.08 250.11 255.11 260.07 265.12 268.98 271.51 275.65 280.14 285.03 288.19 290.19 293.10 295.07 300.07 305.06 310.06 315.05 320.05 325.03 330.05 335.09 340.08 345.07 350.07 355.03 360.08 365.09 370.07 375.14 380.09

1325.80 1317.60 1309.90 1304.40 1290.90 1277.30 1263.20 1252.30 1245.00 1232.90 1219.50 1204.70 1194.90 1188.60 1179.40 1173.00 1156.60 1139.80 1122.40 1104.40 1085.70 1066.40 1045.90 1024.10 1001.10 976.45 949.73 920.84 888.33 851.75 808.77 752.67 666.49

3.371 3.882 4.416 4.817 5.929 7.224 8.760 10.100 11.062 12.792 14.903 17.510 19.379 20.643 22.601 24.010 27.911 32.313 37.294 42.904 49.250 56.393 64.545 73.849 84.363 96.431 110.430 126.700 146.470 170.520 201.100 244.440 318.110

9.515 9.313 9.123 8.992 8.669 8.349 8.023 7.774 7.611 7.344 7.054 6.738 6.534 6.405 6.217 6.090 5.767 5.445 5.125 4.810 4.478 4.157 3.830 3.505 3.176 2.879 2.536 2.217 1.802 1.448 1.076 0.697 0.328

15.663 15.227 14.820 14.539 13.855 13.184 12.509 11.998 11.666 11.127 10.547 9.923 9.525 9.275 8.913 8.670 8.059 7.460 6.873 6.304 5.724 5.171 4.621 4.087 3.565 3.094 2.589 2.132 1.605 1.171 0.761 0.395 0.109

a

Standard uncertainties u are u(T) = 12 mK, u(h) = 0.012 mm, u(r) = 0.0006 mm and the expanded uncertainty U is U(σ) = 0.2 mN·m−1 (0.95 level of confidence, k = 2). Note that ρl and ρg are the literature values.8

Table 6. Fitting Parameters of Equation 2 and Critical Temperature of R1234yf and R1234ze(E)

a

a

Standard uncertainties u are u(T) = 12 mK, u(h) = 0.012 mm, u(r) = 0.0006 mm and the expanded uncertainty U is U(σ) = 0.2 mN·m−1 (0.95 level of confidence, k = 2). Note that ρl and ρg are the literature values.8

sample

σ0/mN·m−1

σ1

σ2

Tc (K)

R1234yf R1234ze(E)

42.36234 63.29305

0.60895 −0.41499

−0.42621 0.34264

367.85a 382.51b

The value is from ref 1. bThe value is from ref 10.

especially at higher temperature. As can be observed in Figure 6, the difference between the experimental data and Tanaka’s values decreases first as temperature increases and then rises with temperature. The deviation from Zhao’s data shows a more complicated trend. Figure 7 shows the experimental data of R1234ze(E) measured in this work, fitted data by present data. Equation 2 represents the obtained data with an average deviation of 0.009 mN·m−1, and a maximum deviation of 0.038 mN·m−1. Comparing the present data in temperature range of each literature source, our experimental results shows better agreement with that of Zhao et al.,3 especially near the critical

respectively, which indicate a great regularity between surface tension and temperature. Comparing our experimental data with the correlation recommended by Tanaka et al.1 in their temperature range of measurement, the average and maximum absolute deviations were 0.083 and 0.148 mN·m−1, respectively. In the experimental temperature range of Zhao et al.,3 the average and maximum absolute deviations were 0.091 and 0.168 mN·m−1. The two sets of data have good consistency, D

DOI: 10.1021/acs.jced.7b00543 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

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measured the surface tension of R1234ze(E) with the differential capillary rise method between 273 and 333 K. Their surface tension correlated data are about 0.312 to 0.710 mN·m−1 larger than our experimental data. As we have already mentioned above, the capillary used for measuring the surface tension should be thin. We supposed the inner radii of two capillaries (r1 = 0.4222 mm and r2 = 0.7526 mm) used in the experiment of Tanaka et al.2 were too large to obtain accurate capillary rise difference. As for the deviation between Grebenkov et al.14 data, the average and maximum absolute deviation are 0.480 and 0.996 mN·m−1. In general, the difference between the experimental data and literature values

Figure 5. Surface tension data of R1234yf. □, Present experimental data; solid line, fitted data by eq 2; △, experimental data of Tanaka et al;1 ▽, experimental data of Zhao et al.3

Figure 8. Deviations of Experimental surface tension of R1234ze(E) compared with data from literature. △, Experimental data of Tanaka et al;2 ▽, experimental data of Zhao et al;3 ○, Grebenkov et al.data.14

decreases as temperature goes up (see Figure 7). As shown in Figure 8, both Zhao et al. data and Tanaka et al. data decrease with temperature. In addition, deviations from Zhao et al. data are always less than that from Tanaka et al. results. At temperature higher than 340 K, results obtained by Zhao et al. are very close to the present data. Data from Grebenkov et al. are close to the present results only at temperature higher than 290 K. It can be concluded in Figures 5 and 7 that surface tensions of both R1234yf and R1234ze(E) decrease as the temperature increases. Surface tensions of R1234ze(E) are always bigger than that of R1234yf. In addition, since the surface of fluids would disappear at the critical temperature, the value of surface tension approaches zero on the critical point.

Figure 6. Deviations of Experimental surface tension of R1234yf compared with data from literatures. △, Experimental data of Tanaka et al;1 ▽, experimental data of Zhao et al.3

4. CONCLUSIONS In this work, surface tensions of R1234yf and R1234ze(E) were measured with the differential capillary rise method. The temperature ranges were from 242 to 365 K for R1234yf and 242 to 380 K for R1234ze(E). These data overlap the ranges of the available literature, and surface tension data in the low temperature region were first presented here. On the basis of the experimental data, simple correlations were developed for representing the surface tension as a function of temperature over a wide range. For R1234yf, the average absolute deviation of experimental surface tension data from correlations was 0.002 mN·m−1, and for R1234ze(E), the corresponding value was 0.009 mN·m−1.

Figure 7. Surface tension data of R1234ze(E). □, Present experimental data; △, experimental data of Tanaka et al;2 ▽, experimental data of Zhao et al;3 solid line, fitted data by eq 2; ○, Grebenkov et al. data.14

temperature region. The average and maximum absolute deviation were 0.083 and 0.248 mN·m−1. Tanaka et al.2 E

DOI: 10.1021/acs.jced.7b00543 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

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AUTHOR INFORMATION

Corresponding Author

*Tel: +86-29-82665445. E-mail: [email protected]. ORCID

Xiaoming Zhao: 0000-0003-2938-8080 Notes

The authors declare no competing financial interest.

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ACKNOWLEDGMENTS We acknowledge the support of the National Natural Science Foundation of China (Grant 51676160) and the 111 Project (No. B16038).

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REFERENCES

(1) Tanaka, K.; Higashi, Y. Thermophysical properties of HFO1234yf(2,3,3,3-tetrafluoropropene). Int. J. Refrig. 2010, 33, 474−479. (2) Tanaka, K.; Higashi, Y. Surface tensions of trans-1,3,3,3tetrauoropropene and trans-1,3,3,3-tetrauoropropene + difluoromethane mixture. J. Chem. Eng. Jpn. 2013, 46, 371−375. (3) Zhao, G.; Bi, S.; Fröba, A. P.; Wu, J. Liquid viscosity and surface tension of R1234yf and R1234ze under saturated conditions by surface light scattering. J. Chem. Eng. Data 2014, 59, 1366−1371. (4) Gao, W.; Zhao, X.; Liu, Z. Surface tension of 2,2-dimethylbutane from (233 to 378) K. J. Chem. Eng. Data 2009, 54, 1761−1763. (5) Fan, J.; Zhao, X.; Guo, Z. Surface tension of ethyl fluoride (HFC161) from (233 to 373) K. Fluid Phase Equilib. 2012, 316, 98− 101. (6) Ghatee, M. H.; Zolghadr, A. R. Surface tension measurements of imidazolium-based ionic liquids at liquid−vapor equilibrium. Fluid Phase Equilib. 2008, 263, 168−175. (7) Ghatee, M. H.; Ghaed-Sharaf, T. An experimental study on the surface properties of Protic Morpholinium-based ionic liquids. J. Mol. Liq. 2017, 241, 694−703. (8) Lemmon, E. W.; Huber, M. L.; Mclinden, M. O. NIST Standard Reference Database 23:Reference Fluid Thermodynamic and Transport Properties(REFPROP), version 9.0; National Institute of Standard and Technology: Gaithersburg, MD, 2010. (9) Tanaka, K.; Higashi, Y. Measurements of the surface tension for R290, R600a and R290/R600a mixture. Int. J. Refrig. 2007, 30, 1368− 1373. (10) Higashi, Y.; Tanaka, K.; Ichikawa, T. Critical parameters and saturated densities in the critical region for trans-1,3,3,3-tetrafluoropropene. J. Chem. Eng. Data 2010, 55, 1594−1597. (11) Mulero, A.; Cachadiña, I. Recommended Correlations for the Surface Tension of Several Fluids. J. Phys. Chem. Ref. Data 2014, 43, 023104. (12) Grigoryev, B. A.; Nemzer, B. V.; Kurumov, D. S.; Sengers, J. V. Surface Tension of Normal Pentane, Hexane, Heptane, and Octane. Int. J. Thermophys. 1992, 13, 453−466. (13) Ghatee, M. H.; Maleki, A.; Ghaedsharaf, H. Extended Generic Nature of Surface Entropy. Langmuir 2003, 19, 211−213. (14) Grebenkov, A. J., Hulse, R., Pham, H., Singh, R. Physical properties and equation of state for trans-1,3,3,3 − tetrafluoropropene. Refrigerantion Conference on Thermophysical Properties and Transfer Progress of Refrigerants, June 2009; paper 191, pp 1−19.

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DOI: 10.1021/acs.jced.7b00543 J. Chem. Eng. Data XXXX, XXX, XXX−XXX