Preparation of Deproteinized Natural Rubber Latex and Properties
of Films Formed by Itself and Several Adhesive Polymer Blends
Wiwat Pichayakorn,*
,†
Jirapornchai Suksaeree,
†
Prapaporn Boonme,
†
Wirach Taweepreda,
‡
and Garnpimol C. Ritthidej
§
†
Department of Pharmaceutical Technology, Faculty of Pharmaceutical Sciences, and
‡
Department of Materials Science and
Technology, Faculty of Science, Prince of Songkla University, Songkhla 90112, Thailand
§
Department of Pharmaceutics and Industrial Pharmacy, Faculty of Pharmaceutical Sciences, Chulalongkorn University,
Bangkok 10330, Thailand
ABSTRACT: This work aimed first to prepare deproteinized natural rubber latex (DNRL) and investigate the properties of
films after it was blended with various adhesive polymers: hydroxypropylmethyl cellulose (HPMC), methyl cellulose (MC),
sodium carboxymethyl cellulose (SCMC), poly(vinyl alcohol) (PVA), poloxamer 407, and sodium alginate. The second aim was
to identify the films that would be the best for medical and pharmaceutical applications. Dibutyl phthalate (DBP), diethyl
phthalate, dibutyl sebacate, triethyl citrate, and glycerin (GLY) were used as plasticizers to improve the elasticity and
adhesiveness of the novel materials. DNRL was prepared by proteolytic alcalase enzyme treatment, followed by centrifugation.
The DNRL was virtually free of protein, produced no significant reaction in the rabbit skin irritation test, and formed a good
elastic film, but it had low skin adhesive properties. Blending DNRL with several polymers produced better films with different
elastic and adhesive properties. Moisture uptake and swelling tests indicated that its films provided increasing hydrophilicity
when blended with several polymers. SEM showed homogeneous films, and water hydraulic permeability tests indicated some
porosity in matrix films. Blending DNRL with HPMC or PVA and DBP or GLY produced films with the best potential for novel
materials. FT-IR, DSC, and XRD studies indicated the compatibility of the blended ingredients. In conclusion, DNRL blends
could be used suitably for medical and pharmaceutical applications.
1. INTRODUCTION
Natural rubber latex (NRL), the colloidal cis-1,4-polyisoprene
polymer obtained from Hevea brasiliensis, is a white or slight
yellow milky liquid that undergoes acid coagulation to an elastic
solid in 4-6 h at room temperature.
1
Freshly tapped latex
contains about 30% rubber fraction, 5% nonrubber, and other
components which are dispersed in water, the serum com-
ponent. The polymer from NRL has interesting physical prop-
erties such as high tensile strength, high elongation at break,
outstanding resilience, impermeability to gases and liquids, and
easiness of forming films.
2
However, the surface of rubber
particles is covered by a continuous monolayer of a negatively
charged phospholipid-protein complex that provides colloidal
stability.
3
There are 14 NRL proteins (Hev b1-14) recognized
by the International Union of Immunological Societies (IUIS)
as causative agents of NRL allergies.
4
Hev b1 and Hev b3 are
two of the major allergenic proteins. Hev b1 is found mainly on
large rubber particles, whereas Hev b3 is more abundant in
smaller rubber particles.
1
Deproteinized NRL (DNRL) pre-
pared by treatment with proteolytic enzymes that removed the
allergenic protein from fresh NRL has been reported else-
where.
5
However, there have been no reports about a specific
DNRL preparation that can be used for medical and phar-
maceutical skin applications, and for producing blends of DNRL
with other substances for formation of nonallergenic films.
Polymer patches are now effective alternative products for
transdermal drug delivery systems to deliver small drug mole-
cules into the systemic blood circulation. For the development
of transdermal drug delivery systems, polymer selection and
product design are important since they directly affect the
physicochemical properties, adhesion-cohesion balance, com-
patibility, and stability of the obtained products.
6
Many types of
polymers such as cellulose derivatives,
7
poly(vinyl alcohol)
(PVA),
8
chitosan,
9
and polyacrylate
10
are being used as mate-
rials to apply to the skin as gelling agents, thickening agents,
and film formers to control drug release.
6
However, there are
only a few reports about using NRL as a material for medical
and pharmaceutical skin applications.
11,12
Recently, applica-
tions of DNRL and its polymer blends in transdermal drug
delivery have been developed by our groups;
13-16
however, the
details of DNRL preparations and characterization have not been
given yet.
This research is focused on the preparation of DNRL and
the improvement of its properties by blending it with other bio-
adhesive polymers and plasticizers. Hydroxypropylmethyl cellu-
lose (HPMC), methyl cellulose (MC), sodium carboxymethyl
cellulose (SCMC), PVA, poloxamer 407 (P407), or sodium algi-
nate (SAG) was chosen to form blended polymers with DNRL.
Dibutyl phthalate (DBP), diethyl phthalate (DEP), dibutyl seba-
cate (DBS), triethyl citrate (TEC), and glycerin (GLY) were used
as plasticizers. The mechanical and physicochemical properties of
these polymers were investigated. Moreover, the feasibility of using
Received: July 25, 2012
Revised: September 16, 2012
Accepted: September 20, 2012
Published: September 20, 2012
Article
pubs.acs.org/IECR
© 2012 American Chemical Society 13393 dx.doi.org/10.1021/ie301985y | Ind. Eng. Chem. Res. 2012, 51, 13393-13404