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Research Article
1
Herbal Medicinal Product Department, Central Institute of Medicinal and Aromatic Plants (Council of Scientific and
Industrial Research), P.O. CIMAP, Lucknow, UP, India and 2Gayatri Institute of Science and Technology, Biju Patnaik
University of Technology, Rourkela (Odisha) India
Abstract
Context: Citronella oil is reported to have excellent mosquito-repellent activity. To develop a stable cream formulation
(emulsion), its hydrophilic–lipophilic balance (HLB) value is important.
Objective: To determine required hydrophilic–lipophilic balance (rHLB) value of citronella oil and to develop stable
cream formulation.
Materials and Methods: Emulsions of citronella oil were prepared by phase inversion temperature technique using
water, Tween 80 and Span 80. A first series of 11 emulsions with HLB values ranging from 5.0 to 15.0 and a second series
of eight emulsions with smaller interval in HLB values from 11.0 to 13.8 were prepared. Emulsions were evaluated
For personal use only.
for creaming index, droplet size and turbidity to determine rHLB. Utilizing determined rHLB, citronella oil cream
was formulated and evaluated for different texture parameters. rHLB of light liquid paraffin was also determined for
validation of methodology.
Results: rHLB of light liquid paraffin and citronella oil was determined to be 11.80 and 12.60, respectively. Stable
citronella oil cream was developed with 10% emulsifier blend. Texture parameters were found to be consistent over
the entire storage period.
Discussion: Creaming index, droplet diameter, percent increase in droplet diameter and turbidity are the established
parameters to determine rHLB and to develop stable emulsion. Emulsions with optimum emulsifier concentration
resulted in less percentage creaming index, smallest droplet, less percentage increase in droplet diameter and
highest turbidity. Texture properties evaluation ensures the stability of the developed cream.
Conclusion: rHLB value of citronella oil was found 12.6 and a stable cream was formulated utilizing determined rHLB.
Keywords: Emulsion, emulsifier, creaming index, droplet size, turbidity, texture analysis
Address for Correspondence: Dr. Narayan Prasad Yadav, Central Institute of Medicinal and Aromatic Plants (Council of Scientific and
Industrial Research), P. O. CIMAP, Lucknow (U.P.) India 226015. Tel.: +91-522-2718657. Fax: +91-522-2342666. E-mail: npyadav@gmail.com
(Received 03 March 2012; revised 29 June 2012; accepted 06 August 2012)
1540
rHLB of citronella oil and cream formulation 1541
properties of citronella oil, which is insoluble in water are Table 1. Hydrophilic–lipophilic balance spread sheet of emulsion
Flash Point: 77°C, Boiling Point: 200°C, Specific Gravity: preparation.
0.897, Refractive Index (25°C): 1.4660–1.4750 and Optical Formulation
Rotation: −5° to 0°12,13. Some conventional and novel drug Formulation Span Tween (Light liquid
(Citronella oil) HLB 80 (%) 80 (%) paraffin)
delivery system of citronella oil for mosquito-repellent
First series emulsions
activity has been reported in the literature14–16.
CE1 5.0 93.46 06.54 LE1
In the present study, a pharmaceutically and cosmeti-
CE2 6.0 84.12 15.88 LE2
cally elegant cream formulation of citronella oil with dif-
CE3 7.0 74.77 25.23 LE3
ferent cream bases was attempted to develop17,18. During
CE4 8.0 65.43 34.57 LE4
the formulation development process, difficulty in selec-
CE5 9.0 56.08 43.92 LE5
tion of suitable emulsifiers was experienced to produce a
CE6 10.0 46.73 53.27 LE6
stable emulsion. These complications further guided to
CE7 11.0 37.39 62.61 LE7
determine the rHLB value of citronella oil, which is not
CE8 12.0 28.04 71.96 LE8
reported in the literature. Therefore in the present inves-
Drug Development and Industrial Pharmacy Downloaded from informahealthcare.com by RMIT University on 09/11/13
Formulation of citronella oil cream Table 3. Percent creaming index of citronella oil and light liquid
Based on the above investigations, rHLB value of cit- paraffin emulsions stored at room temperature.
ronella oil was determined and further utilized in the Emulsions Day 3 Day 5 Day 10 Day 15 Day 30
development of cream formulations which are shown in CE1 2.8 6.6 PS PS PS
Table 2. Oil phase of the cream containing light liquid CE2 2.4 6.3 PS PS PS
paraffin, paraffin wax, cetyl alcohol, stearyl alcohol CE3 2.1 6.1 PS PS PS
and GMS was heated up to 65°C for melting the ingre- CE4 1.9 5.8 PS PS PS
dients. Aqueous phase containing Tween 80 and water CE5 1.8 4.4 PS PS PS
was heated up to 50–55°C. Citronella oil was added to CE6 1.5 4.3 8.4 10.6 PS
oil phase when the temperature came down to 50–55°C CE7 1.1 3.8 6.8 8.3 10.2
and finally aqueous phase was mixed to the oil phase CE8 1.0 3.7 6.6 8.0 10.0
with constant stirring. The mixture was stirred for about CE9 1.0 3.7 6.2 8.0 9.8
30 min until homogenous cream was prepared7,21,24. CE10 1.0 3.9 6.2 8.2 PS
CE11 1.3 3.8 6.4 8.3 PS
Table 2. Citronella oil cream formulationsa. LE1 2.9 5.9 PS PS PS
Formulations/Ingredients (%) CR1 CR2 CR3 CR4 LE2 2.7 5.9 PS PS PS
Light liquid paraffin 8.00 8.00 8.00 8.00 LE3 2.4 5.8 PS PS PS
Citronella oil 2.00 2.00 2.00 2.00 LE4 1.9 5.5 9.8 PS PS
Paraffin wax 3.00 3.00 3.00 3.00 LE5 1.8 4.6 8.8 10.2 PS
Cetyl alcohol 2.00 2.00 2.00 2.00 LE6 1.2 3.2 8.4 8.8 10.4
Stearyl alcohol 2.00 2.00 2.00 2.00 LE7 1.0 3.2 8.1 7.4 9.2
Tween 80 2.95 4.42 5.90 7.37 LE8 1.1 3.3 8.2 7.4 9.4
GMS 1.05 1.58 2.10 2.63 LE9 1.3 3.6 8.5 8.0 10.2
Water (up to 100 mL) q.s. q.s. q.s. q.s. LE10 1.3 3.5 8.6 8.2 PS
a
rHLB of oil phase in citronella oil cream formulation: 12.56. LE11 1.5 3.4 8.8 PS PS
Surfactant Blend is GMS: Tween 80 = 1:2.8. CE, citronella emulsion; LE, light liquid paraffin emulsion; PS,
GMS, glycerol monostearate; q.s, quantity sufficient; CR, cream. phase separation.
citronella oil emulsions turbidity was found to be in the entire 3 months. Extrudability was found to be 25.1 ± 1.04
range of 89.12 ± 2.4 (CE17, HLB = 12.6) and 60.14 ± 2.1 mJ on the day of formulation whereas it was increased to
(CE19, HLB = 13.4) whereas for light liquid paraffin emul- 25.8 ± 1.45 mJ over a period of 90 days.
sions it was found to be 91.2 ± 3.6 (LE15, HLB = 11.8) and
62.9 ± 2.8 (LE19, HLB = 13.4).
Discussion
Creaming index
Regardless of emulsifier concentration and/or combi-
nation, creaming is a natural phenomenon in biphasic
systems and is an indication of destabilization25–27. It
gives a preliminary idea of nearest range of stable emul-
sions which may be useful for determining the rHLB. All
the emulsions (Citronella oil emulsions and light liquid
paraffin emulsions) were studied for creaming for the
period of 30 days and their percent CI was determined
(Table 3). During first two days creaming was not seen
for any of the formulated emulsions, whereas 3rd day
Figure 1. Mean droplet diameter of citronella oil emulsions over a onwards increase in creaming was observed with time.
period of 30 days. Mean value ± SEM, n = 3.
It was also observed that the CI was decreased with the
increase in HLB value of the emulsion. After 30 days cit-
ronella oil emulsions with HLB value 11–13 were found
stable and rest of the emulsions were separated into two
different layers. These results indicate the rHLB of citro-
nella oil lies in between 11 and 13 (CE7–CE9), hence a
second series of eight emulsions with HLB value 11.0–
13.8 (CE13–CE20, Table 1) were prepared and subjected
to other evaluation parameters viz. particle size and
turbidity analysis. Similarly, light liquid paraffin emul-
sions in the HLB range of 10–13 were found compara-
Figure 2. Mean droplet diameter of light liquid paraffin emulsions tively stable and the same evaluations were performed
over a period of 30 days. Mean value ± SEM, n = 3. for these emulsions.
Figure 3. Percent increase in mean droplet diameter of citronella oil emulsions and light liquid paraffin emulsions on day 30.
paraffin emulsions. sions, CE17 (HLB = 12.6) and light liquid paraffin emul-
sions, LE15 (HLB = 11.8) showed minimal droplet size
Table 4. Required HLB of citronella oil and light liquid paraffin over the course of investigation. Percent increase in
(experimentally determined). MDD, over storage is another useful indicator for access-
Methods for determination of HLB
ing the stability of emulsions, because suitable emulsifier
Percent increase Percent
results in to minimum increase in droplet diameter. As
Oils MDD in MDD Turbidity CI
depicted in Figure 3, CE17 and LE15 have shown 16.43
Citronella oil 12.6 12.6 12.6 12.0, 13.0,
14.0 and 27.18% increase in MDD which suggests that these
Light liquid 11.8 11.8 11.8 11.0 emulsions are close to rHLB of the respective oils.
paraffin
MDD, mean droplet diameter; CI, creaming index; HLB, Turbidity
hydrophilic–lipophilic balance. Rate of creaming in a polydisperse system can be
defined as:
Table 5. Texture analysis of stable citronella oil cream formulation
(CR4).
8π
Duration (Days) u = ∑i gni ri5 (d1 − d2 )
Parameters 0 30 60 90 27ηV
Consistency 0.8 ± 0.040 0.9 ± 0.025 0.9 ± 0.038 0.9 ± 0.064
(mJ) Where ni is number of droplets, ri is the radius of drop-
Firmness (g) 6.0 ± 0.25 6.0 ± 0.45 7.0 ± 0.15 7.0 ± 0.55 lets, V is total volume of dispersed phase, η is viscosity
Spreadability 1.8 ± 0.042 1.8 ± 0.045 1.8 ± 0.034 1.8 ± 0.024 of emulsion, g is acceleration due to gravity and (d1–d2)
(mJ) is the density difference between the dispersed and con-
Adhesiveness 1.0 ± 0.22 1.5 ± 0.15 1.5 ± 0.42 1.5 ± 0.32 tinuous phases28. If all the parameters are kept constant,
(g) rate of creaming will depend on droplet diameter. Bigger
Cohesiveness 0.94 ± 0.011 0.99 ± 0.018 0.99 ± 0.022 0.99 ± 0.025 droplet causes more creaming, which leads to poor sta-
Extrudability 25.1 ± 1.04 25.1 ± 1.25 25.8 ± 1.45 25.8 ± 0.95 bility of emulsion, whereas smaller droplet causes slower
(mJ)
creaming, hence better stability is the consequence. The
Mean value ± SEM, n = 3.
emulsions with smaller droplet are turbid in comparison
Droplet size to bigger droplet emulsion; which is determined by tur-
Droplets of dispersed phase have the tendency to bidimetry method29. For citronella oil emulsions highest
coalesce over the storage period, which increases the turbidity was found to be 89.12 ± 2.4 (CE 17, HLB = 12.6),
whereas for light liquid paraffin emulsion it was 91.2 ± 3.6
liquid paraffin was also determined simultaneously. ensure consistent quality of citronella oil cream formu-
Based on the above mentioned evaluation parameters lation. Table 5 exhibits the texture analysis data of citro-
rHLB of citronella oil and light liquid paraffin was found nella oil cream formulation.
to be 12.6 and 11.8, respectively. Reported rHLB of the Spreadability of cream, lotion or gel depends upon the
later is in the range of 11 ± 119,20. Experimentally deter- ingredients used33,34. For instance products with rich con-
mined rHLB value of both citronella oil and light liquid tent of lipid/high molecular weight wax are less spread-
paraffin by three different methods is shown in Table 4. able because of high viscosity and surface tension. The
After the determination of rHLB of citronella oil, it was male female probe (TA15/100: conical probe, Brookfield
implemented for the development of cream formulation. Engineering Laboratories, Inc. USA) for spreadabil-
Blend of Glycerol monostearate and Tween 80 in the ity evaluation is an imitation for human perception
ratio of 1:2.8 at 10% concentration could produce stable of spreading any cream over skin surface30,31. Certain
emulsion. These observations suggest that not only the amount of work is done by these probes to penetrate the
rHLB of oil phase but the appropriate concentration of sample (cream/gel/semisolid products) up to a definite
For personal use only.
emulsifiers is also crucial for the stable cream formula- depth and the energy (mJ) required for this purpose
tion. Further it was found that emulsifier with higher define the spreadability of the formulation. Higher firm-
HLB value (e.g. Sodium lauryl sulfate, HLB 40) could ness and hardness value implies a less spreadability and
stabilize the emulsion at lower concentration. Therefore vice versa. Spreadability of citronella oil cream was found
it can be inferred that the ratio and percentage of specific to be 1.8 ± 0.02 mJ at 25 ± 1°C. Table 5 exhibits the spread-
emulsifier blend is unique to the developed formulation. ability data of citronella oil cream formulation.
If the emulsifiers with different HLB value are used, the Packaging of formulations is an important issue for
concentration of emulsifiers to stabilize the same emul- overall acceptance of product by end users. From con-
sion may vary. sumer’s compliance point of view, extrusion of cream/
lotion/gel from the container (tube, box) is a major con-
Texture profile cern35. A good product with poor extrudability may not
Consistency, firmness, adhesiveness and cohesiveness be acceptable. CR4 was evaluated for forward extrusion
are the different texture parameters that define a specific with TA-DEC probe and work done in extrusion was
type of formulation and imitate human perception for determined to be 25.1 ± 1.04–25.8 ± 1.45 mJ. It was found
any cosmetic/medicated products30,31. These parameters that forward extrusion of citronella oil cream was smooth
do not have any fixed selection criteria or any official and continuous. Table 5 exhibits the extrudability data of
standards (pharmacopoeial/regulatory), but based on citronella oil cream formulation. All the texture parame-
the product specific requirement, these parameters can ters of optimized cream formulation CR4 were reproduc-
be characterized and standardized. ible and consistence over the storage period of 3 months.
Firmness of any semisolid formulation is a reflection of
its hardness. It is the maximum positive force to deform/
Conclusion
penetrate the sample with finger30–32. Based on the type
of product, firmness should be defined. For citronella oil Based on the theory that emulsions with optimum emul-
cream, firmness was found to be 6 ± 0.25–7 ± 0.55 g over a sifier concentration result in smallest MDD, less percent
period of 3 months. Consistency of the sample is related increase in MDD upon storage and highest turbidity value,
to the work done to hardness. For this cream, consistency the rHLB of citronella oil and light liquid paraffin was
was found to be similar over a period of 3 months as indi- found to be 12.6 and 11.8, respectively. Cosmetically ele-
cated by the work done to hardness, which was ranging gant citronella oil cream was developed with 10% emulsi-
from 0.8 ± 0.04 to 0.9 ± 0.06 mJ. fier (glycerol monostearate and Tween 80 in the ratio of 1:
Stickiness of semisolid formulation is a major issue 2.8) concentration. Citronella oil cream was evaluated for
for its acceptance, especially for cosmetic products. different texture parameters viz. consistency (0.8 ± 0.040