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Published in final edited form as: Int J Thermophys. 2022 Jun;43(8):10.1007/s10765-022-03052-7. doi: 10.1007/s10765-022-03052-7

Speed of Sound Measurements of Binary Mixtures of Hydrofluorocarbons [Pentafluoroethane (R-125), 1,1-Difluoroethane (R-152a), or 1,1,1,2,3,3,3-Heptafluoropropane (R-227ea)] with Hydrofluoroolefins [2,3,3,3-Tetrafluoropropene (R-1234yf) or trans-1,3,3,3-Tetrafluoropropene (R-1234ze(E))]

Aaron J Rowane 1, Richard A Perkins 1
PMCID: PMC11459568  NIHMSID: NIHMS1858165  PMID: 39381076

Abstract

Speed of sound data measured using a dual-path pulse-echo instrument are reported for three binary refrigerant mixtures, R-125/1234yf, R-1234yf/152a, and R-1234ze(E)/227ea, at compositions of (0.33/0.67) and (0.67/0.33) mole fraction. The speed of sound was studied at temperatures ranging from 230 K to 345 K from pressures slightly above the bubble point curve up to 20 MPa for the mixtures containing R-1234yf and 49 MPa for the R-1234ze(E)/227ea mixtures. The relative combined expanded speed of sound uncertainty ranged from 0.039 % to 0.317 % with a mean uncertainty over all state points of less than 0.10 %. The reported data are compared to the most recent mixture models in REFPROP for each blend studied. Comparisons of available mixture models for the R-125/1234yf and R-1234yf/152a blends exhibit average absolute deviation values ranging from 0.10 % to 0.27 %, and the average absolute deviations for R-1234ze(E)/227ea blends range from 0.62 % to 0.94 %. The comparisons show that only minor adjustments are required to the R-125/1234yf and R-1234yf/152a mixture models to represent the speed of sound data within its uncertainty. However, significant adjustments are needed to improve the current mixture models for the R-1234ze(E)/227ea blend. Deficiencies with the R-1234ze(E)/227ea mixture model are not unexpected since it (1) utilizes a pure-fluid EOS R-1234ze(E) that has been shown to inaccurately represent R-1234ze(E) speed of sound values and (2) uses binary interaction parameters for the chemically similar mixture of R-1234yf/227ea.

Keywords: Hydrofluorocarbons, Hydrofluoroolefins, REFPROP, Refrigerant mixtures, R-125, R-152a, R-227ea, R-1234yf, R-1234ze(E), Speed of sound

1. Introduction

The next generation of refrigerants are expected to be mixtures of hydrofluorocarbons (HFC) and hydrofluoroolefins (HFO) to meet toxicity, flammability, ozone depletion potential (ODP), global warming potential (GWP), and performance constraints. A database of accurate refrigerant thermophysical properties enables the integration of new low GWP refrigerants into current and future refrigeration systems. The present study expands on a larger project from our group which reports bubble point [1, 2], speed of sound [3, 4], density, thermal conductivity, and viscosity data for several binary mixtures of HFC and HFO refrigerants. The thermophysical property data generated by our group have been used by Bell [5] to improve mixture models for several blends of HFCs and HFOs. The present study expands on this effort and reports speed of sound data for R-125/1234yf, R-1234yf/152a, and R-1234ze(E)/227ea mixtures at nominal compositions of (0.33/0.67) and (0.67/0.33) mole fraction. The data are reported at temperatures ranging from 230 K to 345 K and from pressures just above the bubble point pressure to 20 MPa for blends with R-1234yf and 49 MPa for R-1234ze(E)/227ea blends. The data from the present study are used to assess the performance of mixture models currently in REFPROP [6] for each blend investigated. The mixture models included in REFPROP are constructed from pure-fluid equations of state (EOS) [711] for each blend component and binary interaction parameters [12, 13].

2. Materials and Methods

The sample preparation, dual-path pulse echo, and loading and isochoric measurement procedure used in this study are identical to those reported in previous studies [3, 4, 14]. Therefore, only brief descriptions are provided here, and the reader is referred to our previous work for more detail.

2.1. Sample Preparation

Table 1 lists the refrigerants used in this study along with their short names, CAS numbers, molar mass, source, and purity. As described in our previous studies, [3, 4] degassed pure-component samples were used to prepare vapor-phase samples of each mixture. All mixtures were prepared gravimetrically using the double-substitution method of Harris and Torres [15]. The composition’s estimated standard uncertainty was less than 0.00005 mole fraction when considering contributions from gravimetric preparation, potential contamination of the outside of the sample cylinder with dirt or dust, sorption of sample onto the inner cylinder walls and filling valves, and expansion of the cylinder when filled. The largest contribution to the sample uncertainty was associated with the impurities in the components used to prepare each mixture. The fraction of the impurity for each component was considered in the final composition standard uncertainty by adding it in quadrature with the estimated standard uncertainty from all the aforementioned sources. Table 2 lists the compositions, total sample masses, and standard uncertainties in the composition for each mixture prepared.

Table 1.

Refrigerant samples used in this study listed with their CAS numbers, molar mass, source, and purity

Chemical name CAS Number Molar Mass/ (g·mol−1) Source Purity/mole percent

Pentafluoroethane (R-125) 354–33–6 120.02 Scott Specialty Gas 99.99
1,1-difluoroethane
(R-152a)
75–37–6 66.05 Chemours 99.9355
1,1,1,2,3,3,3-heptafluoropropane
(R-227ea)
431–89–0 170.03 Honeywell 99.97
2,3,3,3-tetrafluoropropene
(R-1234yf)
754–12–1 114.04 Chemours 99.9
1,3,3,3-trans-tetrafluoropropene
(R-1234ze(E))
29,118–24–9 114.04 Honeywell 99.97

All samples were degassed using a freeze–pump–thaw method prior to preparing mixtures and the sample purity was confirmed by gas chromatography

Table 2.

Mixture compositions for the studied binary mixtures listed with total sample mass prepared and standard mole fraction uncertainties

Mixture Composition/mole frac Sample Mass/g uc(x1)/mole frac

R-125/1234yf (0.33351/0.66649) 319.5556 0.00067
R-125/1234yf (0.66643/0.33357) 344.6452 0.00034
R-1234yf/152a (0.33342/0.66658) 281.4816 0.00070
R-1234yf/152a (0.66526/0.33474) 306.3078 0.00055
R-1234ze(E)/227ea (0.33265/0.66735) 378.4553 0.00023
R-1234ze(E)/227ea (0.66803/0.33197) 355.0070 0.00023

2.2. Dual-Path Pulse-Echo Instrument

The dual-path pulse-echo instrument used in this study is identical to that described in our previous studies. Therefore, only selected details are restated here and the interested reader is referred to our previous studies [3, 4, 14] for more information. The dual-path pulse-echo instrument used in this study had a temperature range from 230 K to 423 K and could operate to a maximum pressure of 70 MPa. The standard uncertainties of the temperature and pressure were 0.004 K and 0.014 MPa, respectively. The relative combined expanded uncertainty of the speed of sound for the present measurements ranged from 0.039 % to 0.317 % with an average uncertainty of less than 0.10 %. The speed of sound uncertainty increased as the state point approached the blend’s mixture critical point where lower sound velocities and weaker echo signals were encountered.

2.3. Loading and Isochoric Measurement Procedure

The measuring cell was cooled to 228 K and was then filled by condensing in vapor-phase sample from the supply cylinder until the cell was liquid filled. A majority of the filling manifold, which was at room temperature of 293 K, remained vapor filled immediately following the filling procedure. Measurements commenced at 230 K and a pressure near the saturation pressure; the temperature was increased in 5 K increments, and this caused the liquid to expand into the filling manifold. Once the filling manifold was completely filled with liquid, the pressure would increase by several MPa with each increment in temperature, and this terminated at what we call the “near-saturation trace.” Measurements then proceeded along pseudo-isochores with temperature incremented in 5 K steps until the maximum desired pressure was reached. The pressure was then reduced to a pressure 0.5 MPa above the bubble point determined using the available mixture models in REFPROP [6]. This process was repeated by dropping to a temperature 5 K above the starting temperature of the previous isochore. Up to twelve speed of sound data points were obtained at each state point where measurements were performed. It is important to note that in previous studies [3, 4], pressures for mixtures with R-1234yf were limited to 12 MPa to avoid potential polymerization reactions. However, in the present study, no noticeable polymerization occurred at pressures up to 20 MPa and repeated speed of sound measurements showed no change in the measured speed of sound values.

3. Results and Discussion

The following sections report the experimental speed of sound data measured using the dual-path pulse-echo instrument. The new speed of sound data is then compared to mixture models included in REFPROP, and their performance is discussed.

3.1. Experimental Speed of Sound Data

Figure 1a to f show the relationship between the speed of sound and temperature for the measured Tw points from pressures slightly above the bubble point pressure and several pseudo-isochores for the R-125/1234yf, R-1234yf/152a, and R-1234ze(E)/227ea mixtures. Only every other isochore for each mixture is shown in Figure 1a to f to avoid clutter on the plots. Density labels for each pseudo-isochore are averaged REFPROP values calculated using the measured temperatures and pressures at each state point along a given psuedo-isochore. Lines drawn on each plot are speed of sound values calculated with REFPROP [6]. REFPROP implements the pure-fluid EOS of Lemmon and Jacobson [10] for R-125, Outcalt and McLinden [11] for R-152a, Lemmon and Akasaka [7] for R-1234yf, Thol and Lemmon [8] for R-1234ze(E), and Lemmon and Span [9] for R-227ea. The binary interaction parameters for R-125/1234yf are reported by Bell et al. [13], and for R-1234yf/152a by Bell and Lemmon [12]. No binary interation parameters are available for the R-1234ze(E)/227ea blend, and therefore, parameters for the R-1234yf/227ea mixture of Bell and Lemmon [12] are used in this study. Tables 3, 4 and 5 list the temperature, pressure, speed of sound averaged from up to twelve measurements, and the relative combined expanded uncertainty of the averaged speed of sound measurements for the R-125/1234yf, R-1234yf/152a, and R-1234ze(E)/227ea mixtures, respectively. Data listing up to twelve unaveraged speed of sound measurements and their associated uncertaities can be found in the supplementary information, and these data are also deposited at nist.data.gov (https://doi.org/10.18434/mds2-2642).

Fig. 1.

Fig. 1

Relationship between the speed of sound and temperature for binary mixtures of hydrofluorocarbons (R-125, R-152a, or R-227ea) with hydrofluoroolefins (R-1234yf or R-1234ze(E)) along several pseudo-isochores. The systems and molar compositions are (a) R-125/1234yf (0.33351/0.66649), (b) R-125/1234yf (0.66643/0.33357), (c) R-1234yf/152a (0.33342/0.66658), (d) R-1234yf/152a (0.66526/0.33474), (e) R-1234ze(E)/227ea (0.33265/0.66735), and (f) R-1234ze(E)/227ea (0.66803/0.33197). Symbols represent experimental data points while lines represent predictions with REFPROP [6] along the nominal density; for clarity, only every other isochore is shown

Table 3.

Experimental speed of sound data for the R-125/1234yf mixtures

x1/mole frac x2/mole frac uc(x1)/mole frac T/K p/MPa w/m∙s−1 Uc(w)/%

0.33351 0.66649 0.00067 229.997 0.107 716.21 0.044
0.33351 0.66649 0.00067 235.006 0.744 697.54 0.045
0.33351 0.66649 0.00067 240.002 0.803 675.15 0.047
0.33351 0.66649 0.00067 245.002 0.818 652.50 0.049
0.33351 0.66649 0.00067 250.004 0.825 629.84 0.052
0.33351 0.66649 0.00067 254.994 0.836 607.26 0.055
0.33351 0.66649 0.00067 259.986 0.849 584.75 0.059
0.33351 0.66649 0.00067 269.992 4.667 575.51 0.058
0.33351 0.66649 0.00067 274.995 7.870 582.88 0.055
0.33351 0.66649 0.00067 279.999 11.062 590.02 0.053
0.33351 0.66649 0.00067 269.990 4.084 570.31 0.059
0.33351 0.66649 0.00067 274.995 7.259 577.72 0.057
0.33351 0.66649 0.00067 279.999 10.444 585.08 0.054
0.33351 0.66649 0.00067 284.999 13.619 592.26 0.052
0.33351 0.66649 0.00067 269.989 1.474 545.69 0.066
0.33351 0.66649 0.00067 274.993 4.529 553.43 0.062
0.33351 0.66649 0.00067 279.998 7.594 561.08 0.059
0.33351 0.66649 0.00067 285.000 10.710 568.96 0.056
0.33351 0.66649 0.00067 290.001 13.780 576.34 0.053
0.33351 0.66649 0.00067 274.992 1.591 524.38 0.071
0.33351 0.66649 0.00067 279.998 4.500 532.30 0.067
0.33351 0.66649 0.00067 284.999 7.424 540.15 0.063
0.33351 0.66649 0.00067 290.002 10.348 547.79 0.060
0.33351 0.66649 0.00067 294.996 13.264 555.22 0.057
0.33351 0.66649 0.00067 279.996 1.536 501.19 0.078
0.33351 0.66649 0.00067 284.998 4.294 509.34 0.073
0.33351 0.66649 0.00067 290.000 7.065 517.35 0.068
0.33351 0.66649 0.00067 294.997 9.839 525.16 0.064
0.33351 0.66649 0.00067 284.998 1.500 477.98 0.086
0.33351 0.66649 0.00067 290.001 4.115 486.39 0.080
0.33351 0.66649 0.00067 294.997 6.738 494.59 0.074
0.33351 0.66649 0.00067 299.998 9.369 502.59 0.070
0.33351 0.66649 0.00067 290.000 1.462 454.43 0.096
0.33351 0.66649 0.00067 294.996 3.941 463.24 0.088
0.33351 0.66649 0.00067 299.998 6.425 471.71 0.082
0.33351 0.66649 0.00067 304.997 8.914 479.88 0.076
0.33351 0.66649 0.00067 294.994 1.527 431.92 0.107
0.33351 0.66649 0.00067 299.996 3.868 440.96 0.098
0.33351 0.66649 0.00067 304.997 6.217 449.66 0.090
0.33351 0.66649 0.00067 309.999 8.573 458.02 0.083
0.33351 0.66649 0.00067 299.995 1.727 411.00 0.119
0.33351 0.66649 0.00067 304.996 3.942 420.33 0.108
0.33351 0.66649 0.00067 310.000 6.167 429.22 0.099
0.33351 0.66649 0.00067 314.993 8.391 437.71 0.091
0.33351 0.66649 0.00067 304.993 1.803 388.15 0.136
0.33351 0.66649 0.00067 309.997 3.882 397.71 0.122
0.33351 0.66649 0.00067 314.994 5.967 406.78 0.111
0.33351 0.66649 0.00067 320.004 8.057 415.38 0.102
0.33351 0.66649 0.00067 309.997 2.071 367.74 0.153
0.33351 0.66649 0.00067 314.991 4.030 378.01 0.137
0.33351 0.66649 0.00067 320.004 6.003 387.27 0.124
0.33351 0.66649 0.00067 325.009 7.977 396.01 0.113
0.33351 0.66649 0.00067 314.991 2.342 348.44 0.173
0.33351 0.66649 0.00067 320.002 4.183 357.97 0.154
0.33351 0.66649 0.00067 325.007 6.033 367.70 0.138
0.33351 0.66649 0.00067 330.000 7.883 376.48 0.125
0.33351 0.66649 0.00067 320.001 2.505 326.33 0.202
0.33351 0.66649 0.00067 325.008 4.201 336.07 0.178
0.33351 0.66649 0.00067 330.000 5.910 345.16 0.159
0.33351 0.66649 0.00067 330.000 5.932 346.00 0.158
0.33351 0.66649 0.00067 335.004 7.640 354.50 0.142
0.33351 0.66649 0.00067 325.006 2.664 303.74 0.240
0.33351 0.66649 0.00067 325.006 2.663 303.60 0.240
0.33351 0.66649 0.00067 329.998 4.248 314.22 0.208
0.33351 0.66649 0.00067 335.004 5.836 323.61 0.184
0.33351 0.66649 0.00067 329.997 2.987 284.75 0.279
0.33351 0.66649 0.00067 335.003 4.461 295.33 0.239
0.33351 0.66649 0.00067 340.008 5.942 304.74 0.209
0.33351 0.66649 0.00067 345.012 7.446 314.03 0.184
0.66643 0.33357 0.00034 229.999 0.471 687.99 0.046
0.66643 0.33357 0.00034 235.010 1.062 668.75 0.047
0.66643 0.33357 0.00034 240.003 1.077 645.73 0.049
0.66643 0.33357 0.00034 245.002 1.089 622.55 0.052
0.66643 0.33357 0.00034 250.004 1.120 599.62 0.055
0.66643 0.33357 0.00034 254.994 3.686 598.44 0.054
0.66643 0.33357 0.00034 259.986 7.231 605.38 0.052
0.66643 0.33357 0.00034 265.002 10.792 612.28 0.049
0.66643 0.33357 0.00034 269.992 14.364 619.27 0.048
0.66643 0.33357 0.00034 274.995 17.942 626.20 0.046
0.66643 0.33357 0.00034 279.999 21.515 633.02 0.044
0.66643 0.33357 0.00034 254.991 3.664 598.25 0.054
0.66643 0.33357 0.00034 254.991 1.737 582.05 0.058
0.66643 0.33357 0.00034 259.985 5.206 589.26 0.055
0.66643 0.33357 0.00034 269.991 12.115 603.11 0.050
0.66643 0.33357 0.00034 259.984 1.506 557.12 0.062
0.66643 0.33357 0.00034 259.984 1.440 556.52 0.063
0.66643 0.33357 0.00034 269.990 7.924 570.42 0.056
0.66643 0.33357 0.00034 274.995 11.247 577.89 0.053
0.66643 0.33357 0.00034 269.991 4.788 543.12 0.063
0.66643 0.33357 0.00034 274.995 7.953 550.80 0.059
0.66643 0.33357 0.00034 279.999 11.132 558.41 0.056
0.66643 0.33357 0.00034 269.990 1.601 511.98 0.073
0.66643 0.33357 0.00034 274.994 4.576 519.80 0.068
0.66643 0.33357 0.00034 279.999 7.586 527.73 0.064
0.66643 0.33357 0.00034 285.001 10.594 535.45 0.060
0.66643 0.33357 0.00034 274.993 1.601 488.69 0.080
0.66643 0.33357 0.00034 279.998 4.428 496.85 0.075
0.66643 0.33357 0.00034 285.001 7.269 504.89 0.069
0.66643 0.33357 0.00034 290.002 10.119 512.75 0.065
0.66643 0.33357 0.00034 279.997 1.521 464.28 0.089
0.66643 0.33357 0.00034 284.999 4.185 472.69 0.082
0.66643 0.33357 0.00034 290.002 6.863 480.91 0.076
0.66643 0.33357 0.00034 294.998 9.551 488.94 0.071
0.66643 0.33357 0.00034 284.998 1.626 441.78 0.099
0.66643 0.33357 0.00034 290.001 4.149 450.52 0.091
0.66643 0.33357 0.00034 294.997 6.686 459.01 0.084
0.66643 0.33357 0.00034 299.998 9.233 467.24 0.078
0.66643 0.33357 0.00034 290.000 1.510 416.01 0.114
0.66643 0.33357 0.00034 294.995 3.867 425.01 0.103
0.66643 0.33357 0.00034 299.999 6.240 433.69 0.095
0.66643 0.33357 0.00034 304.996 8.625 442.10 0.087
0.66643 0.33357 0.00034 294.995 1.476 390.66 0.131
0.66643 0.33357 0.00034 299.997 3.687 400.09 0.118
0.66643 0.33357 0.00034 304.995 5.916 409.15 0.107
0.66643 0.33357 0.00034 309.999 8.157 417.85 0.098
0.66643 0.33357 0.00034 299.997 1.466 364.80 0.154
0.66643 0.33357 0.00034 304.996 3.547 374.94 0.137
0.66643 0.33357 0.00034 309.999 5.634 384.42 0.123
0.66643 0.33357 0.00034 314.993 7.728 393.41 0.112
0.66643 0.33357 0.00034 320.003 9.825 401.91 0.102
0.66643 0.33357 0.00034 304.993 1.937 347.12 0.171
0.66643 0.33357 0.00034 309.997 3.889 357.22 0.152
0.66643 0.33357 0.00034 314.989 5.848 366.71 0.136
0.66643 0.33357 0.00034 320.003 7.793 375.31 0.123
0.66643 0.33357 0.00034 325.008 9.761 383.72 0.112
0.66643 0.33357 0.00034 309.995 1.979 321.21 0.207
0.66643 0.33357 0.00034 314.992 3.779 331.71 0.180
0.66643 0.33357 0.00034 320.003 5.598 341.52 0.160
0.66643 0.33357 0.00034 325.007 7.421 350.69 0.143
0.66643 0.33357 0.00034 314.991 2.245 299.27 0.245
0.66643 0.33357 0.00034 320.003 3.919 310.10 0.211
0.66643 0.33357 0.00034 325.008 5.605 319.71 0.184
0.66643 0.33357 0.00034 330.001 7.308 329.48 0.163

Compositions listed (x1, x2) and composition standard uncertainty (uc(x1)) are mole fractions. The standard uncertainties for temperature (T) and pressure (p) are uc(T)= 0.004 and uc(p) = 0.014 MPa, respectively. Speed of sound values listed (w) is averaged from up to twelve measurements at each state point. Relative combined expanded speed of sound uncertainties, Uc(w), are determined with a coverage factor k = 2 and include effects of composition, temperature, pressure, time delay between echo arrivals, and path length calibration as described in detail elsewhere [3, 4, 14]. Lines in the table separate the pseudoisochores

Table 4.

Experimental speed of sound data for the R-1234yf/152a mixtures

x1/mole frac x2/mole frac uc(x1)/mole frac T/K p/MPa w/m∙s−1 Uc(w)/%

0.33342 0.66658 0.00070 229.998 0.258 874.02 0.039
0.33342 0.66658 0.00070 235.012 0.616 852.44 0.039
0.33342 0.66658 0.00070 240.002 0.620 828.74 0.040
0.33342 0.66658 0.00070 245.003 0.629 805.02 0.041
0.33342 0.66658 0.00070 250.005 0.639 781.39 0.043
0.33342 0.66658 0.00070 254.994 0.648 757.80 0.044
0.33342 0.66658 0.00070 259.987 0.663 734.27 0.046
0.33342 0.66658 0.00070 269.991 3.305 709.64 0.048
0.33342 0.66658 0.00070 269.991 3.290 709.46 0.048
0.33342 0.66658 0.00070 274.995 6.843 716.19 0.047
0.33342 0.66658 0.00070 279.999 10.500 723.65 0.045
0.33342 0.66658 0.00070 285.000 14.099 730.67 0.044
0.33342 0.66658 0.00070 269.990 1.083 690.61 0.050
0.33342 0.66658 0.00070 274.993 4.553 697.56 0.049
0.33342 0.66658 0.00070 279.998 8.034 704.54 0.047
0.33342 0.66658 0.00070 285.000 11.524 711.55 0.046
0.33342 0.66658 0.00070 274.992 1.087 667.01 0.053
0.33342 0.66658 0.00070 279.997 4.427 674.27 0.051
0.33342 0.66658 0.00070 284.999 7.776 681.55 0.050
0.33342 0.66658 0.00070 290.002 11.132 688.79 0.048
0.33342 0.66658 0.00070 279.997 1.131 643.60 0.057
0.33342 0.66658 0.00070 284.999 4.339 651.21 0.054
0.33342 0.66658 0.00070 290.002 7.563 658.80 0.052
0.33342 0.66658 0.00070 294.998 10.784 666.26 0.050
0.33342 0.66658 0.00070 284.998 1.054 618.93 0.061
0.33342 0.66658 0.00070 290.001 4.120 626.79 0.058
0.33342 0.66658 0.00070 294.998 7.188 634.51 0.056
0.33342 0.66658 0.00070 299.998 10.264 642.13 0.053
0.33342 0.66658 0.00070 289.999 1.178 596.19 0.065
0.33342 0.66658 0.00070 294.996 4.113 604.32 0.062
0.33342 0.66658 0.00070 299.998 7.056 612.29 0.059
0.33342 0.66658 0.00070 304.996 9.987 619.96 0.057
0.33342 0.66658 0.00070 294.995 1.011 570.00 0.072
0.33342 0.66658 0.00070 299.997 3.806 578.42 0.068
0.33342 0.66658 0.00070 304.997 6.615 586.74 0.064
0.33342 0.66658 0.00070 309.999 9.429 594.83 0.061
0.33342 0.66658 0.00070 299.996 1.209 547.74 0.078
0.33342 0.66658 0.00070 304.996 3.847 556.10 0.073
0.33342 0.66658 0.00070 309.998 6.521 564.52 0.069
0.33342 0.66658 0.00070 314.993 9.198 572.72 0.065
0.33342 0.66658 0.00070 304.994 1.263 523.56 0.086
0.33342 0.66658 0.00070 309.998 3.817 532.72 0.080
0.33342 0.66658 0.00070 314.994 6.372 541.49 0.075
0.33342 0.66658 0.00070 320.003 8.940 550.04 0.070
0.33342 0.66658 0.00070 309.997 1.356 499.49 0.096
0.33342 0.66658 0.00070 314.993 3.833 509.65 0.088
0.33342 0.66658 0.00070 320.003 6.276 518.79 0.082
0.33342 0.66658 0.00070 325.009 8.703 527.34 0.076
0.33342 0.66658 0.00070 314.991 1.651 478.24 0.106
0.33342 0.66658 0.00070 320.002 3.967 487.98 0.097
0.33342 0.66658 0.00070 325.008 6.266 497.03 0.089
0.33342 0.66658 0.00070 329.999 8.556 505.58 0.083
0.33342 0.66658 0.00070 320.003 1.697 452.76 0.120
0.33342 0.66658 0.00070 325.007 3.876 462.80 0.109
0.33342 0.66658 0.00070 329.999 6.042 472.10 0.100
0.33342 0.66658 0.00070 335.004 8.198 480.75 0.093
0.33342 0.66658 0.00070 325.007 1.969 430.73 0.135
0.33342 0.66658 0.00070 329.999 4.027 441.05 0.122
0.33342 0.66658 0.00070 335.003 6.081 450.54 0.111
0.33342 0.66658 0.00070 340.008 8.146 459.65 0.102
0.33342 0.66658 0.00070 329.997 2.042 404.69 0.158
0.33342 0.66658 0.00070 335.002 3.952 415.02 0.141
0.33342 0.66658 0.00070 340.006 5.886 424.93 0.127
0.33342 0.66658 0.00070 345.012 7.830 434.39 0.116
0.33342 0.66658 0.00070 335.000 2.091 377.02 0.189
0.33342 0.66658 0.00070 340.007 3.904 388.49 0.166
0.33342 0.66658 0.00070 345.013 5.729 399.14 0.147
0.33342 0.66658 0.00070 340.007 2.413 354.81 0.220
0.33342 0.66658 0.00070 345.013 4.107 366.51 0.190
0.66526 0.33474 0.00055 229.996 0.135 800.24 0.043
0.66526 0.33474 0.00055 235.011 0.631 780.26 0.041
0.66526 0.33474 0.00055 240.002 0.648 757.43 0.042
0.66526 0.33474 0.00055 245.002 0.654 734.42 0.044
0.66526 0.33474 0.00055 250.004 0.671 711.50 0.046
0.66526 0.33474 0.00055 254.994 0.670 688.76 0.048
0.66526 0.33474 0.00055 259.987 3.819 691.33 0.047
0.66526 0.33474 0.00055 259.985 0.833 667.24 0.050
0.66526 0.33474 0.00055 274.995 11.612 688.91 0.046
0.66526 0.33474 0.00055 269.990 3.405 644.51 0.052
0.66526 0.33474 0.00055 274.995 6.857 652.38 0.050
0.66526 0.33474 0.00055 279.999 10.264 659.74 0.049
0.66526 0.33474 0.00055 269.991 1.171 624.61 0.056
0.66526 0.33474 0.00055 274.994 4.478 632.30 0.054
0.66526 0.33474 0.00055 279.999 7.793 639.91 0.051
0.66526 0.33474 0.00055 285.000 11.120 647.51 0.050
0.66526 0.33474 0.00055 274.992 1.269 602.80 0.059
0.66526 0.33474 0.00055 279.999 4.441 610.74 0.057
0.66526 0.33474 0.00055 285.000 7.628 618.62 0.054
0.66526 0.33474 0.00055 290.002 10.799 626.23 0.052
0.66526 0.33474 0.00055 279.997 1.047 577.69 0.064
0.66526 0.33474 0.00055 284.999 4.067 585.91 0.061
0.66526 0.33474 0.00055 290.002 7.093 593.95 0.058
0.66526 0.33474 0.00055 294.998 10.116 601.80 0.055
0.66526 0.33474 0.00055 284.998 1.082 554.99 0.070
0.66526 0.33474 0.00055 290.001 3.963 563.43 0.066
0.66526 0.33474 0.00055 294.998 6.851 571.70 0.062
0.66526 0.33474 0.00055 299.999 9.742 579.75 0.059
0.66526 0.33474 0.00055 290.000 1.026 531.01 0.076
0.66526 0.33474 0.00055 294.997 3.769 539.79 0.071
0.66526 0.33474 0.00055 299.999 6.519 548.29 0.067
0.66526 0.33474 0.00055 304.997 9.267 556.50 0.063
0.66526 0.33474 0.00055 294.995 1.115 508.59 0.083
0.66526 0.33474 0.00055 299.996 3.725 517.58 0.078
0.66526 0.33474 0.00055 304.997 6.342 526.29 0.072
0.66526 0.33474 0.00055 309.999 8.958 534.65 0.068
0.66526 0.33474 0.00055 299.995 1.325 487.63 0.091
0.66526 0.33474 0.00055 304.996 3.806 496.79 0.084
0.66526 0.33474 0.00055 309.998 6.298 505.65 0.078
0.66526 0.33474 0.00055 314.994 8.789 514.15 0.073
0.66526 0.33474 0.00055 304.994 1.369 464.23 0.102
0.66526 0.33474 0.00055 309.998 3.725 473.73 0.093
0.66526 0.33474 0.00055 314.993 6.084 482.82 0.086
0.66526 0.33474 0.00055 320.004 8.452 491.54 0.080
0.66526 0.33474 0.00055 309.996 1.617 443.53 0.113
0.66526 0.33474 0.00055 314.993 3.849 453.25 0.103
0.66526 0.33474 0.00055 320.003 6.090 462.47 0.094
0.66526 0.33474 0.00055 325.007 8.351 471.47 0.087
0.66526 0.33474 0.00055 314.991 1.659 419.51 0.128
0.66526 0.33474 0.00055 320.002 3.757 429.41 0.116
0.66526 0.33474 0.00055 325.008 5.845 438.60 0.106
0.66526 0.33474 0.00055 329.999 7.970 447.76 0.097
0.66526 0.33474 0.00055 320.000 1.690 394.59 0.149
0.66526 0.33474 0.00055 325.007 3.656 404.85 0.133
0.66526 0.33474 0.00055 329.999 5.625 414.48 0.121
0.66526 0.33474 0.00055 335.003 7.587 423.38 0.110
0.66526 0.33474 0.00055 325.006 2.087 376.15 0.166
0.66526 0.33474 0.00055 329.998 3.941 386.52 0.148
0.66526 0.33474 0.00055 335.003 5.793 396.02 0.133
0.66526 0.33474 0.00055 340.008 7.662 405.17 0.121
0.66526 0.33474 0.00055 329.996 1.939 346.06 0.206
0.66526 0.33474 0.00055 335.003 3.635 356.72 0.181
0.66526 0.33474 0.00055 340.007 5.349 366.76 0.160
0.66526 0.33474 0.00055 345.013 7.070 376.19 0.144
0.66526 0.33474 0.00055 335.001 2.211 324.32 0.241
0.66526 0.33474 0.00055 340.007 3.804 335.47 0.209
0.66526 0.33474 0.00055 345.013 5.407 345.72 0.183
0.66526 0.33474 0.00055 340.007 2.757 309.92 0.266
0.66526 0.33474 0.00055 345.013 4.263 320.63 0.229

Compositions listed (x1, x2) and composition standard uncertainty (uc(x1)) are mole fractions. The standard uncertainties for temperature (T) and pressure (p) are uc(T) = 0.004 and uc(p) = 0.014 MPa, respectively. Speed of sound values listed (w) are averaged from up to twelve measurements at each state point. Relative combined expanded speed of sound uncertainties, Uc(w), are determined with a coverage factor k = 2, and include effects of composition, temperature, pressure, time delay between echo arrivals, and path length calibration as described in detail elsewhere [3, 4, 14]. Lines in the table separate the pseudoisochores

Table 5.

Experimental speed of sound data for the R-1234ze(E)/227ea mixtures

x1/mole frac x2/mole frac uc(x1)/mole frac T/K p/MPa w/m∙s−1 Uc(w)/%

0.33265 0.66737 0.00023 230.010 0.370 736.85 0.040
0.33265 0.66737 0.00023 235.012 0.457 715.38 0.041
0.33265 0.66737 0.00023 240.001 0.462 693.46 0.043
0.33265 0.66737 0.00023 245.003 0.469 671.70 0.044
0.33265 0.66737 0.00023 250.004 0.465 650.04 0.046
0.33265 0.66737 0.00023 254.995 0.458 628.53 0.048
0.33265 0.66737 0.00023 259.987 0.471 607.24 0.051
0.33265 0.66737 0.00023 269.992 3.351 588.48 0.052
0.33265 0.66737 0.00023 274.995 6.712 594.84 0.050
0.33265 0.66737 0.00023 279.999 10.082 601.22 0.049
0.33265 0.66737 0.00023 285.000 13.433 607.45 0.047
0.33265 0.66737 0.00023 290.002 16.668 612.91 0.046
0.33265 0.66737 0.00023 294.997 19.952 618.72 0.045
0.33265 0.66737 0.00023 299.998 23.210 624.35 0.044
0.33265 0.66737 0.00023 304.997 26.420 629.72 0.043
0.33265 0.66737 0.00023 309.999 29.616 635.01 0.042
0.33265 0.66737 0.00023 314.994 32.783 640.19 0.041
0.33265 0.66737 0.00023 320.005 35.925 645.23 0.041
0.33265 0.66737 0.00023 325.010 39.103 650.48 0.040
0.33265 0.66737 0.00023 330.000 42.303 655.89 0.039
0.33265 0.66737 0.00023 335.003 45.456 661.01 0.039
0.33265 0.66737 0.00023 340.008 48.628 666.24 0.039
0.33265 0.66737 0.00023 274.991 3.582 570.38 0.055
0.33265 0.66737 0.00023 279.996 6.857 577.23 0.052
0.33265 0.66737 0.00023 284.997 10.129 583.99 0.050
0.33265 0.66737 0.00023 289.999 13.388 590.58 0.049
0.33265 0.66737 0.00023 294.995 16.634 597.03 0.047
0.33265 0.66737 0.00023 299.997 19.861 603.31 0.046
0.33265 0.66737 0.00023 304.996 23.080 609.49 0.045
0.33265 0.66737 0.00023 309.998 26.280 615.51 0.044
0.33265 0.66737 0.00023 314.994 29.441 621.29 0.043
0.33265 0.66737 0.00023 320.002 32.633 627.19 0.042
0.33265 0.66737 0.00023 325.008 35.791 632.89 0.041
0.33265 0.66737 0.00023 330.000 38.917 638.43 0.041
0.33265 0.66737 0.00023 335.003 41.992 643.65 0.040
0.33265 0.66737 0.00023 340.007 45.084 648.96 0.039
0.33265 0.66737 0.00023 345.013 48.160 654.19 0.039
0.33265 0.66737 0.00023 269.987 0.427 564.48 0.057
0.33265 0.66737 0.00023 274.990 0.887 547.36 0.060
0.33265 0.66737 0.00023 279.995 4.051 554.51 0.057
0.33265 0.66737 0.00023 284.997 7.216 561.58 0.054
0.33265 0.66737 0.00023 289.999 10.386 568.56 0.052
0.33265 0.66737 0.00023 294.995 13.539 575.34 0.050
0.33265 0.66737 0.00023 299.997 16.693 582.02 0.049
0.33265 0.66737 0.00023 304.993 19.799 588.33 0.047
0.33265 0.66737 0.00023 309.998 22.889 594.43 0.046
0.33265 0.66737 0.00023 314.992 25.989 600.59 0.045
0.33265 0.66737 0.00023 320.002 29.081 606.63 0.044
0.33265 0.66737 0.00023 325.008 32.153 612.51 0.043
0.33265 0.66737 0.00023 329.999 35.201 618.26 0.042
0.33265 0.66737 0.00023 335.001 38.214 623.77 0.041
0.33265 0.66737 0.00023 340.008 41.230 629.27 0.041
0.33265 0.66737 0.00023 345.013 44.228 634.66 0.040
0.33265 0.66737 0.00023 279.993 0.975 527.12 0.064
0.33265 0.66737 0.00023 284.995 3.998 534.47 0.060
0.33265 0.66737 0.00023 289.998 7.035 541.78 0.057
0.33265 0.66737 0.00023 294.994 10.056 548.85 0.055
0.33265 0.66737 0.00023 299.996 13.128 556.12 0.053
0.33265 0.66737 0.00023 304.995 16.175 563.14 0.051
0.33265 0.66737 0.00023 309.997 19.195 569.83 0.049
0.33265 0.66737 0.00023 314.993 22.200 576.33 0.048
0.33265 0.66737 0.00023 320.003 25.195 582.67 0.046
0.33265 0.66737 0.00023 325.007 28.171 588.82 0.045
0.33265 0.66737 0.00023 329.999 31.120 594.79 0.044
0.33265 0.66737 0.00023 335.002 34.026 600.43 0.043
0.33265 0.66737 0.00023 340.008 36.936 606.06 0.043
0.33265 0.66737 0.00023 345.013 39.848 611.67 0.042
0.33265 0.66737 0.00023 284.994 0.925 505.60 0.069
0.33265 0.66737 0.00023 289.997 3.800 513.12 0.065
0.33265 0.66737 0.00023 294.993 6.684 520.55 0.061
0.33265 0.66737 0.00023 299.994 9.524 527.43 0.059
0.33265 0.66737 0.00023 304.994 12.394 534.42 0.056
0.33265 0.66737 0.00023 309.997 15.271 541.34 0.054
0.33265 0.66737 0.00023 314.992 18.133 548.04 0.052
0.33265 0.66737 0.00023 320.002 20.996 554.62 0.050
0.33265 0.66737 0.00023 325.008 23.843 561.00 0.049
0.33265 0.66737 0.00023 329.999 26.667 567.19 0.047
0.33265 0.66737 0.00023 335.005 29.464 573.11 0.046
0.33265 0.66737 0.00023 340.007 32.254 578.94 0.045
0.33265 0.66737 0.00023 345.013 35.038 584.69 0.044
0.33265 0.66737 0.00023 289.996 0.986 485.10 0.074
0.33265 0.66737 0.00023 294.993 3.735 492.94 0.070
0.33265 0.66737 0.00023 299.993 6.490 500.58 0.066
0.33265 0.66737 0.00023 304.994 9.299 508.47 0.062
0.33265 0.66737 0.00023 309.996 12.075 515.88 0.059
0.33265 0.66737 0.00023 314.992 14.830 522.96 0.057
0.33265 0.66737 0.00023 320.002 17.582 529.82 0.055
0.33265 0.66737 0.00023 325.007 20.318 536.45 0.053
0.33265 0.66737 0.00023 329.999 23.036 542.79 0.051
0.33265 0.66737 0.00023 335.001 25.715 548.91 0.049
0.33265 0.66737 0.00023 340.008 28.405 554.95 0.048
0.33265 0.66737 0.00023 345.012 31.087 560.88 0.047
0.33265 0.66737 0.00023 294.991 1.091 465.10 0.081
0.33265 0.66737 0.00023 299.993 3.721 473.25 0.075
0.33265 0.66737 0.00023 304.992 6.347 481.07 0.071
0.33265 0.66737 0.00023 309.995 8.983 488.72 0.067
0.33265 0.66737 0.00023 314.991 11.611 496.09 0.063
0.33265 0.66737 0.00023 320.001 14.242 503.27 0.060
0.33265 0.66737 0.00023 325.006 16.854 510.15 0.058
0.33265 0.66737 0.00023 330.000 19.503 517.17 0.056
0.33265 0.66737 0.00023 335.002 22.092 523.63 0.053
0.33265 0.66737 0.00023 340.006 24.669 529.88 0.052
0.33265 0.66737 0.00023 345.012 27.238 535.98 0.050
0.33265 0.66737 0.00023 299.992 1.009 442.88 0.089
0.33265 0.66737 0.00023 304.993 3.494 451.20 0.083
0.33265 0.66737 0.00023 309.995 5.961 459.03 0.077
0.33265 0.66737 0.00023 314.990 8.434 466.60 0.073
0.33265 0.66737 0.00023 320.000 10.921 474.06 0.069
0.33265 0.66737 0.00023 325.007 13.407 481.32 0.065
0.33265 0.66737 0.00023 329.997 15.871 488.25 0.062
0.33265 0.66737 0.00023 335.003 18.295 494.68 0.060
0.33265 0.66737 0.00023 340.007 20.733 501.07 0.057
0.33265 0.66737 0.00023 345.012 23.173 507.39 0.055
0.33265 0.66737 0.00023 304.990 1.109 422.59 0.098
0.33265 0.66737 0.00023 309.994 3.483 431.35 0.091
0.33265 0.66737 0.00023 314.990 5.860 439.72 0.084
0.33265 0.66737 0.00023 320.000 8.241 447.73 0.078
0.33265 0.66737 0.00023 325.007 10.617 455.41 0.074
0.33265 0.66737 0.00023 329.996 12.978 462.75 0.070
0.33265 0.66737 0.00023 335.001 15.291 469.45 0.066
0.33265 0.66737 0.00023 340.007 17.608 475.99 0.063
0.33265 0.66737 0.00023 345.012 19.938 482.52 0.061
0.33265 0.66737 0.00023 309.994 1.305 403.55 0.108
0.33265 0.66737 0.00023 314.991 3.546 412.37 0.099
0.33265 0.66737 0.00023 320.000 5.801 420.82 0.092
0.33265 0.66737 0.00023 325.008 8.053 428.88 0.085
0.33265 0.66737 0.00023 329.997 10.294 436.56 0.080
0.33265 0.66737 0.00023 335.002 12.528 443.85 0.075
0.33265 0.66737 0.00023 340.006 14.762 450.93 0.071
0.33265 0.66737 0.00023 345.012 16.994 457.79 0.068
0.33265 0.66737 0.00023 314.988 1.411 383.28 0.121
0.33265 0.66737 0.00023 319.999 3.535 392.36 0.110
0.33265 0.66737 0.00023 325.006 5.662 400.95 0.101
0.33265 0.66737 0.00023 329.998 7.782 409.07 0.094
0.33265 0.66737 0.00023 335.001 9.886 416.62 0.087
0.33265 0.66737 0.00023 340.007 12.002 424.04 0.082
0.33265 0.66737 0.00023 345.013 14.117 431.21 0.077
0.33265 0.66737 0.00023 319.999 1.467 361.90 0.138
0.33265 0.66737 0.00023 325.005 3.458 371.11 0.125
0.33265 0.66737 0.00023 329.997 5.448 379.87 0.114
0.33265 0.66737 0.00023 335.004 7.431 387.97 0.105
0.33265 0.66737 0.00023 340.005 9.423 395.78 0.097
0.33265 0.66737 0.00023 345.012 11.417 403.31 0.090
0.33265 0.66737 0.00023 325.005 1.545 340.60 0.159
0.33265 0.66737 0.00023 329.996 3.405 350.07 0.143
0.33265 0.66737 0.00023 335.002 5.258 358.70 0.129
0.33265 0.66737 0.00023 340.007 7.124 367.01 0.118
0.33265 0.66737 0.00023 345.012 8.997 374.99 0.108
0.33265 0.66737 0.00023 329.997 1.695 320.21 0.184
0.33265 0.66737 0.00023 335.001 3.431 329.77 0.163
0.33265 0.66737 0.00023 340.006 5.178 338.76 0.146
0.33265 0.66737 0.00023 345.012 6.933 347.28 0.133
0.33265 0.66737 0.00023 335.000 1.674 295.57 0.224
0.33265 0.66737 0.00023 340.006 3.281 305.80 0.196
0.33265 0.66737 0.00023 345.013 4.898 315.09 0.173
0.33265 0.66737 0.00023 340.006 1.985 278.05 0.258
0.33265 0.66737 0.00023 345.012 3.488 288.00 0.224
0.33265 0.66737 0.00023 345.012 2.126 255.72 0.317
0.66803 0.33197 0.00023 230.003 0.053 779.72 0.041
0.66803 0.33197 0.00023 235.014 0.063 757.30 0.041
0.66803 0.33197 0.00023 239.996 0.074 734.91 0.041
0.66803 0.33197 0.00023 245.001 0.088 712.53 0.042
0.66803 0.33197 0.00023 250.004 0.107 690.31 0.044
0.66803 0.33197 0.00023 254.994 0.129 668.28 0.047
0.66803 0.33197 0.00023 259.987 0.152 646.36 0.048
0.66803 0.33197 0.00023 269.988 0.213 602.62 0.053
0.66803 0.33197 0.00023 274.996 0.253 580.89 0.057
0.66803 0.33197 0.00023 279.999 0.298 559.19 0.060
0.66803 0.33197 0.00023 285.001 0.347 537.52 0.065
0.66803 0.33197 0.00023 290.003 0.406 515.85 0.070
0.66803 0.33197 0.00023 235.009 0.447 759.58 0.044
0.66803 0.33197 0.00023 240.003 0.452 737.64 0.043
0.66803 0.33197 0.00023 240.003 0.455 737.19 0.042
0.66803 0.33197 0.00023 245.005 0.462 715.20 0.042
0.66803 0.33197 0.00023 250.002 0.465 693.13 0.044
0.66803 0.33197 0.00023 254.987 0.469 670.84 0.047
0.66803 0.33197 0.00023 259.986 0.475 648.96 0.048
0.66803 0.33197 0.00023 269.990 1.033 609.66 0.052
0.66803 0.33197 0.00023 274.995 4.491 616.43 0.050
0.66803 0.33197 0.00023 280.000 8.049 623.90 0.048
0.66803 0.33197 0.00023 285.001 11.526 630.69 0.047
0.66803 0.33197 0.00023 290.003 14.982 637.28 0.046
0.66803 0.33197 0.00023 294.998 18.419 643.73 0.044
0.66803 0.33197 0.00023 299.999 21.844 650.05 0.043
0.66803 0.33197 0.00023 304.997 25.231 656.12 0.042
0.66803 0.33197 0.00023 309.999 28.622 662.19 0.042
0.66803 0.33197 0.00023 314.995 31.989 668.12 0.041
0.66803 0.33197 0.00023 320.004 35.312 673.76 0.040
0.66803 0.33197 0.00023 320.005 35.204 673.17 0.040
0.66803 0.33197 0.00023 325.009 38.483 678.61 0.040
0.66803 0.33197 0.00023 330.000 41.708 683.81 0.039
0.66803 0.33197 0.00023 335.002 44.866 688.64 0.039
0.66803 0.33197 0.00023 340.007 48.022 693.49 0.038
0.66803 0.33197 0.00023 274.992 1.213 589.52 0.055
0.66803 0.33197 0.00023 279.997 4.543 596.58 0.053
0.66803 0.33197 0.00023 284.999 7.874 603.58 0.051
0.66803 0.33197 0.00023 290.001 11.198 610.44 0.049
0.66803 0.33197 0.00023 294.995 14.510 617.16 0.048
0.66803 0.33197 0.00023 299.999 17.813 623.75 0.046
0.66803 0.33197 0.00023 304.996 21.164 630.60 0.045
0.66803 0.33197 0.00023 309.999 24.461 637.03 0.044
0.66803 0.33197 0.00023 314.994 27.724 643.24 0.043
0.66803 0.33197 0.00023 320.002 30.973 649.28 0.042
0.66803 0.33197 0.00023 325.009 34.192 655.13 0.041
0.66803 0.33197 0.00023 330.000 37.386 660.86 0.041
0.66803 0.33197 0.00023 335.003 40.524 666.24 0.040
0.66803 0.33197 0.00023 340.008 43.670 671.65 0.039
0.66803 0.33197 0.00023 345.013 46.803 677.00 0.039
0.66803 0.33197 0.00023 279.994 1.084 566.73 0.059
0.66803 0.33197 0.00023 284.996 4.255 573.96 0.056
0.66803 0.33197 0.00023 289.999 7.438 581.18 0.054
0.66803 0.33197 0.00023 294.993 10.579 587.99 0.052
0.66803 0.33197 0.00023 299.995 13.705 594.56 0.050
0.66803 0.33197 0.00023 304.995 16.862 601.31 0.048
0.66803 0.33197 0.00023 309.998 20.016 607.96 0.047
0.66803 0.33197 0.00023 314.992 23.151 614.44 0.046
0.66803 0.33197 0.00023 320.003 26.278 620.77 0.045
0.66803 0.33197 0.00023 325.008 29.384 626.92 0.044
0.66803 0.33197 0.00023 329.999 32.463 632.91 0.043
0.66803 0.33197 0.00023 335.003 35.506 638.62 0.042
0.66803 0.33197 0.00023 340.006 38.543 644.27 0.041
0.66803 0.33197 0.00023 345.012 41.571 649.86 0.040
0.66803 0.33197 0.00023 284.994 1.314 547.20 0.062
0.66803 0.33197 0.00023 289.997 4.365 554.74 0.059
0.66803 0.33197 0.00023 294.993 7.420 562.17 0.056
0.66803 0.33197 0.00023 299.995 10.466 569.36 0.054
0.66803 0.33197 0.00023 304.994 13.507 576.39 0.052
0.66803 0.33197 0.00023 309.998 16.549 583.31 0.050
0.66803 0.33197 0.00023 314.991 19.574 590.05 0.049
0.66803 0.33197 0.00023 320.003 22.645 596.98 0.047
0.66803 0.33197 0.00023 325.008 25.638 603.29 0.046
0.66803 0.33197 0.00023 329.999 28.613 609.46 0.045
0.66803 0.33197 0.00023 335.003 31.531 615.19 0.044
0.66803 0.33197 0.00023 340.007 34.458 620.96 0.043
0.66803 0.33197 0.00023 345.012 37.380 626.67 0.042
0.66803 0.33197 0.00023 289.995 1.137 523.75 0.068
0.66803 0.33197 0.00023 294.992 3.997 531.14 0.064
0.66803 0.33197 0.00023 299.994 6.895 538.71 0.061
0.66803 0.33197 0.00023 304.993 9.787 546.05 0.058
0.66803 0.33197 0.00023 309.995 12.667 553.14 0.056
0.66803 0.33197 0.00023 314.992 15.528 559.98 0.054
0.66803 0.33197 0.00023 320.001 18.364 566.48 0.052
0.66803 0.33197 0.00023 325.007 21.179 572.77 0.050
0.66803 0.33197 0.00023 329.999 23.976 578.90 0.049
0.66803 0.33197 0.00023 335.002 26.756 584.82 0.047
0.66803 0.33197 0.00023 340.007 29.549 590.79 0.046
0.66803 0.33197 0.00023 345.012 32.341 596.71 0.045
0.66803 0.33197 0.00023 294.991 1.279 503.42 0.073
0.66803 0.33197 0.00023 299.993 4.055 511.48 0.068
0.66803 0.33197 0.00023 304.993 6.835 519.32 0.065
0.66803 0.33197 0.00023 309.995 9.617 526.94 0.061
0.66803 0.33197 0.00023 314.989 12.347 533.99 0.059
0.66803 0.33197 0.00023 320.002 15.098 540.97 0.056
0.66803 0.33197 0.00023 325.007 17.854 547.90 0.054
0.66803 0.33197 0.00023 329.998 20.587 554.59 0.052
0.66803 0.33197 0.00023 335.002 23.303 561.00 0.051
0.66803 0.33197 0.00023 340.007 26.013 567.28 0.049
0.66803 0.33197 0.00023 345.012 28.714 573.45 0.048
0.66803 0.33197 0.00023 299.992 1.292 481.62 0.079
0.66803 0.33197 0.00023 304.992 3.994 490.59 0.074
0.66803 0.33197 0.00023 309.995 6.699 499.19 0.069
0.66803 0.33197 0.00023 314.991 9.396 507.42 0.066
0.66803 0.33197 0.00023 320.002 12.108 515.43 0.062
0.66803 0.33197 0.00023 325.006 14.789 523.00 0.059
0.66803 0.33197 0.00023 329.998 17.455 530.26 0.057
0.66803 0.33197 0.00023 335.002 20.098 537.17 0.055
0.66803 0.33197 0.00023 340.008 22.742 543.94 0.053
0.66803 0.33197 0.00023 345.012 25.378 550.54 0.051
0.66803 0.33197 0.00023 304.991 1.176 458.03 0.088
0.66803 0.33197 0.00023 309.995 3.732 467.27 0.081
0.66803 0.33197 0.00023 314.989 6.283 476.05 0.076
0.66803 0.33197 0.00023 320.000 8.832 484.35 0.071
0.66803 0.33197 0.00023 325.006 11.370 492.28 0.068
0.66803 0.33197 0.00023 329.998 13.920 500.10 0.064
0.66803 0.33197 0.00023 335.003 16.403 507.12 0.061
0.66803 0.33197 0.00023 340.008 18.918 514.18 0.059
0.66803 0.33197 0.00023 345.013 21.422 521.04 0.056
0.66803 0.33197 0.00023 309.993 1.287 437.02 0.097
0.66803 0.33197 0.00023 314.990 3.694 446.31 0.089
0.66803 0.33197 0.00023 320.001 6.108 455.14 0.083
0.66803 0.33197 0.00023 325.006 8.485 463.18 0.078
0.66803 0.33197 0.00023 329.998 10.848 470.83 0.073
0.66803 0.33197 0.00023 335.001 13.187 478.01 0.070
0.66803 0.33197 0.00023 340.006 15.524 484.95 0.066
0.66803 0.33197 0.00023 345.012 17.878 491.88 0.063
0.66803 0.33197 0.00023 314.988 1.421 416.15 0.108
0.66803 0.33197 0.00023 319.999 3.707 425.71 0.099
0.66803 0.33197 0.00023 325.004 5.990 434.69 0.092
0.66803 0.33197 0.00023 329.997 8.262 443.16 0.085
0.66803 0.33197 0.00023 335.002 10.522 451.08 0.080
0.66803 0.33197 0.00023 340.008 12.787 458.77 0.075
0.66803 0.33197 0.00023 345.012 15.055 466.24 0.071
0.66803 0.33197 0.00023 319.999 1.571 395.33 0.121
0.66803 0.33197 0.00023 325.006 3.713 404.91 0.110
0.66803 0.33197 0.00023 329.997 5.840 413.74 0.101
0.66803 0.33197 0.00023 335.001 7.947 421.83 0.094
0.66803 0.33197 0.00023 340.007 10.060 429.66 0.088
0.66803 0.33197 0.00023 345.013 12.157 437.02 0.083
0.66803 0.33197 0.00023 325.004 1.528 371.16 0.139
0.66803 0.33197 0.00023 329.996 3.533 381.13 0.126
0.66803 0.33197 0.00023 335.002 5.533 390.25 0.115
0.66803 0.33197 0.00023 340.007 7.545 399.01 0.106
0.66803 0.33197 0.00023 345.013 9.561 407.38 0.098
0.66803 0.33197 0.00023 329.997 1.761 351.24 0.158
0.66803 0.33197 0.00023 335.001 3.610 360.73 0.143
0.66803 0.33197 0.00023 340.007 5.462 369.61 0.130
0.66803 0.33197 0.00023 345.012 7.292 377.62 0.120
0.66803 0.33197 0.00023 335.000 1.723 325.61 0.191
0.66803 0.33197 0.00023 340.006 3.470 336.18 0.169
0.66803 0.33197 0.00023 345.012 5.221 345.86 0.151
0.66803 0.33197 0.00023 340.005 2.029 306.65 0.220
0.66803 0.33197 0.00023 345.012 3.661 317.29 0.193
0.66803 0.33197 0.00023 345.013 1.861 275.26 0.292

Compositions listed (x1, x2) and composition standard uncertainty (uc(x1)) are mole fractions. The standard uncertainties for temperature (T) and pressure (p) are uc(T) = 0.004 and uc(p) = 0.014 MPa, respectively. Speed of sound values listed (w) are averaged from up to twelve measurements at each state point. Relative combined expanded speed of sound uncertainties, Uc(w), are determined with a coverage factor k = 2, and include effects of composition, temperature, pressure, time delay between echo arrivals, and path length calibration as described in detail elsewhere [3, 4, 14]. Lines in the table separate the pseudoisochores

3.2. Comparison to REFPROP Mixture Models

Figure 2a to f are deviation graphs comparing the averaged speed of sound data listed in Tables 3, 4 and 5 to the current REFPROP [6] mixture models. Dashed lines in each figure are smoothed curves of the relative combined expanded speed of sound uncertainty of each measurement, which was described previously [3, 4]; these increase as the magnitude of the speed of sound decreases, and as the system approaches the blend’s mixture critical point. The average absolute deviation, ΔAAD, used to characterize the overall performance of each mixture model, is defined by

ΔAAD=1001Ni=0N|wi,expwi,calcwi,exp|, (1)

where wi,exp is an experimental speed of sound value, wi,calc is a calculated speed of sound value, and N is the number of data points evaluated. Additional statistical measures used to assess the present mixture models are the bias, Δbias, given by Eq. 2, and the maximum deviation, Δmax, given by Eq. 3. Table 6 lists ΔAAD, Δbias, and Δmax for each mixture studied.

Fig. 2.

Fig. 2

Deviation graphs comparing experimental speed of sound values, wexp, to speed of sound values calculated using REFPROP [6] mixture models that incorporate pure-fluid EOS [711] and fitted binary interaction parameters [12, 13], wcalc, as a function of wexp. Dashed lines represent the experimental uncertainty of the speed of sound data as a function of the speed of sound. The systems and molar compositions are (a) R-125/1234yf (0.33351/0.66649), (b) R-125/1234yf (0.66643/0.33357), (c) R-1234yf/152a (0.33342/0.66658), (d) R-1234yf/152a (0.66526/0.33474), (e) R-1234ze(E)/227ea (0.33265/0.66735), and (f) R-1234ze(E)/227ea (0.66803/0.33197). Comparisons are shown at temperatures, Inline graphic, 230 K; Inline graphic, 235 K; Inline graphic, 240 K; Inline graphic, 245 K; Inline graphic, 250 K; Inline graphic, 255 K; Inline graphic, 260 K; Inline graphic, 265 K; Inline graphic, 270 K; Inline graphic, 275 K; Inline graphic, 280 K; Inline graphic, 285 K; Inline graphic, 290 K; Inline graphic, 295 K; Inline graphic, 300 K; Inline graphic, 305 K; Inline graphic, 310 K; Inline graphic, 315 K; Inline graphic, 320 K; Inline graphic, 325 K; Inline graphic, 330 K; Inline graphic, 335 K; Inline graphic, 340 K; and Inline graphic, 345 K (Color figure online)

Table 6.

Statistical measures used to evaluate present REFPROP [6] mixture models

Mixture Composition/mole frac ΔAAD/% Δbias/% Δmax/%

R-125/1234yf (0.33351/0.66649) 0.27 − 0.27 0.68
R-125/1234yf (0.66643/0.33357) 0.15 − 0.12 0.31
R-1234yf/152a (0.33342/0.66658) 0.13  0.08 0.28
R-1234yf/152a (0.66526/0.33474) 0.10  0.08 0.18
R-1234ze(E)/227ea (0.33265/0.66735) 0.62 − 0.62 2.48
R-1234ze(E)/227ea (0.66803/0.33197) 0.94 − 0.94 3.57

The average absolute deviation (ΔAAD), bias (Δbias), and maximum deviation (Δmax) defined by Eqs. 1–3 are listed, respectively

Δbias=1001Ni=0Nwi,expwi,calcwi,exp (2)
Δmax=max(100|wi,expwi,calcwi,exp|) (3)

The ΔAAD values vary from 0.10 % to 0.27 % for the R-125/1234yf and R-1234yf/152a mixtures. However, the ΔAAD values for the R-1234ze(E)/227ea mixtures are significantly greater, ranging from 0.62 % to 0.94 %. The maximum deviation ranges from 0.18 % to 0.68 % for the R-125/1234yf and R-1234yf/152a mixtures and as high as 3.57 % for the R-1234ze(E)/227ea mixtures. Figure 2a and b shows that the current REFPROP6 models calculate speed of sound values that are slightly higher (Δbias of − 0.12 % to − 0.27 %) than the reported experimental data for R-125/1234yf mixtures and as shown in Fig. 2c and b slightly lower speed of sound values (Δbias of 0.08 %) for the R-1234yf/152a mixtures. This shows that the current REFPROP mixture models for R-125/1234yf and R-1234yf/152a mixtures only require slight adjustments to accurately represent the blends respective speed of sounds. However, as shown in Fig. 2e and f, the current REFPROP speed of sound calculations for R-1234ze(E)/227ea are substantially higher (Δbias of − 0.62 % to − 0.94 %) than the experimental values reported here. The greater deviations seen with the R-1234ze(E)/227ea mixtures are not unexpected since (1) as shown by McLinden and Perkins [14] and Bell [5] the current EOS for pure R-1234ze(E) requires further adjustments to accurately match experimental speed of sound data, and (2) no binary interaction parameters for the R-1234ze(E)/227ea system exist, and therefore, parameters for the chemically similar system R-1234yf/227ea [12] were used.

4. Conclusions

The data reported in the present study expand on a larger project at NIST providing bubble point, speed of sound, and density data to improve the available models for refrigerant mixtures in REFPROP. The data reported in this study were used to test current mixture models included in REFPROP, which are based on the most recent pure-fluid equations of state [711] and available binary interaction parameters [12, 13]. Comparisons of the current REFPROP mixture models for R-125/1234yf and R-1234yf/152a show that only minor adjustments may be needed to provide an accurate representation of the experimental speed of sound data. However, greater adjustments are required to improve the model for the R-1234ze(E)/227ea system, which is currently based on (1) an EOS for pure R-1234ze(E) that requires further adjustments to accurately reflect experimental speed of sound data [5, 14] and (2) binary interaction parameters for the R-1234yf/227ea system [12]. The speed of sound data from the present study along with bubble point and density data from our group will be used to further improve refrigerant mixture models which will be included in future versions of REFPROP.

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Acknowledgements

We thank Megan Harries and Jason Widegren for providing analysis of the pure fluids used to prepare the binary mixtures studied in this work, Stephanie Outcalt for degassing the pure refrigerant samples, Mark McLinden for his guidance in preparing the gas mixtures for the speed of sound measurements and technical discussions pertinent to this work, Ian Bell for his helpful technical discussions pertaining to the Helmholtz-energy-explicit EOS, and Eric Lemmon and Ryo Akasaka for providing the fluid file for the R-1234yf EOS. We gratefully acknowledge the support of the U.S. Department of Energy, Building Technologies Office under Agreement 892434–19-S-EE000031.

Footnotes

Commercial equipment, instruments, or materials are identified only to adequately specify certain procedures. Such identification does not imply recommendation or endorsement by the National Institute of Standards and Technology, nor does it imply that the identified products are necessarily the best available for the purpose. Contribution of the National Institute of Standards and Technology; not subject to copyright in the United States.

Supplementary Information The online version contains supplementary material available at https://doi.org/10.1007/s10765-022-03052-7.

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