Article pubs.acs.org/jced
pvT Properties of 2,3,3,3-Tetrafluoroprop-1-ene (HFO-1234yf) in the Gaseous Phase Peng Hu,*,† Xu-Dong Cai,† Long-Xiang Chen,‡ Hang Xu,† and Gang Zhao†,§ †
Department of Thermal Science and Energy Engineering, University of Science and Technology of China, Hefei 230027, China Quanzhou Institute of Equipment Manufacturing, Haixi Institutes, Chinese Academy of Sciences, Jinjiang 362200, China § Centre for Biomedical Engineering, Department of Electronic Science & Technology, University of Science and Technology of China, Hefei, 230027, China ‡
ABSTRACT: 2,3,3,3-Tetrafluoroprop-1-ene (HFO-1234yf) is considered as the promising alternative low-global warming potential refrigerant to replace HFC-134a. In this study, the gaseous pvT properties of HFO-1234yf were measured at temperatures from 252 to 345 K and pressures up to 1.91 MPa using a single-sinker densimeter. The density range is from 3.732 to 112.152 kg/m3. The standard uncertainties of the experimental data are estimated as 6 mK and 0.7 kPa for the temperature and pressure, respectively. The relative uncertainty in density is 0.014−0.034% in this study. The average absolute deviation and relative deviation of density from reported equations of state are 0.024 kg/m3 and 0.157%, respectively. A virial equation of state was developed for HFO-1234yf. The calculated results show good agreement with the experimental data.
1. INTRODUCTION Hydrofluorocarbons (HFCs) have been widely used as alternative refrigerants because of their zero ODP (ozone depletion potential). But the most of HFCs including HFC-134a, HFC143a, and HFC-125 still have GWPs (global warming potentials) higher than 150 and will be banned according to the European Union’s F-Gas Regulations.1,2 HFO-1234yf, jointly developed by Honeywell and DuPont, has a very low GWP of about 4, zero ODP, and a very short atmospheric lifetime of 0.03 years.3 Researchers have measured its saturated vapor pressure,4−8 pvT behaviors,8−12 critical parameters, and thermophysical properties in the critical region and developed equations of state for HFO-1234yf.8,9,13 However, the experimental pvT data in the gaseous phase are still very limited, especially in low density region. In this study, the measurement of gaseous pvT properties for HFO-1234yf was carried out using a singlesinker densimeter at temperatures from 252 to 345 K and pressures up to 1.91 MPa.
ρf =
(1)
where W is the weighing mass of the sinker immersed in the fluid and ms and Vs are the calibrated mass and volume of the sinker. The schematic of the densimeter in this study is shown in Figure 1, which mainly includes a comparator balance, a measuring cell, a magnetic suspension coupling (MSC), a sinker, a vacuum vessel, and an automatic controlling and measuring system. The MSC (Rubotherm Company, Germany) is used for the contactless transmission of the gravity and buoyancy force on the sinker to the balance. It consists of an electromagnet, a permanent magnet, a position sensor as Figure 2 shown. The electromagnet has a ferrite core and is attached to the under-pan weighing hook of the balance. The permanent magnet is immersed in the fluid and linked with a lifting fork to pick up the sinker for weighing. The cell is made of nonmagnetic beryllium copper alloy. There are three positions for measurement as Figure 2 shown. In the off position, the coupling system is laid down on the support without suspension. In the zero position (ZP), the permanent magnet is in a low suspension state so that it does not lift the sinker from the support. In the measuring position (MP), both the permanent magnet and the sinker are in a suspension state. In the current densimeter apparatus, a mass comparator balance (Mettler XP205DR) with a resolution of 0.01 mg is used for weighing. It has two compensating weights (Ta, 54.1230 g and Ti, 14.6328 g) with the same volume and the mass difference about 40 g, which is nearly the same with the mass of the sinker.
2. EXPERIMENTAL SECTION 2.1. Chemicals. The HFO-1234yf was provided by Honeywell with a declared purity of 99.9% in mass fraction. As for the confirmation of the reliability of the present apparatus, nitrogen was used. The information on the two samples is summarized in Table 1. The samples were used without any further purification. 2.2. Apparatus. The apparatus is a single sinker densimeter. It is based on Archimedes’ buoyancy principle and using a magnetic suspension coupling technique, which has been described in detail by Wagner and Kleinrahm.14 The density of fluid in the measuring cell can be determined by the following relation: © 2017 American Chemical Society
ms − W (T , P) Vs(T , P)
Received: May 12, 2017 Accepted: September 7, 2017 Published: September 18, 2017 3353
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Table 1. Sample Information chemical name
CAS Registry No.
source
purity
purification method
2,3,3,3-tetrafluoroprop-1-ene (HFO-1234yf) nitrogen
754-12-1 7727-37-9
Honeywell, USA Nanjing Special Gas Factory
99.9 (in mass %) 99.999 (in mole %)
none none
Figure 1. Schematic of the single-sinker densimeter. 1, vacuum vessel; 2, heat exchanger coil; 3, inner shield; 4, outer shield; 5, balance; 6, MSC control panel; 7, SPRT; 8, direct current; 9, pressure sensor; 10, data acquisition instrument; 11, computer; 12, thermostat bath; 13, vacuum pump 1; 14, vacuum pump 2; 15, sample bottle; 16−19, valves.
The Ta weight and Ti weight are alternately placed on the balance pan at ZP and MP states, respectively. In this way, the balance is operated at a nearly constant loading point, and the errors of the balance due to changes in the slope of the characteristic line can be drastically reduced.15 Therefore, eq 1 is modified to incorporate the used external weights as ρf =
ms + (m Ti − m Ta ) − (WMP − WZP) Vs
(2)
where WMP is the reading of the balance when then sinker is in the MP position; WZP is the reading of the balance when the sinker is in the ZP position. For highly accurate density measurements by means of single-sinker densimeter, the force transmission error (FTE) due to the magnetic coupling should be taken into account, which has been described in detail by Richter et al.,8 McLinden et al.,16 and Cristancho et al.17 The density of fluid is ρf =
ms + (m Ti − m Ta ) − (WMP − WZP)/α φVs
(3)
Figure 2. Schematic and positions of the magnetic suspension coupling (MSC).
where α is the balance calibration factor which can be determined by the calibration of standard weight, φ is the coupling factor which can be determined by the relation φ = [(mta − mti) + (WMP0 − WZP0)/α]ms, and the subscript “0” indicates the vacuum condition. The measuring cell is isolated from ambient conditions by a vacuum vessel. A heat exchanger coil is directly attached to the measuring cell and connected with an external thermostat bath (AC200, Thermo Scientific, USA) for temperature controlling.
Multilayer insulation (MLI) is used to reduce heat loss by thermal radiation. The temperature is measured using a standard 25 Ω platinum resistance thermometer (PT25-660-1, Thermo Sensor GmbH, Germany) with a standard uncertainty of 3 mK, which is assembled in the wall of the measuring cell. The pressure is measured using a digital quartz pressure sensor (31K-101, 0−7 MPa, Paroscientific, USA) with an uncertainty of 0.01% of full scale. The data of temperature and pressure are 3354
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Figure 3. Relative deviations of the present experimental density data from the equation of state by Span et al.18 ■, 270.1 K; ○, 298.7 K; ▲, 308.3 K; ▽, 326.8 K; ◆, 345.3 K.
Figure 5. Absolute density deviations of the present experimental density data for HFO-1234yf from the equation of state by Richter et al.8
collected by an Agilent 3458A digital multimeter. During measurement process, the temperature fluctuation is less than 5 mK within 30 min. Therefore, the uncertainties of the experimental data are estimated as 6 mK and 0.7 kPa for the temperature and pressure, respectively. According to eq 3, the density is a function of ms, Vs(T, P), WMP, WZP, WMP0, and WZP0. The error transfer formula, based on the first-order Taylor series, is used to analyze the uncertainty of the experimental density: ⎛⎛ ⎞ 2 ⎞1/2 ⎛ ∂f ⎞2 ⎛ ∂f ⎞2 ∂f u(y) = ⎜⎜⎜ ⎟ u(x1)2 + ⎜ ⎟ u(x 2)2 + ... + ⎜ ⎟ u(x1)2 ⎟⎟ ⎝ ∂x 2 ⎠ ⎝ ∂x1 ⎠ ⎝⎝ ∂x1 ⎠ ⎠
(4)
ur(y) = u(y)/y
Figure 4. Distribution of experimental pvT data for HFO-1234yf in the gaseous phase. , HFO-1234yf vapor pressure;19 ★, critical point;19 ○, Richter et al.;8 △, Di Nicola et al.;9 ◆, this work.
(5)
In this study, y is the experimental density, xi is the variable, u(y) is the uncertainty in density, and ur(y) is the relative
Table 2. Experimental pvT Dataa, Calculated Densities ρref from the Equation of State by Richter et al.,8 Deviations Δρ,b and Relative Deviations δρc of the Experimental Data from EoS, and Relative Standard Uncertainty of Experimental Density ur(ρ)d for HFO-1234yf T/K
p/MPa
ρexp/kg·m3
ρref/kg·m3
Δρ/kg·m3
δρ/%
100ur(ρ)
252.643 252.642 252.642 262.082 262.076 262.078 262.076 262.067 270.191 270.182 270.181 270.181 270.178 279.672 279.664 279.662 279.650 279.651 279.651
0.124 0.110 0.070 0.169 0.157 0.136 0.113 0.081 0.256 0.232 0.172 0.132 0.105 0.352 0.302 0.261 0.219 0.168 0.118
7.097 6.265 3.880 9.424 8.696 7.456 6.190 4.341 14.125 12.710 9.215 6.952 5.505 19.153 16.231 13.822 11.398 8.600 5.957
7.089 6.256 3.882 9.422 8.718 7.472 6.170 4.362 14.170 12.746 9.240 6.971 5.519 19.246 16.246 13.851 11.444 8.637 5.958
0.008 0.009 −0.002 0.001 −0.022 −0.017 0.020 −0.021 −0.045 −0.037 −0.025 −0.020 −0.013 −0.093 −0.015 −0.030 −0.046 −0.037 −0.001
0.109 0.137 −0.049 0.015 −0.256 −0.224 0.330 −0.479 −0.318 −0.288 −0.272 −0.281 −0.240 −0.482 −0.091 −0.214 −0.400 −0.432 −0.015
0.022 0.023 0.033 0.019 0.019 0.021 0.023 0.030 0.016 0.017 0.019 0.022 0.025 0.016 0.016 0.017 0.017 0.020 0.024
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Table 2. continued T/K
p/MPa
ρexp/kg·m3
ρref/kg·m3
Δρ/kg·m3
δρ/%
100ur(ρ)
279.640 289.175 289.172 289.183 289.172 289.181 289.182 289.191 289.190 298.633 298.633 298.632 298.633 298.631 298.633 298.640 298.644 308.142 308.143 308.143 308.144 308.132 308.131 308.128 308.125 308.126 308.119 317.633 317.633 317.632 317.631 317.644 317.645 317.656 317.657 327.252 327.252 327.251 327.252 327.263 327.263 327.260 327.266 327.274 327.271 336.668 336.665 336.667 336.666 336.674 336.672 336.671 336.671 336.668 336.676 336.667 345.744 345.741 345.746 345.752 345.752
0.075 0.502 0.433 0.344 0.279 0.223 0.186 0.143 0.084 0.647 0.599 0.419 0.363 0.312 0.249 0.204 0.134 0.741 0.608 0.551 0.517 0.460 0.367 0.282 0.242 0.188 0.125 0.892 0.613 0.514 0.418 0.351 0.202 0.166 0.116 1.152 0.825 0.597 0.522 0.463 0.372 0.299 0.235 0.153 0.097 1.683 1.254 0.873 0.693 0.667 0.618 0.501 0.424 0.321 0.237 0.110 1.910 1.557 1.229 0.886 0.739
3.732 27.523 23.141 17.869 14.228 11.205 9.245 7.017 4.052 35.336 32.147 21.272 18.154 15.415 12.098 9.779 6.319 39.419 31.080 27.714 25.797 22.624 17.655 13.311 11.284 8.693 5.711 46.934 30.022 24.547 19.560 16.204 9.037 7.365 5.083 61.545 40.447 27.809 23.936 20.996 16.570 13.167 10.227 6.549 4.113 100.038 64.685 41.236 31.586 30.331 27.852 22.051 18.450 13.728 10.013 4.549 112.152 81.658 59.662 40.193 32.609
3.759 27.565 23.186 17.898 14.222 11.220 9.261 7.011 4.059 35.369 32.187 21.293 18.188 15.443 12.117 9.799 6.327 39.481 31.118 27.743 25.813 22.645 17.679 13.322 11.295 8.702 5.696 46.953 29.978 24.551 19.566 16.208 9.039 7.367 5.092 61.612 40.444 27.812 23.949 21.013 16.586 13.187 10.250 6.569 4.137 99.984 64.695 41.235 31.571 30.274 27.796 22.049 18.441 13.728 10.005 4.547 112.200 81.717 59.650 40.190 32.682
−0.026 −0.042 −0.045 −0.029 0.005 −0.016 −0.017 0.006 −0.007 −0.033 −0.040 −0.022 −0.033 −0.028 −0.019 −0.020 −0.008 −0.063 −0.038 −0.029 −0.016 −0.021 −0.024 −0.011 −0.011 −0.010 0.015 −0.019 0.044 −0.004 −0.006 −0.004 −0.002 −0.002 −0.010 −0.067 0.003 −0.004 −0.013 −0.017 −0.017 −0.020 −0.022 −0.020 −0.024 0.054 −0.010 0.001 0.015 0.057 0.056 0.003 0.009 0.000 0.009 0.003 −0.048 −0.060 0.012 0.003 −0.073
−0.700 −0.153 −0.193 −0.161 0.037 −0.142 −0.180 0.089 −0.182 −0.094 −0.125 −0.101 −0.182 −0.182 −0.157 −0.206 −0.128 −0.158 −0.123 −0.104 −0.063 −0.091 −0.135 −0.085 −0.100 −0.109 0.254 −0.041 0.146 −0.016 −0.030 −0.027 −0.020 −0.027 −0.187 −0.109 0.007 −0.013 −0.055 −0.081 −0.099 −0.152 −0.217 −0.300 −0.568 0.054 −0.016 0.002 0.046 0.188 0.201 0.012 0.050 0.001 0.086 0.059 −0.043 −0.073 0.021 0.008 −0.223
0.034 0.015 0.015 0.016 0.016 0.018 0.019 0.022 0.032 0.015 0.015 0.015 0.016 0.016 0.017 0.019 0.023 0.015 0.015 0.015 0.015 0.015 0.016 0.017 0.018 0.019 0.025 0.015 0.015 0.015 0.015 0.016 0.019 0.021 0.027 0.014 0.015 0.015 0.015 0.015 0.016 0.017 0.018 0.023 0.031 0.014 0.014 0.015 0.015 0.015 0.015 0.015 0.016 0.017 0.018 0.029 0.014 0.014 0.014 0.015 0.015
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Table 2. continued T/K
p/MPa
ρexp/kg·m3
ρref/kg·m3
Δρ/kg·m3
δρ/%
100ur(ρ)
345.754 345.761 345.760
0.517 0.305 0.145
21.914 12.598 5.863
22.059 12.615 5.875
−0.148 −0.017 −0.013
−0.669 −0.137 −0.218
0.015 0.017 0.024
Standard uncertainties u are u(T) = 0.006 K and u(p) = 0.7 kPa. bAbsolute deviation of the experimental density from EoS is Δρ = ρexp − ρref. Relative deviation of the experimental density from EoS is δρ = 100 × (Δρ/ρref). dRelative standard uncertainty of the experimental density is ur(ρ) = u(ρexp)/ρexp. a c
Figure 6. Relative density deviations of the present experimental density data for HFO-1234yf from the equation of state by Richter et al.8
Table 3. Coefficients of the Virial Equation of State B0
B1
B2
B3
B4
0.16269981 B5
−0.63657487 C0
0.87595893 C1
−0.44078925 C2
0.04360291 C3
−0.00770065
0.00234218
−0.00613798
0.00452066
−0.00072197
standard uncertainty. The uncertainty of ms is 1 mg, the uncertainty of Vs(T, P) is 0.002 cm3, and the uncertainty of WMP, WZP, WMP0, and WZP0 are 10 μg. Thus, the relative uncertainty in density is estimated to be 0.014−0.034% in this study. 2.3. Experimental Procedure. The measurements were carried out along isotherms and arranged from the highest pressure to the lowest pressure. The cell was evacuated and filled with sample to the pressure just lower than the saturated pressure at the desired temperature. When the deviation of temperature of the measured sample varied within 5 mK for 30 min, the state of this point was considered stable, and the weighing sequence was started. After several replicate measurements were carried out at this point, the pressure was decreased by extracting a portion of the charge into a waste bottle. The measurement of the next point then commenced. The measurements comprised 11 separate fillings of HFO-1234yf for 11 isotherms in this study. The cell was evacuated between fillings and vacuum state points were measured.
nitrogen (purity of 99.999%, Nanjing Special Gas Factory, China) at temperatures from 270 to 350 K and pressures up to 5.90 MPa. The results are in good agreement with the equation of state developed by Span et al.18 The average absolute relative deviation (AARD) of the experimental data from the values calculated from the equation of state is 0.054%, and the relative deviations are shown in Figure 3. A total of 83 gaseous pvT data for HFO-1234yf were measured at temperatures from 252.64 to 345.76 K and at pressure from 0.0695 to 1.91 MPa. The density range is from 3.732 to 112.152 kg/m3. Figure 4 gives the distribution of the present data points and the data points by other authors8,9 in the T−p diagram. The data are listed in Table 2 with the deviations from the equation of state by Richter et al.8 The average absolute deviation and relative deviation of density from the equation of state by Richter et al.8 are 0.024 kg/m3 and 0.157%, respectively. The absolute deviations and relative deviations are also shown in Figures 5 and 6. A truncated virial equation of state was fitted to the data listed in Table 2 and the data by Richter et al.8 and Di Nicola et al.9 for HFO-1234yf. The equation is in the following form:
3. RESULTS AND CORRELATION To verify the accuracy of the apparatus, 25 experimental points in gaseous region along five isotherms were measured for pure 3357
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p = 1 + Bρ + Cρ2 ρR g T
Article
(6)
B = B0 + B1Tr −1 + B2 Tr−2 + B3Tr−3 + B4 Tr−6 + B5Tr−8 (7)
C = C0 + C1Tr −0.5 + C2Tr−1 + C3Tr−2
(8)
−3
where ρ is the density, kg·m ; B and C are the second and the third viral coefficients, respectively; Tr = T/TC, and the critical temperature TC is 367.85 K for HFO-1234yf;19 the gas constant Rg for HFO-1234yf is 92.91 J/K·kg. The values of Bi and Ci were determined by fitting the experimental data to the virial EoS using the least-square method. The objective function is as follows: ⎛ ρ − ρ ⎞2 exp cal ⎟ OF = ∑ ⎜⎜ ⎟ ρ ⎠ exp i=1 ⎝ N
Figure 8. Relative deviations of the experimental data from the virial EoS. ○, Richter et al.;8 △, Di Nicola et al.;9 ■, this work.
(9)
where N is the number of experimental data points and the subscript “cal” and “exp” indicate the calculated results by eq 6 and the experimental data, respectively. The coefficients of the virial equation of state are listed in Table 3. Figures 7 and 8 present the relative deviations and the
data. The average absolute relative deviations and the average absolute deviations of the present data from from the virial equation of state are 0.024% and 0.002 kg/m3, respectively.
■
AUTHOR INFORMATION
Corresponding Author
*E-mail:
[email protected] (P. Hu). ORCID
Peng Hu: 0000-0003-0173-3647 Gang Zhao: 0000-0002-0201-1825 Funding
This work is supported by the National Natural Science Foundation of China (grant no.: 51576187). Notes
The authors declare no competing financial interest.
■
REFERENCES
(1) Regulation (EC) no. 842/2006 of the European Parliament and of the Council of 17 May 2006 on Certain Fluorinated Greenhouse Gases. Official J. EU 2006 (http://eur-lex.europa.eu/legal-content/ EN/TXT/PDF/?uri=CELEX:32006R0842&from=EN). (2) Regulation (EC) no. 517/2014 of the European Parliament and of the Council of 16 April 2014 on fluorinated greenhouse gases and repealing tegulation (EC) no. 842/2006. Official J. EU 2010 (http://eur-lex.europa.eu/legal-content/EN/TXT/PDF/?uri=CELEX:32014R0517&from=EN). (3) Bobbo, S.; Zilio, C.; Scattolini, M.; Fedele, L. R1234yf as a Substitute of R134a in Automotive Air Conditioning. Solubility Measurements in Two Commercial PAG Oils. Int. J. Refrig. 2014, 40, 302−308. (4) Di Nicola, G.; Polonara, F.; Santori, G. Saturated Pressure Measurements of 2,3,3,3-tetrafluoroprop-1-ene (HFO-1234yf). J. Chem. Eng. Data 2010, 55, 201−204. (5) Fedele, L.; Bobbo, S.; Groppo, F.; Brown, J. S.; Zilio, C. Saturated Pressure Measurements of 2,3,3,3-tetrafluoroprop-1-ene (R1234yf) for Reduced Temperatures Ranging from 0.67 to 0.93. J. Chem. Eng. Data 2011, 56, 2608−2612. (6) Yang, Z.; Kou, L.; Mao, W.; Lu, J.; Zhang, W.; Lu, J. Experimental Study of Saturated Pressure Measurements for 2,3,3,3-tetrafluoropropene (HFO-1234yf) and 2-chloro-1,1,1,2-tetrafluoropropane (HCFC244bb). J. Chem. Eng. Data 2014, 59, 157−160. (7) Tanaka, K.; Higashi, Y. Thermodynamic Properties of HFO1234yf (2,3,3,3-tetrafluoropropene). Int. J. Refrig. 2010, 33, 474−479. (8) Richter, M.; Mclinden, M. O.; Lemmon, E. W. Thermodynamic Properties of 2,3,3,3-tetrafluoroprop-1-ene (R1234yf): Vapor Pressure
Figure 7. Absolute deviations of the experimental data from the virial EoS. ○, Richter et al.;8 △, Di Nicola et al.;9 ■, this work.
absolute deviations of the experimental data from eq 6. The average absolute relative deviations and the average absolute deviations of the present data from eq 6 are 0.024% and 0.002 kg/m3, respectively.
4. CONCLUSION The pvT behaviors of HFO-1234yf in the gaseous phase were measured in the temperature range from 252 to 345 K at pressures up to 1.91 MPa using a single-sinker densimeter, which was validated by measuring the pvT properties of pure nitrogen. The standard uncertainties of the experimental data are estimated as 6 mK and 0.7 kPa for the temperature and pressure, respectively. The relative uncertainty in density is 0.014−0.034% in this study. A total of 83 experimental pvT data were obtained for HFO-1234yf. The density range is from 3.732 to 112.152 kg/m3. The results were compared to the EoS by Richter et al. and were in good agreement. A truncated virial EoS for HFO-1234yf was developed to represent the experimental 3358
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