Study of Forced Degradation behavior of Atazanavir
Angirekula Narendra*, Mukthinuthalapati Mathrusri
Annapurna
Department of Pharmaceutical Analysis and Quality
Assurance, GITAM Institute of Pharmacy
GITAM (Deemed to be University), Visakhapatnam-530045,
India
*Corresponding Author E-mail:
naren_angirekula@yahoo.com
ABSTRACT:
A
modified simple and sensitive stability indicating RP-HPLC method has been
developedfor the determinationof Atazanavir in presence of its degradant
products on isocratic mode. The method was validated and forced degradation
studies were performed as per ICH guidelines. Hypersil ODS C-18 Column
(250mmx4.6 mm, i.d.5µ particle size) using methanol:tetra butyl ammonium
hydrogen sulphatemixture with flow rate 1.0 ml/min are the chromatographic
conditions for the present study (UV detection 247 nm) (Isocratic mode).
Atazanavir was eluted at 4.86 min within the total run time of 10 min.
Atazanavir shows linearity 0.5-200 µg/mL (r2 = 0.999). The method
was validated and found to be specific as the degradants were not at
allinterferingwith Atazanavir.
KEYWORDS:
Atazanavir, Stabilityindicating,HPLC, ICH Guidelines.
INTRODUCTION:
Atazanavir (Figure 1) is an antiretroviral drug1.
Literature review describes some of the HPLC methods used for the determination
of Atazanavir 2-6 and in the present study the authors have studied
the forced degradation behavior of Atazanavir in presence of its degradants.
Figure 1: Chemical structure of Atazanavir
MATERIALS
AND METHODS:
Atazanavir
was procured as gift sample from HeteroDrugs (India). Methanol(HPLC Grade),
tetra butyl ammonium hydrogen sulphate(TBAHS) and hydrogen peroxidewere
purchased from MERCK (India). Atazanavir capsules are marketed with brand
namesVirataz (Hetero HC (GenX) (Label claim: 300 mg) and ATAZOR (Label
claim:100, 150, 200 and 300mg) (Emcure. ARV). The HPLC system is of Model SPD
10A Shimadzu LC-Class-Vp version 6.12 equipped with UV-VIS detector and binary
gradient pump (20µl).
Chromatographic
separation was achieved on Hypersil ODS C-18 column (250mmx4.6 mm; i.d.5µ
particle size) using Methanol:10mMtetra butyl ammonium hydrogen sulphate
(85:15) as mobile phase. Flow rate was maintained at 1.0 ml/min with UV
detection at 247 nm. Atazanavir (1000µg/ml) stock solution was prepared in
methanol and diluted with mobile phase. 10 mM tetra butyl ammonium hydrogen
sulphate was prepared, sonicated and filtered.
Method
validation:
The
method was validated by evaluating precision, accuracy, linearity, specificity,
LOD, LOQ and robustness7. 0.5 to 200 µg/mL Atazanavir solutions were
prepared from the stock on dilution with mobile phase and 20 µL of each
solution was injected (n=3) in to the HPLC system and the mean peak area of the
chromatogram was noted. Calibration graph was plotted with concentration versus
mean peak area.Intraday and inter-day precision were performed as per the ICH
guidelines same day and on three consecutive days respectively. Accuracy of the
method was achieved by standard addition method while robustness wasconducted
by introducing deliberate alterations in the optimized conditions such as flow
rate (± 0.1mL), mobile phase ratio (± 2%), pH (± 0.2 units) and detection wave
length (249 nm& 245 nm).
Experimental
applicability to Atazanavir capsules:
Atazanavir
capsules from the two available brands were bought from pharmacy and content
equivalent to 25 mg Atazanavir was extracted with methanol, sonicated, filtered
and diluted with mobile phase. These solutions(n=3) were injected and the mean
peak area was noted from the respective chromatograms obtained.
Forced
degradation studies:
Forced
degradation experiments were performed by treating Atazanavir with different
stress conditions. While performing acidic and alkaline degradations drug
solutions were neutralized and then only diluted with mobile phase. 30% v/v H2O2
was opted for oxidative stress.Thermal degradation and photolysis were
also performed and 20 µL of each solution was injected in to the system and peak
area was noted from the respective chromatograms.
RESULTS AND DISCUSSION:
Method optimization and validation:
A
simple stability indicating RP-HPLCwasestablished for the quantification of
Atazanavir in capsules using methanol and 10mMtetrabutyl ammonium hydrogen
sulphatemixture as mobile phase. During the method development C8 phenomenex
column was initially used with a mixture of mobile phases such as acetonitrile and
formic acid; methanol and formic acidand different aqueous buffers in
combination with acetonitrile and methanol but in some or other manner the
system suitability parameters were not satisfied. But usage of Hypersil ODS C-18 Column with methanol and TBAHS
(85:15, v/v) mixture with 1 ml/min flow rate finally results acceptable system
suitable parameters and Atazanavir was eluted at about 4.8 minFigure 2. The present proposed method was compared
with the reported methods in Table 1. The proposed method was validated and a
calibration curve was shown in Figure 3 demonstrating that Atazanavir obeys
Beer- Lamberts law 0.5 to 200 µg/mL (Table 2) with regression equation y =
20873x + 7458.6 (Correlation coefficient 0.9999). The LOD and LOQ are found to
be 0.1342 µg/mL and 0.413 µg/mL respectively. Intraday and inter-day precision
were studied and % RSD was found to be 0.13-0.65 (Table 3) and 0.17-0.21 (Table
4) respectively. The % RSD in accuracy was found as 1.01-1.39 (Table 5).
Table. 1. Comparison of previously reported HPLC
methods of Atazanavir with the present
|
Mobile phase (v/v) |
Wavelength (nm) |
Linearity |
Ref |
|
0.02M Ammonium dihydrogen phosphate: Acetonitrile: Methanol (30:25:45) |
288 |
5-50 |
2 |
|
Methanol: Water (90:10) (pH adjusted to 3.55 with Acetic acid) |
249 |
10-90 |
3 |
|
Ammonium dihydrogen phosphate buffer: Acetonitrile (55:45) (pH 2.5) |
288 |
30-600 |
4 |
|
Potassium dihydrogen phosphate buffer: Acetonitrile (55:45) |
248 |
25-150 |
5 |
|
Water: Acetonitrile (20:80) (pH adjusted to 3.0) |
255 |
10-80 |
6 |
|
Methanol: 10 mM Tetra butyl ammonium hydrogen sulphate (85: 15) |
247 |
0.5-200 |
Present work |
Table. 2. Linearity studyof Atazanavir
|
Conc. (µg/mL) |
*Mean peak area |
% RSD |
|
0.5 |
10851 |
0.22 |
|
1 |
21901 |
0.16 |
|
2 |
42446 |
0.51 |
|
5 |
103527 |
0.72 |
|
10 |
200733 |
1.20 |
|
20 |
392991 |
1.40 |
|
50 |
1014722 |
0.11 |
|
80 |
1658900 |
0.60 |
|
100 |
2075264 |
0.22 |
|
120 |
2490685 |
0.43 |
|
150 |
3155763 |
0.55 |
|
200 |
4157282 |
0.71 |
*Mean of three
replicates
Table.
3. Intraday precision study of Atazanavir
|
Conc. (µg/ml) |
*Mean Peak Area |
Statistical Analysis |
|
*Mean peak area ± SD (% RSD) |
||
|
20 |
392991 |
392777±2551.739 (0.65) |
|
20 |
390125 |
|
|
20 |
395215 |
|
|
50 |
1014722 |
1015055±4335.621 (0.43) |
|
50 |
1019548 |
|
|
50 |
1010896 |
|
|
100 |
2075264 |
2072349±2602.653 (0.13)
|
|
100 |
2071523 |
|
|
100 |
2070259 |
*Mean of three
replicates
Table. 4. Inter day precision study of Atazanavir
|
Conc. (µg/ml) |
*Mean Peak Area |
*Mean peak area ± SD (% RSD) |
||
|
Day1 |
Day2 |
Day3 |
||
|
20 |
382568 |
381256 |
381155 |
381660±788.259 (0.21) |
|
50 |
1002562 |
1001211 |
1004528 |
1002767±1667.975 (0.17) |
|
100 |
20506582 |
20593561 |
20555769 |
20551971±43613.726 (0.21) |
*Mean of three
replicates
Table. 5. Accuracy study of Atazanavir
|
Conc. (µg/ml) |
Conc. (µg/ml) |
*Mean conc. (µg/mL) ± SD (% RSD) |
% Recovery |
||
|
Formulation |
Pure drug |
Total |
Obtained |
||
|
10 |
5 |
15 |
15.1 |
15.07 ± 0.1527 (1.01) |
101.3 |
|
10 |
5 |
15 |
14.9 |
||
|
10 |
5 |
15 |
15.2 |
||
|
10 |
10 |
20 |
19.9 |
19.97 ± 0.2082 (1.04) |
99.8 |
|
10 |
10 |
20 |
20.2 |
||
|
10 |
10 |
20 |
19.8 |
||
|
10 |
15 |
25 |
25.6 |
25.23 ± 0.3512 (1.39) |
100.9 |
|
10 |
15 |
25 |
24.9 |
||
|
10 |
15 |
25 |
25.2 |
||
Figure 2: Typical chromatograms A) Blank B) Atazanavir
standard (20 µg/mL) C) Atazanavir capsules (20 µg/mL)
Figure
3: Calibration curve of Atazanavir
Experimental
applicability to Atazanavir capsules (Assay):
The
percentage of purity of Atazanavirwas found to be 99.63-99.63 in the marketed
formulations and the results were tabulated (Table 6) and there is no
interference of excipients (Figure 2c).
Table. 6. Assay
of Atazanavir capsules
|
Brands |
Label claim (mg) |
*Amount found (mg) |
*Recovery (%) |
|
I |
300 |
299.53 |
99.84 |
|
II |
300 |
298.89 |
99.63 |
* Mean of three replicates
Stress
degradation studies:
Atazanavir
has shown less than 20 % degradationin all the stress studies indicating that
Atazanavir is highly resistant and the resulting chromatograms during this
study were shown in Figure 4. The system suitability parameters were within the
acceptance criteria (Table 7).
Table.
7. Stress degradation behavior of
Atazanavir
|
Stress Conditions |
% Drug recovered |
% Drug decomposed |
Tailing factor |
Theoretical plates |
|
Standard drug |
100% |
- |
1.129 |
5269 |
|
Acidic Hydrolysis (0.1N HCl, 30 min at 60°C) |
95.8% |
4.2% |
1.381 |
5482 |
|
Alkaline Hydrolysis (0.1N NaOH_30 min at 60°C) |
82.6% |
17.4% |
1.348 |
5698 |
|
Oxidative degradation (3% H2O2 30 min at 60°C) |
96.4% |
3.6% |
1.143 |
5487 |
|
Thermal degradation (80°C, 12 hrs.) |
98.9% |
1.1% |
1.269 |
5367 |
|
Photolytic degradation (24 hrs.) |
99.2% |
0.8% |
1.367 |
5984 |
Figure
4: Chromatogram of Atazanavir (20 μg/ml) on A) Acidic degradation B)
Alkaline degradation C) Oxidative degradation
D)
Thermal degradation E) Photolysis
CONCLUSIONS:
The
proposed stability indicating method for the determination of Atazanavir is
specific and there is no interference of the degradants with the drug peak and
at the same time there is no interference of the excipients. This method can be
applied for the routine assay of Atazanavir in capsules.
ACKNOWLEDGEMENT:
The
authors are grateful to Hetero Labs Ltd. (India) for providing the gift samples
of Atazanavir. The authors do not have any conflict of interest.
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Received on 08.08.2018
Modified on 16.08.2018
Accepted on 23.08.2018
© RJPT All right reserved
Research J. Pharm. and Tech
2018; 11(8): 3693-3697.
DOI: 10.5958/0974-360X.2018.00678.9