IJCCE Volume 38 Issue 5 Pages 221-237
IJCCE Volume 38 Issue 5 Pages 221-237
IJCCE Volume 38 Issue 5 Pages 221-237
5, 2019
Koohyar, Fardad
Division of Computational Physics, Institute for Computational Science, Ton Duc Thang University,
Ho Chi Minh City, VIETNAM
Kiani, Farhoush*+
Department of Chemistry, Faculty of Science, Islamic Azad University, Ayatollah Amoli Branch,
Amol, I.R. IRAN
ABSTRACT: In this research, a theoretical study has been undertaken on the density and also
on the relationship between refractive index and density for aqueous solutions. A simple linear
equation is suggested to show this relationship. Also, a semi-empirical equation has been developed
for estimating the constant of this linear equation. By using our suggested equations, the refractive
indices of aqueous solutions of alkane polyols [R(OH)n, n = 2 to 6 -OH,s) and also polyols with
one ring (monosaccharide) can be calculated. Moreover, the refractive indices of some alcohols
and other components have been collected from the various literature. Our suggested equations
have been tested for aqueous solutions of these molecules. For aqueous solutions of alkane polyols
[R-(OH)n, n = 2 to 6 –OH,s) and monosaccharide, a good agreement is observed between
experimental refractive indices and theoretical ones. Other molecules show positive and/or negative
deviations from the results of our suggested equations. For various liquid solutions, the refractive indices
can be correlated and fitted with our linear equation. Also, the value of the constant of this linear
equation, Kref, shows the power of interaction between solute and solvent molecules. The interaction
between solute and solvent molecules increases when the value of constant, Kref increases.
INTRODUCTION
Refractive index (nD or n) is one of the most industries like pharmaceutical [6,7], food [8], petroleum [9]
important thermodynamic and optical properties of and cosmetic [10]. In pharmaceutical and food industries,
solutions [1-5]. It has many applications in various refractive index (RI) is often used to qualify control
* To whom correspondence should be addressed.
+ E-mail: [email protected] ; [email protected]
Other Address: Faculty of Applied Sciences, Ton Duc Thang University, Ho Chi Minh City, VIETNAM
Other Address: Discipline of Chemical Engineering, School of Engineering, University of KwaZulu-Natal, Howard
College Campus, King George V Avenue, Durban 4041, SOUTH AFRICA
1021-9986/2019/5/221-237 17/$/6.07
of crude intermediate and final products. Also, the refractive In recent years, some researchers have worked
index gives us important information about various engineering on refractive indices of pure compounds and solutions.
calculations, for instance, RI is a key parameter for Shekaari and Jebali reported refractive indices of aqueous
characterizing raw oils. The determination of this index through solutions of (amino acid + Ionic Liquid ([BMIm]Br)
the experiment is capital-intensive and time-consuming [11]. at 298.15 K [26]. Tan and Huang studied the dependence
On the other hand, the refractive index can be modified in of refractive index on concentration and temperature
the cosmetic materials as it is important in making clear in an electrolyte solution, polar solution, nonpolar solution, and
emulsions used in cosmetic formulations [12]. protein solution [27]. Lorimer reported refractive index
Besides, it can be applied in academic and research increments of polymers in solution [28]. Bai and Katz
works. The refractive index information can lead us researched the refractive index of sodium iodide solutions for
to a better understanding of interactions between solute index matching in PIV [29]. Li et al. reported values of sodium
and solvent molecules [13-15]. and potassium aluminate aqueous solutions [30]. Chen et al.
For a medium like an aqueous solution, the refractive determined the refractive index of an aqueous solution of CdTe
index is the ratio of the velocity of light in vacuum and phase quantum dots [31]. Koralewski et al. obtained optical properties
velocity of light in the medium [16]. Also, the refractive index of chitosan in aqueous solution [32]. Proutiere et al. reported
can be obtained from Maxwell’s equation as follow [17]: refractive index variations in pure liquids [33]. Gharagheizi et al.
reported a group contribution model for the estimation of
c
n (1) refractive indices of organic compounds [34].
0 0 In this study, for aqueous solutions, in the first step
we will show that there is a linear relationship between
In Equation (1), c is the velocity of light in vacuum,
refractive index and molar concentration, especially in low molar
v is the velocity of light in the medium, ε and μ are
concentration. In the second step, we will introduce a semi-
the permittivity and permeability for medium and ε0 and μ0
empirical equation for the calculation of Kref for binary aqueous
are the permittivity and permeability for the vacuum,
solutions (water + glycerol, 1- propanol, 1,3-propandiol, butane-
respectively.
1, 3-diol, butane-1, 4-diol, butane-2, 3-diol, pentaerythritol, D-
The Refractive index has no dimension. Most of the
fructose, D-glucose, and D-mannitol) at constant temperature and
materials have positive refractive index values and some
atmospheric pressure (Table 1). However, other solute molecules
others have negative ones [18-20].
(ethylene glycol, ethanol, acetone, lactic acid, acetic acid, citric
Negative Index Metamaterial (NIM) has already been
acid, urea, and 1-amino-2-propanol) show a deviation (negative
introduced in 1968 [21] by the general consideration
or positive) from the proposed equations.
of the electrodynamics properties of the materials with
simultaneously negative values of the dielectric
CALCULATIONS
permittivity and magnetic permeability. In 1996, Pendry
The Gladstone–Dale relation shows the relationship
proposed that a negative epsilon can be made by
between density (ρ) and refractive index (n) for binary
arranging the metal wires in a simple cubic lattice [22].
liquid solutions which is given as follows [35]:
But the main question was how we could get the negative μ.
This question was answered by Smith in 2000 [23]. n 1 B (2)
Smith proposed a structure consisting of a periodic array In Equation (2), B is the Gladstone–Dale constant.
of split-ring resonators and continuous wires that Equation 3 shows the relationship between variations
produced the negative permeability and negative of ρ and n when molar concentration of solute, c, varies
permittivity. in binary liquid solution:
The refractive index of the medium varies as
dn d
the wavelength of light changes [24]. In an apparatus which B (3)
is used for measuring refractive index, a fixed source dc dc
of light (with a certain wavelength) is applied for light We assume that some non-ionic solute molecules
generation. For example, in the Abbe refractometer, a sodium are dissolved in a solvent (water) and a binary aqueous
lamp generates the yellow light (λ = 598.3 nm) [25]. solution, with molar concentration c, is provided.
Table1: The experimental (from Equation (11)) and theoretical (from Equation (13)) values of Kref for aqueous solutions of
some alcohols and polyols at constant temperature and atmospheric pressure.
c(mol.L-1) Kref (exp) (L/mol) Kref (cal) (L/mol) %RD (Kref)
a
Glycerol (at 293.15 K)
Table1: The experimental (from Equation (11)) and theoretical (from Equation (13)) values of Kref for aqueous solutions of
some alcohols and polyols at constant temperature and atmospheric pressure.
c(mol.L-1) Kref (exp) (L/mol) Kref (cal) (L/mol) %RD (Kref)
Table1: The experimental (from Equation (11)) and theoretical (from Equation (13)) values of Kref for aqueous solutions of
some alcohols and polyols at constant temperature and atmospheric pressure.
c(mol.L-1) Kref (exp) (L/mol) Kref (cal) (L/mol) %RD (Kref)
Table1: The experimental (from Equation (11)) and theoretical (from Equation (13)) values of Kref for aqueous solutions of
some alcohols and polyols at constant temperature and atmospheric pressure.
c(mol.L-1) Kref (exp) (L/mol) Kref (cal) (L/mol) %RD (Kref)
dn n n 0 n
(6)
dc c c
n n0 0
B (7)
c c
Fig. 1: The microscopic structure of the liquid solution. It can be seen in some research works and literature
In this figure, the bigger molecules are solute and smaller [26,30,36-38] that for binary aqueous solutions, there is
molecules are solvent. a linear relationship between density and concentration
of solutes, especially in low concentrations, as below:
The microscopic structure of this binary aqueous solution
kc 0 (8)
can be seen in Fig. 1.
It is clear that in aqueous solutions, cₒ = 0. Therefore: In Equation (7), k is a constant. Equation (7) can be
dc c c0 c (4) rewritten as below:
0
On the other hand, we can write: k (9)
c
d 0 Equation (10) can be obtained by combining
(5)
dc c c Equations (7) and (9):
Table 2: The relationship between refractive index, n, and molar concentration, c, for aqueous solutions
of various solutes (species) at T = 293.15 Ka.
Specie Mw (g/mol) Equation (n vs. c)b R2 Molar concentration range
Alkanols and Alkane polyols
Methanol (CH3OH) 32.04 y = 0.0009x + 1.3328 0.9986 0.156 – 10.580
Ethanol (C2H5OH) 46.07 y = 0.0033x + 1.3327 0.9986 0.216 – 7.370
1-Propanol (C3H8O) 60.10 y = 0.0055x + 1.3331 0.9992 0.166 – 3.838
Ethylene glycol (C2H6O2) 62.07 y = 0.0059x + 1.3329 0.9999 0.161 – 8.212
Glycerol (C3H8O3) 92.09 y = 0.0107x + 1.3330 1.0000 0.109 – 6.385
D-Glucose (C6H12O6) 180.16 y = 0.0250x + 1.3333 0.9999 0.056 – 4.081
D-Fructose (C6H12O6) 180.16 y = 0.0251x + 1.3331 1.0000 0.056 – 2.767
D-Mannitol (C6H14O6) 182.17 y = 0.0254x + 1.3332 0.9999 0.055 – 0.867
Lactose (C12H22O11) 342.30 y = 0.0508x + 1.3330 0.9999 0.029 – 0.565
Sucrose (C12H22O11) 342.30 y = 0.0483x + 1.3332 1.0000 0.059 – 2.255
Maltose (C12H22O11) 342.30 y = 0.0493x + 1.3332 1.0000 0.059 – 2.253
Organic acids
Formic acid (CH2O2) 46.03 y = 0.0024x + 1.3332 0.9983 0.109 – 4.074
Acetic acid (CH3COOH) 60.05 y = 0.0041x + 1.3332 0.9996 0.166 – 4.470
Lactic acid (C3H6O3) 90.08 y = 0.0085x + 1.3333 0.9999 0.111 – 5.377
Oxalic acid (C2H2O4) 90.03 y = 0.0095x + 1.3331 0.9995 0.056 – 0.920
Citric acid (C6H8O7) 192.12 y = 0.0233x + 1.3333 1.0000 0.211 – 1.639
Organic solutes
Ammonia (NH3) 17.03 y = 0.0009x + 1.3329 89..04 0.292 – 5.622
Acetone (C3H6O) 58.08 y = 0.0043x + 1.3330 0.9999 0.172 – 1.696
Urea (CH4N2O) 60.06 y = 0.0084x + 1.3333 0.9999 0.167 – 8.234
Ionic solutes
Sodium hydroxide (NaOH) 39.99 y = 0.0099x + 1.3334 0.9989 0.125 – 2.174
Sodium chloride (NaCl) 58.44 y = 0.0092x + 1.3335 0.9992 0.172 – 3.056
Sodium acetate (CH3COONa) 82.03 y = 0.0103x + 1.3335 0.9992 0.122 – 2.993
Sodium nitrate (NaNO3) 84.99 y = 0.0085x + 1.3335 0.9989 0.118 – 2.689
Sodium bromide (NaBr) 102.89 y = 0.0133x + 1.3334 0.9998 0.197 – 2.837
Potassium hydroxide (KOH) 56.11 y = 0.0097x + 1.3335 0.9990 0.179 – 1.938
Potassium chloride (KCl) 74.55 y = 0.0091x + 1.3334 0.9993 0.135 – 2.701
Potassium nitrate (KNO3) 101.1032 y = 0.0085x + 1.3333 0.9991 0.099 – 2.240
Potassium bromide (KBr) 119.00 y = 0.0130x + 1.3334 0.9997 0.084 – 2.914
Potassium iodide (KI) 166.00 y = 0.0207x + 1.3334 1.0000 0.122 – 3.134
Hydrochloric acid (HCl) 36.46 y = 0.0079x + 1.3333 0.9996 0.137 – 4.099
Lithium chloride (LiCl) 42.39 y = 0.0082x + 1.3335 0.9995 0.118 – 4.118
Ammonium chloride (NH4Cl) 53.491 y = 0.0097x + 1.3333 0.9997 0.187 – 3.128
Cesium Chloride (CsCl) 168.36 y = 0.0121x + 1.3334 0.9996 0.120 – 3.877
Nitric acid (HNO3) 63.01 y = 0.0074x + 1.3334 0.9996 0.159 – 3.937
Silver nitrate (AgNO3) 169.87 y = 0.0168x + 1.3334 0.9998 0.120 – 2.758
Manganese(II) sulfate (MnSO4) 151.00 y = 0.0240x + 1.3336 0.9996 0.135 – 1.063
Copper sulfate (CuSO4) 159.61 y = 0.0265x + 1.3335 0.9993 0.063 – 1.013
a) Ref [38] ; b) Eq. [24]
Table 3: Molar concentration ranges of solutes, Δc, for aqueous solutions that in this ranges, the molality is equal to molarity a.
Group 1: the solute molecules which follow Equation (13) group, has free electron pair and free electrons, compared
[Kref(calc) = Kexp(exp)]. These molecules (such as glycerol, to bonding electrons, generate a stronger magnetic field.
propanediol, butane-1, 3-diol, butane-1, 4-diol, It must be taken into account in Eq.(13), N(-O-)
pentaerythritol, D-fructose, D-glucose, D-mannitol) have can be several groups and/or atoms of solute molecules
two or more hydroxyl agents and/or oxygen atoms and that can generate hydrogen bond with solvent molecules.
also, have R- group and/or groups with two or more
carbon atoms (C3, C4, C5,….). These R- groups have Application of Equations (11), (12), and (13)
a good electron donor effect. There are some equations to fit refractive indices data
Group 2: the solute molecules which have a negative of aqueous solutions but Equations (11) and (12) are important
deviation from Equation (13). For these molecules, for fitting refractive indices data of aqueous solutions
the value of experimental Kref is less than calculated Kref. because the parameters of these equations (Kref) help us
These molecules have R- the group with small size, to a better understanding of interactions between solvent
electron acceptor agents, and also, low number of and solute molecules [14]. The interaction between
hydroxyl agents (such as methanol and ethanol). Of course, solute and solvent molecules increases as the value of Kref
ethylene glycol has a negative deviation from Eq.(13), increases.
but in a low amount. We can put the molecules with carbonyl
agents (such as acetone, acetic acid, and citric acid) Determination of refractive index of aqueous solutions
in group 2. Also, the molecules which have –R group For aqueous solutions of alkane polyols (n = 2 to 6 –OH,s)
with seven or more carbons and also, disaccharides (like and monosaccharides, we can calculate the value of Kref
maltose) can be classified as group 2 (please see Table 1). for solutes by Equation (13) and then calculate
Group 3: the solute molecules which have a positive refractive indices at various molar concentrations by
deviation from Equation (13) (such as 1-amino-2-propanol Equations (11) or (12) with high accuracy (%RD < 0.15).
and urea). For these molecules, the value of experimental Please see Table 4. Using Equations (13), (11) or (12),
Kref is more than calculated Kref. In this group, molecules there is no need to refractometer for determination
have agents such as –NH2. The nitrogen atom, an amino of refractive indices of the mentioned aqueous solutions.
Determination of molar concentration of aqueous solutions Therefore, in an aqueous solution of alkane polyols and
For aqueous solutions of alkane polyols [R-(OH)n, monosaccharides, the hydrogen bond which is formed
n = 2 to 6 -OHs) and monosaccharides, with having between solute and solvent molecules, HB(solu-solv), is
theoretical Kref (obtained by Equation 13) and stronger than hydrogen bond between solvent molecules,
experimental refractive index, we can determine molar HB(solv-solv).
concentration using the following equation: The second subject, in alkane polyols, the mass of –R
n exp n 0 (solute molar mass) mostly increases with increasing
c (15) of the number of hydroxyl agents.
K ref calcul
We can reach to the below proportionality with
Where, Kref(calcul) is calculated using Equation (13) and nexp considering two above subjects:
Strength of HB N
and n0 are the experimental refractive index
of aqueous solution and solvent, respectively. As can be seen solu solv O (17)
in Table 4, Equation 15 can be used for the determination of
The proportionality 18 can be obtained by
the molar concentration of alkane polyols (n = 2 to 6 –OH,s)
combination proportionalities 16 and 17:
and monosaccharides aqueous solutions. The values of %RD
for these determinations are less than 2. Equation 15 gives
good results (uncertainty of ±0.001 to ±0.005) especially in
Strength of HB solu solv M WSolute
and N O (18)
low and moderate concentration (between 0.1 and 1 mol/L). Equation (13) shows that Kref depends on MW(solute)
For these solutions, the refractive index can be a good tool for and N(-O-). The Kref,s for 1-propanol, 1,3 propandiol, glycerol,
the determination of concentration. and also, ethanol and ethylene glycol show that the value
of Kref increases (about 0.0026) when the one hydroxyl
group is inserted to –R group.
Study on interaction between solute and solvent
Comparison of Equation (13) and proportionality (18)
molecules
results to the below:
The parameter Kref (from Equation (13)) can show the
strength of the interaction between solvent and solute Kref strength of HBsolu solv (19)
molecules.
The –R group in alkane polyols, [R(OH)n], have Proportionality (19) shows that in an aqueous solution
an electron donor effect on the oxygen atom of hydroxyl of alkane polyols, the value of Kref can indicate the
agents, and this effect increases by increasing the mass of strength of hydrogen bond which is formed between
–R group (or mass of solute molecules). In these molecules, solute and solvent molecules, HB(solu-solv). The strength of
the negative charge (-δ) of the oxygen atom (from hydroxyl HB(solu-solv) increases as the value of Kref increases.
agent) increases as the molar mass of solute increases. The Kref can be used in industrial and research fields.
It means that in alkane polyols and monosaccharides, It is well known that the H-bondings play an important
the strength of hydrogen bond which is formed between role in many organic components and their solutions
solute and solvent molecules, HB(solu-solv), increases which are used in various industries such as pharmacy [48-50],
by increasing the molar mass of solutes. Therefore, food [51,52], detergents and cleaners [53,54].
in an aqueous solution of alkane polyols and monosaccharides: In research works, HB(solu-solv) is a good tool for
investigating interactions between molecules
(Strength of HB(solu-solv))(molecular weight of solute) (16)
in aqueous solutions which have hydroxyl and/or
Two subjects should be considered when the number carboxyl agents [14,55,56]. Of course, in research work,
of hydroxyl agents, N(-O-), increases in alkane polyols and a nonclassical HB (hydrogen bonding involving
monosaccharides. The first subject, the number of HB(solu-solv) a B–H···π interaction) was described [57].
increases when the number of hydroxyl agents, in various As it was mentioned, in aqueous solutions, the Kref
solute molecules, increases. It should be noted that shows the strength of HB(solu-solv) and it can be used in research
the electron donor effect of –R groups (C2Hn, C3Hn, C4Hn, etc) works. For example, we can investigate positive and
is more than the electron donor effect of the hydrogen atom. negative deviations from Equation (13).
Table 4: The values of calculated molar concentration (by Equation (15)) also, experimental and calculated refractive indices
(by Equation (11)), n, for aqueous solutions of some polyol(s) in various molar concentration.
Table 4: The values of calculated molar concentration (by Equation (15)) also, experimental and calculated refractive indices
(by Equation (11)), n, for aqueous solutions of some polyol(s) in various molar concentration.
ccalcul(mol/L)c cexp(mol/L) nexp ncalcb RD (%) for n RD (%) for c
As can be seen in Table 1, 1-amino-2-propanol has can be due to the existing two amine groups.
positive deviation from Equation 13 (Kref(exp) > Kref(calc)). On the other hand, Table 1 shows that some solute
The molecular structure of 1-amino-2-propanol is similar molecules have a negative deviation from Equation (13)
to 1,2- propandiol but there is a difference between (Kref(exp) < Kref(calc)). It can be due to having agents which
structures of these two molecules. 1,2-propandiol has generate HB(solv-solu) with less strength than hydroxyl agent.
two hydroxyl agents while 1-amino-2-propanol has one It can be observed in Table 1 that acetone, citric acid, and
hydroxyl and one amine agent. The oxygen atom ethanol have a notable negative deviation from Equation (13).
(in hydroxyl agent) is more electronegative than nitrogen This deviation for acetone is about - 0.001 and
atom (in amine agent). It means that the free electron pair it can be due to the existing carbonyl group (-C=O).
in the amine group is more available (for production of In aqueous solutions, hydroxyl (from solute molecules)
hydrogen bonding) than that of hydroxyl agent. Therefore, can form three hydrogen bonds (two O solute·····Hsolvent and
the strength of HB[(H)2N·····H-O-H] is more than one Hsolute·····Osolvent) while carbonyl (from solute
HB[R(H)O·····H-O-H]. It can be the reason for this positive molecules) can form two hydrogen bonds (two
deviation. This deviation is +0.002 for 1-amino-2-propanol. Osolute·····Hsolvent). Therefore, the power of the bond
Also, the area has a positive deviation (+0.0024) from between the carbonyl group and water can be less than t
Equation 13 (please see Table 1). This positive deviation hat of between hydroxyl group and the water molecule.
(a) (b)
Fig. 3: The molecular structures of acetic acid (a) and maltose (b).
We can see in Table 1 that the acetic acid (Fig. 3a) of interaction between solute and solvent molecules.
has a negative deviation from Equation (13) (-0.0016). Two important cases must be noted for better comparison
It can be due to the existing one carbonyl group that is between Kref of different molecules. First, this comparison
attached to hydroxyl agent (-COOH). It appears that 0.0015 must be done in a homologous series of chemicals. Second,
negative deviation (from Equation (13)) occurs per each this comparison must be done in the same concentration of
acidic group (-COOH). Citric acid has three acidic groups solutes (for instance, in 0.5 or 1 mol/L). Other components
and shows –0.0045 deviations from Equation (13). Also, show negative or positive deviation from this equation
lactic acid has one acidic group and shows about -0.0015 (Equation (13)). Components with negative deviation have
deviation from Equation (13) (please see Table 1). agents which generate weaker HB(solu-solv) than hydroxyl
Of course, these are weak acids and it guesses that group. Components with positive deviation have agents
the deviation from Equation (13) is too high for strong acids. which generate stronger HB(solu-solv) than hydroxyl group.
Also, there is a negative deviation (from Equation (13)) This information can help us to a better understanding
for maltose. The value of this deviation is about -0.01 of interaction between solutes and solvents in solutions.
(Please see Table 1). As can be seen in Fig. 3b,
the molecule of maltose has 8 hydroxyl groups as well as Nomenclature
3 oxygen atoms. In this molecule, the intramolecular n Refractive index, –
hydrogen bonds can be formed between various hydrogen ρ Density, kg/m3
and oxygen atoms of maltose. For a solute molecule, Kref -, L/mol
the number of hydrogen bonds between solute and Mw Molar mass, kg/mol
solvent molecules can decrease with an increasing c Molar concentration, mol/L
number of intramolecular hydrogen bonds. T Temperature, K
The relative deviation (RD) for refractive indices,
concentration, and Kref can be calculated by: Received : Dec. 19, 2017 ; Accepted :Jul. 30, 2018
Xexperimental Xcalculted
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