Article

pubs.acs.org/jced

Viscosities of Some Saccharides in Aqueous Solutions of Phosphate-

Based Inorganic Salts
Parampaul K. Banipal,* Neha Aggarwal, and Tarlok S. Banipal
Department of Chemistry, Guru Nanak Dev University, Amritsar 143 005, India
*
S Supporting Information

ABSTRACT: The viscosities η of some monosaccharides, their methyl- and

deoxy- derivatives, disaccharides, and trisaccharides have been measured in
(0.25, 0.5, 1.0, and 1.25) mol·kg−1 aqueous solutions of potassium phosphate
(KH2PO4) and (0.5, 1.0, 1.5, and 2.0) mol·kg−1 aqueous solutions of sodium
phosphate (NaH2PO4) and ammonium phosphate (NH4H2PO4) monobasic
salts, and potassium phosphate (K3PO4) tribasic salt over the temperature
range (288.15 to 318.15) K and at atmospheric pressure, P = 0.1 MPa. The
viscosity data have been utilized to calculate the Jones−Dole viscosity B-
coefficients and their corresponding coefficients of transfer, ΔtB. The ΔtB
values were found to be positive and their magnitudes vary depending on the
nature of solutes and cosolutes. The dB/dT coefficients and pair ηAB and triplet
ηABB interaction coefficients have also been calculated and discussed in terms of
solute−solvent/cosolute interactions. The results have been compared in
phosphate-based salts on the basis of the nature of the cation and anion.

1. INTRODUCTION salting-in and salting-out behavior, we have tried to reconcile the

Saccharides and their derivatives are renewable raw materials that
are highly important for life and energy. These play key roles in
biological phenomena including DNA and RNA fingerprinting
and engineering. Saccharides participate in many biological
processes, for example, L-fucose (deoxyhexose) residues in the
carbohydrate chains of glycoconjugates act as cell−cell
recognition sites and as important antigenic determinants such
as blood group antigens. Aqueous solutions of saccharides are
useful in several food processes such as in crystallization and
osmotic dehydration, etc.1−7 Their hydration behavior is
involved in sweet taste chemoreception and environmental
stress tolerance. Deoxy derivatives of saccharides, sugar
phosphates, sulfates, carboxylates, and amino sugars occur in
natural products. L-Rhamnose (6-deoxy mannopyranoside) is
present as glycoside in plant pigments, gums and mucilages.8−11
Viscometric properties play a key role in process design,
modeling, and evaluation. The data are quite useful in various
industrial and physicochemical processes like pump sizing,
extraction, filtration, extrusion, purification, and in the analyses of
flow conditions in food processes, that is, pasteurization,
evaporation, drying, and aseptic processing. The temperature
dependent viscosity data are also useful in determining the
molecular information, such as the pair interaction potential
function.12−16 The saccharide−metal ion interactions have great
importance in biological systems. Na+ and K+ ions are
responsible for the striking difference in the composition of
extra- and intracellular fluids in animals and sap fluids in plants.
Phosphate-based inorganic salts have stabilizing and salting-out
effects on proteins and macromolecules.5,13,17−25 Since the
charge on the anion and cation plays a determinant role in
effects of different salts on the viscometric properties of
saccharides in terms of size, charge, and ionic strength of ions
of phosphate salts.
To the best of our knowledge, the viscometric study of
saccharides and their derivatives in aqueous solutions of
phosphate salts is missing in the literature. However, the
literature of viscometric study in the binary systems that is,
(saccharides + water)10,16,19,22,26,27,29−31 and (phosphate salts +
water)5,13 is available and discussed in the present study. So, we
hereby report the viscosities of some mono-, di-, and
trisaccharides and the methyl- and deoxy-derivatives of some
monosaccharides in aqueous solutions of potassium phosphate,
sodium phosphate, and ammonium phosphate monobasic salts,
and potassium phosphate tribasic salt over the temperature range
(288.15, 298.15, 308.15, and 318.15) K and atmospheric
pressure, P = 0.1 MPa. The viscosity B-coefficients and other
parameters, such as viscosity B-coefficient of transfer, temper-
ature dependent, that is, dB/dT coefficients, and pair and triplet
interaction coefficients, were calculated and compared with the
volumetric properties reported earlier.26,27
2. EXPERIMENTAL SECTION
2.1. Materials. The provenances of chemicals along with
their abbreviations, mass-fraction purity, and CAS numbers are
given in Table 1. Highest purity grade chemicals were dried over
CaCl2(anhy) in a vacuum desiccator for 48 h at room temperature
Received: October 3, 2015
Accepted: April 12, 2016

© XXXX American Chemical Society A DOI: 10.1021/acs.jced.5b00845

J. Chem. Eng. Data XXXX, XXX, XXX−XXX
Journal of Chemical & Engineering Data Article

Table 1. Specifications of the Chemicals Used

C,H,N,S analysis
mass fraction
compound (abbreviations) [molecular formula] molar mass g·mol−1 puritya source CAS no. calculated % observed %
(+)-D-xylose (Xyl) [C5H10O5] 150.13 0.99 Sigma Chemical 58-86-6 C = 40.00 C = 39.97
Co. H = 6.71 H = 6.69
(−)-D-ribose (Rib) [C5H10O5] 150.13 0.99 Sigma Chemical 50-69-1 C = 40.00 C = 39.98
Co. H = 6.71 H = 6.69
(−)-D-fructose (Fru) [C6H12O6] 180.16 0.99 Sigma Chemical 57-48-7 C = 40.00 C = 40.02
Co. H = 6.71 H = 6.74
(+)-D-glucose (Glc) [C6H12O6] 180.16 ≥ 0.99 Sigma Chemical 50-99-7 C = 40.00 C = 40.03
Co. H = 6.71 H = 6.69
(+)-D-mannose (Man) [C6H12O6] 180.16 ≥ 0.99 Fluka 3458-28-4 C = 40.00 C = 40.03
H = 6.71 H = 6.68
2-deoxy-D-ribose (2de-Rib) [C5H10O4] 134.13 0.99 Sisco Research Lab. 533-67-5 C = 44.77 C = 44.75
H = 7.51 H = 7.54
2-deoxy-D-glucose (2de-Glc) [C6H12O5] 164.16 0.99 Sisco Research Lab. 154-17-6 C = 43.90 C = 43.88
H = 7.37 H = 7.39
6-deoxy-D-mannose (6de-Man) [C6H12O5.H2O] 182.18 0.99 Sisco Research Lab. 6155-35-7 C = 39.55 C = 39.53
H = 7.74 H = 7.77
(+)-methyl α-D-mannopyranoside (Me α-Man) 194.18 ≥ 0.99 Sigma Chemical 617-04-9 C = 43.30 C = 43.26
[C7H14O6] Co. H = 7.27 H = 7.30
(+)-methyl α-D-glucopyranoside (Me α-Glc) 194.18 ≥ 0.99 Sigma Chemical 97-30-3 C = 43.30 C = 43.27
[C7H14O6] Co. H = 7.27 H = 7.25
sucrose (Suc) [C12H22O11] 342.30 ≥ 0.99 Sigma Chemical 57-50-1 C = 42.10 C = 42.13
Co. H = 6.48 H = 6.46
(+)-cellobiose (Cel) [C12H22O11] 342.30 0.98 Sigma Chemical 528-50-7 C = 42.10 C = 42.08
Co. H = 6.48 H = 6.49
(+)-lactose monohydrate (Lac) [C12H22O11.H2O] 360.31 ≥ 0.98 Sigma Chemical 64044-51-5 C = 40.00 C = 40.03
Co. H = 6.71 H = 6.69
(+)-maltose monohydrate (Mal) [C12H22O11.H2O] 360.31 0.99 Sigma Chemical 6363-53-7 C = 40.00 C = 40.02
Co. H = 6.71 H = 6.69
(+)-melezitose (Mel) [C18H32O16] 504.48 > 0.99 Sisco Research Lab. 207511-10-2 C = 42.85 C = 42.83
H = 6.39 H = 6.36
(+)-raffinose pentahydrate (Raf) [C18H32O16.5H2O] 594.53 ≥ 0.99 Fluka 17629-30-0 C = 36.36 C = 36.34
H = 7.12 H = 7.15
potassium phosphate monobasic (KH2PO4) 136.09 ≥ 0.99 Sigma Chemical 7778-77-0
Co.
sodium phosphate monobasic (NaH2PO4) 119.98 ≥ 0.99 Sigma Chemical 7778-77-0
Co.
ammonium phosphate monobasic (NH4H2PO4) 115.03 ≥ 0.98 Sigma Chemical 7722-76-1
Co.
potassium phosphate tribasic (K3PO4) 212.27 ≥ 0.98 Sigma Chemical 7778-53-2
Co.
a
Declared by the supplier.

before use. The purity of the chemicals used was analyzed with C,
H, N, and S analysis method using FLASH 2000 Organic
Elemental Analyzer, USA. The carbon and hydrogen contents
obtained in the analysis were similar to expected values from the
molecular formula with zero percentage of nitrogen and sulfur
(Table 1). The hydrogen and oxygen percentage obtained
suggests that the samples were completely dried and the water
content was negligible for anhydrous samples. However, it
should be noted that the elemental analysis cannot reveal any
impurities with same summary chemical formula such as, for
example, isomers.
2.2. Equipment and Procedure. Ubbelohde-type capillary
viscometer was employed for measuring the viscosities of
solutions by measuring the efflux time with a digital stopwatch
(resolution of ±0.01 s) for the average of at least four flow time
readings. The viscometer was calibrated by measuring the efflux
time of water from T = (288.15 to 318.15) K. The temperature of
B DOI: 10.1021/acs.jced.5b00845
the viscometer was maintained by a constant temperature bath
(Julabo F-25) with thermal stability within ±0.01 K. Deionized
water (specific conductance <1.29 × 10−4 S·m−1) procured from
Ultra UV/UF Rions lab water system was used to prepare fresh
solutions by mass using a Mettler balance with a precision of
±0.01 mg. The viscosities for pure water are (1.1382, 0.8904,
0.7194, 0.5963) mPa·s at (288.15, 298.15, 308.15, and 318.15) K,
respectively, taken from the literature.28 The densities of
saccharides and their derivatives in water and in aqueous
KH2PO4, NaH2PO4, NH4H2PO4, and K3PO4 solutions over the
temperature range (288.15 to 318.15) K were measured using a
vibrating tube digital densimeter (Model: DMA 60/602, Anton
Paar, Austria), and the details have been discussed elsewhere.26,27
3. RESULTS AND DISCUSSION
3.1. Viscosity B-Coefficients. The viscosities η of various
saccharides and their derivatives in aqueous KH2PO4, NaH2PO4,
J. Chem. Eng. Data XXXX, XXX, XXX−XXX
Journal of Chemical & Engineering Data
NH4H2PO4, and K3PO4 solutions were obtained over the
temperature range (288.15 to 318.15) K using the expression:
η /ρ = at − b/t
where t is the efflux time; a and b are the viscometric constants; ρ
is density of solution (reported earlier26,27). The viscosity
increases with increase in the molalities of solute and cosolute
while it decreases with the rise of temperature from (288.15 to
318.15) K in all the systems studied (given as Supporting
Information in Table S1). In cases of hydrated solutes such as 6-
deoxy-D-mannose, (+)-lactose monohydrate, (+)-maltose
monohydrate and (+)-raffinose pentahydrate, the molality
corrections have been applied and the data for anhydrous
saccharides have been given in Table S1. The variation in
viscosity with molality and temperature is shown by the
representative 3-D plot of η versus molality of Glc in mB = 2.0
mol·kg−1 K3PO4(aq) at four temperatures (Figure 1).
Figure 1. Plot of viscosity η vs molality mA of (+)-D-glucose at (288.15 to
318.15) K in mB = 2.0 mol·kg−1 K3PO4(aq) solution.
The relative viscosity, ηr data were fitted to the Jones-Dole
empirical equation by least-squares method to obtain the
viscosity B-coefficients for various solutes as
ηr (ηr = η /ηo) = 1 + Bc
where η and ηo are viscosities of solution and solvent,
respectively; c is the molarity in mol·dm−3 (calculated from the
molality and density data26,27).
The viscosity B-coefficients give information about the
kosmotropic or chaotropic ability of solutes. The B-coefficients
for saccharides in water agree well with the literature
values10,16,19,22,29−31 (Table 2). The B-coefficients of studied
solutes are positive and increase in the presence of salts indicating
a kosmotropic nature of saccharides/derivatives in studied
phosphate salts. The B-coefficients also increase with the
complexity of solutes from mono- to di- to trisaccharides,
suggesting structural enhancement in the same order. In the case
of NaH2PO4, the methyl-derivatives have greater magnitudes of
B-coefficients than their respective deoxy-derivatives and
saccharides. Among di- and tri-saccharides, the B-coefficients
follow the order: Raf > Mel > Mal > Lac > Suc > Cel, indicating
that the α or β glycosidic linkage between the monomer units
result in different hydration characteristics of these saccha-
rides.15,18,21 In the cases of KH2PO4, NH4H2PO4, and K3PO4, the
B-coefficients of derivatives are less than their parent saccharides
Article
(Table 2). The size of solute molecule and their interactions with
salts result in such variations in viscometric parameters. The
nature and size of the hydrated radius of the cation or anion also
(1)
have great influences on the B-values. The PO43− anion has
higher ionic strength than H2PO4−, as a result the magnitude of
B-coefficients is quite large in the case of K3PO4 tribasic salt than
in KH2PO4, NaH2PO4, and NH4H2PO4 monobasic phosphate
salts.
The temperature dependence of B-coefficients gives better
information about the kosmo-/chaotropic effects of salts. The
negative dB/dT coefficients (Table S2) for studied solutes in all
the phosphate salts, suggest that saccharides and their derivatives
act as kosmotropes in phosphate salts, except at higher molalities
of NH4H2PO4. Moreover, the dB/dT coefficients increase with
complexity of the solutes.
The viscosity B-coefficients of transfer from water to aqueous
solutions of salts were calculated as following:
Δt B = B (in aqueous phosphate salts solutions)
− B (in water) (3)
The ΔtB values are positive (only representative plots are given
in Figure 2a−f and Figure 3a−f) and increase with increase in
concentration of salt. The ΔtB values show a leveling off effect
from mB = (0.5 to 1.0) mol·kg−1 and then start increasing
afterward in most of the studied systems. However, in the
presence of KH2PO4, the ΔtB values for Rib (Figure 2a), Glc, and
2de-Glc (Figure 2c) show linear behavior and Me α-Glc (Figure
2b) shows negative ΔtB values in mB = 0.25 mol·kg−1 KH2PO4 at
(308.15 and 318.15) K. In the presence of NaH2PO4, the ΔtB
values for Man, 6de-Man, Suc, and Lac (representative Figure
2e) increase almost linearly at all the studied concentrations. In
NH4H2PO4 also the ΔtB show a sharp and linear behavior for Me
α-Man and Mal after mB = 1.0 mol·kg−1 (representative Figure
3d). In K3PO4, the ΔtB increase systematically with increase in
the complexity of solutes. In the cases of NaH2PO4, NH4H2PO4,
and KH2PO4 the transfer values do not increase in a regular
fashion from di- to trisaccharides. The ΔtB values increase with
rise of temperature in NH4H2PO4, whereas the values decrease
with temperature in other salts. The differences in ΔtB values
among various saccharides/derivatives are due to their different
(2) stereochemistry and the nature of cosolute, that is, the size,
charge, and ionic strength of the ions of the salts. The
−CH2OCH3 and −CH3 groups introduce hydrophobicity in
the molecule leading to hydrophobic hydration and lesser
transfer values in methyl- and deoxy- derivatives of Glc and Man.
Similar behavior was observed from volumetric studies.26,27
The average Gibbs free energy of activation of a solute, Δμ1°#
for the viscous flow in a solvent has been calculated by using
Eyring simple model32 as follows:
ηo = [hNA /V1,°ϕ]exp[Δμ1° # /RT ] (4)
where NA, h, R, and T are the Avogadro’s number, Planck’s
constant, universal gas constant, and temperature, respectively;
V°1,ϕ is the average molar volume of salt solution calculated from
density data26,27 at different temperatures. The values of Δμ1°# for
water and aqueous solutions of phosphate salts are given in Table
S3 at different molalities and studied temperatures. The
activation Gibbs free energy, Δμ°2 # (Table S4) for viscous flow
of the solute in aqueous and mixed aqueous solutions is related to
the viscosity B-coefficient according to Feakins et al.33,34 as
follows:
C DOI: 10.1021/acs.jced.5b00845
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Journal of Chemical & Engineering Data Article

Table 2. Viscosity B-Coefficients of Saccharides/Derivatives in Water and in Aqueous Solutions of Phosphate-Based Cosolutes
over the Temperature Range (288.15 to 318.15) K at Pressure (p = 0.1 MPa)a
B·103/m3·mol−1
solute water mB = 0.50 1.00 1.50 2.00 water mB = 0.50 1.00 1.50 2.00
KH2PO4
T/K = 288.15 T/K = 298.15
(+)-D-xylose 0.360 0.393 0.408 0.427 0.437 0.346 0.369 0.384 0.396 0.406
0.368b 0.338b
0.371c 0.339c
0.370d 0.336d,e
(−)-D-ribose 0.338 0.375 0.388 0.407 0.428 0.314 0.340 0.353 0.372 0.386
0.331b 0.317b
0.332d 0.319c,d,e
(−)-D-fructose 0.495 0.556 0.583 0.621 0.646 0.454 0.502 0.526 0.563 0.588
0.485b 0.449b
0.482d 0.451d,g
(+)-D-glucose 0.494 0.583 0.612 0.661 0.687 0.456 0.536 0.561 0.605 0.635
0.497b 0.460b
0.493c 0.458c,g
0.498d 0.461d
0.440e
0.450h
(+)-D-mannose 0.511 0.532 0.566 0.606 0.637 0.472 0.484 0.507 0.558 0.587
0.511b 0.471b,d
0.508c,d 0.469c
2-deoxy-D-ribose 0.391 0.403 0.427 0.472 0.502 0.371 0.378 0.401 0.441 0.465
2-deoxy-D-glucose 0.453 0.475 0.499 0.544 0.574 0.431 0.446 0.469 0.510 0.534
6-deoxy-D-mannose 0.511 0.532 0.556 0.600 0.629 0.480 0.497 0.516 0.559 0.583
(+)-methyl α-D-mannopyranoside 0.543 0.554 0.574 0.614 0.641 0.517 0.519 0.537 0.575 0.601
(+)-methyl α-D-glucopyranoside 0.495 0.518 0.538 0.579 0.609 0.465 0.477 0.495 0.534 0.562
0.496d 0.465d
sucrose 1.032 1.129 1.161 1.191 1.211 0.995 1.073 1.102 1.134 1.149
1.032b 0.995b
1.036c 0.989c
1.035d 0.996d
1.031f 1.006f,g
(+)-cellobiose 0.913 1.198 1.218 1.224 1.229 0.878 1.132 1.155 1.166 1.170
0.913b 0.878b,d
0.912d 0.885f
0.901f
(+)-lactose monohydrate 1.086 1.275 1.302 1.342 1.366 1.048 1.199 1.240 1.259 1.301
1.086b 1.045b
1.090d 1.048d
1.080f
(+)-maltose monohydrate 1.128 1.312 1.362 1.401 1.421 1.091 1.251 1.292 1.333 1.361
1.128b,d 1.088b
1.127c 1.081c
1.121f 1.086d
(+)-melezitose 1.432 1.542 1.598 1.677 1.718 1.384 1.453 1.515 1.595 1.642
1.434b 1.379b
(+)-raffinose pentahydrate 1.542 1.706 1.766 1.840 1.870 1.478 1.617 1.671 1.747 1.770
1.543b,d 1.477b
1.479d
T/K = 308.15 T/K = 318.15
(+)-D-xylose 0.327 0.339 0.350 0.372 0.375 0.311 0.318 0.325 0.341 0.347
0.327b 0.311b
0.323c 0.310c
0.324d 0.309d
(−)-D-ribose 0.294 0.311 0.323 0.342 0.352 0.283 0.291 0.302 0.316 0.332
0.291b 0.282b
0.292d 0.280d
(−)-D-fructose 0.436 0.471 0.491 0.526 0.552 0.373 0.396 0.415 0.453 0.473

D DOI: 10.1021/acs.jced.5b00845
J. Chem. Eng. Data XXXX, XXX, XXX−XXX
Journal of Chemical & Engineering Data Article

Table 2. continued
B·103/m3·mol−1
solute water mB = 0.50 1.00 1.50 2.00 water mB = 0.50 1.00 1.50 2.00
T/K = 308.15 T/K = 318.15
0.422b 0.377b
0.420d 0.381d
(+)-D-glucose 0.427 0.485 0.510 0.554 0.582 0.406 0.434 0.462 0.503 0.531
0.432b 0.410b
0.436c 0.412c
0.433d 0.409d
(+)-D-mannose 0.440 0.446 0.467 0.512 0.534 0.418 0.420 0.435 0.472 0.499
0.440b 0.418b
0.444c,d 0.415c,d
2-deoxy-D-ribose 0.349 0.345 0.368 0.408 0.432 0.330 0.310 0.336 0.374 0.401
2-deoxy-D-glucose 0.407 0.413 0.435 0.475 0.499 0.384 0.386 0.402 0.438 0.466
6-deoxy-D-mannose 0.451 0.463 0.477 0.521 0.541 0.421 0.426 0.439 0.479 0.500
(+)-methyl α-D-mannopyranoside 0.491 0.483 0.503 0.541 0.560 0.466 0.448 0.469 0.507 0.525
(+)-methyl α-D-glucopyranoside 0.443 0.440 0.466 0.504 0.530 0.413 0.401 0.425 0.463 0.481
0.443d 0.412d
sucrose 0.956 1.023 1.046 1.072 1.086 0.918 0.977 0.989 1.005 1.018
0.955b 0.918b
0.952c 0.916c,d
0.960d 0.911f
0.970f
(+)-cellobiose 0.842 1.074 1.091 1.101 1.112 0.807 0.997 1.016 1.027 1.032
0.843b 0.807b,d
0.845d 0.796f
0.850f
(+)-lactose monohydrate 1.022 1.135 1.167 1.195 1.223 0.991 1.049 1.074 1.109 1.146
1.027b 0.976b
1.025d 0.980d
(+)-maltose monohydrate 1.053 1.193 1.226 1.273 1.295 1.007 1.121 1.148 1.190 1.211
1.053b 1.006b
1.049c 1.009c
1.051d 1.005d
(+)-melezitose 1.322 1.366 1.437 1.518 1.564 1.279 1.295 1.355 1.444 1.489
1.325b 1.279b
(+)-raffinose pentahydrate 1.431 1.549 1.594 1.665 1.689 1.364 1.457 1.496 1.559 1.580
1.430b 1.367b
1.428d 1.365d
NaH2PO4
T/K = 288.15 T/K= 298.15
(+)-D-xylose 0.360 0.467 0.504 0.558 0.602 0.346 0.426 0.474 0.521 0.548
(−)-D-ribose 0.338 0.455 0.499 0.542 0.594 0.314 0.409 0.452 0.494 0.539
(−)-D-fructose 0.495 0.613 0.642 0.673 0.721 0.454 0.554 0.586 0.608 0.668
(+)-D-glucose 0.494 0.643 0.681 0.709 0.839 0.456 0.583 0.621 0.663 0.761
(+)-D-mannose 0.511 0.563 0.619 0.648 0.679 0.472 0.517 0.562 0.596 0.627
2-deoxy-D-ribose 0.391 0.526 0.567 0.614 0.654 0.371 0.483 0.528 0.565 0.611
2-deoxy-D-glucose 0.453 0.607 0.643 0.690 0.756 0.431 0.555 0.591 0.626 0.680
6-deoxy-D-mannose 0.511 0.563 0.608 0.644 0.681 0.480 0.522 0.561 0.602 0.644
(+)-methyl α-D-mannopyranoside 0.543 0.711 0.791 0.848 0.916 0.517 0.658 0.714 0.766 0.852
(+)-methyl α-D-glucopyranoside 0.495 0.657 0.702 0.752 0.831 0.465 0.607 0.621 0.674 0.781
sucrose 1.032 1.185 1.296 1.383 1.501 0.995 1.121 1.232 1.321 1.414
(+)-cellobiose 0.913 1.180 1.236 1.264 1.283 0.878 1.119 1.177 1.196 1.218
(+)-lactose monohydrate 1.086 1.292 1.401 1.483 1.567 1.048 1.210 1.319 1.403 1.464
(+)-maltose monohydrate 1.128 1.372 1.498 1.566 1.646 1.091 1.283 1.407 1.470 1.552
(+)-melezitose 1.432 1.607 1.695 1.754 1.811 1.384 1.543 1.623 1.682 1.713
(+)-raffinose pentahydrate 1.542 1.774 1.889 1.948 2.028 1.478 1.688 1.778 1.834 1.887
T/K = 308.15 T/K = 318.15
(+)-D-xylose 0.327 0.392 0.432 0.480 0.516 0.311 0.354 0.383 0.418 0.464
(−)-D-ribose 0.294 0.371 0.424 0.457 0.495 0.283 0.339 0.374 0.405 0.468
(−)-D-fructose 0.436 0.521 0.546 0.579 0.637 0.373 0.446 0.469 0.497 0.563

E DOI: 10.1021/acs.jced.5b00845
J. Chem. Eng. Data XXXX, XXX, XXX−XXX
Journal of Chemical & Engineering Data Article

Table 2. continued
B·103/m3·mol−1
solute water mB = 0.50 1.00 1.50 2.00 water mB = 0.50 1.00 1.50 2.00
T/K = 308.15 T/K = 318.15
(+)-D-glucose 0.427 0.534 0.558 0.599 0.708 0.406 0.489 0.520 0.564 0.658
(+)-D-mannose 0.440 0.474 0.515 0.549 0.579 0.418 0.440 0.469 0.506 0.536
2-deoxy-D-ribose 0.349 0.444 0.486 0.528 0.558 0.330 0.397 0.439 0.484 0.514
2-deoxy-D-glucose 0.407 0.517 0.546 0.584 0.623 0.384 0.460 0.481 0.529 0.578
6-deoxy-D-mannose 0.451 0.486 0.525 0.552 0.588 0.421 0.451 0.477 0.510 0.536
(+)-methyl α-D-mannopyranoside 0.491 0.599 0.652 0.695 0.788 0.466 0.542 0.595 0.635 0.710
(+)-methyl α-D-glucopyranoside 0.443 0.561 0.583 0.624 0.713 0.413 0.509 0.516 0.564 0.628
sucrose 0.956 1.031 1.167 1.257 1.340 0.918 0.993 1.069 1.180 1.272
(+)-cellobiose 0.842 1.055 1.109 1.136 1.147 0.807 0.996 1.045 1.073 1.090
(+)-lactose monohydrate 1.022 1.147 1.254 1.336 1.417 0.991 1.086 1.171 1.265 1.357
(+)-maltose monohydrate 1.053 1.214 1.317 1.383 1.474 1.007 1.125 1.226 1.304 1.391
(+)-melezitose 1.322 1.458 1.533 1.583 1.629 1.279 1.373 1.457 1.504 1.557
(+)-raffinose pentahydrate 1.431 1.613 ± 1.694 1.746 1.807 1.364 1.521 1.578 1.631 1.693
NH4H2PO4
T/K = 288.15 T/K= 298.15
(−)-D-ribose 0.338 0.372 0.392 0.414 0.445 0.314 0.365 0.391 0.415 0.446
(+)-D-glucose 0.494 0.547 0.580 0.592 0.628 0.456 0.542 0.569 0.579 0.639
(+)-D-mannose 0.511 0.573 0.619 0.665 0.738 0.472 0.559 0.612 0.666 0.757
2-deoxy-D-glucose 0.453 0.495 0.525 0.546 0.580 0.431 0.493 0.531 0.550 0.585
(+)-methyl α-D-glucopyranoside 0.495 0.531 0.559 0.581 0.623 0.465 0.522 0.558 0.579 0.621
(+)-methyl α-D-mannopyranoside 0.543 0.554 0.585 0.656 0.791 0.517 0.542 0.583 0.684 0.805
sucrose 1.032 1.146 1.237 1.333 1.453 0.995 1.171 1.261 1.359 1.492
(+)-cellobiose 0.913 1.036 1.094 1.242 1.435 0.878 1.040 1.117 1.265 1.472
(+)-maltose monohydrate 1.128 1.131 1.179 1.396 1.608 1.091 1.104 1.165 1.415 1.659
(+)-raffinose pentahydrate 1.542 1.696 1.862 2.009 2.163 1.478 1.713 1.868 2.022 2.223
T/K = 308.15 T/K = 318.15
(−)-D-ribose 0.294 0.368 0.402 0.426 0.461 0.283 0.377 0.414 0.439 0.477
(+)-D-glucose 0.427 0.521 0.562 0.599 0.677 0.406 0.518 0.574 0.626 0.707
(+)-D-mannose 0.440 0.553 0.616 0.679 0.767 0.418 0.563 0.632 0.703 0.793
2-deoxy-D-glucose 0.407 0.486 0.531 0.556 0.592 0.384 0.483 0.524 0.553 0.598
(+)-methyl α-D-glucopyranoside 0.443 0.525 0.561 0.597 0.660 0.413 0.518 0.557 0.592 0.661
(+)-methyl α-D-mannopyranoside 0.491 0.532 0.586 0.718 0.845 0.466 0.526 0.589 0.729 0.863
sucrose 0.956 1.191 1.287 1.399 1.538 0.918 1.212 1.326 1.430 1.563
(+)-cellobiose 0.842 1.053 1.136 1.283 1.526 0.807 1.066 1.156 1.311 1.555
(+)-maltose monohydrate 1.053 1.099 1.173 1.424 1.676 1.007 1.068 1.179 1.455 1.745
(+)-raffinose pentahydrate 1.431 1.746 1.918 2.072 2.252 1.364 1.758 1.950 2.126 2.279
K3PO4
T/K = 288.15 T/K = 298.15
(−)-D-ribose 0.338 0.419 0.430 0.448 0.453 0.314 0.378 0.391 0.406 0.416
(+)-D-glucose 0.494 0.630 0.681 0.701 0.736 0.456 0.581 0.625 0.640 0.667
2-deoxy-D-glucose 0.453 0.534 0.568 0.589 0.622 0.431 0.503 0.533 0.551 0.584
(+)-methyl α-D-glucoside 0.543 0.593 0.618 0.639 0.660 0.517 0.550 0.571 0.590 0.612
(+)-maltose monohydrate 1.128 1.341 1.437 1.504 1.540 1.091 1.291 1.376 1.437 1.488
(+)-raffinose pentahydrate 1.542 1.835 1.904 1.954 2.018 1.478 1.745 1.812 1.859 1.923
T/K= 308.15 T/K = 318.15
(−)-D-ribose 0.294 0.346 0.359 0.375 0.389 0.283 0.324 0.335 0.353 0.369
(+)-D-glucose 0.427 0.536 0.578 0.596 0.614 0.406 0.492 0.530 0.547 0.579
2-deoxy-D-glucose 0.407 0.470 0.498 0.518 0.548 0.384 0.434 0.467 0.486 0.516
(+)-methyl α-D-glucoside 0.491 0.514 0.532 0.557 0.577 0.466 0.469 0.487 0.509 0.534
(+)-maltose monohydrate 1.053 1.248 1.319 1.371 1.438 1.007 1.193 1.258 1.308 1.371
(+)-raffinose pentahydrate 1.431 1.666 1.740 1.786 1.843 1.364 1.579 1.650 1.693 1.750
a
Standard deviation for fitting in eq 2 lies in the range of (0.001 to 0.008)·103 m3·mol−1. bReference 16. cReference 22. dReference 19. eReference
10. fReference 29. gReference 30. hReference 31.

B = [(V1,°ϕ − V 2°)/1000] Δμ2° # = Δμ1° # + (RT /V1,°ϕ)[1000B − (V1,°ϕ − V 2°)] (6)

# #
+ V1,°ϕ[(Δμ2° − Δμ1° )/1000RT ] (5) According to the transition-state theory, every solvent molecule
in one mole of solution must pass through the transition-state
F DOI: 10.1021/acs.jced.5b00845
J. Chem. Eng. Data XXXX, XXX, XXX−XXX
Journal of Chemical & Engineering Data Article

Figure 2. Plots of viscosity B-coefficients of transfer ΔtB vs molalities mB of KH2PO4 for (a) (−)-D-ribose, (b) (+)-methyl α-D-glucopyranoside, (c) 2-
deoxy-D-glucose, (d) (+)-maltose monohydrate; of NaH2PO4 for (e) (−)-D-fructose, (f) 6-deoxy-D-mannose at ⧫, 288.15 K; ■, 298.15 K; ▲, 308.15 K;
×, 318.15 K.

and also interact more or less strongly with the solute molecules.
Hence, the Gibbs free energy of transfer of a solute from the
ground-state to transition-state solvents, ΔG°2 (1 → 1′) is the first
contribution and the Gibbs free energy of the solute through its
own viscous transition state, ΔG2°(2 → 2′) which is equal to
Δμ1°#, is the second contribution to Δμ2°#. The ΔG2°(1 → 1′)
values thus obtained from Δμ°2 # and ΔG°2 (2 → 2′) values are
found to increase with concentration of salt and decrease with
rise of temperature in all the cases (Table S5). The ΔG°2 (1 → 1′)
values follow the order: K3PO4 > NaH2PO4 > KH2PO4 >
NH4H2PO4, due to high ionic charge and ionic strength of PO43−
ion as compared to H2PO4− ion. The ΔG2°(1 → 1′) values also
increase with complexity of the solute. The large positive values
of Δμ°2 # and ΔG°2 (1 → 1′) suggest that the formation of
G DOI: 10.1021/acs.jced.5b00845
transition-state is less favorable for the solutes in phosphate-
based salts.
Activation entropy, ΔS2°# and enthalpy, ΔH2°# for the viscous
flow of solutes have been calculated in water and mixed aqueous
solutions as
ΔS2° # = −d(Δμ2° # /dT ) (7)
ΔH2° # = Δμ2° # + T ΔS2° # (8)
It is evident from the data (Tables S6 and S7) that ΔH°2 # and
TΔS2°# values are positive and further ΔH2°# > TΔS2°#. This
suggests that the formation of transition-state is associated with
bond breaking and a decrease in structural order. Hence it
J. Chem. Eng. Data XXXX, XXX, XXX−XXX
Journal of Chemical & Engineering Data Article

Figure 3. Plots of viscosity B-coefficients of transfer ΔtB vs molalities mB of NaH2PO4 for (a) methyl α-D-glucopyranoside, (b) (+)-cellobiose; of
NH4H2PO4 for (c) methyl α-D-glucopyranoside, (d) methyl α-D-mannopyranoside; of K3PO4 for (e) 2-deoxy-D-glucose, (f) (+)-raffinose pentahydrate
at ⧫, 288.15 K; ■, 298.15 K; ▲, 308.15 K; ×, 318.15 K.

indicates that for the studied saccharides/derivatives, the solute−
solvent interactions are nearly complete in the ground state.
3.2. Solvation. The ratio of viscosity B-coefficient to partial
molar volume, V°2 at infinite-dilution, that is, B/V°2 helps in
understanding the solvation of solutes. B/V°2 values lie between
zero and 2.5 for unsolvated spherical species and the values
higher than 2.5 indicate spherical solvated species.35,36 B/V°2
values in the present study are greater than 2.5 (Table S8), and
the values are more in the presence of salts as compared to those
in water, hence indicating that saccharides/derivatives are more
solvated in the presence of studied phosphate salts. The B/V°2
values increase with increase in molalities of salts, but decrease
H DOI: 10.1021/acs.jced.5b00845
with rise of temperature, except for a few cases in NH4H2PO4.
The B/V2° values follow the order: Glc > 2de-Glc > Me α-Glc;
Man > Me α-Man > 6de-Man, indicating that saccharides are
more solvated than their respective derivatives.
3.3. Interaction Coefficients. The viscometric interaction
coefficients were calculated using the McMillan-Mayer
theory37,38 in order to study the solute−cosolute interactions
as follows:
Δt B = 2ηABmB + 3ηABBmB 2 (9)
where A and B represent solute and cosolute. Generally, the pair
η AB interaction coefficients are positive and triplet η ABB
J. Chem. Eng. Data XXXX, XXX, XXX−XXX
Journal of Chemical & Engineering Data
interaction coefficients are negative for the studied solutes
(except for Me α-Man and Mal in NH4H2PO4) (Table S9). The
plot (Figure 4) clearly shows that the contribution of pair
Figure 4. Contributions of viscometric interaction coefficients to ΔtB at
various molalities mB of K3PO4 for (−)-D-ribose at (⧫,∗) 288.15 K,
(■,●) 298.15 K, (▲,+) 308.15 K, (×,−) 318.15 K [⧫,■,▲,× (ηAB) and
∗,●,+,− (ηABB)].
interaction coefficients to ΔtB at various molalities of K3PO4 for
(−)-D-ribose varies linearly while that of triplet coefficients varies
nonlinearly. Both coefficients increase systematically from
mono- to di- to trisaccharides. The magnitude of ηAB coefficients
is large compared to that of ηABB values suggesting the pairwise
interactions among solute and cosolute. Similar results were
obtained for the volumetric studies for these solutes in
phosphate-based salts.26,27
4. CONCLUSIONS
The viscometric properties have been studied for various mono-
and di-, trisaccharides and methyl- and deoxy-derivatives of
monosaccharides in aqueous solutions of potassium, sodium, and
ammonium phosphate monobasic and potassium phosphate
tribasic salts at different temperatures. The viscosity B-
coefficients are positive and increase with the molalities of the
cosolutes, indicating an increase in kosmotropicity of solutes in
the presence of phosphate-based cosolutes. Similarly, the
viscosity B-coefficient of transfer, ΔtB are positive in all the
studied cosolutes except for 2de-Rib, Me α-Glc and Me α-Man at
mB = 0.25 mol·kg−1 KH2PO4 at (308.15 and 318.15) K. The dB/
dT values are negative for the solutes in all the cosolutes except in
case of NH4H2PO4. Overall, the results suggest that saccharides/
derivatives exhibit more kosmotropic behavior in K3PO4 as
compared to other phosphate-based salts. This has been
attributed to high charge and ionic strength of PO43− anion
compared to H2PO4− anion.
■
ASSOCIATED CONTENT
*
S Supporting Information
The Supporting Information is available free of charge on the
ACS Publications website at DOI: 10.1021/acs.jced.5b00845.
Viscosities, η (Table S1), dB/dT values (Table S2),
activation parameters (Tables S3−S7), B/V2° values
(Table S8) and interaction coefficients (Table S9) of
saccharides/derivatives in water and in aqueous solutions
of phosphate-based cosolutes (PDF)
I DOI: 10.1021/acs.jced.5b00845
■
Article
AUTHOR INFORMATION
Corresponding Author
*E-mail: pkbanipal@yahoo.com. Tel.: +91 183 2451357. Fax:
+91 183 2258819/20.
Funding
Neha Aggarwal is grateful for the award of fellowship to the
Council of Scientific and Industrial Research (09/254(0228)/
2011-EMR-I) New Delhi, India.
Notes
The authors declare no competing financial interest.
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J. Chem. Eng. Data XXXX, XXX, XXX−XXX