Saturated Liquid Dynamic Viscosity and Surface Tension of

Article Cite This: J. Chem. Eng. Data XXXX, XXX, XXX−XXX

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Saturated Liquid Dynamic Viscosity and Surface Tension of trans-1Chloro-3,3,3-trifluoropropene and Dodecafluoro-2-methylpentan-3one Junwei Cui, Shaomin Yan, Shengshan Bi,* and Jiangtao Wu Key Laboratory of Thermo-Fluid Science and Engineering, Ministry of Education, School of Energy and Power Engineering, Xi’an Jiaotong University, Xi’an, 710049, China ABSTRACT: A surface light scattering (SLS) method was applied to investigate the saturated liquid dynamic viscosity and surface tension of trans-1-chloro-3,3,3-trifluoropropene (R1233zd(E)) and dodecafluoro-2-methylpentan-3-one (also known as Novec1230 and Novec649) at a temperature range from 303 to 403 K and 303 to 433 K, respectively. The typical expanded uncertainty (k = 2) of the saturated liquid dynamic viscosity and surface tension is 3% and 1.5%, respectively. The liquid viscosity and surface tension were correlated with a simple polynomial equation and van der Waals equation, respectively.

of sound,5 thermal conductivity,9 the liquid viscosity,4 and surface tension.4,10 Regarding the liquid viscosity, Hulse et al.4 carried out the measurements over the temperature range from 270 to 380 K and pressure range up to 1.35 MPa. In connection with the surface tension, Hulse et al.4 and Kondou et al.10 investigated the surface tension with a differential capillary rise method from 273 to 323 K and 279 to 350 K, respectively. Regarding Novec1230, only the vapor pressure,11 density,11,12 speed of sound,11 and saturated liquid dynamic viscosity13 are available. The liquid viscosity experiments were performed by Wen et al.13 in our group over a temperature range of (243 to 373) K and pressure up to 40 MPa. For a more comprehensive knowledge of the two interesting fluids, in this work the saturated liquid viscosity and surface tension are studied by the surface light scattering (SLS) method covering a temperature range of 303 to 403 K and 303 to 433 K along the saturation line.

1. INTRODUCTION Ozone depletion and global warming caused by working fluids have attracted a worldwide concern and stimulated a search for alternatives that have low environmental impact. 1,1,1,3,3Pentafluoropropane (R245fa) is a commonly used working fluid in the Organic Rankine Cycle (ORC). However, it has a high global warming potential (GWP) of 1030 and a long lifetime of 7.7 y. trans-1-Chloro-3,3,3-trifluoropropene (R1233zd(E)) has a GWP of 7, an ozone depletion potential (ODP) of 0.00024 to 0.00034, and a relatively short atmospheric lifetime of 26 days, which make R1233zd(E) a friendly alternative to R245fa in the ORC. Eyerer et al.1 and Datla et al.2 compared the drop-in performance of R245fa and R1233zd(E) in the ORC. The results show that R1233zd(E) can be used as a substitute for R245fa in existing ORC systems and R1233zd(E) behaves better in thermal efficiencies. Dodecafluoro-2-methylpentan-3-one has also been proposed as an ORC working fluid. (It is also known by the trade names of Novec649 and Novec1230. Novec649 is used by the manufacturer for ORC applications, and Novec1230 is used for fire-suppression applications; we use “Novec1230” as a shorthand nomenclature throughout this paper.) Additionally, Novec1230 has been used as a total flooding agent for fire suppression by the U.S. Environmental Protection Agency due to its relatively low heat of vaporization, which makes it easy to transit from liquid phase to vapor phase.3 Accurate thermophysical properties which determine the heat transfer and flow process of the working fluids are necessary for their industrial use. Table 1 gives a brief literature review on the thermophysical properties of the two interesting fluids. For R1233zd(E), the investigated properties include the vapor pressure,4−6 density,4,5,7,8 ideal gas heat capacity,4 speed © XXXX American Chemical Society

2. EXPERIMENTAL SECTION 2.1. Material. R1233zd(E) was purchased from Honeywell with a declared purity of 0.999 in mass fraction. Novec1230 was obtained from Zhengzhou Alfachem Co., Ltd., and the stated mass fraction purity was more than 0.995. The complete specifications for the two samples are given in Table 2. R1233zd(E) was purified by freeze−pump−thaw cycles using liquid nitrogen and a high vacuum pump in order to get rid of the noncondensable gas. During the purification process, the pressure is less than 10 Pa with the vacuum pump. The Received: October 13, 2017 Accepted: February 9, 2018

A

DOI: 10.1021/acs.jced.7b00902 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

Journal of Chemical & Engineering Data

Article

Table 1. Literature Review Thermophysics Properties of R1233zd(E) and Novec1230a T/K

authors R1233zd(E) Hulse et al.4

Kondou et al.10 Mondéjar et al.5

Tanaka et al.7 Nicola et al.6 Perkins et al.9 Romeo et al.8 Novec1230 McLinden et al.11

Tanaka et al.12 Wen et al.13

p/MPa

points

property

method

p ρ Cpid η σ σ p ρ cs ρ p λ ρ

float technique quantum mechanical methods capillary tube method differential capillary rise method differential capillary rise method static mode two-sinker densimeter with a magnetic suspension coupling spherical acoustic resonator the isochoric methoda static vapor−liquid equilibrium (VLE) apparatus a constant-volume apparatus transient measurements hot-wire systems vibrating tube densimeter

ρ p cs ρ η

two-sinker densimeter a static technique a spherical acoustic resonator constant volume vibrating wire method

263−352 243−293 100−1000 270−380 273−323 279−350 280−438 215−444 290−420 328−443 234−375 204−453 273−333

saturated saturated 0.1−1.35 saturated saturated saturated up to 24.1 up to 2.1 gas phase up to 10 saturated 0.1−67 up to 30

16 13 11 6 3 10 23 611 155 97 81 2404 30

225−470 325−440 315−500 333−523 243−373

up to 0.085 up to up to up to

381 20 75 155 90

36 1.7 10 40

a Note: p, saturated pressure; ρ, density; Cpid, the ideal gas heat capacity; η, saturated liquid dynamic viscosity; σ, surface tension; cs, speed of sound; λ, liquid thermal conductivity.

the time-dependent intensity correlation function. The normalized intensity autocorrelation function (ACF) takes the form:

Table 2. Specifications of Chemical Samples chemical

CAS

source

R1233zd(E)

102687-65-0

Novec1230

756-13-8

Honeywell International Inc. Zhengzhou Alfachem Co., Ltd.

purity (mass fraction) 0.999 0.995

purification method

g 2(τ ) = A + B cos(ωτ + ϕ) exp( −τ /τc)

freeze− pump− thaw filtering

(1)

where A and B are experimental parameters, ω and τc represents the frequency of propagation and mean lifetime of the surface waves, the phase term ϕ largely accounts for the deviations of the spectrum from the Lorentzian form. At a given wave vector, combined with the liquid density, vapor density, and vapor viscosity, the liquid viscosity and surface tension can be simultaneously obtained by numerically solving the dispersion relation. A more comprehensive description of the fundamentals and methodological principles of SLS can be found in refs 16−18. The SLS apparatus employed in this work was described thoroughly in ref 19 and it is already used to study several refrigerants19,20 and binary mixtures.21,22 The experimental system consists of a diode-pumped solid state laser (SpectraPhysics Excelsior, 300 mW) with a wavelength of λ0 = 532 nm, a digital correlator with a single-tau structure (ALV-LinCorr) for the computation of the pseudo cross-correlation function, optical path, and experimental cell (stainless steel and equipped with quartz windows; inner diameter, 70 mm; volume, 160 cm3). The temperature of the cell is regulated through resistance heating and measured by two calibrated 100 Ω platinum resistance probes with a total uncertainty of 0.03 K. The incident angle was adjusted by an electric rotation table (DaHeng, GCD-011080) with a standard uncertainty of 0.05%. The measurements at each temperature were performed at different six angles (±3.0°, ±3.1°, ±3.2°) to guarantee no line broadening as well as correct the misalignment, and the average values were used in this work. During the experiment, the color of the laser beam in the sample and the diameter of the laser beam after the cell are always checked in order to make sure the laser heating can be neglected.

Novec1230 was filtered under room temperature by syringe filters with a pore size of 200 nm to remove the small particle and improve the signal characteristic during the SLS measurement. 2.2. Surface Light Scattering. In comparison with the conventional methods, the surface light scattering (SLS) method has the advantage of contactless measurement. The SLS method has been successfully applied to investigate the liquid viscosity and the surface tension of refrigerants,14 ionic liquids,15 and alkanes.16 Under macroscopic thermal equilibrium, there are surface waves caused by the thermal movement of molecules in the vapor−liquid interface. A thermally excited surface can be represented by a sum of Fourier components. Each Fourier component of the rough surface behaves optically as a weak phase grating and scatters a small fraction of the incident light around both the reflected and refracted beams. In the experiments of this work, the scattering light around the refracted beam is analyzed with a photon correlation spectroscopy under a heterodyne scheme for which the reference light is much stronger than the scattering light. To realize heterodyne conditions, part of the incident laser light is split by a glass plate and superimposed with the scattered light behind the sample cell. In the present case, for the liquid having a relatively low viscosity, the amplitude of the surface fluctuations decreases with time in the form of a damped oscillation. The mean decay times and the frequency of the surface fluctuations are analyzed by calculating B



Article

Table 3. Saturated Liquid Dynamic Viscosity η and Surface Tension σ of R1233zd(E) and Novec1230 under Saturation Conditions Determined by SLS Combined with Liquid Density ρ′ and Vapor Density ρ″ Reproduced According to the EOS Developed by Mondejar et al.5 and Mclinden et al.11 and Vapor Dynamic Viscosity η′ Predicted by Extended Corresponding Statesa

2.3. Data Evaluation and Uncertainty Analysis. Figure 1 shows an ACF of the scattering light from the surface wave

T K R1233zd(E) 303.14 313.15 323.19 333.18 343.16 353.19 363.15 373.14 373.17 383.15 393.17 403.15 Novec1230 303.16 313.12 313.18 323.15 333.12 343.15 353.16 363.14 373.14 383.13 393.15 403.17 413.18 423.15 433.02

Figure 1. Measurement example of a normalized experimental correlation function of the scattering light for Novec1230 at 3.0° under 303.15 K. □, experimental data; , the fit according to eq 1.

fluctuation at the surface of the Novec1230 under saturation conditions at a temperature of 303.15 K with an incident angle of 3 degrees. To get the frequency ω and the decay time τc, the ACF was fitted according to eq 1 by a nonlinear regression based on a Levenberg−Marquardt (LM) algorithm. The uncertainties (k = 2) obtained from the fit are given in Figure 1 and are below 0.6% for ω and 2.9% for τc. In all of the cases, uncertainties below 1% for ω and 3% for τc could be obtained. The uncertainty analysis of dynamic viscosity and surface tension is on the basis of the first order approximation of the dispersion relation which is described in detail in refs 16 and 17. In the error propagation, the standard deviation of the dynamic viscosity and surface tension obtained by the SLS measurements together with the liquid density, vapor density, and vapor dynamic viscosity is needed. The uncertainty of the liquid density is estimated to be 0.2%. The uncertainty of the vapor density is estimated to be 10% at a lower density region and decreasing to 1% when the reduced temperature is higher than 0.9. The uncertainty of vapor viscosity is estimated to be 10%. The typical expanded uncertainty (k = 2) of the saturated liquid dynamic viscosity and surface tension are 3% and 1.5%, respectively.

kg·m

ρ″ −3

kg·m

−3

η′

η

σ

μPa·s

μPa·s

mN·m−1

1250.6 1225.6 1199.6 1172.7 1144.5 1114.7 1083.3 1049.5 1049.4 1012.9 972.3 926.6

8.5 11.7 15.7 20.7 27.0 34.8 44.3 56.2 56.2 70.9 89.4 113.2

11.24 11.61 11.98 12.36 12.76 13.18 13.65 14.17 14.18 14.79 15.56 16.55

285.7 250.4 226.5 207.9 189.1 169.5 159.5 140.6 144.8 131.8 119.1 104.7

13.30 12.37 10.89 9.74 8.62 7.58 6.40 5.38 5.38 4.37 3.41 2.45

1587.0 1556.1 1555.9 1523.9 1490.6 1455.6 1418.9 1380.2 1338.9 1294.4 1245.6 1191.0 1128.1 1051.5 946.3

6.5 9.4 9.4 13.2 18.2 24.6 32.7 42.9 55.8 72.1 92.8 119.6 155.3 205.7 286.9

11.34 11.72 11.72 12.09 12.47 12.84 13.22 13.60 13.99 14.40 14.84 15.33 15.93 16.79 18.41

585.0 493.9 503.3 435.7 377.6 329.0 290.7 256.9 228.0 199.8 171.9 147.1 130.9 104.0 76.8

10.09 9.26 9.24 8.43 7.56 6.70 5.84 4.99 4.19 3.44 2.71 2.02 1.37 0.78 0.27

a

The combined expanded uncertainties Uc are Uc(T) = 0.03 K, the typical uncertainty for Uc(η) = 0.03·η and Uc(σ) = 0.015·σ (k = 2).

nonlinear regression based on a LM algorithm using the inverse values of the relative uncertainties of the experimental dynamic viscosity as a weighting factor. ηi (i = 0, 1, 2, 3) is the fitting parameters which are given and listed in Table 4. The temperature-dependent saturated liquid dynamic viscosity of R1233zd(E) combined with literature data is given in Figure 2. In the residual plots, the correlation eq 2 acts as a basis. The absolute maximum deviation and absolute average deviation between our experimental results and the correlation are 2.24% and 0.92%, respectively. Hulse et al.4 measured the compressed liquid dynamic viscosity of R1233zd(E) using the capillary tube method with a declared uncertainty of 1.2%. Because its condition is close to the saturation line and limited experimental data, the fitted Vogel equation given by Hulse et al.4 was directly used for the comparison. The results of Hulse et al.4 are around 30% to 55% larger compared to the dynamic viscosity of R1233zd(E) in this work. The huge deviation maybe ascribed to the systematic error of the capillary tube setup. R1233zd(E) is proposed to be an alternative for R245fa; Figure 2 also included the dynamic viscosity of R245fa which was calculated from Refprop 9.1. The

3. RESULTS AND DISCUSSIONS 3.1. Results. The experimental results for the saturated liquid dynamic viscosity η and surface tension σ of R1233zd(E) and Novec1230 determined by SLS under saturation conditions were shown in Table 3. The liquid density ρ′, vapor density ρ″ were reproduced on the basis of the equation of state (EOS),5,11 while the vapor dynamic viscosity η′ is predicted based on the extended corresponding states.23 3.2. Correlation and Discussion. For the liquid viscosity, an polynomial equation with inverse temperature η = η0 + η1T −1 + η2T −2 + η3T −3

ρ′

(2)

was adopted to represent the viscosity over the complete investigated temperature range. The correlation is fitted by a C



Article

Table 4. Fitting Coefficients of Saturated liquid Dynamic Viscosity Correlation for R1233zd(E) and Novec1230 η0

η1

η2

η3

sample

μPa·s

μPa·s·K

μPa·s·K2

μPa·s·K3

R1233zd(E) Novec1230

−3363.47 −5477.66

3.49322 × 106 5.89981 × 106

−1.21070 × 109 −2.16870 × 109

1.47604 × 1011 2.84139 × 1011

Figure 2. Temperature-dependent liquid dynamic viscosity of R1233zd(E) obtained by SLS and a comparison with reference data as well as with R245fa, R1234yf, and R1234ze(E): , the fit of R1233zd(E); -·-·-·, Hulse et al.;4 --- □, this work; the fit of R245fa;24 ▽, R1234yf;19 △, R1234ze(E).19

Figure 3. Temperature-dependent liquid dynamic viscosity of Novec1230 obtained by SLS and a comparison with reference data: , the fit; □, this work; ○, Wen et al.13

shown in Figure 3. It is in good agreement with our results, in which a maximum deviation of 2% can be found. To represent the surface tension of R1233zd(E) and Novec1230, a van der Waals-type equation was used:

viscosity of R1233zd(E) was smaller than that of R245fa, and the difference decreased from 33.8% at 303 K and got closer with increasing temperature. The dynamic viscosity is connected with the flow, heat, and mass transfer process. A small viscosity usually means a weak flow resistance, fast heat, and mass transfer coefficients. R1233zd(E) is more favorable without considering the environmental impact. 2,3,3,3-Tetrafluoroprop-1-ene (R1234yf) and trans-1,3,3,3tetrafluoropropene (R1234ze(E)) are also two kinds of lowGWP alternatives in the Organic Rankine Cycles. In view of their similar carbon numbers to that of R1233zd(E), a comparison was made for the viscosity of the three compounds which was also shown in Figure 2. R1234yf has the lowest dynamic viscosity which may be due to its spherical molecular shape, while R1233zd(E) has the highest dynamic viscosity which can be ascribed to its bigger molecular size. The saturated liquid dynamic viscosity of Novec1230 obtained from SLS together with the fits and the comparison with the literature data were plotted in Figure 3. The absolute maximum deviation and absolute average deviation between the experimental data and the fit are 4.75% and 1.09%, respectively. The big discrepancy at 433 K can be ascribed to the temperature fluctuations. Similar temperature instability at higher temperature (above 430 K) can lead to the huge density fluctuation. The scattering vector cannot be perfectly defined because of the fluctuation of the transmitted beam which leads to the increasing uncertainty of the dynamic viscosity. Wen et.al13 measured the compressed liquid dynamic viscosity of Novec1230 by the vibrating wire method with a declared uncertainty of 2%, and an equation for viscosity of Novec1230 was also developed. The viscosity equation is extrapolated to the saturation, and the results were compared to our data

σ = σ0(1 − Tr)n

(3)

where σ0 and n are the fitting parameters listed in Table 5. In eq 3, Tr (=T/Tc) is the reduced temperature; Tc is the critical Table 5. Fitting Coefficients of 3 for R1233zd(E) and Novec1230 sample R1233zd(E) Novec1230 a

TC

σ0

K

mN·m−1

n

59.317 43.655

1.2714 1.2556

a

439.60 441.81b

From Mondejar et al.5 bFrom Mclinden et al.11

temperature. The fitting procedure was the same as the dynamic viscosity fitting, a LM scheme was adopted with a weighting factor of inverse values of the relative uncertainties. The surface tension of R1233zd(E) in this work together with the literature data is plotted in Figure 4. Figure 4 also included the surface tension of R245fa calculated from NIST Refprop 9.1.24 The surface tensions of the two compounds are quite similar and the difference increase to 0.38 mN·m−1 at 360 K and up to 0.77 mN·m−1 in the critical region of R245fa. The surface tension correlation of R1233zd(E) according to eq 3 serves as a baseline in the residual plot. The absolute maximum deviation and absolute average deviation between our experimental data and the fit are 0.20 mN·m−1 and 0.05 mN· m−1. Kondou et al.10 investigated the surface tension of D



Article

Figure 4. Temperature-dependent surface tension of R1233zd(E) obtained by SLS and a comparison with reference data as well as R245fa, R1234yf, and R1234ze(E): , the fit of R1233zd(E); □, this work; -----, the fit of R245fa;24 ○, Kondou et al.;10 △, Hulse et al.;4 ◇, R1234yf;19 ▽, R1234ze(E).19

Figure 5. Temperature dependent surface tension of Novec1230 obtained by SLS. , the fit; □, this work.

between the experimental data and the correlations were mostly within the combined uncertainty. Our results were compared with the available literature. In terms of the dynamic viscosity, the discrepancies from the literature were within 2% for Novec1230. The differences of the surface tension for R1233zd(E) were mostly within 0.5 mN·m−1. The results supplement the data set of the two fluids and can be used in the industry.

R1233zd(E) using the differential capillary rise method with an estimated uncertainty of 0.2 mN·m−1. The impurity of the sample is better than 99.9% by mole. Hulse et al.4 also measured the surface tension of R1233zd(E) with the differential capillary rise method with a uncertainty of 1.0%. The declared impurity of the compound is 99% by mass. The discrepancy of the surface tension measured by Hulse et al.4 and Kondou et al.10 is larger than 2.20 mN·m−1 at 323 K. The surface tension obtained by Kondou et al.10 is always larger than our results. The maximum deviations is about 0.5 mN·m−1 at 310 K, which is beyond the combined uncertainty. The surface tension of Hulse et al.4 at 323 K is 1.95 mN·m−1 smaller than our result which also exceeds the stated uncertainty. The impurities which have a significant influence on the surface tension can be one reason for the large discrepancy. In addition, the differential capillary rise method has the limitation that the inner surface of the capillary cannot be perfectly wetted by the liquid, and actual differential capillary rise height cannot be obtained exactly due to the sharp meniscus in each capillary tube. The surface tension comparisons of R1234yf and R1234ze(E) were given in Figure 4. The surface tension of R1234ze(E) is greater than that of R1234yf because of the stronger polarity of R1234ze(E) in the trans arrangement. R1233zd(E) has the greatest surface tension may be because of its stronger interaction between different molecules. The surface tension of Novec1230 along with the fit were shown in Figure 5. The correlation was fitted by the 15 experimental data and covers the temperature range of 303 to 433 K. From the residual plot, it can be seen that the deviations are within 0.1 mN·m−1.

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AUTHOR INFORMATION

Corresponding Author

*E-mail: [email protected]. Tel.: +86-29-82663737. ORCID

Shengshan Bi: 0000-0002-6818-9124 Jiangtao Wu: 0000-0003-1123-4307 Funding

This work was supported by the National Natural Science Foundation of China (Grant No. 51776171) and the Fundamental Research Funds for the Central Universities. Notes

The authors declare no competing financial interest.

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REFERENCES

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CONCLUSIONS In this work, the saturated liquid dynamic viscosity and surface tension of R1233zd(E) and Novec1230 were measured from 303 to 403 K and 303 to 433 K, because the liquid dynamic viscosity and the surface tension data available in the literature were scarce or even absent. On the basis of the present results, a simple polynomial equation with inverse temperature and a van der Waals equation were used to represent the liquid viscosity and surface tension, respectively. The deviations E



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Saturated Liquid Dynamic Viscosity and Surface Tension of

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