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Microencapsulation of Zanthoxylum limonella Oil (ZLO) In

.
Genipin Crosslinked Chitosan-Gelatin Complex for
Mosquito Repellent Application

Tarun K. Maji, Md R. Hussain


Department of Chemicill Sciences, Tezpur University, Assam-784 028, India

Received 30 July 2007; accepted 24 July 2008


DOllO.lO02/app.29001
Published online 13 October 2008 in Wiley TnterSCience (www.interscience.wiley com).

ABSTRACT: Essential oil containmg chitosan gelatin com- improved with the mcrease in the amOlmt of chitosan in chi-
plex microcapsules crosslmked with gem pin were prepared tosan-gel,'tin matrix as revealed by thermogravimetric anal-
by complex coacervation process. The effects of various pa- YSIS. FT-IR spectroscopy and differenlial scanmng
rameters such as oil loading, ratio of chltosan to gelatin, calorimetry study indicated that there was no significant
degree of crosslinking on oil content, encapsulation effi- interaction between chitosan-gelatin complex and oil. 02008
ciency, and the release rate of the essential oil were studied. WIley' Periodicals, Inc J Appl Polym Sci Ill. 779-785,2009
Scanning electron nucroscopy study indicated that the sur-
face of the microcapsules were more irregular as the amount Key words: chitosan; gelatin; essential oil; microencap-
of oil loading Increased. Thermal stability of microcapsules sulation; genipin; mosquito repellent

INTRODUCTION can cause physiological toxicity. Therefore, a system


is looked for which can produce product having ei-
Recently, considerable efforts are made worldwide
ther very less or nil toxicity. Genipin, a natural
to proJ'!lote the use of environmentally friendly and
crosslinker, can react spontaneously with amino
biodegradable natural insecticides and repellents. A
acids or proteins. Its toxicity is much less than glu-
large number of essential oils have been evaluated
taraldehyde. 23 Chitosan, gelatin, and genipin are nat-
and forind to possess mos~uito repellency against
urally occurring materials and have attracted much
various mosquito vectors. -7 The essentIal oil
attention from scientists all over the world. The
obtained from 21lntlwxylum limonella (ZLO) has been
v"hole system will be fully biodegradable. Genipin
found to possess mosquito repellent properties
crosslinked alginate-chitosan microcapsule for live
against different mosquito vectors. 8 However, the
cell encapsulation was reported by Chen et a1. 2.t
repellency of these plant based products is lower
Chen et al. 25 investigated the flu orogenic characteris-
both in efficacy and duration than those of synthetic
tics of chitosan-genipin reaction for microencapsula-
repellents. Furthermore, essential oils are subjected
tion purposes.
to environmental deterioration by heat, humidity,
The present work 1S aimed at to produce chito-
light, and oxygen. 9
san-gelatin complex mlcrocapsules containing ZLO
Controlled release by microencapsulation seems to
by complex coacervation technique using the. natural
be the b~st way to protect essential oil from environ-
crosshnker, genipin. Efforts have also been made to
mental damage and thus securing a long shelf-life. 10
study the release characteristics of oil from micro-
The vast majority of publications on microencapsu-
capsules prepared under different conditions
lated repellents are patents. l l Coacervation,12-17 mo-
lecular inclusion,18 and spray drying9,19 techniques
are generally used for microencapsulation. EXPERIMENTAL
Varieties of crosslin king agents like glutaralde-
hyde, formaldehyde, epoxy compounds 20-22 are Materials
reported to be employed for improving the con- Gelatin type B from Bovine skin with a bloom
trolled release behavior. These crosslinking agents strength", 225 and chitosan with a medium molecu-
lar weight vyith Brookfield viscosity '" 200 cps were
Correspondellce to: T K. Maji (tkm@lezu.ernet.in). purchased from Sigma-Aldrich (USA). Sodium
Contract grant sponsor: DI{L, Tezpur, india
hydroxide (E. Merck, Mumbai, India), glacial acetic
. Journal of Applied Polymer Science, Vol. 111, 779-785 (2009) acid (E. Merck, India), Tween 80 (E. Merck), Genipin
© 2008 Wiley PeriodIcals, Inc. (Mol. wt. ,226.22) (Challenge Bioproducts Co.,
780 MAJI AND HUSSALN

Taiwan), and silicone oil (Ranbaxy Fine Chemical,s, range 0.005 to 0.1 gilOO mL, a sharp peak at 256 nm
Delhi, India) were used as such received.: TJ;1e core was noticed. 'The absorbance values at 256 run
material, essential oil from ZLO, was extracted in ,obtained "yith the respective concentrations were
our laboratory. DOl (double-dIstilled deionized) recorded and plotted. From the calibration curve,
water was used throughout the study. Other the unknown concentration of ZLO was obtained by
reagents used were of analytical grade. knowing the absorbance value

Extraction of essential oil


Encapsulation efficiency, oil content, and oil load
The seeds of ZLO, a big tree available in Tezpur,
were collected and shed dried, Essential oil was A known amount of ac.curately weighed microcap-
obtained by steam distillation of the seeds.' The oil sules was grounded in a crucible, transferred with
precaution to a volumetric flask containing a known
obtained was separated from the aqueous phase and
dried by treating with anhydrous sop.ium sulfate. amount of 0.3 wt % aqueous Tween 80 solution, and
The dried oil was transferred into a dark glass bottle kept for about 3 days with continuous stirring to
ensure complete extraction of oil in Tween 80 solu-
and kept inside the refrigerator at low temperature
for subsequent use. tion The encapsulation efficiency (%), oil content
(%), an9. oil loading (%) were calculated by using
the calibration curve and the following formulae
Microencapsulation procedure
To a beaker, certain ammmt of 2% (w Iv) chitosan Encapsulation efficiency (%) = WI/W2 X 100
solution previously made in 1% (v Iv) aqueous acetic
Oil content (%) = wI/w x 100
acid and 2% (w Iv) aqueous gelatin solutJon were
taken. Total amount of polymer was kept constant at Oil load (%) = WdW3 x 100
1 g. The mixture of polymer solution was stirred by
mechanical stirrer under high agitation after adding where w, weight of microcapsules; WI, actual amolmt
one drop of silicon anti foaming agent at 40"C. The of oil encapsulated in a known amount of microcap-
temperature was maintained at 40°C. To this, essen- sules; w~, amount of oil introduced in the same
tial oil (1-4 mL) was added under high agitation to amount of microcapsules; and W3, total amount of
form an emulsion. Using O.lN NaOH the pH of the polymer used including crosslinker.
emulsion was brought to the range of 5.4-5.9 to
attain the maximum coacervation. Once the coacer-
vation took place with the formation of microcap- Oil release studies
sules, the system was brought to room temperature
('" 30°C) to harden the microcapsules. The crosslink- Oil release studies of encapsulated oil were done by
ing of the polymer capsule was achieved by slow using UV-visible spectrophotometer (UV-200l Hita-
addition of certain amount of -genipin (0.05-0.5 chi). A known quantity of microcapsules was placed
mmol/ g of polymer) solution (0.5% w Iv aq. solu- into a known volume of 0.3 wt % Tween 80 surfac-
tion). The temperature of the vessel was then raised tant solution. The microcapsule-Tween 80 mixture
to 40°C and stirring was continued for about 3-4 h was magnetically stirred at a constant rate and the
in order to complete the crosslinking reactlOn. The temperature throughout was maintained at 30°C
vessel was then cooled to room temperature. The (room temperature). An aliquot sample of known
microcapsules were filtered, washed with 0,3% volume (5 mL) was removed at appropriate time
Tween 80 surfactant solution, dried and stored intervals, filtered and assayed spectrophotometri-
inside a refrigerator in a glass ampule. cally at 256 nm for the determination of cumulative
amount of oil release up to a ti.me t. Each determina-
tion was carried out in triplicate, To maintain a con-
Measurements stant volume,S mL of 0.3 wt % Tween 80 solution
Calibration curve of oil was returned to the container.
A cahbration curve IS required for the determination
of release rate of oil from the microcapsule~. It was
Scanning electron microscopy study
found that 1 g of oil could be easily dissolved in
100 mL of water. containing 0,3 g Tween 80. The samples were deposited on a brass holder and
A known concentration of essential oil in DOl sputtered with gold. Surface characteristics of the
water containing 0.3 wt % Tween 80 was scanned in microcapsules were studied using scanning electron
the range of 200-400 nm by using UV visible spec- microscope (model JEOL, JSM-6360) at an acceler-
trophotometer. For ZLO having concentration in the ated voltage of 10-20 kV and at room temperature.
Journal of Applied Polymer Science 001 10,1002/app
MlCROENCAPSULATlON OF Zanthoxylum ll1llonelln OIL 781

Thermal properties study determined by measuring the coacervate yield as


well as turbidity.
Thermal properties of chitosan, gelatin, ZLO, and
Celatin and chitosan solutions were mixed at differ-
ZLO containing microcapsules were evaluated by
ent ratio (1 : 1 to 1 : 40) at room temperature under
employing thelmogravimetric analyzer (TCA) and
stirring condition. The pH of the solution, prepared at
differential scanning calorimeter (DSC). TCA study
different ratio, was varied from 5.0 to 6.0. In this pH
was carried out using TCA (model TA 50, shi-
range, no precipitation of chitosan occurred and also
madzu) at a heating rate of 10°C/min up to 600°C.
it :·vas above the isoelectric point of gelatin. Turbidity
DSC study was done in a differential scanning calo-
would appear due to the formation of coacervate par-
rimeter (model DSC-60, shimadzu) at a heating rate
ticles. The change in transmittance due to turbidity
of IO°C/min upto 400°C. Both the studies were done
was monitored using UV spectrophotometer at 450
under nitrogen atmosphere.
nm. The pH at which maximum absorption noticed
was recorded. The coacervate yield was measured at
fourier transform infrared (FTIR) study different pH by decanting the supernatant and drying
the coacervate phase. The optimum raho of gelatin-
FrIR spectra were recorded using KBr pellet in
chitosan and pH at which max'imum coacervation
a Nicolet (model Tmpact-410) spectrophotometer.
observed were 1 : 10 and 5.9, respectively. Similar
Microcapsules, chitosan, gelatin, and ZLO were each
results were reported by Lopez and Bodmeler. 26
separately finely grounded with KBr· and FTIR spec-
tra were recorded in the range of 4000-400 cm -1.
Oil release studies
RESUL TS AND DISCUSSION Effect of variation of oil loading on release rate
Pure gelatin B solution was scanned between 450 The effect of variation of oil loading on encapsula-
and 600 nm at different pH using UV spectropho~ tion efficiency and release rate for I : 1 chitosan-gel-
tometer. The % transmittances studied in the above atin microcapsules are presented in Table I and
wavelength were found to follow more or less simi- Figure 1. The more the oil-load, the higher was the
lar trend at different pH. For chitosan, the % trans- release rate. The lower in encapsulation efficiency
mittance at the above scaruled wavelength remained might be due to the higher % of oil loss during isola-
unchanged up to a certain pH (~ 6.00), beyond that tion of microcapsules.
the % transmittance decreased due to precipitation. At low oil load, small oil droplets were formed as
Chitosan-gelatin mixture of different ratios the dispersive force of the stirrer was more effective.
showed ):he trend similar to those of chitosan. How- The % of chitosan-gelatin mixture was enough to
ever, in the case of both chitosan and chitosan/ gela- encapsulate properly the oil droplets. With the
tin mixture, the maximum absorption occurred at incrcase in oil-load, the dispersive force of the stirrer
lower wavelength. Therefore all the successive meas- became less efficient which resulted in the formation
urements were done at 450 nm and reported. of large oil droplets. At this stage, chitosan-gelatin
To optimize the coacervation behavior, tl.1C study mixture cO\lld be able to. encapsulate the large oil
of phase separation behavior is essential. ThIS was droplets only at the expense of decrease in thickness

TABLE I
Effect of Variation of Oil Loading, Chitosan to Gelatin Ratio, and Genipin
Concentration on the Behavior of Microcapsules
Sample parhculars
Chitosan (gm) : Genipin Oil load Oil content EncapsulJ tion
Gelatm (gm) (mmol) ZLO (mL) (%) (%) efflciency (%).
0.25·1 O.OS 4 308.75 26.45 == 1.20 3414 ± 1.74
066· 1 005 4 30875 25.15 :!: 057 32.47 ± 1.07
2.1 0.05 4 30875 3065 ± 0.54 3956 ± 1.74
4.1 005 4 30875 37.65 ± 075 48.60 ± 1.14
1.1 D.D5 1 77.20 22.32 ± D.l5 48.31 ± 0.84
1: I 0.05 2 154.37 23.68 ± 051 44.3 ± 0.35
1:1 0.05 3 231.56 28.0 ± 0.12 32.87 ± 0.96
1:1. 0.10 4 280.27 42.0 ± 0.45 54.22 ± 1.12
1:1 0.20 4 236.60 4534 ± 087 58.53 ± 1.36
1: I 050 4 161.26 46.50 ± 0.64 60.05 ± 0.89

Total polymer = 1 g; genipin == (0.05-0.5 mmol/gm of polymer; oil == (1-4 mL); water
= 100 mL; Temperature = (40 ± 1)"C.

Tournai of Applied Polymer Science 001 1O.1002/app


782 MAJI AND HUSSAlN

10 100

SO
GO
III

i7'O
:EO
.Ja
~«>
=
~010
~30

20 L~~~de
10 II) ~
O~~---r--~--r-~---r--'---~~---'
0
0 10 20 110 ~ 60 110 10 110 110 100
o ro ~ ~ ~ ~ R 10 U ~ 100
TirIuo.h nn•. h

Figure 1 Effect of variation of oil loadmg on release pro- Figure 2 Effect of variation of chitosan to gelatin ratio on
file. (a) Polymer 1.0 gm, crosslinker 0.05 mmol, ZLO 1.0 mL; release profile. Total polymer 1.0 gm, ratio of chitosan to
(b) polymer 1.0 gm, crossJinker 0.05 mmol, ZLO 2.0 mL; gelatin m (a) 0.25 . 1; (b) 0.66 : 1; (c) 2 : 1; (d) 4 : 1, ZLO
(c) polymer 1.0 gm, crosslinker 0 05 nunol, ZLO 3.0 mL 40 mL; crosslmker 0.05 mmol.

of microcapsule wall. Besides this, the amount of during the study of the release behavior of triclosan
. chitosan-gelatin mixture might not be sufficient to encapsulated within chitosan-gelatin microcapsules .
encapsulate all the oil droplets. Some oil droplets Both oil content (%) and encapsulation efficiency
might present without encapsulation. These oil were also found to increase with the increase in the
droplets might get exhausted during recovery of chitosan concentration. As explained earlier, the
microcapsules. As wall thickness decreased, the dif- increase in viscosity of the medium resulted in
fusional path for the oil became short27,2~ which the formation of large oil droplets. These large oil
resulted in an increase of release rate. droplets had a tendency to coalesce at higher oil
Again oil content (%) was found to increase with load to form further large oil droplets and therefore
the increase in the % of oil load. At low oil load, more oil could be encapsulated with the same
many of the microcapsules probably contained few amount of encapsulating material.
oil droplets indicating that there was an abundance
of encapsulating polymer for the oil present. As oil
load ('Yo) increased, the number of oil droplets in the Effect of variation of concentration of genipin on
release rate
microcapsules increased which resulted in an
increase in oil content. Results showing the oil load (%), oil content (%) and
encapsulation efficiency are shown in Table I. The
release profile of the oil is shown in Figure 3. The
Effect of variation of chitosan/ gelatin ratio on trend shown by both oil loading and oil content was
release rate as per expectation. Encapsulation efficiency increased
The effect of variation of chitosan-gelatin ratio on oil 71
loading, encapsulation efficiency and release rate are
shown in Table I and Figure 2. The release rate of oil 6.
was governed by the o,{, of chitosan present in the chito-
san-gelatin mixture. With the increase 10 the concentra-
tion of chitosan in chitosan-gelatin mixture, the release
f'..
~

rate was found to decrease. Again an increase in the vis- g 3'


'tJ
cosity of the chitosan-gelatin mixture was noticed with
~
'lit
2t -I>
the increase in the concentration of chitosan. -<

The higher viscosity might decrease the dispersive 11


force of the stirrer. As a result large oil droplets were
formed. The decrease in surface area could be respon- o tID 10 70 08 eo 100
sible for the decrease in release rate. Moreover, chi to- T..... h
san has more average moieties of primary amine
groups than gelatin. Chitosan could react with genipin Figure 3 Effect of variatIOn' of crosslinker concentra-
tion on release proftle. (a) Polymer 1.0 gm, crosslinker
to form sufficient crosslink bridges compared with gel- 0.1 mmol, ZLO 4.0 mL; (b) polymer 1.0 gm, crosslinker
atin. This might also playa role in reduction of release 0.2 mmol, ZLO 4.0 mL, (c) polymer 1.0 gm, cross linker
rate. Similar observations were r~ported by Kim et al 29 0.5 mmol, ZLO 4.0 mL.

JOllrnal of Applied Polymer Science 001 1O.1002/app


MICROENCAPSULATlON OF Lanthoxylu11l IImonelln OIL 783

FIgure 4 Scam-ung electron rruClogIaph~ of mICrocapsules prepared '\lth Oll load ('Yo) (a) 15437, (b) 30875, (c) 61702,
(d) 15437 (after 011 rdea~e)

wIth the ll1Crea6e m gempm concentratIOn The con- of 011 The burface of the mlcrocap~ule6 con tamed a
centratIOn of gempm was vaned from a 1 to 050 'ilgnlficant numbel of pm holes (arrow marked)
mmol/g of polymer mIxture The mClea::.ed effICIency These pm holes might be formed due to the release of
was due to the hIgher 011 retentIon capacIty of the 011 by dlffu'iIOn Moreover, on phYSical venficatJOn,
mIcrocapsules caused by the formatIOn of crosshnk- the mICrocapsules prepared at higher Oil loadmg
mg The cros~lmkmg reachon took place between appeared OIly and agglomerated where as tho::.e pre-
gempm, gelatm, and chltoc;an The release rate of 011 pared at low OIlloadmg appeared dry and powdery
was found to decrease as the % of gempm mCl eased
The mIcrocapsule wall became compact a::. degree of
crosslmkmg mcrea'ied ThIS re'iulted m the decrease ThermogravImetric analYSIS
of dIffuSIOn rate through the mIcrocapsule ,·vall Simi- Table II showb the mlhal decompositIOn tempelature
lar fmdmgs were cIted m the hterature 1030 (T,) and residual weIght (RW, %) of vlrgm polymer,;
(chltosan and gelatm), ZLO and ZLO contammg
Scarming electron microscopy study TABLE II
Scannmg electron mlcrobcopy (SEM) mlcrograph~ of Thermal Analyhcal Data for Vlfgm Polymer and OIl
Contammg MIcrocapsules
gempm crosshnked dutosan-gelatm microcapsules
havmg dIfferent percentage of 011 content ale ~hown SamplE' palhcu!ar:,
m FIgure 4 At low Oliloadmg [FIg 4(a)], the burface Gelatm (gm) 011 RW(%)
of the microcapsules appeared smooth compaled Chltosan (gm) (mL) T,CC) ilt 600 "C
With those of microcapsules prepared at hIgher all J 0 236 875
loadmg [FIg 4(b,c)] At hIgher OIlloadmg, a burstmg 1 05 40 175 933
look was observed due to the presence of large per- ! 1 40 190 2306
centage of 011 Sirrular observatIons were reported In 0 1 273 3774
Olla
the hterature 10 14 The burface of the mlcrocapbule6
became more megular as the percentage of 011 load- T" Imtlal d€'compo<;ltlOn temperature, RW, lesldua!
mg mcreabed Figure 4(d) bhow::. the microgiaph of \\ eIght
the microcapsule,; after release of 'iubc;tanhal amount 1 Stal ted decompo'img flom the vely begmnmg

Journal of Applted Polymer SClellLc DOL 10 1002/app


784 MAJI AND HUSSAlN

TABLE III
Temperature of Decomposition (TD) at Different Weight Loss (%) of Virgin Polymer and
Oil Containing Microcapsules
Temperature of decomposition (To) (0C)
Sample particulars at dIfferent welght loss (%)
Gelatin (gm) : Chitosan (gm) Oli (mL) 20 40 60 70 80
1:0 286 331 394 438 529
1 : 0.5 4 236 300 354 370 446
1'1 4 200 302 366 448
0:1 294 320 543
Oil 90 115 155 228

microcapsules. Both the Ti (0C) and RW ('Yo) were tosan. The reaction rate of chitosan and genipin was
found to increase with the increase in chitosan con- reported more compared with that of gelatin?l So
centration in the chitosan-gelatin mixture. The chitosan could form more crosslink bridges com-
decomposition of ZLO started at an early stage and pared with that of gelatin and thereby would lead to
there was no residue at 600°C. more thermally stable microcapsules.
Temperature of decomposition (To) values of The difference in T, values for vClrious samples
ZLO/chitosan/gelatin microcapsules, chitosan, gela- could be explained on the baSIS of their difference in
tin and oil at different weight loss (%) are shown in rate of decomposition. The crosslinking reaction of
Table III. T D values for the microcapsules increased . genipin with chitosan was higher compared with
with the increase in the % of chitosan in the micro- that of gelatin as per explanation given above. More-
capsules. This observed high values might be due to over oil decomposed at fast rate. Both of these influ-
the decreasing chance of elimination of small mole- enced the rate of decomposition and were
cules like NH 3, CO 2, etc. with the formation of cross- responsible for different T, values.
linking by genipin. Gelatin contains lower 01<. of
lysine and arginine residues as primary amll1e
groups. Chitosan contains gluco~amine unit in larger FTlR study
percentage. Genipin could react with the pnmClry
amine group of gelatin and glucosar11ine unit of chi- FTIR spectra of chltosan, gelatin, ZLO, and chi to-
san/gelatin microcapsules containing ZLO were
recorded and presented in Figure 5. The spectrum of
chitosan displayed a strong amide characteristic
peak at 1632 cm- 1 . Similarly gelatin spectrum also

J;
..
==

1
3alO ~ 2500 2000 1eoo 1000 SIO 100.00 200.00 300.00 COO.IO
WU\'C number (ern ') Tempertturc(C)-

Figure 5 FTTR spectra of (a) geJatlll B, (b) ehitosan, (e) Figure 6 DSC thermograms of (a) chitosan, (b) gelatin B,
oli, (d) oil contaIning microcapsules. (c) oil, (d) oil containi.ng microcapsules.

Journal of Applied Polymer Science DOl IO.1002/app


MiCROENCAPSULATiON OF Zanthoxylum llmonelln OIL 785

showed an ammo band at 1547 cm- l and carbonyl to decrease as the concentration of chltosan m the dl1-
peak at 1624 cm- l In ZLO, the peaks appeared tosan-gelatm mixture mcreases SEM study show1>
between 1638 and 1720 cm- 1 were due to carbonyl that the surface of the mIcrocapsules became Irregular
stretchmg band Besides thiS, the other notable peaks due to presence of Oil Thermal stabIlIty has been
appeared at 1457 cm- 1 and 1378 cm- l were due to found to be 1l1l.proved WIth the mcrea5e m the per-
CH 2 asymmetnc deformation and ,CH 2 symmetrIc centage of chltosan lli the chltosan/gelatIn matnx A
deformation In the mlcrocapsules, the carbonyl low compatibility lli thermal properties lli the I elation
band &hlfted to 1641 cm- 1 mdICatmg an mterachon between 011, gelahn, and chltosan eXIsts as revealed
between chltosan and gelatm complex The posItion by DSC study FTIR .,tudy shows that there IS no
of these peaks remamed almost unchanged when remarkable lliteractlon between polymer and 011
compared wIth that of &pectrum of ZLO The POSI-
tion of other peaks which were due to CH 2 asym- References
metnc deformatIOn was also remamed unchanged
Thl<; suggested that there was no slgmfICant mterac- 1 ['>man, M B Pe~hc Outlook 1999, 10, 68
2 Peterson, C J, Coats, J R Pe,tIc Outlook 2001, 8, 154
tIon between ZLO and dutosan gelatin complex 1 An~an, M A, Vawdevan, p, Tand(ln, M, Razdan, R K
BlOresour Techno1 2000, 71, 267
4 Omolo, M 0, Okmyo, D, Ndlege, I 0, Lwande, W , Ha,~a­
Differential sc~nning calorimetry study nal!, A PhytochemIstry 2004, 65, 2797
The DSC thermogram of pure crutosan (a), pure gel- 5 Chalthong, U , Kamsuk, K, Choochote, W , Jltpakdl, A, Tlp-
pawangkosol, P, R'yong, D, Pltasawat, B Fltoterapla 2007, 77,
ahn' B (b), OJI (c), and 011 loaded chitosan/gelatm 359
mIcrocapsules (d) are presented In Figure 6 Pure 6 Tawatsln, A , Wralten, S D, Scott, R R, Thavara, U, Techa-
chitosan 1>hovVed peaks at 98°C, 271°C, and 340°C, damrongsm, Y J Vector Etcl 200L 26, 76
respectively Pure gelatm B showed peaks at 95°C 7 Plta'XlWat, B, Kam~uJ.., K, Choochote, W, Chalthong, U,
Jltpakdl, A, Tlppawangkosol, p, Rlyong, D Parasltol Res
and some multiple peaks In the temperature range
2007, 100, 339
226-323°C Pure 011 showed a peak at 90°C and 8 D.1s, N G, Baruah, 1, Talukdar, P K, Das, S C J Vector
another bload peak havmg average peak tempera- Borne DJ' 2003, 40, 49
ture at 200°C Oil encapsulated chitosan/gelatm 9 Edns, A, Bergn,taN, B Nahrung/Food 2001, 45, 133
mICrocapsules showed a sharp peak at 120"C and 10 MaJl, T K, Baruah, I, Dube, S, Hl1~'>dm, M R BlOre~our('e
Technol 2007, 98, 840
another tvvo peaks (m shoulder fmm) havmg avel-
11 Calton, J G, Siemer, R S Wood, I L US Pat 6,180,127
age peak temperature at 240°C and 320°C The peaks (2001)
appeared m the temperature range 95-98u C ...vere 12 Rosenbldt, J , Magd"%I, 5 ,Garh, N J MlcroenLapsul1989, 6, 515
due to the removal of mOisture The posItion of one 13 Bachtsl, R A, Klppamsldt's, C J Control ReI 1996,38, -19
peak appeared m the thermogram (not shown) of 14 Chan, L W, Lim, L T, Heng, P W S J MicroCnCdpS111 2000,
17, 757
phYSICal mixture of chltosan/ gelatm/ Oil at 95°C was
15 Legrand, J , Mauguet, M C, Brujes, L, Carnella, G, Larre, C,
found to dIsappeared and a new peak appeared Popmcilu, Y J 1vhcrocncap~ul 2002, 19,377
(shown at 120"C) when gempm was used (CIOSS- 16 KIm, J C, Song, ME, Lee, E, Park, S, Rang, M J, Ahn, H
lmked samples) The posItion of other two peaks m J J DI'> SCI Technol 2001, 22, 591
the thermogram of phySIcal mIxture remamed 17 Xmg, F, Cheng, G, Yang, B, Ma, L J Appl Polym SCI 2004,
91, 2669
almost unchanged Irrespective of addltIon of gem-
18 D71e7ak, J D Food Technol 1988,42,136
pm The peaks found at 240°C and 320°C m cross- 19 Grosso, C R F, Tnndadc, M A J MKroencapsul2000, 17, 169
lmked 011 loaded microcapsules were mam]y due to 20 Nlmm, ME, Cheung, D, Kodama, M, SheIkh, K Colldgen,
the decompoSItion of 011 and cruto&an-gelatm com- CRC Press Boca Ranton, FL, 1988
plex respectIvely The pOSItion of these peaks exhlb- 21 GOISSIS, G, JuntO!, E tv! , Marcantomo, R A C, Lta, R C C,
CanClan, D C J , Oe Caevallho, W M BlOmatenals 1999, 20, 27
lted m both the thermograms of phySIcal mIxture-
22 NOl~hlkl, y, Kodalfa, K, Furu~e, M, Mlyatil, T U SPat
and cros&lmked 111lcrocapsules suggested that a low 4,806,599 (1989)
compatibility 111 thermal propertIes eXisted III the 21 Sung, H W, Huang, L L H, T~aJ, C C J BlOmater Sci Polym
relatIOn between oll and gelat1l1-chltosan complex Ed 1999, 10, 63
24 Chen, H, OUyilng, W, LauduYI, B, Martol1l, C, Praka~h, 5
BlOmacromolecules 2006, 7,2091
CONCLUSIONS 25 Chen H, Ouyang, W , LauduYI, B, M"rtol1l, C, Praka~h, S
J BIOInt'd Mater Res A 2005 75, 917
The 011 from ZLO can be encapsulated successfully 111 26 LopeL, C R, Bodmeler, R Int J Pharmacul 1996, 135,63
the chltosan-gelatl11 matnx usmg gellJpm as ClOSS- 27 S~nJokovlc, R, JalsenJuk, L J ['harm Pharmacol 1%1,33 279
hnker The release rate of 011 depends on 011 content, 28 l\ladan, P L J Phann Su 1988, 70,430
29 KIm, J C, Song, M [, Lt'E', E J, Park,S Rang, M J J.hn
crosshnkmg den&lty, polyme\ concentratIOn, etc The
1\1 J J 01, ScI Technol 2006, 22, 591
release rate Increases With the 1I1crease 111 the 011 load- 10 Dma] "and, R, Mahmood], S, Faruoud, E, Saleh], M, Artyabl,
mg The higher the percentage of gempl11, the lower I~ FActa Pharm 2005, 55, 57
the release rate The release rate ha& also been found 31 MI, F L BlOmacromolccl1le~ 2005, 6, 975

!ournlll of AppllCd Polymer SCience 001 10 1002/app

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