Hybrid Advances 5 (2024) 100142

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Hybrid Advances
journal homepage: www.journals.elsevier.com/hybrid-advances

Designing aloe vera-sterculia gum based copolymeric hydrogel dressings

for drug delivery
Diwanshi Sharma , Baljit Singh *
Department of Chemistry, Himachal Pradesh University, Shimla, 171005, India

A R T I C L E I N F O A B S T R A C T

Keywords: Herein the present work, aloe vera (AV) and sterculia gum (SG) based polymer network hydrogels have been
Aloe vera designed for use in wound dressing and drug delivery (DD) applications. The hydrogels were prepared by graft
Sterculia gum copolymerization reaction of poly(2-(methacryloyloxy) ethyl trimethylammonium chloride) [poly (METAC)]
Antibiotic drug
onto AV and SG. Polymers were characterized by FESEM, SEM, EDS, AFM, C13 NMR, FTIR, XRD and TGA-DTG
Wound dressings
analysis. Swelling, drug delivery and biomedical properties of dressings have been evaluated. Sustained diffusion
of moxifloxacin drug from dressings exhibited a non-Fickian diffusion mechanism and the release profile was best
fitted in the Korsmeyer-Peppas kinetic model. Various interactions of polymers with blood and goat membranes
revealed the biocompatible and mucoadhesive nature of the dressings. Hydrogel dressings were found permeable
to O2 and water vapour and impermeable to microbes. Overall, these properties revealed that these hydrogels
could act as suitable materials for design of wound dressings. Furthermore, antioxidant properties of AV, wound
healing characteristic of SG, antibacterial properties of poly(METAC) and encapsulated moxifloxacin drug in
hydrogel dressings may enhance the wound healing potential of hydrogel wound dressings (HWD).

1. Introduction
Recently, considerable progress has been made in research area to
develop the materials for use in wound dressings. Chronic wounds have
affected a large world population both in terms of health and economy.
The rapidly spreading problems of wounds are responsible for great loss
of human life. Hence, cost-effective wound dressings for healthcare
deserve a special level of prioritization [1,2]. The development of
polysaccharide hydrogel wound dressing (HWD) materials is
well-recognized strategy in this area of research. Hydrogels developed
from bioactive polysaccharides exert their therapeutic effect in wound
healing, besides their ideal characteristic properties required for dres­
sing materials [3]. These HWD have been recognized as alternatives to
traditional dressing materials [4]. Polysaccharide-based hydrogels have
also been applied in drug delivery (DD) and tissue engineering appli­
cations beside their wound dressing applications [5,6]. Wounds treated
with bioactive polysaccharide aloe vera (AV) enhances wound healing
processes. The hyaluronic acid and dermatan sulphate in AV have
increased collagen formation by stimulating macrophage cytokine pro­
duction. Acemannan of AV acts as a macrophage stimulator. Presence of
ascorbic acid in AV enhances the collagen synthesis and counter
balances its breakdown [7]. The anti-diabetic effect of AV leaf extract
has been demonstrated by performing in vitro experiments on isolated
pancreatic islets of adult female albino rats. AV has been applied in
formation of various materials for use in biomedical applications. AV
extract in olive oil has been found helpful for chronic wound treatment
due to its antibacterial and anti-inflammatory properties. AV has also
been applied in the preparation of DD systems [8–12]. Joshy and co­
workers [10] prepared AV modified lipidic nano-composites which were
analyzed as nano-carriers of zidovudine medicine used for the treatment
of HIV.
Sterculia gum (SG) is an exudate extracted from the Sterculia urens
plant comprising of hetero-polysaccharides (glucuronic and galactur­
onic acids) along with galactose and rhamnoses units. SG is a biocom­
patible and antioxidant natural polymer that has been explored for
design of wound dressings for a better healing. It has been found
effective as wound and skin healing agent that increases cell prolifera­
tion and cell granulation during healing processes. It increases wound
closer or healing rate during healing process [13]. SG is also used in
pharmaceutical industries due to its high swelling, high viscosity [13],
antiulcer and cholesterol lowering activity [14,15]. SG based hydrogel
dressings have displayed buffer actions and bacteriostatic activity

* Corresponding author.
E-mail address: baljitsinghhpu@yahoo.com (B. Singh).

https://doi.org/10.1016/j.hybadv.2024.100142
Received 4 November 2023; Received in revised form 10 January 2024; Accepted 12 January 2024
Available online 14 January 2024
2773-207X/© 2024 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-
nc-nd/4.0/).
D. Sharma and B. Singh
during wound healing tests. Packing of SG powder in open wounds has
increased granulation tissue and resulted epidermal growth [16]. Its
exudates sorption and bacteriostatic effects at surgical site has reduced
various infections [17]. Teshima and coworkers [18] have demonstrated
the role of karaya gum adhesive in the prevention of infection at surgical
sites. Dhabhar and coworkers [19] prepared the karaya gum-derivatized
cellulose-poly(ethylene oxide) based copolymers for prolonged delivery
of drugs.
Poly(METAC) is a hydrophilic monomer containing -+N(CH3)3 units
which has been found to have biocompatibility, adhesion, and hydro­
philic properties. Matricardi and coworkers [20] prepared poly(METAC)
based alginate copolymers and reported their biocompatible and anti­
microbial properties. Moxifloxacin is a broad spectrum antibiotic drug
used for skin and wound infections especially those caused by antibiotic
resistant Gram-positive and Gram-negative bacteria. The mode of action
of drug involves inhibition of DNA gyrase, a type II topoisomerase, and
topoisomerase IV, an enzyme necessary to separate bacterial DNA
strands that inhibits cell division. Topical applications of moxifloxacin
on animal models have promoted wound healing processes [21,22].
Talekar and coworkers [23] have explained that the combination of two
or more than two herbal medicinal plant products can enhance their
therapeutic potential especially for wound healing.
The main objective of this study was the formation of dressing ma­
terials encapsulated with antibiotic drug. Herein present work, inclusion
of bioactive polysaccharides AV and SG in HWD along with the anti­
biotic drug moxifloxacin has been done for better wound healing. These
HWD were fabricated by grafting reactions which were performed by
free radical polymerization of poly(METAC) onto AV and SG poly­
saccharides in the presence of a crosslinker. The copolymeric hydrogels
were used to evaluate the water sorption, drug delivery and biomedical
properties. The swelling and drug release properties were evaluated
from drug encapsulated HWD. The biomedical properties of HWD like
blood compatibility, antioxidant activity, oxygen, water and microbial
permeability, mucoadhesion, mechanical properties, and antimicrobial
properties were also evaluated. This innovative approach aims to elevate
the dressing’s therapeutic potential by ensuring a gradual and sustained
delivery of the active compound (moxifloxacin) and contributing to­
wards healing process useful for better wound management.
2. Experimental
2.1. Materials used
2-(Methacryloyloxy) ethyl trimethylammonium chloride) (METAC)
[Sigma-Aldrich, Ukraine], Sterculia gum (SG) (Sigma-Aldrich, USA)
[molecular weight 9,500,000], Aloe vera (AV) (GIDC, Umargaon, -
Gujarat, India) [molecular weight of approximately 1000 kDa]. NNMBA
(Sigma-Aldrich, USA) and moxifloxacin was obtained from Cipla Ltd.
Mumbai, India.
2.2. Synthesis of hydrogel dressings
The synthesis of the hydrogel was done via copolymerization re­
actions. Covalent bonding was formed by the grafting of poly(METAC)
onto AV and SG to develop network structure in the presence of a cross
linker (NNMBA). Definite contents of monomer METAC (2.1 × 101
molL− 1), initiator APS (8.76 × 10− 3 molL− 1), cross linker NNMBA (0.51
× 10− 2 molL− 1), and plasticizer glycerol (2.73 × 10− 1 molL− 1) were
added into solutions of definite concentrations of SG (4 % w/v) and AV
(2 % w/v) after hydration. After stirring for 3 h at 100 rpm reaction
content was transferred to petri plates and polymer films were made by
the solvent casting method at 65 ◦ C for 2 h. The washing of hydrogels
was done by distilled water to remove the soluble content of the initi­
ator, crosslinker and monomer left as residue after polymerization re­
action. Thereafter, drying of polymer sample was performed under
reduced pressure at 45 ◦ C in a vacuum oven to maintain the shape and
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Hybrid Advances 5 (2024) 100142
structural integrity of HWD. The product was named as SG-co-AV-poly
(METAC) hydrogel films. Optimization of reaction conditions for the
synthesis of hydrogel dressings was done by varying monomer METAC
from 0.9 to 4.51 × 10− 1 molL− 1 and cross-linker NNMBA from 0.51 to
1.55 × 10− 2 molL− 1. The optimization of conditions was done by
varying METAC from 0.4 to 2.1 × 101 molL− 1 and [NN-MBA] from 0.51
to 1.55 × 10− 2molL− 1. The optimized parameters from swelling were
recognized as [sterculia gum] = 4 % (w/v), METAC = 2.1 × 101 molL− 1,
[aloe vera] = 2 % (w/v), [N,N-MBA] = 0.51 × 10− 2 mol/L, [APS] =
8.76 × 10− 3molL− 1 and glycerol = 2.73 × 10− 1 molL− 1. Copolymers
formed from optimized parameters were subjected to DD and biomed­
ical assays.
2.3. Characterizations
Characterization of SG-AV- cl -poly(METAC) copolymers was carried
out via FESEM, EDS, AFM, 13C NMR, FTIR, XRD and TGA. FESEM and
EDS were recorded on instrument (SU8010, Hitachi). Surface
morphology and roughness were studied by AFM (INTEGRA,NT-MDT,
Russia) in semi-contact mode, using antimony doped, N-type, single
crystal silicon probe, with resistivity (0.01–0.025 Ohm. cm) at a scan
frequency of 1 Hz.Imaging was done in 5 μm2 area, with set point cur­
rent 5 nA. The AFM images provide qualitative data (topographic im­
ages) as well as quantitative data (roughness). Images obtained were
processed by using NOVA Px software to calculate roughness of polymer
sample surface. FTIR of dried powdered samples was collected in KBr
pellets and FTIR was recorded on BRUKERALPHA-Platinum-ATR in­
strument. A solid state 13C NMR spectrum (JEOL ECZR Series 600 MHz
NMR Spectrometer, Japan) was recorded and instrument operated at
14.09 T magnetic field and at 600 MHz frequency for carbons. XRD was
taken from 2θ (10◦ to 80◦ ) (PAN-analytical X’pert Pro system, Nether­
land) and X-ray generator was operated at 40 kV and 40 mA using Cu-kα
radiation. TGA-DTG was recorded on METTLER TOLEDO-STARe TGA 2,
USA instrument by heating the sample between temperature range
25 ◦ C–800 ◦ C with heating rate 10 ◦ C/min in the presence of nitrogen
flow at flow rate 20 mL/min by taking alumina as reference.
2.4. Swelling and drug release properties
The swelling characteristics of copolymers were determined by the
gravimetric method [24]. The difference in gain in mass of the polymer
sample in simulated wound fluid (SWF) and other solution gave wound
sorption and swelling of copolymers [24]. Drug content during loading
& release was measured from calibration curves of moxifloxacin were
prepared in (distilled water (λmax = 290 nm), pH 2.2 (λmax = 295 nm),
pH 7.4 (λmax = 288 nm), and simulated wound fluid (λmax = 288 nm)
using UV visible spectrophotometer. Swelling equilibrium approach was
applied in drug impregnation by keeping polymers in known concen­
tration of moxifloxacin (500 μg/mL) at 37 OC temperature for 24 h.
Polymers were dried at 37 ◦ C and drug release was observed in different
releasing mediums. Diffusion mechanisms for drug moxifloxacin release
from polymer was evaluated by applying data in Ritger and Peppas [25,
26] equation (i)
Mt/M∞ = ktn (i)
Where, Mt/M∞ was fractional drug release in time t, k was constant and
n was diffusion exponent characteristic. Mt and M∞ were drug release at
time t and at 24 h respectively. Release data was applied to different
kinetic model equations to evaluate kinetic model [27,28].
2.5. Biomedical properties
The sorption of SWF by hydrogel was evaluated gravimetrically. The
biocompatibility test of HWD gave the thrombogenicity of materials by
gravimetric mass formed as clot while RBC rupturing by polymer
D. Sharma and B. Singh
expressed haemolysis which was analyzed by solution absorbance [29].
Mucoadhesive properties of dressings were determined with texture
analyzer using bio-membrane of goat intestine detachment force (Fmax)
and work of adhesion (Wad). Antioxidant properties were analyzed by
F–C reagent and DPPH assay [30,31]. O2 permeability was obtained by
Winkler’s method [32,33]. Permeability to water vapour (WP) was
carried out gravimetrically using the desiccant method. The porosity of
HWD was obtained by ethanol diffusion test. The pores formed in
grafted copolymer films in the presence of crosslinker were measured by
determining the porosity of network copolymeric hydrogels by alcohol
displacement method. Briefly, 0.2 g of copolymers was immersed in 10
mL of absolute ethanol for 24 h at 37 ◦ C in a sealed vessel. % porosity of
Fig. 1. FESEM images of (a,b) aloe vera (c,d) sterculia gum (e,f) SG-AV-cl- poly(METAC) polymeric films at different magnification.
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Hybrid Advances 5 (2024) 100142
copolymeric hydrogel was calculated using equation (ii).
W2 − W1
%Porosity = (ii)
ρV
Where, w1 (Initial weight), W2 (final weight), ρ (density of alcohol), and
V (volume of hydrogels).
The turbidity of nutrient broth gave microbial penetration through
HWD [32]. The mechanical properties, such as tensile strength (TS),
burst strength (BS), resilience, stress relaxation folding endurance and
gel strength, were determined were determined by using texture
analyzer equipped with 50 kg load cell [34]. TS of polymeric film of
fixed dimension (length = 50 mm, breath = 20 mm, thickness: 1 mm),
D. Sharma and B. Singh
was held between two clamps of texture analyzer, where the upper
clamp pulled the film in upward direction at a fixed speed of 0.5 mm/s
until it was broken. The breaking force of film (N) and extension in
length (mm) of the film at break were recorded. The length of polymer
film held within the clamps was 10 mm from each side.
For all other mechanical properties of polymeric film of fixed
dimension (length = 30 mm, breath = 30 mm, and thickness = 1 mm)
was used. For BS film was held in a sample holder, and ball probe (P/5s)
was pressed in downward direction at a prefixed speed and distance to
rupture film. Force (N) & distance (mm) at break were recorded. The
resilience of polymer film of fixed dimension was determined by moving
the instrument probe downwards to strain the film up to 2 mm distance.
The total work done for compression/return of the sample was recorded.
Fig. 2. (a) EDS (b) 3-D AFM image of SG-AV- cl -poly(METAC) polymer.
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Hybrid Advances 5 (2024) 100142
For the stress relaxation test of polymer film this constant strain was
applied for 30 s & relaxed force was recorded in terms of retained force
(%). During the folding endurance test, the polymer film was repeatedly
folded and de-folded at the same place until it breaks. Agar well method
was applied for antimicrobial test of grafted SG-co-AV-poly(METAC)
polymer [35] using S. aureus and P. aeruginosa bacteria.
3. Results and discussion
3.1. Characterizations
3.1.1. FESEM &EDS
FESEM images of AV, SG and SG-AV-cl-poly(METAC) are presented
D. Sharma and B. Singh Hybrid Advances 5 (2024) 100142

in Fig. 1. It demonstrated the change in the morphological features of AV

and SG after formation of network hydrogels. SEM images of HWD
revealed the heterogeneous morphology of copolymer surfaces in com­
parison to the smooth homogenous surfaces of SG and AV. Some irreg­
ular uneven morphology has also been ascribed to intermolecular
interactions among various constituents. The heterogeneous porous
morphology of HWD has helped to absorb wound fluids wherein a moist
environment could be maintained for better healing and to prevent
microbial contamination during wound healing. It has been considered
as useful for wound fluid sorption for hydrogel dressings. Kumar and
coworkers [36] have also reported that the morphology of surface got
changed into irregular and porous after grafting of METAC on to the
dextrin. Mandal and coworkers [37] have also demonstrated change in
morphology of polysaccharide grafted product of CMC- poly (METAC).
The EDS of SG-AV-cl-poly (METAC) was analyzed by characteristic
peaks of carbon, oxygen, nitrogen and chlorine elements appeared in
EDS spectrum (Fig. 2a). It revealed carbon = 37.2 %, oxygen = 52.1 %,
nitrogen = 3.0 % and chlorine = 8 % elements in cross linked copoly­
meric hydrogels. This may be because of graft copolymerization of poly
(METAC) onto SG in presence of the cross linker NN-MBA. After for­
mation of SG-AV-cl-poly (METAC) polymers, the presence of nitrogen
and chlorine depicted monomer METAC grafting onto SG-AV. Wang and
coworkers [38] also reported similar observations during the formation
of xylan-poly(METAC) copolymer.

3.1.2. AFM
AFM image of SG-AV-cl-poly(METAC) has illustrated surface topog­
raphy (Fig. 2b). The values of root mean square roughness and average
roughness were found 23.5 nm, 17.8 nm respectively. Visibility of some
valleys in AFM indicated heterogeneity in sample and surface roughness.
It may be due to the grafting of poly (METAC) onto SG-AV. A rough
surface in polymeric film can increase the film surface area and leads to
more absorption and drug diffusion. Rough surface of polymer matrix
can also increase cellular activities and cellular adhesion for a better
healing process during applications of copolymers as hydrogel wound
dressings. Grafting has induced surface roughness to polymer films
which has not only provided adhesion but has also enhanced absorption
of wound fluid from wound site. Zauro and coworkers [39] reported that
the grafting of METAC monomer onto pectin which has changed the
topography of polymeric films that led to the formation of a heteroge­
neous rough surface. Further rise in AV content has enhanced the
roughness in surface of materials composed of starch and chitosan [40].

3.1.3. FTIR
FTIR spectra of AV, SG and SG-AV-cl-poly(METAC) polymeric films
are presented in Fig. 3. The spectrum of grafted product SG-AV-poly
(METAC) demonstrated bands at 3286 cm− 1 [due to OH-bonded in­
teractions of SG and AV], at 290 3 cm− 1 [due to C–H asymmetric
stretching vibrations of SG,AV & poly(METAC)], 1721 cm1[due to C– –O
stretching of carboxylic acid SG,AV and poly(METAC) ester],1412
cm− 1[corresponds to the methyl of -+N(CH3)3 salt] [41], 1360 cm− 1
[due to –CH2 bending of SG,AV and C–N of quaternary ammonium
group poly(METAC)] [42],1034 cm− 1 [due to C–O–C stretching fre­
quency of gum and grafted poy(METAC)] and 1012 cm− 1 [due to C–N
bending vibration of quaternary nitrogen group present in poy
(METAC)] along with peaks found in FTIR of AV and SG [38,43]. Liu and
coworkers [41] reported that a peaks at 1728 cm− 1 and 1480 cm− 1 were
associated with the ester group of METAC and trimethyl group of qua­
ternary ammonium salt. Wang and coworkers [38] have also reported
spectrum of poly (METAC) with peak at 1718 cm− 1[due to C– –O
stretching of poly (METAC], and 947 cm− 1 [because of -+N(CH3)3 in
poly(METAC)]. Presence of bands at 1721 cm− 1 due to C– –O stretching
of poly(METAC) and at 1012 cm− 1 because of C–N bending vibration of
quaternary nitrogen of poly(METAC) indicated the grafting of poly
(METAC) and AV onto SG during copolymerization reactions.
FTIR spectrum of AV demonstrated peaks at 3253 cm− 1 [H-bonded
Fig. 3. FTIR spectrum of (a) aloe vera (b) sterculia and (c) SG-AV- cl -poly
(METAC) polymer.
interactions], 2889 cm − 1 (C–H stretching of aliphatic –CH and –CH2
groups), 1743 cm− 1 and 1602 cm− 1 (due to asymmetrical & symmetrical
stretching vibration of –COO- group and the presence of O-acetyl ester in
gel polysaccharide), bands at 1040 cm− 1 (C–O stretching associated
with rhamnogalacturonan, which is a side-chain constituent of pectin
present in the AV gel). Band at 849 cm− 1 and 781 cm− 1 were due to
glucose & mannose units present in the AV [44,45]. FTIR spectrum of SG
illustrated bands at 3360 cm− 1 [due to H-bonded interactions of –OH
groups], at 2914 cm− 1 [due to –CH stretching of –CH2 group], 1716
cm− 1 and 1601 cm− 1 (due to –C– –O stretching vibrations of carboxylic
acid of and methylated galacturonic acid ester of SG), at 1414 cm− 1(due
to –CH2 bending vibrations) and at 1043 cm− 1 (due to –C-O-C stretching
vibrations) [46].
3.1.4. 13C NMR
13
C NMR of AV, SG and SG-AV-cl-poly(METAC) copolymers are

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D. Sharma and B. Singh Hybrid Advances 5 (2024) 100142

represented in Fig. 4. 13C NMR of grafted copolymers revealed peaks at
177.35 and 173.09 ppm [C– –O of galactouronic acid of SG and AV along
with carbonyl carbon of poly(METAC)], at 102.19 ppm [anomeric C-1
carbon of galacto-glucopyranose ring of SG,AV], at 72.89 ppm [attrib­
uted to C-2 to C-5 of ring of galacto-glucopyranosyl of SG,AV], at 60.35
[-C-O-C of grafted monomer], 63.65 ppm [due to sequential methylene
group (-CH2-CH2–+N(CH3)3)], 54.56 ppm [sharpest characteristics peak
assigned to methyl carbon atom attached to quaternary nitrogen –+N
(CH3)3Cl group in poly(METAC)], at 45.30 ppm [due to carbon –
(–CH2–C(CH3)n-] of poly(METAC) [47], peak at 21.48 and 18.07 ppm

13
Fig. 4. C NMR spectrum of (a) aloe vera (b) sterculia and (c) SG-AV- cl -poly(METAC) polymer.

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D. Sharma and B. Singh Hybrid Advances 5 (2024) 100142

[corresponds to CH3 group of rhamnose of SG, and (–CH2–C(CH3)n-] of

poly(METAC)] beside the peaks observed in SG and AV [36].
NMR of AV demonstrated peaks at 182.5 ppm [because of carbonyl
carbon of acetylated mannans of AV], 102.7 ppm [due to anomeric C of
β-mannopyranosyl units], 97.01 and 92.9 ppm [due to α-and β-anomers
of glucose reducing units]. Spectrum also demonstrated peaks at 82.03
ppm [because of C-3 and C-5], at 72.77 ppm [C-2 and C-4] and at 60.7
ppm of C-6 and C-3 of CH2–OH of aloin component of AV [48,49]. NMR
spectrum of SG indicated these peaks at 173.6 ppm [C– –O group of
galactouronic acid], broad peak between 103 and 100 ppm [C-1 of
rhamnopyranose rings], 71.8 ppm [ring carbons i.e. C-2, C-3, C-4 and
C-5 of galactopyranose ring] and peak 20.7 ppm [due to -CH3 of
rhamnose residues] [50]. 13C NMR spectrum revealed the conversion of
monomer into polymer because there was no peak recorded around 135
ppm which illustrated conversion of sp2 carbon to sp3 carbon during
grafting &crosslinking reaction (CH2=CHX) to -(-CH2-CHX-)n- and this
peak was record at 45.30 ppm.
Further, there exist the correlation between spectral techniques for
the grafting of poly(METAC) onto polysaccharides. In FTIR spectra
bands were found at 1721 cm1 due to C– –O stretching of carboxylic acid
SG, AV and poly(METAC) ester and in case of 13C NMR of copolymers
revealed peaks at 177.35 and 173.09 ppm [C– –O of galactouronic acid of
SG and AV along with carbonyl carbon of poly(METAC)]. In FTIR
stretching frequency at 1412 cm− 1corresponds to C–N stretching of -+N
(CH3)3 group of poly(METAC) while in 13C NMR peak at 54.56 ppm
assigned to methyl carbon atom attached to quaternary nitrogen –+N
(CH3)3Cl group in poly(METAC)]. While band at 1034 cm− 1 [due to
C–O–C stretching frequency of gum and poly(METAC) grafted polymers]
and in 13C NMR spectra peak found at 60.35 was due to grafted carbon of
monomer i.e. -C-O. In FTIR spectra, stretching observed at1012 cm− 1
was due to C–N bending vibration of quaternary nitrogen group present
in poy(METAC)] while in13C NMR peak appeared at 63.65 ppm was due
to sequential methylene group (-CH2-CH2–+N(CH3)3)] of poly(METAC).

3.1.5. XRD
XRD analysis of AV and SG recorded broad peak at 2θ = 19.59 O and
O
20 respectively which revealed their amorphous nature (Fig. 5). There
was no sharp peak present in diffraction pattern of these poly­
saccharides. During XRD of grafted product SG-AV a broad diffraction
pattern peak was appeared at 2ϴ = 19.88O which demonstrated modi­
fication in amorphous region. Amorphous state of copolymers has been
found to be beneficial for various biomedical properties of the materials.
This region is important for fluid sorption and diffusion of drugs during
drug release analysis. Relaxation of the polymer chain occurred during
fluid absorption and transportation of drugs because of the presence of
amorphous region in hydrogel films. Heydarifard and coworkers [51]
reported that after the modification of chitosan by METAC led to a
change in crystallinity of the network structure this was due to the
destruction of H- bonded interaction of chitosan –NH2, –OH groups of Fig. 5. XRD spectra of (a) aloe vera (b) sterculia and (c) SG-AV- cl -poly
network hydrogels. (METAC) polymer.

3.1.6. TGA
Thermal degradation analysis of SG, AV and SG-AV-cl-poly(METAC)
copolymers is represented in Fig. 6. Thermal degradation (TD) revealed
that polymeric samples undergo degradation with a rise in decomposi­
tion temperature (DT). TG analysis copolymer of SG-AV-poly(METAC
revealed four stages TD after ignoring the initial stage of physically
sorbed water from grafted product. After loss of moisture in polymer
(about 12.9 % weight loss), first stage was started at initial DT 124.8 ◦ C
and ended at 205 ◦ C with 7.89 % weight loss and during this stage minor
degradation occurred because of loss of bounded water and glycerol
present in sample. The second decomposition stage was between 205
and 350 ◦ C (45.54 % weight loss) and it was the major stage of TD
wherein, maximum loss of weight of polymer sample occurred. It was
some condensation reactions which provided some degree of thermal
stability and thereafter gradual degradation of polymer sample took
place. It has been also been inferred from successive stages of TD. Hence,
third and fourth stages of DT were gradual and occurred between 350
and 540 ◦ C (with 15.92 % weight loss), & 540–790.5 ◦ C (16.798 %
weight loss) respectively with negligible residue left. These stages may
be due to de-polymerization and aromatization reactions. In these stages
scission of polymeric chains and fragmentation of sample occurred and
reduction in weight of sample was due to loss of volatile byproducts
[39]. These observations were further supported by DTG peaks appeared
at 179.6 ◦ C, 264.3 ◦ C, 361.1 ◦ C and 583.9 ◦ C corresponding to four
thermal degradation stages in which major peak observed at 264.34 ◦ C
(− 57.24 mg/ C) (due to major degradation reaction while other were
◦

due to decomposition of quaternary ammonium groups of poly(METAC) minor that indicated gradual degradation of polymer sample.
during TD. Thereafter, formation of cyclic anhydrides occurred due to

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D. Sharma and B. Singh
Fig. 6. TGA/DTG graphs of (a) aloe vera (b) sterculia and (c)SG –AV- cl -poly
(METAC) polymer.
AV illustrated two stages of TD after ignoring mass loss (6.095 %) up
to 161.20O C due to the desorption of water in AV during rise in DT. First
stage was recorded between 161.20 and 389.18 OC (66.72 % weight
loss) was attributed to a polysaccharide degradation reaction, while the
second stage was found between 389.18 and 678.89 OC (27.21 % weight
loss). SG also indicated two stages of TD and the first stage was between
186.73 and 398.08 OC with 49.58 % mass loss and second stage was
found between 398.08 and 710.95 OC with 30.81 % mass loss. Overall,
some degree of thermal stability has been induced after modifications.
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Hybrid Advances 5 (2024) 100142
3.2. Swelling properties
The influence of feed monomer and crosslinker content during the
synthesis of hydrogels in the reaction mixture influenced the network
density of hydrogel dressings (Fig. 7). With the rise in monomer content
from 0.5 × 10− 1 molL− 1 to 2.66 × 10− 1 molL− 1 during the synthesis of
hydrogels, swelling of resultant polymers enhanced. This may be
because of rise in the hydrophilicity of the copolymeric network with the
increase in METAC monomer content. More quaternary nitrogen groups
(–+NR3) groups in a hydrogel network enhanced the hydrophilicity of
the hydrogel and caused a greater affinity for water. This may be
probably because of the incorporation of polar vinylic monomers into
the hydrogels in the form of grafted and cross linked products. Ilgin and
coworkers [43] reported similar results and pH-sensitive water uptake of
poly (acrylamide-co-METAC)/montmorillonite - composite hydrogels
wherein swelling enhanced with rise in METAC concentration. The rise
in crosslinker NNMBA content in the reaction mixture from 0.51 × 10− 2
molL− 1 to 1.62 × 10− 2 molL− 1 during synthesis has developed the
network with a higher crosslinking density which reduced the swelling
of resultant hydrogels. The results demonstrated that cross linking
density of hydrogel dressings could be controlled by varying the cross­
linker content as per requirement of the wound fluid in the wound. The
rise in cross linker content increased covalent linkages between polymer
chains of SG, AV and poly(METAC) and as a result there was a reduction
in pore size between the network chains of HWD. Wang and coworkers
[52] also found the similar results of swelling of copolymers with an
increase in the content of crosslinker NNMBA. With rise in pH and
temperature of the swelling medium, the swelling of copolymers
increased. With rise in pH increased swelling was may be probably due
to opening of the pores of hydrogels dressings by ionic repulsions of the
polymeric chains caused by ionization of the functionalities of SG and
AV present in the hydrogel dressings. Swelling was observed more in
solutions of higher pH i.e. SWF, 7.4 pH buffer, as compared to 2.2 pH
buffer. This may be attributed due to various polar functional groups
such as carboxylic group (-COOH) in polymer matrix because of pres­
ence of AV and SG in hydrogels which at higher pH medium get partially
ionized and caused ionic repulsions which open pores and increase
water diffusion and swelling characteristic of hydrogel dressings. Zauro
and coworkers [39] also reported the similar trends of water uptake by
poly(METAC) copolymers in various pH mediums. Water diffusion into
hydrogels during swelling was approaching towards Fickian type
diffusion process. It was inferred from the values of the diffusion
exponent ‘n’ which were obtained to be less than 0.5 (see Table 1).
3.3. Drug release properties
The release of the drug moxifloxacin was found more in SWF as
compared to pH 2.2 buffer solution (Figs. 8a and b and Table 2). Higher
swelling of HWD in higher pH buffer was the reason for these trends of
drug release. The higher release of drug in SWF was occurred by virtue
of more diffusion rate of drug in SWF. The release occurred in sustained
manner which has been confirmed from values of the diffusion coeffi­
cient. The values of initial diffusion coefficient were found more than
the later time diffusion coefficient which illustrated that after main­
taining a certain concentration diffusion of drug occurred in a sustained
manner SWF. The release was not abrupt from drug encapsulated HWD.
Data of the release profile was applied to various kinetic models gov­
erning the release of moxifloxacin from films involving the Zero order
model, First order model, Korsmeyer-Peppas model, Higuchi model and
Hixson-Crowell model. Kinetic models were explained from values of
regression coefficients that indicated Korsmeyer-Peppas as best fitted
kinetic model for drug moxifloxacin release profile (Fig. 8b, Table 3). In
case of the Korsmeyer-Peppas kinetic model simple power law is obeyed
to describe moxifloxacin release mechanism from drug encapsulated
hydrogels. Sustained release was also observed in the fact that various
polymer drug interactions present because of different functionalities
D. Sharma and B. Singh
Fig. 7. Effect of (a) poly(METAC) (b) N,N-MBA(c) pH medium (d) temperature on swelling kinetics of SG-AV-cl-poly(METAC) polymers.
Fig. 8a. Release profile of antibiotic drug (a) moxifloxacin from drug loaded
SG-AV-cl-poly (METAC) hydrogels in different mediums at 37 ◦ C.
carboxylic (-COOH), (-OH), -N-C–O
– and quaternary ammonium salt
(–+N(CH3)3) of constituents of hydrogels and carboxylic (-COOH),
(OCH3),(NH2) constituents present in drug moxifloxacin.
9
Hybrid Advances 5 (2024) 100142
3.4. Wound fluid absorption
Hydrogel dressings absorbed 6.270 ± 0.33 g of fluid while kept in
SWF solutions for 24 h of swelling (Table 4). SWF sorption by polymeric
films was due to the hydrophilicity of HWD which comprises of various
polar functionalities such as carboxylic groups (-COOH), hydroxyl
groups (-OH) and quaternary ammonium salt (–+N(CH3)3) present in the
SG, AV and poly(METAC). Under SWF conditions of a solution of pH 8
functional groups present in the dressing get ionized and open network
pores because of ionic repulsion and simultaneously expand pore size in
copolymeric structure. It also enhanced polarity and hydrophilic nature
of functional moieties present in polymeric matrix. It revealed that these
HWD can provide moist surroundings to the wound site. Wound exu­
dates sorption property of HWD material was required for sorption of
excess exudates from wound site that can prevent wound mercerization.
The presence of large exudates in the wound site is responsible for mi­
crobial growth and microbial infections that made the wound chronic.
Peles and coworkers [53] prepared antibiotic loaded soy protein
hydrogels that provided protection to wound from mercerization. The
presence of covalent linkage in HWD can maintain the structural
integrity and stability of network hydrogel dressing. The AV-SG based
material could be applied as dressing for fluid absorption and to main­
tain their physical dimensions. Tolba and coworkers also reported [54]
copolymers that exhibited good capacity of wound fluid absorption.
Hence, these dressings can help in exudates uptake and can maintain
moist environment around wound to enhance healing process.
D. Sharma and B. Singh Hybrid Advances 5 (2024) 100142

Fig. 8b. Different drug release models for kinetics of release profile of moxifloxacin from drug loaded SG-AV-cl-poly(METAC)polymers in different mediums at 37 ◦ C.
(a) Zero order model, (b) First order model, (c) Korsmeyer-Peppas model, (d) Higuchi model and (e) Hixson-Crowell model.

3.5. Blood compatibility
The interactions of polymeric films with blood demonstrated the
compatibility of SG-AV-cl-poly(METAC) hydrogels with body systems.
The thrombogenicity characteristic of copolymeric gels revealed the
non-thrombogenic character of HWD and samples gave 84.16 ± 2.23 %
thrombogenicity with citrate blood. The clot formation was lower in
hydrogels as compared to positive control. The haemolytic index values
of polymer dressings was 2.49 ± 0.058 (Table 4) which has been
recorded as less than 5 % and standard of biomedical materials classifies
them as non-haemolytic [55]. These results elucidated less rupturing of
RBC after the interaction of hydrogel with blood cells and polymeric film

10
D. Sharma and B. Singh Hybrid Advances 5 (2024) 100142

Table 1
Results of the swelling, diffusion exponent ‘n ‘, gel characteristic constant ‘k’ and various diffusion coefficients for the swelling kinetics of SG-AV-cl-poly(METAC)
hydrogel films.
S. Parameters Swelling after 24 h (g/g of Diffusion exponent Gel characteristic constant ‘k’ × Diffusion coefficients (cm2/min)
No. gel) ‘n’ 102
Initial Di × Average DA × Late time DL ×
106 106 106

Effect of [METAC] £ 101 (molL¡1)

1. 0.4 2.43 ± 0.12 0.97 0.26 27.5 6.5 20.4
2. 0.8 2.92 ± 0.05 0.90 0.36 20.7 12.2 14.3
3. 1.2 3.27 ± 0.07 0.73 0.10 15.4 5.2 13.5
4. 1.7 3.71 ± 0.14 0.42 0.73 12.5 11.3 21.6
5. 2.1 4.10 ± 0.31 0.26 18.3 5.6 16.0 15.7
Effect of [NN-MBA] £ 102 (molL¡1)
6. 0.51 5.26 ± 0.6 0.35 11.3 10.1 16.4 21.1
7. 0.77 4.61 ± 0.14 0.29 15.2 7.05 15.3 16.8
8. 1.03 4.33 ± 0.26 0.43 6.7 12.3 10.7 18.8
9. 1.29 4.10 ± 0.31 0.26 18.3 5.65 16.04 15.7
10. 1.55 3.87 ± 0.07 0.46 5.9 13.9 10.3 22.3
Effect of medium of swelling
11. pH 2.2 buffer 4.37 ± 0.15 0.46 4 9.6 5.2 11.8
12. Distilled water 5.25 ± 0.61 0.35 11 10.1 16.3 21.2
13. pH 7.4 buffer 5.44 ± 0.36 0.40 8.1 7.8 7.7 10.7
14. Simulated wound 6.27 ± 0.34 0.3 15 7.6 11.9 16.8
fluid
Effect of Temperature
15 27 ◦ C 3.23 ± 0.43 0.45 0.6 8.69 8.88 12.9
16 37 ◦ C 5.25 ± 0.61 0.36 11.3 10.1 16.4 21.4
17 47 ◦ C 6.71 ± 0.23 0.19 27.9 4.08 7.36 17.4

Table 2
Results of diffusion exponent ‘n’, gel characteristic constant ‘k’, of different models for release profile of moxifloxacin from drug loaded SG-AV-cl-poly(METAC)
hydrogels.
Release medium Diffusion Gel characteristic Maximum amount of Constant of the Initial release rate Diffusion coefficients (cm2/min)
exponent constant released drug, kinetic of release krel ro (mgL− 1s− 1)
Initial Average Late time
‘n’ ‘k × 102’ Cmax(mgL− 1) × 105(s-n)
(Di) × 106 (DA) × 106 (DL) ×
106

pH 2.2 Buffer 0.67 1.58 41.9 8.21 0.14 12.7 8.2 11.2
Distilled water 0.72 1.26 78.4 3.53 0.22 14.8 8.4 12.7
pH 7.4 Buffer 0.75 1.01 123 7.73 0.26 16.1 8.05 13.5
Simulatedwound 0.84 0.5 278.5 0.405 0.31 22.6 9.22 17.8
fluid

was safe for biomedical use. Non-thrombogenic and non-hemolytic

Table 3
character of films was attributed due to different polar moieties
Results of correlation coefficients (R2) of different models for release profile of
including –COOH, hydroxyl group (-OH), –+NR3. Hence, AV-SG-poly
moxifloxacin from drug loaded SG-AV-cl-poly(METAC) hydrogels in different
mediums at 37 ◦ C.
(METAC) dressings can be applied for wound dressings in the form of
HWD. Polymeric material exhibited blood compatible characteristics
Kinetic Drug release mediums
useful for healing process. The copolymeric hydrogels of poly
model
(HEMA)-poly(METAC) polymers have also been illustrated biocompat­
pH 2.2 Distilled pH7.4 Simulated ible in nature in other research reports [56].
Buffer water buffer wound fluid
2
Zero order R 0.922 0.929 0.974 0.991
Ko × 1.7 1.9 2.0 2.1 3.6. Mucoadhesion
103(min− 1)
First order R2 0.981 0.986 0.995 0.975 Results of mucoadhesion revealed that force of 97.0 ± 6 mN was
K1 × 4.03 4.69 4.79 5.14
103(min− 1)
needed for detachment of copolymeric film from goat membrane during
Higuchi R2 0.976 0.980 0.998 0.997 test which required work of adhesion 0.156 ± 0.017 Nmm with
KH × 4.86 5.30 5.43 5.81 debonding distance 3.85 ± 0.195 mm mm (Table 4). The polymer was
102(min− 1/ kept in contact membrane only for 60 s along with a 0.1 N force before
2
)
the test experiment. Results of the adhesion test concluded that poly­
Korsmeyer- R2 0.976 0.977 0.993 0.998
Peppas meric films exhibited mucoadhesive properties because of the presence
KKP × 1.58 1.26 1.01 0.57 of SG and AV and poly(METAC) in hydrogels which showed non-
102(min-n) covalent supramolecular interactions and hydrophilic forces between
Hixson- R2 0.967 0.975 0.999 0.994 polymer and bio-surface. Hydrophilic nature was introduced due to
Crowell
KHC × 1.01 1.15 1.18 1.26
–COOH, –OH, and –+NR3 functional groups. All constituents in HWD
103(min− 1/ were capable of forming these interactions with mucosal membrane
3
) Mucoadhesive nature of polymeric film was found advantageous for site
specific DD. Due to the increase in functional groups in the polymeric
films their interactions with bio-surface increase along with an increase

11
D. Sharma and B. Singh Hybrid Advances 5 (2024) 100142

Table 4 mg/L in the open flask (positive control) (Table 4). The covered flask
Results of wound fluid absorption, thrombogenicity, hemolytic potential, with HWD revealed 7.3 ± 0.57 mg/L O2 permeability. These observa­
mucoadhesion test, antioxidant activity, water vapour permeability, oxygen tions elucidated that these films were permeable to oxygen and its
permeability, porosity, microbial penetration and mechanical properties of SG- supply is a desirable feature for tissue repair and to enhance healing
AV-cl-poly(METAC) polymeric films. process. These observations revealed the permeability of hydrogel
Properties Inference dressings to oxygen. Hosseini and coworkers [60] described that oxygen
Wound fluid absorption permeability in dressings is useful for healing and it describes the inbuilt
Wound fluid 6.27 ± 0.33 g/g of Wound fluid absorption ability of a hydrogel film to transport oxygen. Oxygen permeability re­
absorption hydrogel. sults demonstrated the suitability of hydrogel films in the field of wound
Blood compatibility
dressing uses. Wound healing process has been carried out through
Thrombogenicity(%) 84.16 ± 2.23 % Non-thrombogenic
Haemolytic index (%) 5.49 ± 0.05 % Non-Haemolytic various phases that require O2 in wound environments. The extent of
Mucoadhesion free volume and porosity of network increased with the addition of
Debonding distance 3.85 ± 0.195 mm glycerol (plasticizer) which allowed a certain content of oxygen to
Work of adhesion 0.156 ± 0.017 N mm penetrate and was suitable for cell regeneration [61].
Peak detachment force 97 ± 6 m N
Anti-oxidant activity
DPPH assay 46.62 ± 0.89 % inhibition 3.9. Water vapour permeability
F–C reagent assay 25.68 ± 0.51 μgGAE Antioxidant in nature
Water vapour permeability The results of the water vapour permeability of the open vial, sealed
Water permeability 32.87 ± 7.35 g/m2/hour Permeable to water
vials with SG-AV-cl-poly(METAC) films and for closed vial were found as
vapour
Oxygen permeability 1646 ± 56.0,788.89 ± 176, 234.3 ± 174 g/m2/day (Table 4). The water
Oxygen permeability 7.33 ± 0.57 mg/L Permeable to oxygen vapour permeability of the polymeric films was significantly less than
Porosity that of the open vials. HWD prevented excess dehydration at wound site
Porosity 34.03 % Porous in nature and maintained a moist atmosphere which is also a characteristic
Microbial penetration
requirement of ideal dressing. Kamoun and co-workers [62] found that
Microbial penetration No turbidity after 30 days. Impermeable to microbes.
Mechanical properties Burst Strength moist dressings have prevented excess loss of water-vapour and reduced
Burst strength 1.75 ± 0.15 N Mechanically stable the bacterial population and enhanced recovery.
Distance at burst 4.79 ± 0.44 mm
Tensile Strength
3.10. Microbial penetration
Tensile Strength 20.5 ± 2 mm NN/mm2
Extensibility 41.85 ± 6.16 %
Resilience The results of the microbial penetration test of SG-AV-cl-poly
Resilience 73.90 ± 12.5 % (METAC) revealed that grafted polymeric materials remained imper­
Relaxation meable to microorganisms for a period of one month during microbial
Force at target distance 0.17 ± 0.001 N
60 ± 12.5 %
penetration evaluation. However, contamination in the open test tube
Folding Endurance 319 was clearly visible during microbial penetration. The impermeable na­
ture of HWD was due to crosslinking density of the polymeric films and
the antimicrobial activity of AV, SG and poly(METAC) which inhibited
in adhesion. Bahulkar and coworkers [57] explained adhesion of the microbial penetration. It can reduce secondary infection probability
dressings because of various –OH groups in its structure. These –OH during wound healing. Poly(METAC) hydrogel inhibits the cationic
groups have formed weak bonds such as hydrogen bonds, Vander Waal’s bacteria, when cationic –N+ moiety of hydrogel comes in contact with
interaction or ionic interactions with mucus glycoprotein. cell membranes of bacteria cationic –N+ interacts with the negative
charge of the bacterial membrane to make membranes lose fluidity and
3.7. Antioxidant activity kill bacteria. Amin and coworkers [63] have revealed that microbes
were impermeable into hydrogel dressing that has accelerated wound
The antioxidant characteristics of the polymeric films were demon­ healing. Nonaka and coworkers [64] have confirmed antibacterial ac­
strated by DPPH and F–C reagent assays. It has been observed from the tivity of graft product of loofah fibers -g-METAC) because of presence of
results that the percent scavenging of free radicals by films was 46.62 ± the poly(METAC).
0.89 % during the DPPH assay. F–C reagent assay showed antioxidant
activity 25.68 ± 0.51 (μg) gallic acid equivalents (Table 4). These results 3.11. Porosity
showed that SG-AV based copolymeric HWD exhibited antioxidant
properties. The composition of HWD which composed of natural poly­ The porosity of HWD was measured 38.52 % (Table 4). It is an ideal
saccharides AV and which were having antioxidant characteristics due characteristic of functional HWD materials for DD. The porous structure
to their phenolic and phytosterols. AV contains active constituent aloin enhances the wound healing ability of the hydrogel dressing material
which is generally used for cancer treatment and it shows the antioxi­ which leads to the promotion of oxygen supply to the wound site and
dant properties [58]. Rubio-Elizalde [59] have illustrated the wound also keeps the moist surroundings towards the wound site. The moist
healing role of HWD formed with the grafting of poly (methyl methac­ surface around the wound site helps to prevent the colonization of the
rylate) onto AV-alginate copolymers. They explained that antioxidant microbes around the wound [65]. Porous network structure is an ideal
property of material was because of presence of phenolic of natural property of dressing material along with DD [66]. Proliferation and cell
gums. Overall, these results demonstrated antioxidant activity in poly­ adhesion are facilitated by high water uptake, hydrophilicity and
meric films which may enhance wound healing effect during its use in interconnectivity of a porous network and is useful for dressings which
wound dressing applications. can absorb wound exudates.

3.8. Oxygen permeability 3.12. Antimicrobial properties

SG-AV-cl- poly(METAC) polymeric films elucidated permeability to The antimicrobial property of the hydrogel dressings was tested with
O2 during the permeability experiment. Dissolved oxygen content was S. aureus and P. aeruginosa (Fig. 9). AV showed inhibition area zone from
4.6 ± 0.15 mg/L in the airtight flask (negative control) and 9.6 ± 0.21 5 to 8 mm against S. aureus bacteria and 14–16 mm against P. aeruginosa.

12
D. Sharma and B. Singh Hybrid Advances 5 (2024) 100142

Fig. 9. Antibacterial activity of (a,b) aloe vera (c,d) sterculia gum (e,f) SG-AV-cl-poly(METAC) polymers and (g,h) drug loaded polymers against bacteria P. aeru­
ginosa and S. aureus respectively.

SG indicated inhibition area zone from 4 to 9 mm against S. aureus and 6
to 5 mm against P. aeruginosa. In case of SG-AV-cl-poly(METAC) poly­
mers inhibition zone was from 14 to 15 mm against S. aureus bacteria
and 10–13 mm against P. aeruginosa. In case of drug loaded polymeric
samples diameters of inhibition were observed 25 and 27 mm against
S. aureus as well as P. aeruginosa respectively. Both AV and SG exhibited
antimicrobial activities which were enhanced by the encapsulation of
antimicrobial drug into hydrogel dressings. It is concluded from the
results that an antibacterial drug increased diameter of the inhibition
area in the case of drug loaded polymers. Garcia and coworkers [67]

13
D. Sharma and B. Singh
performed the experiment and found that METAC in resin-based seal­
ants, showed antibacterial activity.
3.13. Mechanical properties
These properties of hydrogel dressing demonstrated TS = 20.5 ± 2
mN/mm2, BS = 1.75 ± 0.157 N, extensibility = 26.36 ± 1.242, stress-
relaxation = 18.90 ± 1.80 %, percentage resilience = 41.85 ± 6.16 %
and folding endurance = 329 (Table 4). Tensile strength was low
because of the presence of AV in the polymeric films. The addition of AV
into the composition was responsible for a slight decrease in maximum
TS and elongation at break values. Moreover, data values successively
decreased with the increment of AV contents during the test. A decrease
of the hardness of polymeric film can be seen due to the presence of AV
content and accompanied by higher flexibility [68]. The glycerol
(plasticizer) content influenced folding endurance and improved the
flexibility of the film [69]. However, mechanical properties elucidated
considerable mechanical strength in hydrogel dressings which can
withstand stress or strains during application as wound dressing.
Overall, hydrogel dressings SG-co-AV-poly(METAC) were flexible,
porous and had rough surfaces. The analysis of the physical and me­
chanical aspects of the dressing revealed tensile strength 20.5 ± 2 mN/
mm2 and burst strength 1.75 ± 0.157 N. The dressings were of golden-
brown coloration having thickness about 0.2 cm of and diameter 7.5 cm.
The image of the SG-AV-cl-poly(METAC) hydrogel dressing is shown in
Scheme 1.
The in vivo experiment of the hydrogel dressings has not been per­
formed. However, materials used for the design of hydrogel dressings i.e.
aloe vera, sterculia gum and poly(METAC) have demonstrated their non-
cytotoxic nature to the animals during wound healing experiments in
various research reports [70–73]. Genesi and co-workers [70] illustrated
the non-toxic nature of aloe-vera based polymer composites prepared for
wound healing applications. Cytotoxicity, and in vivo proof has also
been demonstrated in this research report [70]. Aloe-vera gels have also
been found better in wound healing during comparison of burn treat­
ment with and without silver sulfadiazine in animal models [71]. Nar­
ayanan and coworkers [72] have demonstrated the anti-inflammatory
activity of aloe vera extract. Albumin de-naturation process has been
adopted to investigate the anti-inflammatory activity of aloe vera.
Scheme 1. The image of the SG-AV-cl-poly(METAC) hydrogel.
14
Hybrid Advances 5 (2024) 100142
Cytotoxicity test of aloe vera has also been performed by mice fibroblast
L929 cells and material has been found non-toxic. Sterculia gum has
been found effective in wound repair and has increased cell proliferation
and granulation during healing process [13]. Packing of SG powder in
open wounds has increased granulation tissue and resulted epidermal
growth [16]. Cytotoxic properties of modified sterculia gum have been
demonstrated during MTT assay. Gum did not show cytotoxicity against
macrophages up to 100.0 to 0.78 μg mL concentration [73]. A biological
characterization of gum based hydrogels have also been performed in
terms of protein absorption on polymeric hydrogels surfaces, cytotox­
icity and cell adhesion and proliferation studies using both murine 3T3
and human fibroblasts. Hydrogels have been proved as non-cytotoxic
materials and facilitated cell proliferation during biomedical applica­
tions [56]. Therefore, the present hydrogel dressings could be used for
wound dressing applications.
4. Conclusions
In concluding remarks, it has been observed that the composition of
the copolymers and the content of the crosslinker NN-MBA used during
synthesis of hydrogels have controlled the crosslinking of hydrogel
dressings which has been inferred from the results of swelling properties
of HWD. XRD analysis revealed the amorphous nature of copolymers.
Wound fluid absorption (6.27 ± 0.34 g/g) capacity in simulated con­
ditions has demonstrated that hydrogels have good capacity to absorb
wound fluid which can maintain a moist environment. Further, there
exist the correlation between spectral techniques for the grafting of poly
(METAC) onto polysaccharides. In FTIR spectra bands were found at
1721 cm1 due to C– –O stretching of carboxylic acid SG, AV and poly
(METAC) ester and in case of 13C NMR of copolymers revealed peaks at
177.35 and 173.09 ppm [C– –O of galactouronic acid of SG and AV along
with carbonyl carbon of poly(METAC)]. In FTIR stretching frequency at
1412 cm− 1corresponds to C–N stretching of -+N(CH3)3 group of poly
(METAC) while in 13C NMR peak at 54.56 ppm assigned to methyl
carbon atom attached to quaternary nitrogen –+N(CH3)3Cl group in poly
(METAC)]. While band at 1034 cm− 1 [due to C–.–C stretching frequency
of gum and poly(METAC) grafted polymers] and in 13C NMR spectra
peak found at 60.35 was due to grafted carbon of monomer i.e. -C-O. In
FTIR spectra, stretching observed at1012 cm− 1 was due to C–N bending
vibration of quaternary nitrogen group present in poy(METAC)] while
in13C NMR peak appeared at 63.65 ppm was due to sequential methy­
lene group (-CH2-CH2–+N(CH3)3)] of poly(METAC). The release of drug
moxifloxacin was exhibited through a non-Fickian mechanism. Polymer
bio-surface interactions have revealed their mucoadhesive property (97
± 6 mN detachment force) and polymer-blood interactions indicated
bio-compatible nature (<5 % haemolysis) with their antioxidant (46.62
± 0.89 % free radical scavenging in DPPH assay) characteristics. The
porous dressings were permeable to O2 and water vapour and imper­
meable to microbial penetrations. Overall, these antibiotic drug moxi­
floxacin encapsulated HWD could be applied as wound dressing
materials. Further, the healing potential of dressings could be enhanced
by virtue of wound healing therapeutic role of AV (anti-inflammatory
and anti-microbial properties) and SG (wound healing and anti-oxidant
properties).
CRediT authorship contribution statement
Diwanshi Sharma: Writing – original draft, Validation, Methodol­
ogy, Investigation, Formal analysis, Data curation. Baljit Singh: Writing
– review & editing, Visualization, Supervision, Resources, Formal
analysis, Data curation, Conceptualization.
Declaration of competing interest
XThe authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
D. Sharma and B. Singh
the work reported in this paper.
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