Effect of Different Polyoxyethylene Matrices on Extended Release Formulation of Cephalexin Trihydrate

 

Sarita Garg1, Meenakshi Bhatia1 and Pradeep Kumar2*

1Division of Pharmaceutics, Department of Pharmaceutical Sciences,

Guru Jambheshwar University of Science and Technology, Hisar-125001, Haryana, India

2Chitkara College of Pharmacy, Chandigarh Patiala National Highway, Rajpura-140401, Patiala, Punjab, India

 

ABSTRACT

The present study was undertaken to evaluate the effect of different viscosity grades of polyoxyethylene, their content level and the method of tablet preparation on the release profile of cephalexin trihydrate from matrix systems. Matrix tablets were prepared using Polyox N-10, Polyox N-80, Polyox N-60 K, Polyox 301 and Polyox 303 as rate-retarding agents by direct compression process. The release of drug from these hydrophillic matrices was studied over 12-hours in buffer media of pH 1.2. Statistically significant difference was found among the drug release profile from different matrices. The release kinetics was found to be governed by the type and content of hydrophillic materials in the matrix. Tablets granulated by PVP K-30 solution have higher hardness than those prepared by direct compression. However, drug release was not influenced by the method of tablet preparation. Formulations containing Polyox N-60K, Polyox 301 and Polyox 303 released 82%, 76% and 70% of the drug respectively, indicating that increasing viscosity can drastically reduce the release rate. Further, a decrease in polymer concentrations resulted a slight increase in thickness and friability, while a increase in polymer level resulted a increase in hardness and decrease in release rate. Numerical fits indicated that the formulations followed the Zero order release pattern which was further confirmed by the domination of super case-II transport in polyox tablets.

 

KEYWORDS: Polyoxyethylene, Cephalexin trihydrate, hydrophilic matrix, release kinetics

 

INTRODUCTION

The development of oral modified-release dosage forms has attracted much attention in recent years. Many strategies are available for design and development of modified-release drug delivery formulations.1-2 The primary purpose of these drug delivery devices is to improve the state of disease management by modifying the pharmacokinetic profiles of therapeutic agents normally administered as conventional tablets. Conventional oral dosage forms often produce fluctuations of drug plasma level that either exceed safe therapeutic level or quickly fall below the minimum effective level; this effect is usually totally dependent on particular agent’s biological half-life, frequency of administration, and release rate. It is recognized that many patients can benefit from drugs intended for chronic administration by maintaining plasma levels within a safe and effective range.3 Cephalexin is a broad spectrum bactericidal antibiotic. It is almost completely absorbed from the gastrointestinal tract, its plasma half-life is about 1 h, and more than 80% of the dose is excreted unchanged in the urine during the first 6 h.4 However, because the physical properties of the trihydrate are superior to those of the tetra- and monohydrate, a number of attempts have been made in recent years at the production of trihydarte. As compared with the tetrahydrate, the trihydrate has higher nascent oxygen content, and it can be stored better at higher temperatures as a result of its higher melting point and its low water vapor partial pressure.


Compared with the monohydrate, trihydrate has advantages also; for instance, it possess a better mechanical stability and a better ability to be stored, the monohydrate being hygroscopic.5 The use of CR formulations offers many potential advantages like sustained blood levels, attenuation of adverse effects, and improved patient compliance, it is realized that in case of antibiotics with short half-life, it is necessary to maintain the constant blood levels as otherwise microorganisms will become resistant to the antibiotic. Therefore, formulating cephalexin in CR dosage forms will increase the therapeutic efficacy and patient compliance.6

 

Therefore, to reduce the frequency of administration and to improve the patient compliance, an extended release formulation of cefalexine trihydrate is desirable. The most commonly used method of modulating the drug release is to include it in a matrix system. Hydrophilic polymer matrix systems are widely used in oral controlled drug delivery because of their flexibility to obtain a desirable drug release profile, cost effectiveness, broad regulatory acceptance and no complex production procedures such as coating and pelletization are required. Hydrogels are being increasingly investigated for controlled-release. In addition the hydrogels have the ability to release the entrapped drug in aqueous medium and to regulate the release by controlling the swelling. Hydrogels can be applied for the release of both hydrophilic and hydrophobic drugs and charged solutes.7

 

Polyox (Polyethylene oxide) is the most commonly and successfully used hydrophilic retarding agent for preparation of oral controlled drug delivery systems. Polyox resins are among the fastest hydrating water-soluble polymers in pharmaceutical systems. They very quickly form hydrogels that initiate and regulate release of active ingredients. Systems using Polyox resins are often superior to others in approaching zero order release models. Polyox resins are available in wide range of molecular weight.8 Maggi et al., 2002, reported that higher molecular weight polyethylene oxide swells to greater extent and tends to form, upon hydration, a stronger gel, which is therefore less liable to erosion, if compared to the lower molecular weight polyethylene oxide.9

 

In the present study, various matrix systems were designed and tested for extended delivery of cefalexine trihydrate. The objectives of the study were (I) to investigate the performance of hydrophilic matrix system with polyethylene oxide in extending the release of drug and (II) to find out the release kinetics and mechanism of release from these matrices.

 

MATERIALS AND METHODS:

Materials:

Cephalexin trihydrate was a kind gift sample from Ranbaxy Research Laboratories, Hoshiarpur, PB, India. Polyethylene Oxide (Polyox) of different grades was obtained from Dow Chemical Company, USA. Polyvinylpyrrolidone (PVP K-30) was obtained from BASF Corporation, USA. Microcrystalline cellulose (Avicel PH-101 and Avicel PH-102) and Lactose monohydrate (Phramatose 200M) were obtained from FMC Biopolymer, USA and DMV International, Netherlands, respectively. Magnesium Stearate and Colloidal Silicon Dioxide were obtained from Mallinckrodt, USA and Evonik Industries, Germany, respectively.

 

 

Table 1: Composition with different method of preparation in Polyox matrix

 

mg/tab

 

Ingredients

15 B

20 A

 

Cephalexin Trihydrate

200

200

 

Avicel PH 101

111

-

 

 

Avicel PH 102

-

115

 

Polyox 301

75

75

 

PVP K-30

10

-

 

Water

q.s.

-

 

Magnesium stearate

4.0

2.0

 

Aerosil 200

-

8.0

Total weight

400

400

 

 

 

Methods:

Batch 15B was prepared by wet granulation method and other batches by direct compression method. Polymers of different grades and levels were adopted to obtain an optimized composition as shown in Table 1, Table 2 and Table 3.

 

Procedure for direct compression:

Drug, diluent and polymer were weighed accurately, sifted through BSS #30 sieve and they were mixed in a polybag properly for 10 min. Blend was lubricated for 2 min and compressed into tablets (400mg) using a round punch (10.5 mm) (Cadmach Machinery Co. Pvt. Ltd., India).

 

Procedure for wet granulation:

All intragranular ingredients were weighed accurately and sifted through BSS #30 sieve. The premix was granulated with a 10%w/w Polyvinylpyrrolidone (PVP K-30 grade in water) binder solution. The wet granules were dried in a lab scale fluid bed drier or by using tray drier at a temperature of 600C till a LOD of less than 2.0% (1050C, 10 min) was achieved. Dried granules were sized, lubricated and compressed into tablets using a round punch of size 10.5 mm for 400mg tablet and caplet punch of size 20´9 mm.

 

Assessment of tablets:

Tablets were assessed for the following parameters:

Weight variation:

Total weight and individual weight of 20 tablets were checked using electronic weighing balance (ER 200 A, Afcoset, India).

 

Hardness:

Hardness of tablets (5 units) was determined by using Schleuniger hardness tester (VK-200, Schleuniger Pharmatorn, Switzerland).

 

Thickness:

Thickness of tablets (5 units) was measured by using Digital Vernier Caliper (500-144, Mitutoyo, Thailand).

 

Friability:

Preweighed tablets (10 units) were placed in Roche’s Friabilator (Serwell Instruments) and subjected to 100 rotations in 4 minutes. The percentage difference between initial and final weight (after dedusting) was calculated.

 

 

 

 


Table 2: Composition with different level of Polyox N -60K, Polyox 301 and Polyox 303

 

mg/tablet

Ingredients

23D

23E

11A

15A

20A

23A

20B

11B

23B

23C

Cephalexin trihydrate

200

200

200

200

200

200

200

200

200

200

Avicel 102

55

115

55

90

115

140

165

55

115

140

Polyox N-60 K

135

75

-

-

-

-

-

-

-

-

Polyox 301

-

-

135

100

75

50

25

-

-

-

Polyox 303

-

-

-

-

-

-

-

135

75

50

Aerosil

8.0

8.0

8.0

8.0

8.0

8.0

8.0

8.0

8.0

8.0

Magnesium stearate

2.0

2.0

2.0

2.0

2.0

2.0

2.0

2.0

2.0

2.0

Total weight

400

400

400

400

400

400

400

400

400

400

 

 


Drug Content:

Tablets (10 units) were powdered using mortar and pestle. An amount equivalent to 50 mg drug was extracted with 200 ml of 0.1N HCl and sonicated for 30 minutes. The solution was filtered through nylon filter and properly diluted with 0.1N HCl. Drug content was then calculated spectrophotometrically with absorbance maximum set at 260 nm.

 

In vitro Release Study:

The level of the drug release from the tablets was measured by the paddle method at 50 rpm. Tablets equivalent to 75 mg drug content were placed in USP dissolution apparatus II (Distek Dissolution System-2100C, USA) in 900 ml hydrochloric acid 0.1N (pH 1.2), 37˚C containing sinker BSS # 10 and at different time intervals, 5 ml of the solution was withdrawn until 12 hr. An equal volume of the medium was introduced into the container after each withdrawal to maintain a constant volume. The amount of the drug release was measured spectrophotometrically employing a UV-spectrophotometer (Shimadzu UV-1601) at 260 nm. The mean values of drug released were plotted as percentage cumulative release vs. time.

 

Erosion study:

For conducting erosion studies, the dissolution jars were marked with the time points of 4, 8 and 12 hrs. One tablet was placed in each dissolution jar containing 900 ml of 0.1N HCl and the apparatus was run at 50 rpm using paddle. The tablets were taken out after completion of the respected stipulated time span as mentioned above. The wetted samples were then dried in an oven at 60 0C up to constant weight. The dried samples were weighed. The degree of erosion was determined using following formula:

 

% Erosion = (Initial weight of tablet - final weight of dried tablet)  ´ 100

                                       Initial weight of tablet

 

RESULTS AND DISCUSSION:

Polyox was used as matrix forming polymer. They very quickly form hydrogels that initiate and regulate release of active ingredients.

 

Effect of method of preparation:

Formulations were developed by wet granulation (15B) and direct compression (20A) method. Physical properties of developed tablets such as, average weight, hardness, thickness, friability and drug content were determined and shown in Table 4. Tablets granulated by PVP K-30 solution have higher hardness than those prepared by direct compression. These results might be ascribed to the better binding properties of the PVP K-30 solution in water. In vitro release profile of drug from 15B and 20A is shown in Figure 1.

 

Figure 1: Percentage drug released data depicting the effect of method of preparation (n=3).

 

No significant changes were found in drug release rate from 15B and 20A indicated that the drug release was not influenced by the method of tablet preparation (Figure 1). So further formulations were preceded by Direct Compression method because of low equipment costs, short processing time and limited steps. As has been found previously by Dow Chemical Company that Polyox resins perform well as binders in economical direct compression systems. They often provide better flow and compaction properties than other binders.10

 

Effect of different viscosity grades:

Formulations were designed with different viscosity grades of polyox. Formulations prepared with 70% Polyox N-10 (44A) and with 70% Polyox N-80 (44B). Other formulations were composed of 18.75% Polyox N-60K (23E), 18.75% Polyox 301 (20A) and 18.75% Polyox 303 (23B).

 

Physical properties are presented in Table 4.  In vitro release profile of drug from 44A, 44B is shown in Figure 2 and from 23E, 20A, 23B is shown in Figure 3.

 

Figure 2: Percentage drug released from matrices with 70% polymer content, (n=3).

 

Figure 3: Percentage drug released from formulations with different grades of Polyox.

 

Formulation 44A and 44B released 94% and 84%of the drug respectively, over 6 hrs (Fig. 2). Release was very fast even using high concentration of polymer that means the grades are not successful in controlling the drug release. To avoid the higher concentration (70%) of these polymer grades, we prepared other formulations with higher viscosity grades in low concentration.

 

Formulations containing Polyox N-60K, Polyox 301 and Polyox 303 released 82%, 76% and 70% of the drug respectively, over 12 hrs (Fig. 3). As we moved towards higher viscosity grades, there was decrease in release rate. Increasing viscosity can drastically reduce the release rate as observed in 44A and 23B due to large difference in molecular weight. These results might be attributed to the higher molecular weight polyox swells to greater extent and tends to form a stronger gel upon hydration, which is therefore less liable to erosion, if compared to the lower molecular weight polyox. These results are in confirmation with those obtained by Maggi L., 2004.9

 

Table 3: Composition with different viscosity grades of Polyox

Ingredients

23 E

20 A

23 B

44 A

44 B

Cephalexin trihydrate

200

 

200

 

200

 

200

 

200

 

Avicel 102

115

115

115

-

-

Lactose

-

-

-

90

90

Polyox N-10

-

-

-

700

-

Polyox N-80

-

-

-

-

700

Polyox N-60 K

75

-

-

-

-

Polyox 301

-

75

-

-

-

Polyox 303

-

-

75

-

-

Aerosil 200

8.0

8.0

8.0

-

-

Magnesium stearate

2.0

 

2.0

 

2.0

 

10

 

10

 

Total weight

400

400

400

1000

1000

 

 

Effect of polymer level:

Formulations were designed with Polyox N-60K, Poyox 301, and Polyox303 in different concentrations. Polyox N-60K formulations were prepared with 33.75% (23D) and 18.75% (23E) of polymer. Polyox 301 formulations were prepared with 33.75% (11A), 25% (15A), 18.75% (20A), 12.50% (23A) and 6.25% (20B) of polymer. Formulations composed of Polyox 303 were prepared with 33.75% (11B), 18.75% (23B) and 12.50% (23C) of polymer.

Physical properties data is presented in Table 4. In vitro release profile of drug from Polyox N-60K formulations, Polyox 301 formulations and Polyox 303 formulations is shown in Figure 4, Figure 5 and Figure 6 respectively.

 

Figure 4: Percentage drug released from different level of Polyox N-60K, (n=3).

 

Figure 5: Percentage drug released from different level of Polyox 301, (n=3).

 

Figure 6: Percentage drug released from different level of Polyox 303, (n=3).


 

Table 4:  Physical properties of tablets of Polyox formulations

Parameters

15B

20A

44A

44B

23E

20A

23B

11A

15A

20A

23A

20B

23D

23E

11B

23B

23C

Average wt. (mg)

404

398

1001

999

402

398

405

401

397

398

398

402

399

402

403

399

401

Hardness (Kp)

10 ±0.5

 

8.1 ±1.0

15  ±2

15  ±2

8 ± 1.0

8.1 ±1.0

8.6   ± 0.6

9.5   ± 0.5

9 

± 0.5

8.1   ± 1.0

8.0   ± 1.0

7.5   ± 1.2

8.5    ± 1.5

8      ±1.0

9      ± 0.7

8.6    ± 0.6

8.2     ± 0.5

Thickness (mm)

4.21 ±0.04

 

4.6 ±0.3

6.8 ±0.02

6.8 ±0.05

4.80 ±0.06

4.6  ±0.3

4.50 ±0.04

4.40 ±0.03

4.45 ±0.02

4.6  ±0.03

4.72 ±0.06

4.80 ±0.04

4.50 ±0.03

4.80 ±0.06

4.4 ±0.03

4.5  ±0.04

4.90 ±0.07

Friability (%)

0.08

0.10

0.20

0.18

0.14

0.10

0.08

0.03

0.08

0.10

0.12

0.13

0.06

0.14

0.06

0.08

0.10

Drug Content (%)

95.5

97.0

96

95

97.5

95.4

98

96

97.2

95.4

98.5

96.7

96

97.5

96.2

98

97.5

 


 

 

It was observed that decrease in polymer concentrations resulted in slight increase in thickness of tablet formulations (Table 4). These results might indicate that the polymers have high binding properties. The friability of prepared tablets increased by decreasing the polymer level. Decreased polymer concentration resulted in decrease in the hardness of the tablets. These results were in good agreement with those of thickness and friability.

 

Formulation 23D and 23E released 73% and 82% of the drug respectively, over 12 hrs (fig. 4). Drug release was slow by using 33.75% of Polyox N-60K as observed in 23D. Release profile matched with an ideal target in 23E, which was composed with 18.75% of Polyox N-60K.11

 

Formulations 11A, 15A, 20A, 23A and 20B released 67%, 69%, 76%, 84% and 90% of the drug respectively, over 12 hrs (fig. 5). Release profile was slow in 11A, 15A and 20A that were composed of 33.75%, 25% and 18.75% of Polyox 301, respectively. Release profile matched with target in 23A, which is having 12.5% of polymer. In formulation 20B release of drug was very fast from starting points, so 6.25% of Polyox 301 is not suitable for controlling the drug release.

 

Formulation 11B, 23B and 23C released 39%, 70% and 79% of the drug respectively, over 12 hrs (fig. 6). Drug release was very slow by using 33.75% of polymer in 11B. The drug release was slow also in 23B that was composed of 18.75% of Polyox 303. Formulation 23C which was composed with 12.5% polymer appeared to achieve our designed objective in terms of drug release.

 

It was observed that increasing the polymer level resulted in decrease in release rate. These results might be ascribed to the increase in polymer concentration increases the gel viscosity on the surface of tablets, which retards the diffusion of drug from the gel layer. These results are in accordance with the findings of Dow Chemical Company in Polyox brochure and Efentakis et al., 2000, also reported that an increase in content of polymer polyox results in a decrease in the release rate of drug.10, 12

 

Erosion study:

Since the rate of erosion may affect the mechanism and kinetics of drug release, the penetration of dissolution medium and the erosion of hydrated tablets; was determined. The percentage erosion of tablet at various time intervals is shown in Table 5 and figure 7. Figure 7 shows that 81%, 80% and 78% of tablet eroded in formulation 23E, 23A and 23C respectively, over 12 hrs after contact with aqueous medium.

 

 

Figure 7: Percentage erosion of tablet in selected formulations, (n=2).

 

Table 5: Erosion study for selected formulations

0.1N HCl/ 900ml/ USPII/ 50rpm/ #10 sinker

Time (hrs)

23E

23A

23C

0

0

0

0

4

28

33

26

8

60

61

58

12

81

80

78

 

Release kinetics and mechanism of release:

Drug release rate was predicted by fitting drug release data into different mathematical models to selected formulations (23E, 23A and 23C) based on release profile according to reference (Table 6).11 To know the mechanism of drug release from these formulations, the data were treated according to Zero order (cumulative % drug released vs time), First order (log of cumulative % drug remaining vs time), Higuchi’s (cumulative % drug released vs square root of time), Korsmeyer equation (log cumulative % drug released vs log time) pattern.13 When the data were plotted according to zero order equation, the formulations showed a fair linearity with regression values between 0.9945 and 0.9977, clearly indicating that the formulations followed the Zero order release pattern. The R2 value in case of first order equation was found between 0.5412 and 0.555 indicating that formulations did not follow first order release pattern. Similarly, the R2 value was found between 0.8205 and 0.8385 in case of Higuchi model indicating that formulations did not follow Higuchi’s release pattern.


 

Table 6: Drug release parameters from various mathematical models

Form.

Code

Zero order

First order

Higuchi

Peppas

Release Mechanism

k

r2

k

r2

k

r2

n

k

r2

23E

21.54

0.9945

0.0325

0.5412

74.873

0.8205

1.0764

1.2318

0.9948

Super Case-II

23A

23.20

0.9977

0.0325

0.5412

81.079

0.8385

1..0530

1.2988

0.9976

Super Case-II

23C

21.72

0.9960

0.0337

0.5551

75.669

0.8281

1.0646

1.2529

0.9968

Super Case-II

 

 


To confirm the Zero order release pattern, the data were further fitted into Peppas’s equation as the Peppas equation offers a clear illustration of drug release mechanism. The formulations showed good linearity (R2: 0.9948 to 0.9968), with slope (n) values ranging from 1.0530 to 1.0764 in polyox matrix tablets indicating that domination of super case-II transport in polyox tablets (Table 6). The n value nearer to 1 in all formulations, indicated the tendency towards drug release kinetics nearer to zero order.

 

CONCLUSION:

The present study was to carried out to make a comparative evaluation among the various grades of polyoxyethylene those can be potential candidates as release retarding agents. The study implies that, the kinetics and mechanism of release exclusively depends on the type and loading of these materials. A critical polymer-filler ratio is necessary to get an acceptable release profile and counter the complexities of sustained release effect. The wide range of matrix-formers available in this group endows the formulator with higher degree of flexibility, greater scope of optimization and wider approach to comply with compendial specifications. The study also reveals that, it is possible to formulate matrix tablet by appropriate combination of these hydrophillic matrices with rate controlling agents to get an acceptable pharmacokinetic profile in the fluctuating in vivo environment.

 

REFERENCES:

1.        Merkus FWHM. In: Rate Controlled Drug Administration and Action (Struyker- Boundier, H.A.J., Eds.), CRC Press, Boca Raton, FL, USA 1986; pp.15-47.

2.        Jantzen GM and Robinson JR. In: Modern Pharmaceutics (Banker, G.S. and Rhodes, C.T., Eds.), Marcell Dekker, Inc., New York, USA 1996; pp. 575-609.

3.        Cardinal JR. Matrix systems. In: Medical application of controlled release, Vol.1, Classes of systems (Langer, R.S. and Wise, D.L., Eds.),.CRC Press, Boca Raton, FL, 1984; pp. 41-67.

4.        M Horii, T Morinaga, S Shimada, T Takeuchi, H Yamanaka, T Nishimura, Y Noshi, T Okada, T Sasaki, S Ikeda, S Takada, O Iizuka, J Kimura, S Sagara, Y Inada, Y Nishioka and M Kimata. Double-blind comparison of L-keflex and cephalexin (Keflex) in dental infections. Jpn. J. Antibiot. 1980; 33: 1194–1214.

5.        Helmut Dillenberg, Helmut Honig and Rudolf Siegel, inventors; Kali-Chemie Aktiengesellschaft, Hannover, Germany, assignee. Method for producing sodium perborate trihydrate. US Patent 3,832,447. 1974.

6.        Agnihotri SA, Jawalkar SS and Aminabhavi TM. Controlled release of cephalexin through gellan gum beads: Effect of formulation parameters on entrapment efficiency, size, and drug release. European Journal of Pharmaceutics and Biopharmaceutics. 2006; 63: 249–261.

7.        Reza MS, Quadir MA and Haider SS. Comparative evaluation of plastic hydrophobic and hydrophilic polymers as matrices for controlled release. J. Pharm. Sci. 2003; 6: 282-291.

8.        Anonymous, The Dow Chemical Company, USA, Polyox water-soluble resins NF in pharmaceutical applications, 2004.

9.        Maggi L, Segale L, Torre M. Dissolution behaviour of hydrophilic matrix tablets containing two different PEOs for controlled release of a water-soluble drug. Biomaterials 2002; 23: 1113-1119.

10.     The Dow Chemical Company, USA, Polyox water-soluble resins NF in pharmaceutical applications, 2004.

11.     Richard I and Currie R. Novel formulations and method of treatment. United States Patent Application, publication no. US2004/0192690 A1, 2004.

12.     Efentakis M and Viachou M. Evaluation of high molecular weight polyox polymer: studies of flow properties and release rates of  furosemide and captopril from controlled release hard gelatin capsules. Pharmaceutical Development and Technology 2000; 5: 339-346.

13.     Shoaib MH, Tazeen J, Merchant HA and Yousuf RI. Evaluation of drug release kinetics from Ibuprofen matrix tablets using HPMC. Pak. J. Pharm. Sci. 2006; 19: 119-124.

 

Received on 22.10.2009

Accepted on 20.11.2009        

© A&V Publication all right reserved

Research Journal of Pharmaceutical Dosage Forms and Technology. 1(3): Nov. – Dec. 2009, 269-274