International Journal of Biological Macromolecules

International Journal of Biological Macromolecules 94 (2017) 10–27
Contents lists available at ScienceDirect
International Journal of Biological Macromolecules

journal homepage: www.elsevier.com/locate/ijbiomac
Blends and composites of exopolysaccharides; properties and

applications: A review
Abid Hussain a , Khalid Mahmood Zia a , Shazia Tabasum a , Aqdas Noreen a ,
Muhammad Ali b , Rehana Iqbal c , Mohammad Zuber a,∗
a
Institute of Chemistry, Government College University, Faisalabad 38030, Pakistan
b
Department of Biotechnology, Government College University, Faisalabad 38030, Pakistan
c
Institute of Pure and Applied Biology, Bahauddin Zakariya University, Multan.60800, Pakistan
a r t i c l e i n f o a b s t r a c t
Article history: Exopolysaccharides are synthesized by bacteria and secreted into the external environment and they
Received 14 August 2016 may be homopolymeric or heteropolymeric in configuration. They are believed to protect bacterial cells
Received in revised form from heavy metals, desiccation or other environmental effect. EPS exhibit antitumor, anti-HIV, emulsion
23 September 2016
stabilization capacity, shear-thinning activity, suspension ability, high viscosities, excellent biocompat-
Accepted 29 September 2016
ibility, high biodegradability and immunomodulatory properties. They are widely used in herbicides,
Available online 3 October 2016
functional food, nutraceuticals, cosmeceuticals, pharmaceuticals, insecticides, immunomodulation and
anticoagulants. This review shed light on the properties and versatile applications of xanthan, curdlan,
Keywords:
Curdlan
hyaluronic acid and dextran blends and composites with natural and synthetic polymers.
Xanthan © 2016 Elsevier B.V. All rights reserved.
Dextran
Hyaluronic acid
Biomedical applications
Food industry
Contents
1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
1.1. Polysaccharides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
1.2. Exopolysaccharides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
1.2.1. Homopolysaccharides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
1.2.2. Heteropolysaccharides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
1.3. Structure of exopolysaccharides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
1.4. Reason for choosing exopolysaccharides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
1.5. Limitations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
2. Modifications of exopolysaccharides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
2.1. Exopolysaccharides blend and composites with natural polymer . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
2.1.1. Blends and composites of xanthan with natural polymers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
2.1.2. Blends and composites of curdlan with natural polymers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
Abbreviations: HPAM, anionic polyacrylamide; BSA, bovine serum albumin; CDI, carbonyldiimidazole; CMC, carboxymethyl curdlan; CPAM, cationic polyacrylamide;
CS, chondroitin sulfate; Cur, curcumin; Dx, dextran; DMSO, dimethyl sulfoxide; DOX, doxorubicin; DR, drag reduction; DDS, drug delivery system; EGCG, epigallocatechin-
3-gallate; EPS, exopolysaccharides; GA, gallic acid; GLG, gellan gum; AuNPs, gold nanoparticles; LAB, lactic acid bacteria; HMW, high molecular weight; HLC, human-like
collagen; HA, hyaluronic acid; KGM, konjac glucomannan; Lyz, lysozyme; MGs, microgel; MIPs, molecular imprinting; PEG, poly(ethylene glycol); PLGA, poly(lactide-Co-
Glycolide); PAMs, polyacrylamides; PAA, polyacrylic acid; PPy, polypyrrole; QCS, quaternized chitosan; Ag NPs, silver nanoparticle; NaA, sodium alginate; XG, xanthan gum;
XRD, x-ray powder diffraction.
∗ Corresponding author.
E-mail address: [email protected] (M. Zuber).
http://dx.doi.org/10.1016/j.ijbiomac.2016.09.104
0141-8130/© 2016 Elsevier B.V. All rights reserved.
A. Hussain et al. / International Journal of Biological Macromolecules 94 (2017) 10–27 11
2.1.3. Blends and composites of hyaluronic acid with natural polymers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16

2.1.4. Blends and composites of dextran with natural polymers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18
2.2. Exopolysaccharides blends and composites with synthetic polymers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
2.2.1. Blends and composites of xanthan with synthetic polymers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
2.2.2. Blends and composites of hyaluronic acid with synthetic polymers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21
2.2.3. Blends and composites of dextran with synthetic polymers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
3. Conclusion and future prospects . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
1. Introduction has currently opened a new opportunity for the researchers to uti-
lize new bacteria that inhabit unfamiliar marine ecosystems. EPS
1.1. Polysaccharides can be modified by combination or blending with natural and syn-
thetic polymer, as a result of blending they change their properties
Polysaccharides are the high molecular weight molecules linked and have wide applications in several fields [45].
through a glycosidic linkage. They usually contain 100 to 90,000
monomer units and on hydrolysis give monosaccharides. They dif- 1.5. Limitations
fer from each other by their monomers, molecular weight, mole and
other structural features. They may be linear or highly branched. The main challenges for the commercialization of new EPS is the
Microbial polysaccharides are produced in two forms, capsular identification of strains and nature of EPS, improvement of novel
polysaccharide (CPS) and exopolysaccharides (EPS) [1,2]. structures, cost of production and development of downstream
process. For production and commercialization of EPS a suitable
1.2. Exopolysaccharides downstream method is required. EPS have unique properties such
as high gel strength, foaming and viscosity that can create sev-
Exopolysaccharides (EPS) are high-molecular-weight polymers eral problems during fermentation processes for their production.
that are secreted by a microorganism into the surrounding Genetic engineering of microbes requires further developments to
environment by cell wall-anchored enzymes and are composed convert inexpensive raw materials to EPS. In the light of current
of sugar residues. Microorganisms synthesize a wide-ranged knowledge, an emphasis should be given to produce new EPS with
spectrum of multifunctional polysaccharides including structural potential multifarious applicability [45].
polysaccharides, intracellular polysaccharides and extracellular
polysaccharides (i.e. EPS). EPS usually consist of monosaccharides 2. Modifications of exopolysaccharides
and non-carbohydrate substituents such as pyruvate, acetate, phos-
phate and succinate [8–10]. They are divided into two groups Exopolysaccharides have a wide range of applications depend-
(Table 1) homopolysaccharides and heteropolysaccharides [11,12]. ing on their nature, composition and structure. Generally some
specific monosaccharides form EPS and its structural diversity
1.2.1. Homopolysaccharides determines its possible applications [46]. EPS are used in the food,
These polysaccharides on hydrolysis give only one type of pharmaceutical, biomedical, bioremediation and bioleaching fields
monosaccharide units e.g. cellulose, alginate, dextran etc. because of their physical, rheological, some unique properties and
wide structural diversity [47–49]. EPS plays a key role in biofilm
1.2.2. Heteropolysaccharides formation, facilitating initial adhesion leading to development of
These polysaccharides on hydrolysis produce more than one complex architecture [50]. In this review, we discussed only four
type of monosaccharide units. Heteropolysaccharides are com- EPS viz., xanthan, curdlan, hyaluronic acid and dextran that can
posed of repeating units, varying in size from disaccharides to be blended with natural and synthetic polymers. The techniques
heptasaccharides e.g. xanthan, hyaluronic acid, heparin etc. [3–7] employed for characterization of EPS and their potential applica-
tions in various fields are summarized in Table 2.
1.3. Structure of exopolysaccharides
2.1. Exopolysaccharides blend and composites with natural
Bonds between monomeric units at the backbone of the poly- polymer
mers are 1,4-␤- or 1,3-␤-linkages and 1,2-␣- or 1,6-␣-linkages
(Fig. 1) [44]. 2.1.1. Blends and composites of xanthan with natural polymers
Xanthan is an exopolysaccharide produced by the bacterium
1.4. Reason for choosing exopolysaccharides Xanthomonas campestris. It is a heteropolysaccharide with repeated
pentasaccharide units consisting of glucose, mannose and glu-
Due to the unique functionality and reproducible physicochem- curonic acid [94,95]. It consists of ␤ 1,4-linked d-glucose backbone
ical properties along with stable cost and supply, exopolysaccha- and also substituted with a trisaccharide side chain linkage
rides are widely used in many industries [36,37]. The increased alternately with every second glucose residue [96,97]. Xanthan
demand of natural polymers for many industrial applications in has remarkable emulsion stabilization, suspension ability, shear-
recent years has increased the importance of EPS production by thinning activity and high viscosities [98]. It is biocompatible, water
new sources [38]. Intelligent screening of microorganisms for EPS soluble, has limited electrical conductivity and thermal stability
is necessary for its further exploration toward commercialization. [99].
An advanced approach is needed for applications of EPS in the med-
ical or pharmaceutical field and food sectors [39–41]. In future, 2.1.1.1. Xanthan gum blend with alginate. Alginate (Alg), the most
there will be further development of prebiotic and probiotic-based common encapsulating agent and linear polysaccharide consist-
dairy goods where bacterial EPS will play an important role [42,43]. ing of 1 → 4 linked ␤-(d)-guluronic(G) and ␣-(l)-mannuronic (M)
Applicability and acceptability of EPS in pharmaceutical industries acids derived from brown algae. Alginate has been widely used
12 A. Hussain et al. / International Journal of Biological Macromolecules 94 (2017) 10–27
Table 1
Types properties and application of exopolysaccharides [13–35].
Sr. No. EPS Source Properties Applications Refs.
1 Alginate Pseudomonas aeruginosa, Azotobacter Film forming, gelling capacity. Food hydrocolloid, medicine [13–16]
sp. surgical dressings, controlled drug
release
2 Dextran Leuconostoc mesenteroides, Non-ionic character, good Foods and Pharmaceutical [15–18]
Lactobacillus hilgardii, Leuconostoc stability and fluid behavior. industry.
dextranicum, Streptococcus mutans
3 Cellulose Acetobacter xylinum, Pseudomonas sp., High tensile strength Foods as a indigestible fiber, [16,19,20]
Agrobacterium Rhizobium sp. biomedical for wound healing
purpose and tissue engineered
blood Vessels.
4 Curdlan Alcaligenes faecalis, var. Myxogenes Gel-forming ability, water Foods and pharmaceutical industry [21,15]
insolubility, and Non-toxic. as a heavy metal removal.
5 Xanthan Xanthomonas Campestris Stable over wide temperature petroleum industry, [22]
and high viscosity. Pharmaceuticals, cosmetics and
personal care products.
6 Succinoglycans Alcaligenes faecalis, var. Myxogenes High viscosity, acid stability Food and oil recovery [16,19]
7 Glucuronans Sinorhizobium meliloti, Gelling and thickening capacity Food and cosmetics products [23]
Gluconacetobactaria
8 Colanic acid E. coli, Shigella spp., Salmonella spp., Gelling capacity. Cosmetics and personal care [23]
Enterobacter spp. products
9 Hyaluronan Streptococcus sp. Cell adhesion, cell motility, Cosmetic market, viscosurgery, [24–28]
(Hyaluronic acid) wound healing, pseudo plastic skin moisturizers, ophthalmic
and viscoelastic. surgery, wound healing, and
surface coating
10 Emulsan Acinetobacter calcoaceticus Ability to form stable Consumer products and drug [29,30]
oil-in-water emulsions. delivery
11 Welan Alcaligenes sp. stable and viscous at high Stabilizer and viscosifiers in [31–33]
temperatures cement systems and oil
well-drilling sites.
12 Levan Alcaligenes viscosus, Zymomonas Polymeric medicinal properties Food, medicine, cosmetic, [23]
mobilis, Bacillus subtilis pharmaceutical, and commercial
industrial sectors
13 Kefiran Lactobacillus hilgardii, L. rhamnosus, L. Antibacterial, antifungal, Improve texture of fermented food. [32,34]
kefir, L. kefiranofasciens antitumor activity and
Prebiotic non-digerible fibers.
14 Gellan Aureomonas elodea, Sphingomonas High yield stress and low Food industry production of liquid [15,19,33–35]
paucimobilis, Sphingomonas elodea viscosity. gels, edible films, gelatin desserts,
jams and microcapsules
for “burst release” under acidic conditions pH < 2.0 [114]. Sodium interact with the surrounding zeolite particles. XG–alginate hydro-
alginate (NaA), found in marine brown algae, possesses varying gel are formed by the contribution of strong intermolecular
compositions of ␤-1,4 linked l-guluronic acid and d-mannuronic hydrogen bonding between carboxyl and hydroxyl groups of
acid [117]. XG and alginate [108,109]. For making hybrid NaA/XG–alginate
Zeolite is vital porous aluminosilicate materials that have wide composites, the zeolite NaA particles are dispersed into binary
application in several fields such as catalysis, ion exchange and XG–alginate hydrogel networks. These are utilized for the removal
separation [100–102]. The hydrogels that are formed by cross link- of Co2+ and Ni2+ from nuclear wastewater. Zhang et al. [92] pre-
ing of calcium ion with alginate are biodegradable and nontoxic pared novel hybrid NaA/XG–alginate composites (Fig. 2) applicable
[103,104]. But, the NaA zeolite particles with large surface energy in industrial wastewater treatment. In comparison to NaA/alginate
tend to form agglomerates inside the alginate-based composite composites, the NaA/XG–alginate composite showed improved
[105]. Xanthan gum (XG) was exploited to modify highly con- sorption kinetics, capacity and operation stability.
centrated zeolite NaA particles suspension [106,107]. On heating, Much attention has been paid to lactic acid bacteria (LAB)
the double helical XG chains get separated rendering them apt to because it has wide range of applications. LAB are considered as
Fig. 1. Structure of Exopolysaccharides [44].

Table 2
Different techniques for the synthesis and characterization of functionalized by different exopolysaccharides and their prospective applications in different fields [51–93].
Sr. No Material Composition Techniques For Properties/Applications Refs.

Characterization
1 Curdlan/Gellan Gum FTIR Adhesion prevention properties/applicable to [51]

reduce post-operative adhesion during healing.
2 Glucomannan/curdlan FT-IR, XRD, DSC, SEM Edible food films and coatings purpose. [52]
3 Carboxylic Curdlan-capped gold UV–vis, XRD, HR-TEM, Molecular diagnostics, bimolecular imaging, [53]
nanoparticles–protein EDX, FTIR bioengineering and drug delivery
4 Carboxylic curdlan–deoxycholic acid FTIR, SEC, XRD Carrier of hydrophobic antitumor drug. [54]
5 Curdlan–Histidine NMR, FTIR Protein delivery system [55]
6 Protein–novel Carboxymethyl-curdlan FTIR, SEM Analyze the experimental data of BSA adsorption. [56]
7 polyaniline/xanthan gum AFM, FTIR Determine the swelling amount of nanocomposite [57]
in aqueous solution
8 novel xanthan gum/polypyrrole nanocomposite AFM, FTIR. Enhance the thermal stability of nanocomposite. [58]
9 Poly(ethylene oxide), Polyacrylamide/Xanthan SEM Drug reduction process [59]
Gum
10 Xanthan–lignin hydrogels FTIR, DSC Used in the manufacturing of eco-friendly items on [60]
various usages.
11 chitosan,␤-cyclodextrin–xanthan FTIR, DSC, SEM, TGA. Encapsulation of drugs. [61]
12 calcium alginate–xanthan gum FTIR Recycling of lead from current industrial [62]
wastewaters.
13 Lysozyme–xanthan gum FTIR Great quality emulsifier, foam fabricator or natural [63]
antibacterial agent in food and pharmaceutical
industries.
14 xanthan conformation-based silver nanoparticles UV–vis, TEM, FT-IR Antibacterial and catalytic application in [64]
biotechnology and biomedical.
15 co-polymer(polyethylene XRD, FTIR Controlled drug delivery. [65]
oxide)–xanthan-O-Carboxymethyl
16 Chitosan coated alginate–xanthan gum FTIR, DSC, XRD Food and pharmaceutical industry. [66]
17 xanthan gum–lysozyme XPS, SEM, AFM, FTIR It can provide several valuable information in [67]
protein/polysaccharide NP fabrications and
physical interactions
18 xanthan/polypyrrole FTIR, AFM, DSC Electrical control properties/Biomedical devices. [68]
19 alginate shell–xanthan gum FTIR Food packaging. [69]
20 poly(acrylamide)–Carboxymethyl xanthan gum NMR, FTIR, XRD SEM Drug delivery system. [70]
21 Poly(vinyl amine)–dextran SEM Drug delivery system. [71]
22 Dextran/chitosan-graft-polyaniline FTIR, NMR UV–vis Tissue engineering. [72]
23 Dextran–polyethylenimine NMR Clinical application. [73]
24 Dextran–sulfate coated chitosan FTIR EGCG delivery in food processing. [74]
25 Dextran–polyethylene glycol SEM Used for differentiating of different protein [75]
structures.
26 Dextran-based flocculant FTIR, TG, XRD Wastewater flocculating treatment. [76]
27 Dextran based curcumin FTIR,1 H NMR XRD, TG/DTG, Drugs delivery system. [77]
TEM, SEM, AFM, DLS
28 Dextran-poly(4-substituted- ␧-caprolactone) DLS, TEM Targeted drug delivery system. [78]
29 polypyrrole-/hyaluronic acid AFM, SEM Applied to detect tryptamine in real sample [79]
30 gelatin/hyaluronic acid SEM Adipose tissue engineering. [80]
31 hyaluronic acid/human-like collagen FTIR Tissue engineering. [81]
32 Hyaluronic acid/chondroitin sulfate-based FTIR Drug delivery carrier. [82]
hydrogel
33 xanthan gum/Gellan gum/hyaluronan FTIR Anti-adhesive barriers/tendon surgeries for clinical [83]
trial in human
34 hydroxyethyl cellulose–hyaluronic acid SEM, FTIR Skin lesions for transdermal delivery systems [84]
35 polycarboxylic/amino–hyaluronic acid UV–vis, SEM, HPLC Biomedical surfaces to prevention of bacterial [85]
adhesion.
36 Poly(Lactide-Co-Glycolide)/Hyaluronic Acid FTIR, SEM, XRD, TEM Tissue Engineering. [86]
37 Hyaluronic acid-polyacrylic acid NMR, FTIR Drug delivery. [87]
38 Poly(Ne-acryloyl l-lysine)/hyaluronic acid NMR, FTIR 3D in vitro model of breast cancer. [88]
39 Hyaluronic acid- chitosan-based nanoparticles NMR, DSC Drug carrier. [89]
40 Curdlan-␣-amylase NMR, FTIR Preparation of oligosaccharides [90]
41 Polyacrylamide/Xanthan Gum SEM, FTIR It is very important for developing NGH(natural [91]
gas hydrate) drilling fluid to improve borehole
stability and cutting carriage
42 xanthan gum–alginate binary biopolymer XRD, SEM,TGA Industrial wastewater treatment. [92]
43 hyaluronic acid–poly(ethylene glycol) composite NMR, FTIR Cell delivery and soft tissue regeneration. [93]
GRAS (generally recognized as safe), by the production of organic food packaging applications. Chitosan is formed by deacetylation
acids, phages, lytic agents enzymes, defective hydrogen peroxide of chitin and it is widely used polycationic and non-toxic polysac-
and antimicrobial peptides, or bacteriocins and it can inhibit the charide. To improve the mucoadhesivity and stability of the beads,
growth of different fungi, yeasts and bacteria [110]. Due to its non- their entire surface was coated with chitosan [115]. Fareez et al.
toxicity, biocompatibility and low cost, alginate has been widely [66] prepared chitosan coated alginate–XG beads. The Lactobacillus
used as microencapsulation material [111–113]. Bekhit et al. [69] plantarum LAB12, a Malaysian LAB with exceptional probiotic fea-
prepared aqueous-core microcapsules with sodium alginate hydro- tures [116], was selected as the model bacterial strain. The prepared
gel in membrane and XG in core using ionotropic gelation method beads had improved pH resistance, temperature tolerance storage
to encapsulate bacteriocin-producing LAB that can be used for durability and targeted release of L. plantarum LAB12 in vitro.
Fig. 2. The fabrication procedures of NaA/XG–alginate composites by facile controlling the zeolite NaA dispersion into the composites [92].
The alginate can form three-dimensional gel beads upon expo- release [127]. Chitosan has great potential applications in the phar-
sure to aqueous calcium ions. The adsorption property of calcium maceutical industry [94] as a lipophilic encapsulation for drugs
ion cross-linked alginate (CA) gel beads has been used for metal [95] and in food industry as an encapsulation for probiotics and
ions bearing wastewater treatment [118–120]. CA gel beads served prebiotics [96] and aromatic compounds [128–131]. Cyclodextrin
as a template, for porous TiO2 /ZrO2 millimeter sized beads which consists of glycosidic bonds. [132]. Cleonice et al. [61] carried out
are used for urinal adsorption [121]. While the prepared alginate- microencapsulation of gallic acid (GA) with chitosan, cyclodextrin
template macroporous titania beads of uniform size and high or xanthan by the lyophilization method. GA is encapsulated in
surface area for heavy metal removal [122]. The silica/CA–XG com- chitosan, ␣-cyclodextrin and xanthan matrices by lyophilization
posite were prepared by in situ incorporation of amorphous silica method to calculate encapsulation efficiencies and also determine
into CA–XG gel beads via easy and cost-effective tetraethoxysilane antioxidant capabilities of the encapsulated gallic acid. The blend of
(TEOS) sol–gel approach. The silica could be entrapped and con- xanthan with chitosan matrix exhibited encapsulation efficiency,
densed within the three–dimensional network structures of CA–XG and capsules with characteristic shape were obtained.
gel beads involving the hydrolysis and condensation of TEOS. Zhang
et al. [62] prepared silica modified calcium alginate–XG hybrid bead 2.1.1.4. Xanthan blend with lignin. Lignin is a highly branched,
composites for the removal and recovery of Pb(II) from aqueous three-dimensional phenolic polymer that has variety of functional
solution with inherent macro/mesoporosity, large surface area, and groups [133,134]. The presence of hydrophilic functional groups
excellent mechanical stability. in lignin provide good feedstock, which are important ingredients
for the preparation of hydrogels and widely used in petroleum oil
2.1.1.2. Xanthan gum blend with lysozyme. Lysozyme (N-acetyl- drilling, biomedical, agriculture, engineering and daily life [135].
muramic-hydrolase) is found abundantly in many secretes of Irina et al. [60] prepared xanthan/lignin hydrogels for the devel-
biological cells. It is well-known bacteriolytic enzyme that has the opment of eco-friendly products of different usages. Atomic force
ability to lyse bacterial cells. The hen egg is the major source of microscope showed that the lignin type influences the hydrogel
this enzyme and it is also manufactured commercially [124]. Nano morphology leading to formation of different permeable structures
particulate delivery systems possess environmental and social ben- with a smooth surface, except the hydrogel containing aspen wood
efits [123]. Xu et al. [67] prepared XG/lysozyme nanoparticles lignin which forms a fibrilar structure.
(NPs) through alkali and thermal treatments (Fig. 3). XG can be
attached to lysozyme via the controlled Maillard reaction to form 2.1.2. Blends and composites of curdlan with natural polymers
protein-polysaccharide conjugate [124]. Marjan et al. [63] prepared Curdlan is an exopolysaccharides produced by bacteria, such
lysozyme-XG conjugate with greater antimicrobial activities than as Alcaligenes faecalisvar with linear structure and is com-
unmodified lysozyme, for use in formulated food or drug systems. posed of (1–3)-␤-d-glycosidic linkages [136–138]. Curdlan exhibits
anti-tumor, anti-HIV, immunomodulatory effects, poor solubil-
2.1.1.3. Xanthan blend with chitosan. Gallic acid is 3,4,5- ity in water [139–141], good gelling ability, thermal stability,
trihydroxybenzoic acid which is biosynthesized from the enzyme biodegradability and nontoxicity [142,143]. It is widely used in
dihydroshikimate. It is abundant in different kinds of plant king- pharmaceuticals, drug delivery, protein drug delivery, various
dom especially in berries, cereals, tea, wine citrus fruits and herbs, foods, meat products, cosmetics and building industries.
occurs naturally both in an ester or salt and in free form [125]. The
purpose of microencapsulation is to maintain the bioactivity of 2.1.2.1. Curdlan blend with protein. Proteins have a tendency to
compound. [126]. Lyophilization method of microencapsulation accumulate at the interface between solutions and solid sur-
in a polymer matrix maintained its bioactivity and controlled its faces and they are relatively large biomolecules [144]. Purified
Fig. 3. Tentative model of XG/Ly NPs formation during the harsh alkali coupled thermal treatment [67].
proteins have important application in pharmaceutical indus- water-soluble CC derivatives [163]. The obtained CC derivatives
try, in biofuel cell, biosensors and bioreactors [145,146]. Gold were non-toxic, biodegradable, biocompatible and exhibited more
nanoparticles (AuNPs) are widely used in biotechnology, catalysis, flexible chain conformations. CM-curdlan exhibited rigid triple
biomedicine, sensors, and electronics [147–149]. The interactions helical conformation in aqueous solution and convenient for the
between protein and nanoparticles are utilized in bimolecular preparation of amphiphilic conjugates [164,165]. Yana et al. [54]
imaging, molecular diagnostics, drug delivery for cancer therapeu- prepared nanoparticles of carboxylic curdlan-deoxycholic acid
tics and bioengineering [150–154]. Carboxymethyl curdlan (CMC) (CCD) conjugates as a carrier of doxorubicin (DOX) (Fig. 6) and
is biocompatible, non-toxic and biodegradable and is widely used hydrophobic antitumor drugs.
in biomedicine and bio analytical field. Yan et al. [53] prepared
biocompatible CMC-capped AuNPs from chloroauric acid (HAuCl4 )
(Fig. 4). Particle size of the AuNPs can be changed by changing the 2.1.2.4. Curdlan blend with gellan gum. Gellan gum (GLG) consists
reaction time and concentrations of CMC and HAuCl4 . After six of repeating units of glucose glucuronic acid-glucose-rhamnose,
months storage spherical AuNPs showed high stability and were and is a linear anionic heteropolysaccharide. Due to its ease of pro-
well dispersed. The carboxylic groups (COO ) in the CMC molecules cessing into transparent gels at high temperatures using divalent
tend to adsorb and stabilize the surface of the AuNPs. Rafigh et al. cations, it is used in the food industry and biomedicine [166] as an
[56] discussed protein adsorption using novel CMC microspheres. anti-adhesion barrier [167–169]. Kim et al. [51] prepared curdlan
Bovine serum albumin (BSA) was used as a model protein adsorp- and GLG hydrogels for prevention of post-surgical peritoneal adhe-
tion. sion. To prevent the adhesion between injured tissues the barriers
can be easily applied during surgery.
2.1.2.2. Curdlan blend with Boc-histidine. Histidine is a biocom-
patible and eco-friendly amino acid due to imidazole side group
possesses pH-responsive properties [155–157]. Yang et al. [55] 2.1.2.5. Curdlan blend with glucomannan. Konjac glucomannan
prepared pH-responsive hydrogels by conjugating curdlan with (KGM) is high molecular weight water-soluble non-ionic natu-
Boc-histidine (CUR-HIS) for protein delivery (Fig. 5) with porous ral polysaccharides composed of ␣-1,4 linked of d-glucose and
structures and good biocompatibility. Bovine serum albumin (BSA) d-mannoses backbone lightly branched, with branches through
are taken as a model protein drug which can be encapsulated into −1,6-glucosyl units [170,171]. KGM exhibits good biocompatibility,
CUR-HIS hydrogels and the release profiles of BSA at different pH biodegradability and excellent film-forming ability [172,173]. Wu
values from CUR-HIS hydrogels were significantly different. [158]. et al. [51] prepared KGM/curdlan blend films with potential appli-
cations as edible films and biodegradable food packaging materials.
2.1.2.3. Carboxylic curdlan blend with deoxycholic acid. Due to poor This blend film (70 wt%) had high tensile strength as compared to
solubility in water and less bioactive nature, derivatives of curd- neat curdlan film. Tensile strength increased from 4.54 ± 1.89 MPa
lan such as carboxylic curdlan (CC) are prepared [159–161]. CC to 42.93 ± 1.92 MPa as KGM content increased from 0 to 70 wt%
is negatively charged curdlan derivative which is widely used to while the presence of curdlan enhanced the moisture barrier prop-
manufacture amphiphilic CM-curdlan [162]. Under mild conditions erties of the KGM/curdlan films.
4-acetamido-TEMPO/NaClO/NaClO2 system was used to prepare
Fig. 4. Proposed scheme for the preparation of AuNPs by CMC [53].

Fig. 5. Synthesis of curdlan/Boc-histidine hydrogel [55].
2.1.3. Blends and composites of hyaluronic acid with natural engineering. For successful tissue engineering, the scaffold must
polymers be biodegradable and biocompatible, with a 3-D porous architec-
Hyaluronic acid (HA) is an exopolysaccharides having a repeat- ture and inter-pore connections and the appropriate mechanical
ing unit of d-glucuronic acid and N-acetyl-d-glucosamine linked properties similar to those of the regenerative tissue [195].
by (1 → 4) and (1 → 3) linkages [174]. HA is a hydrophilic polymer Gelatin, a partially degraded product of collagen, is believed to
that can absorb large amount of water and retain up to 1000 fold have a lower antigenicity than collagen. Moreover, it is not only
more water than its solid volume due to hydrogen bonding between more economical than collagen, but it also contains amino acid
carboxyl and N-acetyl groups of HA with water [174]. HA shows sequences, such as the RGD of collagen, which can enhance cell
bacteriostatic, non-immunogenic, non-inflammatory, highly bio- attachment. Therefore, gelatin has been blended with other natural
compatible, antiviral and also biodegradable properties [175] but it or synthetic biomaterials to fabricate 3-D scaffolds using vari-
has poor mechanical stability [176]. It is used in drug delivery, scaf- ous methods for different tissue engineering applications. Gelatin
folds for tissue engineering, as an ingredient in cosmetics provides microspheres containing basic fibroblast growth factor were shown
anti-aging and moisture supplying effects to the skin [174,177,178], to induce preadipocytes to form adipose tissue at the implant site
as a postsurgical adhesion prevention and construction of 3D tumor [194].
models [179,180] Macroporous elastic cryogels could be fabricated from gelatin
and HA, two biopolymers suitable as adipose tissue engineering
2.1.3.1. Hyaluronic acid blend with chitosan. Ionotropic gelation scaffolding materials. The GH cryogel is endowed with unique
is most successful techniques to produce chitosan NPs. In this mechanical properties, such as high extensibility, moderate tough-
technique chitosan chains are ionically cross-linked with penta- ness and total recovery from large strains. Furthermore, the
sodium tripolyphosphate (TPP) in the presence of cargo molecules superior physicochemical properties, such as high porosity, large
[181,182]. The physicochemical properties of chitosan NPs were pore size, fast swelling kinetics and high swelling ratio, combined
improved by incorporating HA [183–185]. with mechanical properties similar to those of adipose tissue, make
HA selectively binds to CD44 receptors expressed on lung the GH10 cryogel a suitable scaffold for adipose tissue engineering.
epithelial cells. These receptors have ability to over-express in cer- Chang et al. [80] prepared gelatin/HA (GH) cryogels for adipose tis-
tain cancer cell therefore it is use as a targeting ligand [187]. The sue engineering. The growth arrest, morphological changes, actin
synergistic effects provided by both chitosan and HA improved the cytoskeleton expression and leptin secretion of the ADSCs in GH
toxicity profile, [186,184] mucoadhesivity [188,189] and therapeu- cryogel were consistent with the differentiation process that occurs
tic outcome of the resulting hybrid chitosan/HA NPs both in vivo under adipogenic induction. The mRNA expression of adipogenic
and in vitro [190–193]. Al-Qadi et al. [89] reported the synergistic marker genes also supported the adipogenesis of ADSCs in the GH
effect of chitosan/HA NPs for drug delivery. HA physically consol- cryogel in vitro. Based on the IHC and ICC staining of the phenotypic
idates the hydrophilic NP matrix, enabling a greater control over markers for adipocytes (PPARc and leptin) the angiogenic marker
drug release. CD31, and the expression of adipogenic marker genes, successful
adipose tissue engineering using committed ADSCs in the GH10
2.1.3.2. Hyaluronic acid blend with gelatin. Hydrogels, which are cryogel was also demonstrated in the nude mouse and porcine
widely used biomaterials, are prepared by chemical or physical animal models.
cross-linking [195] and can be used for drug delivery, substitution
of damaged tissue, filling soft tissue, etc. [196–199]. Soft tissue defi- 2.1.3.3. Hyaluronic acid blend with collagen. Collagen is a major
ciency is a common problem after traumatic injury, tumor ablation, part of connective tissues and it contributes to the formation, sup-
congenital underdevelopment and the natural changes of the aging port and protection of tissues and organs. Human-like collagen
process. Adipose tissue engineering is a promising method to solve (HLC) is efficiently expressed by recombinant Escherichia coli BL21.
these problems [188]. Scaffolds have an important role in tissue Zhang et al. [81] synthesized HA/HLC hydrogels, by cross linking of
Fig. 6. Synthetic scheme for CCD conjugates and DOX-loaded CCD self-aggregated nanoparticles [54].
1,4-butanedioldiglycidyl ether (BDDE) with HA/HLC, which showed and cartilage and it can bind to a core protein to produce extremely
low residual crosslinker (Fig. 7), excellent antienzyme proper- permeable aggrecan, which is a major structure inside cartilage and
ties and strength as compared to HA-based hydrogels, as well as performs as a shock absorber [201–203]. Zhao et al. [82] prepared
superior crosslinking density. The potential application for these HA/CS based hydrogel by using by gamma irradiation technique to
hydrogels are in tissue engineering field. be used as a drug delivery carrier or scaffold material for biomedical
applications. HA/CS/PVA hydrogels showed moderately high water
2.1.3.4. Hyaluronic acid blend with chondroitin sulfate. Chondroitin contents >90% and reached an equilibrium swelling state within
sulfate (CS) consists of repeating disaccharide units of d-glucuronic 24 h.
acid and N-acetyl galactosamine and sulfated glycosamino-glycan
(GAG), the sulfate groups are attached at either the 4- or 6-positions 2.1.3.5. Hyaluronic acid blend with hydroxyethyl cellulose. In trans-
[200]. It is an important structural component in connective tissues dermal delivery systems pH is an important parameter. The range
Fig. 7. Schematic diagram of crosslinking of HA/HLC hydrogels [81].
of pH for the skin surface, or stratum corneum (SC), is 5.0–6.0, (1 → 6) linkage in the main chains with ␣ (1 → 3) linkage at branch
to provide an effective barrier, as well as maintaining physiolog- points [207]. Dextran is highly biodegradable and biocompatible
ical processes [204,205]. To improve the solubility of cellulose, [208] and is used as a drug delivery vehicle in plasma/blood volume
cellulose-based derivatives including ethyl cellulose (EC), hydrox- expanders and as blood plasma substituent. It also used as a molec-
yethyl cellulose (HEC), methylcellulose (MC), hydroxypropyl ular sieve for separation and purification of bio-macromolecules
methylcellulose (HPMC), and sodium carboxymethylcellulose (Na- [208].
CMC) have been developed [206]. Kwon et al. [84] prepared
pH-sensitive hydrogels based on hydroxyethyl cellulose–HA for
2.1.4.1. Dextran blend with sulfate coated chitosan. Liposomes
transdermal delivery systems for skin lesions that are caused by
trap hydrophobic molecules and are used as carriers for drugs
pH imbalance and antimicrobial therapeutics.
and genes [209]. The amphiphilic chitosan derivatives of N,N
dimethyl hexadecyl carboxymethyl chitosan (DCMC) were suc-
2.1.4. Blends and composites of dextran with natural polymers cessfully synthesized from carboxymethyl chitosan (CMC). A
Dextran is produced from sucrose by enzymes on the cell surface novel amphiphilic chitosan derivative based liposome (DCMC-
of lactic acid bacteria or by Leuconostoc mesenteroides, is a water- L) containing certain functional groups (including amino group,
soluble glucan. It consists of d-anhydroglucosyl units joined by ␣ carboxymethyl salt group and alkyl quaternized group) have
Fig. 8. Synthesis of amphiphilic DCMC from CMC [74].

Fig. 10. Scheme of graft copolymerisation CMXG-g-PAAm [70].
simulated intestinal fluid (SIF). This novel delivery system has

strong EGCG (Epigallocatechin-3-gallate) protective capability,
high EGCG encapsulation capacity and quite good EGCG sustained
release property therefore DS-DCMC-NL was capable as a carrier
for EGCG delivery. The potential application of DCMC-NL is in food
processing.
2.1.4.2. Dextran blend with curcumin. Curcumin (Cur) is yellow col-

ored natural phenolic pigment having low molecular weight and
isolated from Curcuma longa (turmeric) [213]. It has many poten-
tial applications in medicine, coloring agent and dietary [214] and
is well-known for its antioxidant, antitumor, antibacterial, antimi-
crobial, anticoagulation, anti-inflammatory, anti HIV, antiamyloid,
antihyperlipidemic, antidiabetic, antineoplastic, antiangiogenic
and liver antifibrotic properties and due to these properties it can
Fig. 9. (a) Schematic representation for the synthesis of GAAm [77]; (b) Schematic
representation for the synthesis of GHDX by free radical graft copolymerisation of
inhibit cancer in variety of cell lines [215–217]. Encapsulation of
HEMA, and GAAm onto Dx using CAN and EGDMA [77]. Cur in nanoparticle based drug delivery system (DDS) with target-
ing ligands can decrease the dosage and enhance the efficiency of
drug [218]. NPs are suitable for the controlled and targeted delivery
been developed [210–212]. Zou et al. [74] prepared dextran sul- of anti-cancer drugs to tumor by enhanced permeation and reten-
fate coated amphiphilic chitosan derivatives-based nanoliposome tion (EPR) effect [219,220]. Anirudhan et al. [77] prepared dextran
(DCMC-NL) by dynamic high pressure microfluidization (DHPM) based nano sized carrier for the controlled and targeted delivery
combined with a film evaporation method (Fig. 8). DCMC-NL exhib- of curcumin to liver cancer cells by graft copolymerization from
ited high zeta potential, high encapsulation efficiency and low 2-hydroxyethylmethacrylate (HEMA) and glycyrrhetinic acid (GA),
mean particle size as well as easily precipitated after mixing with (Fig. 9a) [221,222] using ethylene glycol dimethacrylate (EGDMA)
Fig. 11. (a) Mechanism of Cation Action on CPAM/XG Macromolecules [91]; (b) Mechanism of Cation Action on HPAM/XG Macromolecules [91].
as crosslinker and ceric ammonium nitrate (CAN) as an initiator depends upon the concentration of XG i.e. DR efficiency falls by
(fig. 9b). The ideal concentration of Dx, CAN and EGDMA for graft- increasing XG concentration.
ing was found to be 1.0 g L−1 , 0.005 M and 0.001 M, respectively at Natural gas hydrate (NGH) consists of water and natural gas
ideal time of 300 min and a temperature of 55 ◦ C. molecules with a cage structure and is an ice-like crystalline com-
pound [232]. It is a metastable material that is stable only under
high pressure and low temperature. The drilling fluids used in
NGH drilling are mainly water-based and oil-based [233]. In the
2.2. Exopolysaccharides blends and composites with synthetic water-based drilling fluid, inorganic salt cations can not only reduce
polymers the freezing point of the drilling fluid but also have a negative
impact on the rheological properties of the drilling fluid [234].
2.2.1. Blends and composites of xanthan with synthetic polymers Both PAM and XG are common low cost, effective flocculant, poly-
2.2.1.1. Xanthan gum blend with poly(acryalamide). After derivati- electrolyte polymers. Anionic polyacrylamide (HPAM) is widely
zation of xanthan into carboxymethyl xanthan (CMX), solubility used to treat industrial and municipal wastewater. Cationic poly-
and reactivity of xanthan is increased because of the presence and acrylamide (CPAM), a highly efficient organic flocculant, can cause
ionization of CM group [223–226]. Badwaika et al. [70] synthesized colloidal particles to coalesce through “charge neutralization” and
carboxymethyl xanthan gum grafted poly(acryalamide) (CMXG-g- “absorption-bridging” effects with anions in waste water, thus puri-
PAAm) copolymers by free radical polymerisation in a nitrogen fying the water. This has many advantages, such as lower dosage,
atmosphere using ammonium persulphate as an initiator (Fig. 10). better flocculating effects, wide pH range, low toxicity and safety
CMXG-g-PAAm copolymers can be used as a potential carrier for [235,236]. Zhao et al. [91] mixed two types of polyacrylamide
drug delivery system. (CPAM and HPAM) with XG to form macromolecules. CPAM/XG
The drag reduction (DR) phenomenon is very dependent on the mixture has a strong cation-resistant stability as compared to
kind of drag reducer used. Fibrous particles, surfactants and poly- HPAM/XG (Fig. 11a,b). CPAM/XG is very important for developing
mers are used as a drag reducer [227,228]. Poly (ethylene oxide), NGH drilling fluid to improve borehole stability.
polyacrylamide and polyisobuthylene undergo mechanical degra-
dation, so they are blended with exopolysaccharides such as guar
gum and xanthan gum [229–231]. Anselmo et al. [59] analyzed 2.2.1.2. Xanthan blend with polypyrrole. Polypyrrole (PPy) is a
DR over time for three polymers, poly(ethylene oxide) (PEO), poly- conducting polymer that has unique physical properties such
acrylamide (PAM), XG as well as DR induced by flexible and rigid as ion exchange capacity, electrical conductivity, hydrophobicity
molecules. PEO and PAM are flexible polymers but XG is a rigid [237–246], cytocompatibility, electrical conductivity and environ-
polymer. The process of DR in rigid polymers is very different from mental stability [239,240,242]. Due to insolubility in common
that in flexible ones. By increasing concentration of PEO and PAM solvents and limited biocompatibility, PPy has restricted appli-
the level of DR and its efficiency also increases. However DR also cations [247–249]. Bueno et al. [68] prepared biocompatible
Fig. 12. (a) Schematic representation of the experimental setup for the production of XCA-PPy hybrid materials [68]; (b) Schematic representation of xanthan chains (blue)
cross linked with citric acid (red) and electropolymerized PPy chains (black) [68]. (For interpretation of the references to colour in this figure legend, the reader is referred
to the web version of this article.)
xanthan/PPy scaffolds for tissue engineering by electropolymer- peritoneal adhesion. As compared to unmodified HA, the grafted
ization (Fig. 12a). PPy chains are arranged parallel to XCA surface HA (HA-g-PAA) showed less degradation.
as a result porous stratified structure XCA-PPy is formed and in
this stratified structure of XCA-PPy films are arranged parallel to
PPy chains that enhance the strain as compare to XCA hydrogels
(Fig. 12b). Due to larger hydrophobicity and larger surface rough-
ness of XCA-PPy, it makes better scaffolds for fibroblasts than XCA.
Darzi et al. [58] synthesized novel XG/PPy nanocomposite by
oxidative polymerization of pyrrole in presence of XG and ammo-
nium peroxydisulfate. The thermal stability of nanocomposite
enhanced by increasing the amount of XG.
2.2.1.3. Xanthan gum blend with polyaniline. Polyaniline is most

well-known conducting polymer that, has good environmental sta-
bility and simple method of preparation [250–254]. The insolubility
among common solvents and non-biodegradability properties are
two main facts that restrict its applications [255,256]. Laramie et al.
[57] discussed fabrication, conductivity and thermal properties of
polyaniline/XG nanocomposite aqueous solution by oxidative poly-
merization of aniline in the presence of xanthan gum, in which
ammonium persulfate (APS) is as an oxidant. Xanthan gum is a
water soluble biopolymer that can affect the hydrophilic property
of polyaniline. By the addition of xanthan into polyaniline, elec-
trical conductivity and thermal stability of the nanocomposites is
improved.
2.2.2. Blends and composites of hyaluronic acid with synthetic

polymers
2.2.2.1. Hyaluronic acid grafted with polyacrylic acid. Grafting is an
effective method to functionalize native polysaccharides and there
are two methods of grafting such as “grafting to” and “grafting
from” [257,258]. The sodium salt of polyacrylic acid (PAA) is a
grafting polymer [259]. Nakagawaa et al. [87] developed a biocom-
patible calcium salt of HA grafted with PAA (HA-g-PAA) (Fig. 13) Fig. 13. (a) Schematic illustration of HA-g-PAA and formation of an insoluble cal-
for drug delivery in the peritoneum and for materials preventing cium salt of HA-g-PAA. (b) Synthetic route to HA-g-PAA [87].
Fig. 14. (a) Schematics for synthesis of HA–SH from HA; (b) Four-arm PEG–VS based on four-arm PEG; (c) Formation of the HA–PEG composite hydrogel via the Michael
addition reaction between HA–SH and four-arm PEG–VS [93].
2.2.2.2. Hyaluronic blend acid with polypyrrole. Molecular imprint- carriers to the disc [268,274–280]. The advantages of the
ing (MIPs) technology have excellent sensitivity, simplicity, rapid HA-composite hydrogels include an ability to “tune” physical prop-
response, low cost, in vivo detection and electrochemical sensors erties for the HA hydrogel as scaffolds or cell carriers [281–283].
properties, due to which it has been applied in sensor development Jeong et al. [93] prepared HA based poly(ethylene glycol) com-
and wide applications in medical, biological and environmental posite hydrogels by using artificial neural network analysis, in
fields [260–265]. Graphene is a two-dimensional sheet of carbon which Michael-type addition of thiolated HA (HA–SH) and four-arm
atoms having high electrical conductivity, high thermal and good PEG–vinylsulfone (PEG–4VS) of several molecular weights were
mechanical properties therefore it is considered as an ideal mate- used (Fig. 14). The main purpose of artificial neural network analy-
rial for the preparation of biosensors and electrochemical sensors sis to identify relationships between HA–PEG composite hydrogel
[266,267]. (Fig. 15).
Xing et al. [79] prepared electrochemical sensors based on MIPs
film of PPy – sulfonated graphene/HA – multiwall carbon nano- 2.2.2.4. Hyaluronic acid blend with poly(Ne-acryloyl l-lysine). Breast
tubes (PPy-SG/HA-MWCNTs/GCE) using tryptamine molecule by cancer is very dangerous disease that can cause death and in world-
electropolymerization. The function of PPy-SG composite films is wide about one in eight women develops metastatic breast cancer
to enhance conductivity and electrochemical performance and HA in their lifetime [284]. The new anticancer drugs are being hin-
act as dispersing agent to solubilize MWCNTs, therefore electro- dered by the lack of effective tumor models that closely mimic the
chemical sensor showed high selectivity, sensitivity and speed, human disease [285,286]. Due to biodegradable, non-immunogenic
appropriate for tryptamine detection in sample. and non-inflammatory characteristics HA has been used to con-
struct 3D tumor models and it is also used to promote tumor
2.2.2.3. Hyaluronic acid blend with poly(ethylene glycol). HA is a key progression through cell signaling as well as protects tumor tis-
component of the native extracellular matrix. HA biomaterials have sues against immune surveillance and chemotherapeutic agents
several advantages i.e., they are biocompatible with a long history [287,288]. However, HA hydrogels have poor mechanical proper-
of clinical use, non-immunogenic, and their side chains can be read- ties because a single cross-linked network lacks structural integrity
ily manipulated to present various functional groups [267–273]. [289]. In 3D cultures, cells are often fixed within a matrix material
HA-based biomaterials are combined with a second constituent that can mimic the tumor microenvironment (TME), where they
such as collagen, gelatin or poly(ethylene glycol) (PEG), as cell can migrate and experience cell-matrix interactions and cell–cell
Fig. 15. Schematic diagram for the preparation of pLysAAm/HA hydrogels with dually cross-linked networks [88].
Fig. 16. Schematic representation of the formation of QCS–polyaniline/oxidized dextran hydrogel [72].
contacts in all directions [290–294]. It is big challenge to design 3D breast cancer. An ideal 3D model has good mechanical properties
culture model for tumor engineering. Weijun et al. [88] prepared matching with the tumor tissue, similar microstructure and chem-
poly(Ne-acryloyl l-lysine)/HA hydrogel by photo-polymerization ical components to the tumor tissue, controllable degradability,
and this pLysAAm/HA hydrogels provided a more physiologically controlled release of bioactive substances and allowing the vas-
relevant 3D in vitro model for breast cancer (Fig. 16). The obtained cularization of matrix in vivo [295,296]. pLysAAm and PLL have a
pLysAAm/HA hydrogels displayed a double-network structure as similar chemical structure and ability to promote cell attachment
compared to in 2D monolayer culture, therefore this hydrogels through electrostatic interactions [297].
can provide a more physiologically relevant 3D in vitro model for
Fig. 17. Preparation of MG–Dexox composite hydrogels. (a) Gel formation and (b) the proposed reaction scheme. The MG particles and Dexox for (a) are not drawn to scale
to enhance clarity [71].
as a hydrophilic block and poly(4-methyl–caprolactone) (PMCL) or

poly(4-phenyl–caprolactone) (PBCL) acts as a hydrophobic block.
3. Conclusion and future prospects
Xanthan, curdlan, HA and dextran are EPS having multi-

dimensional properties such as non-toxicity, biocompatibility,
biodegradability and good mechanical properties. The composites
that are formed by the blending of EPS with natural and synthetic
polymers can be utilized in tissue engineering, protein delivery
system, targeted drug delivery system and encapsulation of drugs.
They are also used in food industry as an edible food film, coating
and food packing purpose. Consequently, wide use of EPS invites
great attention of researchers for preparing their blends with other
Fig. 18. Synthesis of amphiphilic photocleavable Dex-ONB-PMCL [78]. natural and synthetic polymers to explore novel applications in
various areas in future.
2.2.2.5. Hyaluronic acid blend with poly(Lactide-Co-Glycolide). Poly

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International Journal of Biological Macromolecules 94 (2017) 10–27

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International Journal of Biological Macromolecules

Blends and composites of exopolysaccharides; properties and

2.1.3. Blends and composites of hyaluronic acid with natural polymers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16

Sr. No. EPS Source Properties Applications Refs.

Fig. 1. Structure of Exopolysaccharides [44].

Sr. No Material Composition Techniques For Properties/Applications Refs.

1 Curdlan/Gellan Gum FTIR Adhesion prevention properties/applicable to [51]

Fig. 4. Proposed scheme for the preparation of AuNPs by CMC [53].

Fig. 5. Synthesis of curdlan/Boc-histidine hydrogel [55].

Fig. 7. Schematic diagram of crosslinking of HA/HLC hydrogels [81].

Fig. 8. Synthesis of amphiphilic DCMC from CMC [74].

Fig. 10. Scheme of graft copolymerisation CMXG-g-PAAm [70].

simulated intestinal ﬂuid (SIF). This novel delivery system has

2.1.4.2. Dextran blend with curcumin. Curcumin (Cur) is yellow col-

2.2.1.3. Xanthan gum blend with polyaniline. Polyaniline is most

2.2.2. Blends and composites of hyaluronic acid with synthetic

as a hydrophilic block and poly(4-methyl–caprolactone) (PMCL) or

3. Conclusion and future prospects

Xanthan, curdlan, HA and dextran are EPS having multi-

2.2.2.5. Hyaluronic acid blend with poly(Lactide-Co-Glycolide). Poly

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