Vapor Pressure Measurement of Two Quaternary Systems LiBr +


Apr 1, 2014 - Vapor Pressure Measurement of Two Quaternary Systems LiBr +. LiNO3 + LiCl + H2O and LiBr + LiCl + 1,3-Propanediol + H2O. Xizhuo Jiang,...
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Vapor Pressure Measurement of Two Quaternary Systems LiBr + LiNO3 + LiCl + H2O and LiBr + LiCl + 1,3-Propanediol + H2O Xizhuo Jiang,† Wenjie Xiong,‡ Yun Li,‡ Danxing Zheng,‡ Xiao Wang,† and Lin Shi*,† †

Key Laboratory for Thermal Science and Power Engineering of Ministry of Education, Department of Thermal Engineering, Tsinghua University, Beijing 100084, P. R. China ‡ College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, P. R. China ABSTRACT: This research introduced two new absorption working pairs which have better energy storage performance than LiBr + H2O and lower cost than other working pairs in literature. The two working pairs are both quaternary systems: LiBr + LiNO3 + LiCl + H2O and LiBr + LiCl + 1,3-propanediol + H2O. Vapor pressures of the two quaternary systems were measured with the boiling point method at temperatures from (318.07 to 443.02) K and (324.78 to 419.40) K, respectively, with the both mass fractions of absorbent species from 0.40 to 0.65. The experimental data agree well with the calculated data from the Antoinetype equation. Compared with traditional working fluids of absorption cycle and ionic liquids, results show that the two quaternary systems studied in this work have lower vapor pressures, which will benefit energy release process in absorption energy storage/release systems. absorbed species mass fraction of 62 %.15 Organics, such as 1,3propanediol, working as additives can also contribute to the decrease of crystallization temperature of LiBr aquatic solution. Park and Kim et al. proved that two quaternary systems of LiBr + LiNO3 + 1,3-propanediol + H2O and LiBr + LiI + 1,3propanediol + H2O had lower crystallization temperatures than LiBr aquatic solution.16−18 More research about basic data of vapor pressure and crystallization should be studied. However, additives should not be expensive.19 Wang calculated costs of the mentioned working pairs and noted that using LiI as an additive would increase the cost of industrial application. Thus, LiI is not recommended as additives in spite of good performance. Considering both performance and cost, this research introduced two new working pairs, which are economical14 in the absence of LiI, and studied vapor pressures of the two working pairs to provide basic data for industrial application. The two working pairs can be used in cold generation with absorption systems as working fluid for substitution of LiBr/H2O. Moreover, these two working pairs can also be applied in absorption energy storage systems aiming at storing and releasing extra energy during cooling generation process. The first new working pair (NWF1) is composed of LiBr, LiNO3, LiCl, and water, and the mass ratio of LiBr, LiNO3, and LiCl is 5:1:2. Vapor pressures were measured at the temperature range from 318.07 K to 443.02 K and the mass ratio of all absorbed species (LiBr, LiNO3 and LiCl) from 40 % to 65 %. The second new working pair (NWF2) is composed of

1. INTRODUCTION With increasing interest in renewable energy, researches on energy storage/release systems are reactivated and have become vigorous.1−4 Multicriteria analysis proves that LiBr/ H2O as storage media is suitable on long-term solar thermal storage by absorption process in building heating5 which is commonly seen in combined cooling, heat, and power (CCHP) systems. Previous research showed that using LiBr + H2O alone in energy storage/release devices caused corrosion and crystallization at a high mass fraction.6,7 Corrosion should be prevented, but crystallization becomes new interest of researchers. Crystallization in the solution tank can increase the storage density by several times.8 However, according to current reports, only ClimateWell has dealt with crystallization during the energy storage process, and the process duration cannot be long.5 Therefore, avoiding crystallization is still a hot topic in present research. Many scientists try to improve the characters of LiBr solution by adding various additives such as lithium salt, ionic liquids, and alchohol.9−13 Wang stated that good refrigeration performance of LiBr absorption system also resulted in good energy storage/release performance. For example, low vapor pressure will benefit the energy release process. Usually, using LiNO3 as an additive will decrease the crystallization temperature and increase the vapor pressure of LiBr solution. In contrast, using LiCl as an additive will decrease the vapor pressure but increase the crystallization temperature of LiBr solution. However, adding LiI into LiBr solution will both decrease the crystallization temperature and the vapor pressure.14 Koo et al. studied a new working pair composed of LiBr, LiNO3, LiI, LiCl, and water and indicated that the crystallization temperature of the new working pair is lower than LiBr aquatic solution by about 30 °C at the © 2014 American Chemical Society

Received: January 2, 2014 Accepted: March 24, 2014 Published: April 1, 2014 1320

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0.05 K, a U-tube mercury manometer with the minimum calibration of 1 mm, and a set of vacuum system. The atmospheric pressure was measured with a calibrated barometer with minimum calibration of 0.01 kPa,20 comparable with the accuracy of the U-tube mercury manometer. Aqueous alcohol solution was used in the condenser to reach a sufficiently cooled temperature (270.15 K), so that the amount of condensed vapor can be minimized to avoid variation of initial concentrations of sample solution caused by the water evaporation in the condenser.21 2.3. Validity of the Method. The vapor pressures of pure water and NaCl aqueous solution (with mass fraction of 0.25) were measured to verify the reliability of the experimental system used in this research. Compared with vapor pressures in previous literature,22,23 the average absolute relative deviation (ARDs) for the vapor pressure of water was 0.68 % and that for NaCl solution was 1.01 %, respectively. Therefore, the experimental system is valid and reliable and can be applied to measurements of vapor pressures of NWF1 and NWF2.

LiBr + LiCl + 1,3-propanediol and water and the mole ratio of LiBr/LiCl = 4 and mass ratio of (LiBr + LiCl)/1,3-propanediol = 4. Vapor pressures were measured at the temperature range from 324.78 K to 419.4 K and mass ratio of all absorbed species (LiBr, LiCl, and 1,3-propanediol) from 40 % to 65 %.

2. EXPERIMENTAL METHODS 2.1. Materials. Lithium bromide (w ≥ 99.9 %), lithium chloride (w ≥ 99.9 %), and lithium nitrate (w ≥ 99.9 %) were supplied by Aladdin Chemistry Co., Ltd. without further purification. 1,3-Propanediol (w ≥ 99.0 %) was supplied by Alfa Aesar, A Johnson Matthey Company. The specifications of all used chemicals are presented in Table 1. Table 1. Information of Chemicals in This Work chemical name lithium bromide lithium chloride lithium nitrate 1,3propanediol

initial mass fraction purity

purification method

final mass fraction purity

analysis method

Aladdin

0.999

none

-

-

Aladdin

0.999

none

-

-

Aladdin

0.999

none

-

-

Alfa Aesar

0.990

none

-

-

source

3. RESULTS AND DISCUSSION The vapor pressures for NWF1 were measured at temperatures from (318.07 to 443.02) K, and the mass fractions of absorbent species were from 0.40 to 0.65. Meanwhile, the vapor pressures for NWF2 were measured at temperatures from (324.78 to 419.4) K, and the mass fractions of absorbent species were from 0.40 to 0.65. The experimental results for both systems were listed in Tables 2 and 3, respectively. Moreover, the vapor pressure results were correlated with an Antoine-type equation, expressing vapor pressure as a function of temperature and concentration, as shown in eq 1.

All solutions were prepared with deionized water, which was supplied by Aladdin Chemistry Co. Ltd. The required concentrations of solution were obtained by weighing the corresponding quantity of salts on a precision balance (Mettler, AL204), with an accuracy of 0.0001 g. 2.2. Apparatus and Procedure. The boiling point method was used to measure the vapor pressures of two solutions. The experimental system of vapor pressure measurement and the operating procedures are described in detail in early literature.20,21 Moreover, this research is valid because vapor pressures of the absorbent species, which are LiBr + LiCl + LiNO3 and LiBr + LiCl + 1,3-propanediol, respectively, in this research, can be neglected compared with the vapor pressure of water. As shown in Figure 1, the system consists of an equilibrium vessel with a volume of 0.25 L, an oil bath with a magnetic stirrer, a condenser cooled by refrigerant, a temperature sensor, and a temperature transmitter calibrated within uncertainty of

4

log(p /kPa) =



∑ ⎢⎣Ai + i=0

⎤ i 1000Bi ⎥w T /K − 43.15 ⎦

(1)

In eq 1, p represents vapor pressure with the unit of kPa, T represents temperature in K, and w is the mass fraction of all the absorbent species. The parameters Ai and Bi were determined by the least-squares method, and the results are listed in Table 4. As listed in Tables 2 and 3, estimated values calculated by eq 1 are also included for NWF1 and NWF2, respectively. Also, relative deviations between calculated and experimental data are shown in Figures 2 and 3. The high deviations of NWF2 at mass fraction of 0.65 can be due to the significant vapor decreases and the high viscosity of solution. After solution boiling, the remaining solution of high viscosity will blur the vessel wall, which increases observation difficulties. Moreover, the absolute values of pressures are lower than other mass fractions, so the relative deviations seem higher. However, considering all of the experimental and calculated data, the ARDs for the vapor pressure between all experimental and theoretical values were found to be 0.68 % for NWF1 and 0.77 % for NWF2. Therefore, the experimental data agree well with calculated data. Figures 4 and 5 show that vapor pressures change with mass fractions and temperatures of NWF1 and NWF2, respectively. Pressures increase with temperatures but decrease with mass fractions, which implies that adding absorbents will help decrease vapor pressure. Figures 4 and 5 also include experimental data and theoretical fitted curves from the Antoine-type equation, and both of the figures show the goodness of fittings.

Figure 1. Schematic diagram of the measurement system for saturated vapor pressure: 1, temperature transmitter; 2, U-tube mercury manometer; 3, condenser; 4, refrigerator; 5, temperature sensor; 6, equilibrium vessel of 0.25 L; 7, oil bath; 8, magnetic stirrer; 9, pressure buffer; 10, vacuum control valve; 11, vacuum pump. 1321

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Table 2. Experimental and Calculated Vapor Pressures of the LiBr + LiNO3 + LiCl + H2O (LiBr/LiNO3/LiCl Mass Ratio = 5:1:2) System and Standard Uncertaintiesa,b T/K

p/kPa

pcal/kPa

T/K

318.07 325.49 337.73

4.07 6.08 10.57

4.08 5.97 10.75

351.85 361.05 367.35

331.45 339.45 347.15

5.60 8.53 12.53

5.69 8.58 12.48

353.25 356.55 360.95

333.60 345.53 354.28

3.47 6.13 9.07

327.74 354.25 375.07

2.13 7.47 16.93

2.14 7.34 16.82

382.72 391.13 400.65

365.23 375.29 384.2

5.87 9.07 12.93

5.81 9.08 13.18

389.95 424.04 434.29

3.466 6.127 9.05

360.28 371.01 378.85

p/kPa w = 0.4 19.73 29.20 36.93 w = 0.5 16.67 19.33 23.33 w = 0.55 11.60 18.00 24.53 w = 0.6 22.13 29.73 40.26 w = 0.65 16.67 57.33 78.39

pcal/kPa

T/K

p/kPa

pcal/kPa

19.99 29.06 37.10

377.87 387.65 396.05

54.44 76.93 101.325

54.65 76.68 101.05

16.58 19.24 23.35

372.96 379.39 382.54

38.80 49.33 55.86

38.61 49.78 56.19

11.68 18.004 24.27

385.70 399.45 410.88

31.06 49.60 72.39

31.16 49.98 72.06

22.24 29.80 40.83

411.75 422.97 431.30

57.20 80.66 101.325

57.73 80.27 101.268

16.60 56.42 78.18

436.78 443.02

83.86 101.325

84.41 101.87

a w is the mass fraction of all absorbent species. pcal is calculated pressure data from the Antoine-type equation. bStandard uncertainties u are u(T) = 0.05 K, u(w) = 0.0001, and u(p) = 0.01 kPa.

Table 3. Experimental and Calculated Vapor Pressures of LiBr + LiCl + 1,3-Propanediol + H2O (LiBr/LiCl Mole Ratio = 4, (LiBr + LiCl)/1,3-Propanediol Mass Ratio = 4) System and Standard Uncertaintiesa,b T/K

p/kPa

pcal/kPa

T/K

p/kPa

pcal/kPa

T/K

p/kPa

pcal/kPa

24.32 41.88 50.15

373.32 381.95 387.43

61.46 84.26 101.325

61.24 84.28 102.38

19.41 25.60 32.42

372.65 380.9 390.25 398.9

40.13 54.66 75.59 101.325

39.92 54.51 76.19 102.26

338.03 343.25 347.43

13.60 17.40 21.06

13.66 17.43 21.07

350.67 363.61 368.14

331.96 343.57 349.72

6.53 11.60 15.47

6.63 11.63 15.39

355 361.55 367.35

w = 0.4 24.34 42.21 50.53 w = 0.5 19.60 25.86 32.53

332.91 340.09 353.05

5.07 7.07 12.80

5.02 7.12 12.86

359.35 364.2 371.1

w = 0.55 16.80 20.66 27.06

16.84 20.58 27.10

377.7 385.88 397.46 408.63

34.93 46.80 70.26 101.325

34.88 47.06 70.22 100.86

347.41 356.31 362.95

7.73 11.47 15.33

7.65 11.43 15.21

370.05 375.93 381.9

w = 0.6 20.66 25.73 32.26

20.37 25.70 32.28

388.87 397.87 408.2 415.4

41.46 57.06 80.13 101.325

41.71 57.19 80.62 101.27

324.78 356.83 369.77

1.73 8.35 13.81

1.69 8.06 13.88

375.19 389.43 398.61

w = 0.65 17.07 29.33 41.20

17.21 29.31 40.40

405.73 414.80 419.40

52.00 70.13 80.39

51.24 68.44 78.85

a w is the mass fraction of all absorbent species. pcal is calculated pressure data from Antoine-type equation. bStandard uncertainties u are u(T) = 0.05 K, u(w) = 0.0001 and u(p) = 0.01 kPa.

Figure 6 shows comparison between vapor pressures of the two quaternary systems mentioned in this paper at different mass fractions and the LiBr + H2O system at the mass fraction of 0.5,24 which was commonly used in the real LiBr absorption cycle. Results show that quaternary systems both have lower vapor pressures than the LiBr + H2O system. Moreover, the

vapor pressures of NWF1 are lower than those of NWF2, which implies that additives of NWF1 decrease vapor pressure more significantly than NWF2 at the same mass fractions. This can be explained as principle of “Vapor Pressure Lowering”. Nonvolatile solutes added in solvents block some liquid-state water molecules to escape to vapor and result in vapor pressure 1322

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Table 4. Correlation Parameters of the Antoine-Type Equation (eq 1) for Two Quaternary Systems

application range A0 A1 A2 A3 A4 B0 B1 B2 B3 B4 ARDa for p

LiBr + LiNO3 + LiCl + H2O

LiBr + LiCl + 1,3-propanediol + H2O

0.4 ⩽ w ⩽ 0.65

0.4 ⩽ w ⩽ 0.65

−195.141498 1373.967584 −3365.708621 3498.639943 −1286.133307 −28.028900 258.713235 −909.276338 1364.626673 −743.866670 0.68 %

−219.451001 1758.356373 −5053.002353 6382.413358 −2994.266678 52.665828 −422.724940 1216.987058 −1541.193715 724.403066 0.77 %

Figure 3. Relative deviations Δp/p = (pcal − p)/pcal of the calculated pcal from the Antoine-type equation and experimental p for NWF1. □, w(LiBr + LiNO3 + LiCl) = 0.4; red ○, w(LiBr + LiNO3 + LiCl) = 0.5; blue △, w(LiBr + LiNO3 + LiCl) = 0.55; blue ▼, w(LiBr + LiNO3 + LiCl) = 0.6; pink ☆, w(LiBr + LiNO3 + LiCl) = 0.65.

ARD = 100∑Ni=1[(cali − expi)/cali]/N, where N = number of measurement points, expi = experimental value, and cali = calculated value. a

Figure 2. Relative deviations Δp/p = (pcal − p)/pcal of the calculated pcal from the Antoine-type equation and experimental p for NWF1. ■, w(LiBr + LiNO3 + LiCl) = 0.4; red ●, w(LiBr + LiNO3 + LiCl) = 0.5; blue ▲, w(LiBr + LiNO3 + LiCl) = 0.55; teal ▼, w(LiBr + LiNO3 + LiCl) = 0.6; pink ★, w(LiBr + LiNO3 + LiCl) = 0.65.

Figure 4. Vapor pressures changing with temperatures and mass fractions of NWF1 (LiBr/LiNO3/LiCl mass ratio = 5:1:2): ■, w(LiBr + LiNO3 + LiCl) = 0.4, experimental data; red ●, w(LiBr + LiNO3 + LiCl) = 0.5, experimental data; blue ▲, w(LiBr + LiNO3 + LiCl) = 0.55, experimental data; light blue ▼, w(LiBr + LiNO3 + LiCl) = 0.6, experimental data; pink ★, w(LiBr + LiNO3 + LiCl) = 0.65, experimental data; -----, calculated data from the Antoine-type equation.

declining. All solutes of NWF1 can disassociate in water, which means that n mole solutes will become 2n mole ions and anions to block water molecules to escape from liquid. In contrast, 1,3propanediol of NWF2 will still stay in molecular state when added into water, which means that n mole solutes will become less than 2n mole ions and anions. There are more ions and anions in NWF1 than in NWF2 to prevent water molecules escaping from liquid to vapor. Therefore, NWF1 has lower vapor pressures than NWF2 at the same temperatures and mass fractions. Furthermore, a comparison between vapor pressures of the two quaternary systems and LiBr/H2O was shown in Figure 6 at different absorbed species mass ratios.24 Figure 7 shows that NWF1 and NWF2 have lower vapor pressures than ionic liquids at own largest mass ratios. According to previous literature,19 low vapor pressure and wide ranges of solution mass fraction will benefit the energy release process. Moreover, additives of NWF1 and NWF2 are common drugs which cost less than both LiBr and additives of ionic liquids, so NWF1 and

NWF2 are more economical than LiBr + H2O and ionic liquids. Estimated costs of NWF1 and NWF2 with mass fractions of 55 % were both less than $60 per kilogram solution (for lab use), while LiBr solution was $75 per kilogram solution at the same mass fraction in this research. Usually, ionic liquids cost more than LiBr. Therefore, NWF1 and NWF2 will be good choices in absorption energy storage/release systems.

4. CONCLUSIONS This research introduced two new absorption working pairs which have better performance than LiBr + H2O and lower cost than other working pairs in the literature. Furthermore, the boiling point method was used to measure vapor pressures of two quaternary systems LiBr + LiNO3 + LiCl + H2O (LiBr/ 1323

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Figure 5. Vapor pressures changing with temperatures and mass fractions of NWF2 (LiBr/LiCl mole ratio = 4, (LiBr + LiCl)/1,3propanediol mass ratio = 4): □, w(LiBr + LiCl + 1,3-propanediol) = 0.4, experimental data; red ○, w(LiBr + LiCl + 1,3-propanediol) = 0.5, experimental data; blue △, w(LiBr + LiCl + 1,3-propanediol) = 0.55, experimental data; light blue ▽, (LiBr + LiCl + 1,3-propanediol) = 0.6, experimental data; pink ☆, w(LiBr + LiCl + 1,3-propanediol) = 0.65, experimental data; -----, calculated data from the Antoine-type equation.

Figure 7. Vapor pressure comparison between the two quaternary systems in this research and ionic liquid systems in literature.15 purple ◆, w(LiBr + [Dmin]BF4) = 0.57; purple ◇, w(LiBr + [Dmin]Cl) = 0.55; pink ★, w(LiBr + LiNO3 + LiCl) = 0.65; pink ☆, w(LiBr + LiCl + 1,3-propanediol) = 0.65.



AUTHOR INFORMATION

Corresponding Author

*Tel. and fax: +86-10-62787613. E-mail: [email protected] edu.cn. Funding

This work was supported by the National Basic Research Program of China (Grant No. 2010CB227305), the State Key Program of the National Natural Science Foundation of China (Grant No. 51236004) and the Science Fund for Creative Research Group (No. 51321002). Notes

The authors declare no competing financial interest.



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Figure 6. Vapor pressure comparison between the LiBr/H2O system and the two quaternary systems in this research: red ○, w(LiBr) = 0.5; blue ▲, w(LiBr + LiNO3 + LiCl) = 0.55; pink ★, w(LiBr + LiNO3 + LiCl) = 0.65; blue △, w(LiBr + LiCl + 1,3-propanediol) = 0.55; pink ★, w(LiBr + LiCl + 1,3-propanediol) = 0.65.

LiNO3/LiCl mass ratio = 5:1:2) and LiBr + LiCl + 1,3propanediol + H2O (LiBr/LiCl mole ratio = 4, (LiBr + LiCl)/ 1,3-propanediol mass ratio = 4) in the mass fractions of absorbent species range from 0.40 to 0.65 and in the temperature ranges from (318.07 to 443.02) K and (324.78 to 419.4) K, respectively. Results showed that the two quaternary systems both have lower vapor pressures than LiBr + H2O system and relative ionic liquids in the literature. Low vapor pressures will also benefit energy release process. Therefore, both the quaternary systems have potential to use in absorption energy storage/release system in CCHP systems. 1324

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