Journal of Polymers and the Environment

https://doi.org/10.1007/s10924-020-02034-w

REVIEW

Utilization of Cereal Crop Residues, Cereal Milling, Sugarcane

and Dairy Processing By‑Products for Sustainable Packaging Solutions
Gaurav Kr Deshwal1 · Tanweer Alam2 · Narender Raju Panjagari1 · Aastha Bhardwaj3

Accepted: 31 December 2020

© The Author(s), under exclusive licence to Springer Science+Business Media, LLC part of Springer Nature 2021

Abstract
Residues and by-products are the unavoidable outputs of cereal, sugarcane and dairy processing industry which can be
resorted economically. Widespread focus on plastic replacement, residue burning and waste reduction had led to charac-
terization and identification of by-products for economic packaging applications. Extensive research work had been done
on whey usage in eco-friendly packaging but packaging applications of cereal crop residues, cereal milling by-products and
sugarcane bagasse are still in nascent stage. However, research studies on extraction and exploitation of cellulose, hemicel-
lulose and other film forming components from these by-products had been reported for packaging applications but described
processes have low techno-commerciality. Current status and innovations in utilization of cereal residue (rice straw, wheat
straw and corn cob), cereal milling by-products (husk, hull and bran), sugarcane processing waste (bagasse and sugar beet
pulp) and whey based packaging applications as well as application in bio-composites, are discussed briefly in this review.

Keywords  Cereal · By-products · Biodegradable · Whey · Agro-residue · Sugarcane · Packaging

Introduction presence of pesticides and other synthetic additives makes

Agricultural plastics represent the mulch, green house films,
bale wraps, fertilizer sacks and irrigation channels with
technique termed as ‘plasticulture’, which is a significant
contributor to plastic waste. However, if the boundaries of
agricultural plastics are expanded to include food packaging,
agricultural storage and transport containers, it will amount
to more than billion kilograms of plastic waste. Incinera-
tion and landfilling are costly ventures for such plastics and
* Aastha Bhardwaj
aasthabhardwaj90@gmail.com
Gaurav Kr Deshwal
ndri.gkd@gmail.com
Tanweer Alam
amtanweer@rediffmail.com
Narender Raju Panjagari
pnr.ndri@gmail.com
1 several other functional properties [2]. After harvesting the
Dairy Technology Division, National Dairy Research
Institute, ICAR​, Karnal, Haryana, India
2 ley etc., residues in the form of stems and stalks (stubble)
Indian Institute of Packaging, Mumbai, India
3
Department of Food Technology, Jamia Hamdard,
New Delhi, India
recycling a tortuous response. Conversely, technological
advances across the world had led to the development and
commercialization of various biodegradable packaging
materials though at higher cost but with comparable prop-
erties similar to their orthodox plastic analogue from non-
renewable sources. Some of the globally traded bio-plastics
available in the market are Mater-Bi™ (Novamont, Italy),
NatureWorks™ Polylactide (Cargill Dow, LLC), Bioska™
(Plastiroll®), Bioplast™, Solanyl™, Potatopac™, Green-
fil™ and Eco-Foam™ [1]. The use of such expensive bio-
degradable materials from costly raw materials will never
be a wise solution; rather finding some cheap source of raw
material for development of sustainable packaging solution
for agricultural plastics, food packaging and other packaging
applications will be accepted with both hands.
There are various by-products, waste and residues which
have the potential of their valorization and waste reduction
by their usage as a substrate for edible, biodegradable, anti-
microbial, antioxidant, agricultural films or coatings with
grains from the cereal crops like wheat, rice, maize, bar-
are generated. The residues are exploited as animal feed or
left in the field for reducing erosion but these methods are

13
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less cost effective and may lead to growth of undesirable
pests respectively. The burning of residues for clearing the
field leads to tremendous air pollution and loss of nutrients
whose effects on ecosystem and human health are severe. So,
the best choice is to exploit these residues as an important
source of fibrous biomass which holds the potential for paper
and bio-plastics production commercially [3]. The usage of
agricultural residues as substrate for production of bioplas-
tics reduces disposal problems, lowers environmental pollu-
tion, cuts the usage of petroleum based synthetic polymers
and produces biodegradable plastics at much lower cost [4].
Statistics
Every year nearly 500 million tons of agricultural residues
is generated in North America singly out of which around
25% is from wheat crops [5]. More than 100 million
tons of wheat residue is generated every year in United
States of America which is sufficient to fulfill the supply
of medium density paperboard. In South and East Asia,
nearly 26 million hectares of land is under rice and wheat
cultivation. Rice is the most residue-producing crop in
Asia (826 million tons) contributing 84% of total produc-
tion of the world [6]. Among the South Asian countries,
India is one of the highest contributors of agricultural
Fig. 1  Crop-wise residue
generated (million ton) in
various states of India during
2019–2020
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Journal of Polymers and the Environment
residues and by-products owing to ample irrigation land
per state. Figure 1 shows crop-wise residue generated (in
million tons) in various states of India, an agriculture-
based country, during 2019–2020.
In 2014, the worldwide demand of biodegradable plas-
tics was 1.4 million tons, which was anticipated to reach
6 million tons in 2019 with a compound annual growth
rate of 32.7%. According to a study, by the end of 2020,
about 30% of total plastics will be bio-plastics [7]. Accord-
ing to an expert estimate in USA, renewable/natural raw
substance will be contributing to 10% of materials by the
end of 2020 and 50% by 2050 [3]. Figure 2 depicts the
data pertaining to average generation of different cereal
residues and sugarcane bagasse worldwide. Addressing
the concern and headway in sustainable packaging mate-
rial from by-products/waste, this review is designed. The
low-cost raw materials for development of sustainable
packaging materials are broadly divided in four different
categories in this review article for a better understanding.
• Cereal crop waste (or residues): e.g. Straw, leaves and
stalks
• Cereal processing by-products: e.g. Bran, husk and hulls
• Sugarcane processing waste: e.g. Sugarcane bagasse and
sugar beet pulp
• Dairy by-products: e.g. Whey
Journal of Polymers and the Environment

Fig. 2  Average cereal residues

and sugarcane bagasse gener-
ated (in million tons) worldwide
during 2010–2020

Cereal Crop Residues and Cereal Milling
By‑Products
Cereals, the most widely consumed staple foods are cul-
tivated on 80% of world’s arable land. At large, around
50% of world’s population is dependent on cereals i.e.
wheat, rice, corn, millet, rye, barley etc. for their food
supply. Cereals are ground or milled to make them pro-
cessable into variety of products. The milling process
generates a variety of by-products like bran, middlings
etc. that possess a potential of their use in packaging mate-
rial, have been discussed in this review. Greater weight
loss which implies better degree of biodegradation in
agricultural crop residues (rice hulls, rice straw, wheat
residues, corn residues) as compared to wood shavings by
white rot fungus (Pleurotus ostreatus) signposts towards
their exponential upcoming use as counterpart/replace-
ment in paper or board manufacture processes [3]. Any
type of agricultural residues, irrespective of its origin and
composition (Table 1) has to be pretreated or modified
through physical, chemical or biological interventions for
their apt usage in material development process [8–11].
Physical process like crushing, grinding, sieving, mill-
ing, sifting, defibrillation is done for size reduction and
making it suitable for any further treatment. Heat treat-
ment sterilizes the raw material, prevents any microbial
growth and also enhances the level of substrate utiliza-
tion by augmenting the reaction rate. Chemical treatment
like addition of coupling agents, plasticizers, adhesives,
alkali or acid treatment modifies the properties of agro-
residues for better assimilation and adhesion properties.
Alkali treatment is generally given to agro-crop residues
(rice straw, maize straw and wheat straw) for impurity

Table 1  Agro-residues/wastes and their composition. All the values are on dry matter basis (% of mass)
Waste/By-product Water (%) Protein (%) Fat (%) Fiber (%) Minerals (%) Carbohydrates (%) References

Wheat straw 10.4 4.3 1.5 37.8* 7.1 – [8]

Rice straw 23.9 – – 36.0* 18.0 –
Corn cob 12.0 3.40 0.56 38.6 0.87 40.9* [9]
Sugarcane bagasse 47.8 – – – 1.1 70.9# [10]
Rice husk 13.1 8.3 2.5 – 1.4 87.8 [11]
Rice bran 9.0 13.0 14.0 15.2 – 57.8
Oat bran 9.2 8.9 3.5 2.8 – 84.8
Broken grains, husk 10–15 15 4–5 20–30 1–3 53–60
Sugar beet pulp 9.4 10 0.9 20.6 – 68.5
Whey 93.4–94.4 12.1–17.9 – – 7.6–14.3 76.8–80.3

*Cellulose on dry matter basis

#
 Total reducing sugars

13

(generally lignin and pectin) removal. The lignin removal
usually produces smooth fibres but the extent of impurity
removal varies with the raw material type [12]. Biological
methods involve the addition of microorganisms for lignin
removal and also degrade the waxy cuticle and hemicel-
luloses in the straw without much cellulose removal. These
treatments also improve the performance properties of
the composite structures by altering the extent of inter
linkages and impurity removal. This section, henceforth,
mainly deals with utilization of cereal crop residues and
cereal milling by-products in packaging material or com-
posite material development, either after minimal process-
ing, after extraction of useful component or as a reinforce-
ment filler.
Rice Straw
China, India and Indonesia are the largest rice producing
countries encompassing 60% of total world’s production.
As per an estimate, 2 lakh hectares of rice crop produces
1.5 million tonnes of residues which on burning generates
0.5 lakh tons of carbon monoxide [3]. Rice straw is often
reflected as solid trash owing to its insolvability in typical
organic solvents and low thermoplastic property. Chemical
modification by introduction of acetyl group in rice straw
with acetic anhydride in presence of mild acids have been
attempted to develop transparent biodegradable thermoplas-
tic films [13]. Rice straw-based copolymers, with enhanced
thermoplasticity, have been also developed by employing
graft copolymerization of ε‑Caprolactone onto acetylated
rice straw using ultrasonic-microwave co-assisted technol-
ogy [14]. A different facet showed the conversion of cellu-
lose removed from rice stubble residues into carboxymethyl
cellulose for its utilization in production of flexible packag-
ing material. The material developed with glycerol as plas-
ticizer was found to have appropriate mechanical properties,
water vapour barrier properties, opacity and biodegradabil-
ity which make it a preferable eco-friendly alternative for
food packaging purpose [15]. A study also reported pulping
methods of rice straw to obtain cellulosic fibres by potas-
sium hydroxide, soda and sodium sulphate (Kraft) process.
The extracted fibres when utilized for making paper sheets
showed satisfactory results with soda processed pulp (added
with 1% anthraquinone) retaining the best performance prop-
erties in terms of burst factor, stretch and drainage degree
[16]. Another study by Chollakup et al. (2020) aimed at
developing rice straw paper, through soda pulping of fibers,
and subsequent coating with pomelo peel extract intended
for bio-based and antibacterial food packaging [17].
Another technological intervention includes the devel-
opment of natural fiber-reinforced bio-composites, to
suffice the high cost of synthetic fibers and address the
13
Journal of Polymers and the Environment
environmental concerns over polymer based materials. The
rice straw characteristics (such as fibre length and fibre
extraction conditions) and quantity in composite material,
affects the performance properties of the developed bio-
composite. For instance, the flexural strength in poly lactic
acid and rice straw based green composites increased with
increasing fiber proportion and molding temperature with
maxima being attained at 30% fibre loading and 180 °C
molding temperature [18]. Another bio-composite, with
high tensile strength, has been developed based on poly
(hydroxybutyrate-co-hydroxy valerate) copolymer and rice
straw as reinforced agent [19]. Properties of bio-composites
involving rice straw based microfillers thus show promising
future in the water soluble plastic packaging applications.
Additionally, rice straw cellulose nanofibers and nano-crys-
tals, extracted via acid and alkali treatment, enzymes, ultra-
sonication, high-pressure homogenization, etc., have gained
prevalence owing to their high tensile strength, large sur-
face to volume ratio, and significant mechanical attributes.
Incorporation of rice straw CNCs as reinforcement fillers in
biopolymers such as PLA, PVA, and PVOH has also been
successfully demonstrated as a green alternative to develop
bio-nanocomposites with improved tensile, thermal and
morphological properties [20]. Table 2 shows recent devel-
opments in packaging material and bio-composite develop-
ment utilizing rice straw [21–24].
Rice Milling By‑products (Rice Bran, Husk
and Hull)
The annual production of rice is estimated at 550 million
tons globally and roughly 100 million tons of it is rice
hull [23]. It is considered that for each ton of rice milled,
approximately 0.23 ton of rice husk consisting 25–35% cel-
lulose and 18–21% hemicellulose is generated. Rice husk
has extensively been used as reinforcing material, in poly-
mer composites consisting of polyethylene, polypropylene,
polyvinyl chloride and polylactic acid as matrix, alongwith
other additives (like compatibilizer, adhesives, cross link-
ing and coupling agents) like montmorillonite, maleic anhy-
dride, urea–formaldehyde etc. [25]. Rice hulls and milling
by-products, after alkaline and acidic pretreatment were
incorporated in biodegradable starch films in form of cel-
lulose nanofibres. The films having rice, bleached rice hull
and rice hull nanofibers as reinforcing agents were having
better mechanical, barrier and optical properties, thus indi-
cating the potential of cereal milling waste in biodegradable
packaging films [26]. Majeed et al. [27], used rice husk as
reinforcing agent in low density polyethylene (LDPE) blown
films which decreased the barrier and mechanical proper-
ties above 5% rice husk loading weight but increased the
biodegradability. Similarly, rice bran is a low cost milling
 Table 2  Recent studies employing rice and wheat straw for film as well as bio-composite production
Type of material Method of film formation Methodology Film characterization Observation/Conclusion Reference
Journal of Polymers and the Environment

Rice straw (in films and in bio-composites)

Rice straw nano-fibrillated cellulose
film
Rice straw nanofiber blended in cel-
lulose acetate film
Chitosan based film with rice straw
and nano rice straw fibres as rein-
forcement
Rice straw cellulose nanofibrils-
enhanced polyvinyl alcohol films
Wheat Straw (in films and in bio-composites)
Poly(3‐hydroxylbutyrate‐co‐3‐
hydroxyvalerate) (PHBV)/wheat
straw fibers (WSF) bio composites
Wheat straw hemicelluloses film with
wheat straw cellulose nanocrystals
Suspension casting Supramolecular modification of XRD, TEM, FTIR Improvement in tensile strength, [21]
TEMPO-oxidized NFC porosity and water permeability;
Antimicrobial potential; application
in active packaging and healthcare
paper products
Solution casting Soda Pulping followed by Xylanase AFM, SEM, Thermal Stability Enhanced mechanical performance of [22]
pre-treatment the films
Wet mixing and casting Nano-fiber extraction by soda and acid FTIR, XRD, SEM Biodegradable food packaging bags [23]
pre-treatment by ultrasonication
Solution casting Willey mill grinding and high pressure FTIR, SEM, thermal properties Increase in tensile strength and modu- [24]
homogenization lus values
Extrusion Impact milling Overall Migration tests Low migration values. Application as [38]
food contact packaging material in
the case of food products with an ­aw
equal or lower than 0.90 (fruits and
vegetable, bread, and cheese)
Solution casting Steam explosion and alkali-acid diges- FTIR, SEM, Opacity Enhanced water resistance and water [39]
tion vapor barrier; use as biodegradable
wrapping or coating to a variety of
foods

13

by-product with approximately 70% starch, which shows the
possibility of its incorporation in biodegradable films. Rice
bran, used as a filler in a blow molded LDPE film at a rate of
5–10%, using twin screw extruder, showed enhanced tensil-
ity as well as biodegradability [28]. However, mechanical
and barrier attributes decreased for rice bran incorporated
films but it was suitable for normal packaging applications
and weight loss in films was observed during biodegrada-
tion [29]. The use of rice bran in its crude form (i.e. without
extracting starch) instead of utilizing extracted starch for
film preparation, could be a highly cost effective and novel
use of rice bran. The similar approach could also be used for
other by-products of cereal milling industry.
Wheat Straw
China is a leading producer of wheat, followed by India,
the United States, and Russia, together which contribute to
approximately 45% of the total world wheat production. This
clearly implies ample generation of wheat straw residues;
more than 650 million tons of wheat straw available per year
[30]. The possibilities of wheat straw exploitation as filler in
composite packaging material has not only aided in signifi-
cant reduction of the cost of the material, but also making
it light weight, thus improving its suitability for food pack-
aging applications. Delignification of wheat straw is com-
monly done by hydrogen peroxide, alkali (sodium hydrox-
ide) and acid treatment to produce uniform stable films else
cracked films are obtained [7]. Pretreatments like cutting,
drying, milling and sieving are performed to make wheat
straw suitable for mixing with thermoplastic pellets and
then co-extruding them to develop bio-composites for food
packaging. Advanced techniques like alkali steam explosion
combined with high shear mixing have also been used for
producing uniformly dispersed wheat straw nanofibres vary-
ing in size between 10 and 50 nm [31]. However, various
research studies on managing wheat straw in bio-composite
packaging material development had been reported previ-
ously [6, 7], but augmentation of their mechanical properties
still remains unanswered. Various coupling agents upgrade
the performance properties of agro-residue based composite
material as they enhance the level of linkages in the inter-
nal structure. An intermediate polymerization product of
polyurethane manufacturing process (prepolymer) when
introduced in recycled wheat straw-LDPE (low density poly-
ethylene) composites boosted its mechanical properties. The
free isocyanate end group in polyurethane prepolymer acted
as interfacial coupling agent, making it suitable for high load
carrying applications even under humid environment [32].
Similarly, citric acid in hemicellulose (extracted from wheat
straw and wheat based by-products) films improved the
water barrier and tensile property because of cross linking
13
Journal of Polymers and the Environment
and plasticization effect, thus providing a flexible film fit for
food packaging [6, 33].
Alkali treatment of wheat straw nanofibres doubled its
cellulose content due to hydrolysis of lignin and hemicel-
lulose impurities from the straw’s internal structure [34].
The adhesion and mechanical properties of injection molded
wheat straw HDPE (high density polyethylene) composites
had also been improved by removing lignin using white-
rot fungus Pleurotus ostreatus. In an effort to improve the
thermal properties, cellulose extracted from soy hull, a mill-
ing by-product of soybean oil production process and wheat
straw fibres were used for reinforced polymer manufactur-
ing. After proper chemical treatment (acid and alkali solubi-
lization), cryocrushing, milling and defibrillation of blended
raw material pulp, thermal properties of wheat straw and
soy by-product nanofibres improved efficiently i.e. thermal
degradation temperature above 290 °C was obtained [34].
Polyhydroxyl-3-butyrate-co-3-valerate (PHBV) is a fully
biodegradable polymer produced by microbial source and
processed into films using extrusion or injection process.
The fusion of wheat straw fibres in PHBV pellet-based
composite affected the mechanical properties adversely i.e.
loss of ductility and decrease in elongation at break [35].
Similarly, Berthet et al. [36] reported an inverse relation-
ship between wheat straw fibre size (millimeter to microm-
eter) and tensile properties of PHBV-wheat straw compos-
ites obtained after different preparatory (grinding, sifting,
impact milling, ball milling and selection sieving) steps.
Correspondingly, the adverse effects on mechanical proper-
ties were overcome by alkali treatment of wheat straw for
attaining microfibers and additional mechanical treatment of
alkali treated wheat straw microfibers to get nanofibres. In
another study, wheat straw’s micro and nanofibres showed
significant potential as reinforcing agent for polyvinyl alco-
hol based composite material having improved mechanical
(tensile modulus increased from 2.1 to 3 Giga pascal) and
thermal properties [37]. Table 2 shows recent developments
in packaging material and bio-composite development utiliz-
ing wheat straw [38, 39].
Wheat Milling By‑Products (Wheat Bran,
Husk and Hull)
Wheat bran is referred to as technological waste of mill-
ing process. The particle size and proportion of wheat bran
is inversely correlated with tensile strain and mechanical
properties of packaging materials [40]. Similarly, amount
of starch, protein and nature of plasticizer also affects prop-
erties of wheat bran extruded sheets. Sheets with higher
starch content had better tensile strength, water vapour bar-
rier properties and elongation at break. The best results in
terms of mechanical and barrier properties were obtained
Journal of Polymers and the Environment
for sorbitol plasticized sheets with higher starch and lower
protein [41]. Wheat bran having different particle size (0.4 to
0.8 mm) was studied for its aptness in injection molding of
LDPE based packaging material without any pro-adhesives.
The incorporation of wheat bran improved the biodegrada-
bility and reduced the mechanical properties, thermal deg-
radation point (160 °C), longitudinal shrinkage and cost.
In another study, combination of wheat and corn hulls as
reinforcing agent in starch matrix improved the tensile and
impact strength but reduced the elongation [42].
Corn Agro‑residues (Cob and Husk)
Corn is a cereal crop produced across the world and agro-
residues like corn cob, stalk, leaves and husk are left after
harvesting which are collectively referred as corn stover
[43]. In the year 2018, approximately a billion tons of corn
was produced worldwide generating huge amount of corn
cob and 70 million tons of corn husk [44]. The by-prod-
ucts of corn harvest are used for animal feeding, ethanol
production and also as filler in packaging materials. In the
recent past, corn husk had been used for the evolution of
bio-packaging materials either directly as pulp [45] or after
extracting cellulose [46] or as reinforcing agent in form of
nanofibres [47]. Pulverized corncobs are used in paper mak-
ing as it contains 47% cellulose and 37% hemicellulose, and
also as reinforcing agent in polypropylene composites [48].
The incorporation of corn cob into the packaging materials
provides the economic advantage but it reduces the mechani-
cal properties. The mechanical properties mainly depend
on the interaction between two substrates (surface energy,
wettability and roughness) and their chemical properties
(hydrophilicity and chemical sites). The corn cob introduc-
tion in chitosan bio-composites reduced the tensile property
and elongation at break while acrylic acid treated corn cob
powder enhanced the mechanical properties due to better
interfacial bonding [49]. Enhanced protein complexation
with corn polysaccharide in any bio-composite prerequisites
latter to be anionic due to which various chemical modifica-
tions like carboxymethylation, maleiation and succination
have been tried. The incorporation of carboxymethylated
corncob in soy protein isolate composite material possessed
tensile strength in range of 20 to 28 MPa (mega pascal)
which is equivalent to those of polytetrafluorethylene and
high-density polyethylene [48]. Similarly, the cross-linking
agent glutaraldehyde upgraded the tensile strength, thermal
stability and elongation at break of the corn cob and chitosan
biocomposite material [50]. Other cross-linking agents like
epichlorohydrin and adipic acid showed the same effect in
similar biocomposites [51].
Another dimension of corn agro-residue utilization in
packaging is extraction of xylan from corn cob followed
by its extrusion. The extracted arabinoglucuronoxylan
and extruded biopolymers based on it had very good ten-
sile strength (76 MPa) and elongation at break (35%). The
developed material was better than polylactic acid based bio-
plymers and use of twin screw extruder instead of solvent
casting demonstrated its commerciality [52]. Norashikin and
Ibrahim [42], created a biodegradable film using corn husk
waste, chitosan and acetic acid which had complete degrada-
bility within 7 to 9 months under soil burial test and the film
was also found suitable for developing pots (BioPot) for sap-
ling plantation. All these material development and property
enhancement research works demonstrate the huge potential
of rice, wheat and corn agro-residues in packaging arena.
Barley Straw and Husk
Barley is the fourth major cereal crop with 50 million of
cultivated area and 150 million tons of grain production
globally. Barley straw has a high carbon/nitrogen ratio
which causes nitrogen deficiency if left on the fields. Barley
husk, by-product of milling and brewing industry is used for
feeding animals. However, substantial amount of cellulose
in barley straw and husk brands them for packaging film
manufacture. Majority of the studies have advocated for the
use of barley straw and husk as a reinforcing agent. This
had been demonstrated by Borjesson et al. [53], that sug-
gests incorporation and transformation of barley husk into
new bio-based composites. In addition to this, the cellulose
nanocrystals present in barley straw and husk were extracted
by alkaline and enzymatic treatment and studied as reinforc-
ing agent in polyvinyl alcohol and chitosan biocomposites.
The optical, thermal and mechanical properties were found
to vary depending on the method of extraction, but showed
the potential of their introduction in active packaging [54].
Correspondingly, antimicrobial packaging is also a type of
active food packaging which interacts with the food product
and extends its shelf-life. Antioxidants derived from barley
husks by acid hydrolysis and delignification, were dispersed
over LDPE for wrapping frozen swordfish. The LDPE film
with sprayed antioxidants prevented the lipid damage and
also increased the oxidative stability of frozen swordfish
[55].
Miscellaneous Packaging Applications
of Cereal Residues and Milling by‑Products
(Oat Husk, Oat Hull, Corn Hull) with Other
Biodegradable Wastes
Each year approximately 4 million tons of corn hull, the
major by-product of corn milling industry is produced in
USA [56]. Oat hulls principally consist of approximately
13

30–35% cellulose and hemicelluloses and 2–10% lignin
while corn husk fibres have about 80–87% of cellulose and
6–8% of lignin. It has been reported that isolation of cellu-
lose nanofibrils from corn husks and oat hulls by oxidation
and high-pressure homogenization, can generate possibili-
ties of their exploitation in development of nano-packaging
material from agro-residues [57]. Development of biocom-
posites by incorporating oat hulls (hydrolyzed cellulose and
lignin) in biodegradable polymers (polylactic acid and poly-
propylene blend) was reported to have improved tensile and
flexural strength [58]. Yet another process of corn husk’s
etherification generated food grade carboxymethyl cellulose
which may be employed for development of sustainable food
packaging materials in near future [59]. Oxy-biodegradable
linear density polyethylene (LDPE) based packaging mate-
rial constituting pulverized husk of four different agricul-
tural crops i.e. wheat, corn, rice and soybean demonstrated
good mechanical properties at 50 µm thickness and suitable
biodegradability (51.5%) [60]. Likewise, introduction of
corn husk fibre in baked starch foam trays after mild pro-
cessing (cutting, hydrating, homogenizing and sifting) not
only reduced the cost but also improved the surface quality,
tensile strength and flexibility [61]. The incorporation of
nanocellulose extracted from oat husk at 5% concentration
strengthened the tensile property, young’s modulus, elon-
gation at break, water vapour barrier and opacity of whey
films [62].
Arabinoxylans are a heterogenous class of hemicelluloses
found in cereal milling by-products that have complex side
chains as compared to whole grain, thus making former the
best choice for development of biodegradable packaging and
coatings. Arabinoxylans and other hemicelluloses from most
of the cereal milling by-products i.e. corn hull [56], barley
husks [63], wheat bran [64] have good film forming ability
which reflect their importance and suitability as a sustain-
able raw material. Arabinoxylan is extracted using water,
mechanical (ultrasound, steam explosion, microwave, super-
critical ­CO2), chemical (sodium hydroxide and hydrochloric
acid) and enzymatic (endoxylanase) methods [65]. Ultrafil-
tration and diafiltration process purified the barley husk’s
arabinoxylan, thereby augmenting oxygen barrier property
of paperboard [63]. The wheat straw arabinoxylan films for-
tified with beta-glucan fatty acid from oat flour improved the
water vapour barrier, thermal stability and opacity due to
formation of laminar structure [66]. Exceptional mechanical
strength of films, in terms of puncture resistance, modulus
of elasticity, and tear resistance, made from arabinoxylan
extracts of wheat bran, along with sorbitol as a plasticizer,
indicate its utility in packaging application where it could be
used to protect food product from mechanical stress during
transportation and storage [67]. Arabinoxylan from maize
bran is most extensively used for sustainable and edible
packaging material after grafting it with fatty acids, sucro
13
Journal of Polymers and the Environment
esters and stearyl (meth) acrylate and glycerol as plasticizers
[65]. Seed coatings, edible films for encapsulating flavour
compounds, tough transparent films and several remark-
able applications of hemicelluloses extracted from cereal
milling products had been appraised thoroughly by Hansen
and Plackett [68]. However, sophisticated extraction meth-
ods and compromised mechanical properties of arabinoxy-
lan based films are still the major hurdles in upscaling as
it involves massive investment and technological barriers.
Wood plastic composites generally consist of thermoplas-
tic polymer as matrix and cellulosic material as reinforcing
material. Wood plastic composites consisting of thermoplas-
tic polymer polypropylene (PP) and rice husk fibres, bagasse
fibres and Kilka (Clupeonella engrauliformis) waste fish as
reinforcing material were developed using extruder and
evaluated for their biodegradability. As compared to pure
PP material, composites containing waste fish were having
higher degradation rates under soil burial tests while the
rice husk and bagasse fibres improved the tensile strength,
elongation at break, impact strength and flexural ability [69].
Extrusion process to fabricate the pellets demonstrated sig-
nificant engineering and functional potential of biodegrad-
able packaging prospects from agricultural wastes encom-
passing rice husk, rice bran, potato peels, deoiled rice bran,
banana peels and cashew nut shell [70].
Polyhydroxybutyrates (PHBs) are the macromolecules
produced during bacterial fermentation and most signifi-
cantly used for bioplastics’ production because of their 100%
biodegradability. However, very high contribution of initial
raw material in its production cost had forced researchers
to search for alternative substrates for bacterial fermenta-
tion. Agricultural residues like sugarcane bagasse, corn cob,
banana peel and teff (Eragrostis teff) straw had been utilized
as carbon source for PHB producing microorganisms and
development of biodegradable plastics. In a study, agro-
residues were dried, milled and hydrolyzed by zinc chloride
for their use as carbon source resulting sugarcane bagasse as
the cheapest carbon source followed by corn cob. PHB pro-
duction was least (27%) in banana peel inspite of significant
bacterial growth because of relatively less reducing sugar
content in pretreated banana peel [71].
Sugarcane Processing By‑products (Bagasse
and Sugar Beet Pulp)
An estimated amount of 540 million metric tons of sugarcane
bagasse (SB) is produced worldwide annually from distiller-
ies and sugar factories. Sugarcane bagasse, at large is used as
fuel or burnt down in fields or as an animal feed in develop-
ing countries, and has also been used in various biotechno-
logical (enzyme extraction) and non-biotechnological (single
cell protein) applications. The valued 33.5% hemicellulose
Journal of Polymers and the Environment
present in sugarcane bagasse has been acknowledged as a
key ingredient in development of biodegradable packag-
ing films and coatings for food industries. Hemicellulose
is extracted from sugarcane bagasse using alkali treat-
ment alone, alkali-peroxide treatment, acid hydrolysis [72]
and enzymatic treatment [73] and films can be developed
using casting or extrusion techniques. The application also
expands to production of foam trays by baking process [74,
75], which points out to the fact that these can replace the
expanded polystyrene (EPS) based materials. The hemicel-
lulose-based films and their characterization have shown the
potential for production of biodegradable films for various
packaging applications [76]. Some researchers had even
utilized the hemicellulose of sugarcane bagasse as a plas-
ticizer in cellulose acetate films developed from acetylated
bagasse cellulose [77]. An all-cellulose nanocomposite film
and sheets i.e. having both fibre and matrix of cellulose was
developed using sugarcane bagasse cellulose nanofibres.
Both films and sheets were not only fully biodegradable but
were also found to be suitable for food packaging applica-
tions based on their acceptable water barrier properties and
toughness [78]. Sugarcane bagasse derived nano-cellulose,
has been a subject of intense research in recent decades due
to their renewability, high strength as well as eco-friendly
nature [79]. Techniques for nano-fibrillation include ultra-
sonication; homogenization, microfluidization, mechanical
grinding etc. [80–82]. Sugarcane bagasse fiber cellulose
nanocrystals have witnessed prevalence and have been
regarded as the next generation green material for packaging
purposes. Furthermore, sugarcane bagasse cellulose based
functional film impregnated with a cashew nut extract, using
interfacial assembly, resulted in an active packaging film
with pH-triggered release mechanism and showed potential
for enhancing the shelf life of perishable food commodities
[83].
The development of advanced bio-composite materials,
such as, sugarcane bagasse fiber reinforced polymer com-
posites have also demonstrated excellent specific strength
and high modulus, in addition to being environmentally at
stages of production, processing as well as disposal [84].
Nano-composites are also significant in achieving remark-
able barrier properties. Additionally, eco-friendly nano-bio-
composite films using 0.5–10% cellulose nanocrystals from
sugarcane bagasse in polyvinyl alcohol/carboxymethyl cel-
lulose blend matrix showed good tensile strength, high water
vapour barrier and almost equivalent transparency in com-
parison to control films (i.e. without any cellulose nanocrys-
tals) [85]. Poly-(butylene succinate adipate) (PBSA) is
the most vital biodegradable plastic because of its better
mechanical strength and hydrophobicity but its high produc-
tion cost is a barrier in its wide commercialization. Sugar-
cane bagasse incorporation in PBSA based composite mate-
rial had positive effect on mechanical properties because
of better interaction between carboxyl groups of PBSA and
hydroxyl groups of bagasse cellulose and the material also
degraded completely in microbial compost within 60 days
[86]. Table 3 shows several recent developments in regard
to SB nano-cellulose based films and bio-composites, hav-
ing potential to be employed in food packaging applications
[83, 87–91].
Sugar beet pulp is another by-product of sugar refin-
ing industry having 20% cellulose, 25% hemicellulose and
25–30% pectin. During 2011, the sugar industries of USA
singly threw away 26.7 million tons of sugar beet pulp based
on dry matter basis. It finds miscellaneous applications in
the form of energy rich animal feed supplement, fuel source
and platform chemicals. However, the presence of sugar beet
lignocellulose also makes it a suitable alternative for flex-
ible and biodegradable packaging films. Different treatments
like cryo-crushing, homogenization, alkali extraction and
bleaching using sodium chlorite are given to the raw sugar
beet pulp for film preparation. Casting and hot press methods
create self-supported films with good mechanical and optical
properties (i.e. transparency) [92]. Another dimension of
sugar beet pulp usage in packaging is the use of compression
heating technique for composite materials based on sugar
beet pulp and polylactic acid with high cost effectiveness
as compared to single polylactic acid-based films [93]. An
equal proportion of sugar beet pulp and polyvinyl alcohol
(PVOH) had been reported as the best suitable biodegrad-
able composite film material based on tensile strength, ther-
mal and barrier properties [94].
Dairy By‑Products
A dairy by-product could be defined as the product achieved
through the processing/manufacturing of any major dairy
product. Skim milk, buttermilk, whey and ghee residue
are the major rudimentary by-products of dairy processing
industry. Skim milk and buttermilk are either used for direct
consumption or in other dairy products (yoghurt, cheese,
probiotic drinks and ice-cream) to enhance their functional
properties. Ghee residue is a by-product with very high
nutritive value and has been incorporated in chocolate,
candy, edible paste and other bakery products at laboratory
scale. Currently, consequential research and development for
ghee residue utilization in high worth products is impera-
tive. Casein-rich water is another plentiful, but underuti-
lized protein source which is generated during the clean-
ing of dairy plants. Ryder et al. [95] suggested the use of
casein rich material (referred to as DAF-casein) harvested
from dairy wastewater using a dissolved air flotation (DAF)
procedure having potential for the formation of biopolymer
composites, upon inclusion with κ-carrageenan, sodium
13
 Journal of Polymers and the Environment

Table 3  Sugarcane bagasse (SB) nanocellulose based packaging films and bio-composites

Formulations Technique involved Functional Properties/Key findings and References
proposed application

SB nanocellulose/nanofibrils
SB microcrystalline cellulose film incorpo-
rated with cashew nut extract
SB cellulose nanofibrils/nisin nano-hybrid
films
SB based nanofibrillated CNF with hydro-
phobic fluorinated polymer coating
Sugarcane bagasse nanocellulose-based
hydrogel
SB as bio-composite/bio-nanocomposite
CMC-Starch film reinforced with SB
nanocrystals
PVA/Starch film reinforced with SB nano-
cellulose
Interfacial assembly
Solution casting
Aqueous counter collision
Ionic-crosslinking and induced gelation Colorimetric freshness indicator for moni-
Sulfuric acid hydrolysis; extraction and Good optical transparency, eco-friendly,
solution casting for film formation
Akaline digestion and ultrasonication
Anti-oxidant and anti-microbial film with [83]
pH-triggered release mechanism as an
active packaging film for perishable food
commodities
Antimicrobial film with low oxygen and [87]
water vapor permeability for active pack-
aging of foods
Transparent, water resistant and oxygen [88]
barrier property for food that require high
oxygen barrier
[89]
toring spoilage of chicken breast (applica-
tion in intelligent packaging of foods)
[90]
reduced WVP and increased tensile
strength, required for packaging applica-
tions
Strong adhesion and interfacial bonding [91]
between polar molecules of PVA starch
blend and SB nanocellulose resulted in
water resistant packaging film

carboxymethylcellulose (NaCMC) and gelatin to produce
excellent physical strength and self-associating properties
(Table 4).
Whey is utilized to produce other valuable products like
whey powder, whey protein isolate, lactose powder and
demineralized whey which prerequisites expensive equip-
ment and complex manufacturing process. Whey protein has
been explored for development of coatings alongwith edible,
active, biodegradable, stand-alone and flexible packaging
materials which have penetrated the market to a great extent
and are not very far from assembly line production.
Whey
Whey is the most abundant green coloured translucent liq-
uid by-product of dairy industry, obtained through the pro-
duction process of cheese, casein, co-precipitate and other
traditional Indian dairy products like paneer, chhana and
chakka. Approximately 186 million tons of whey was pro-
duced worldwide in 2008 and 70% of it was contributed
by European Union and United States. Due to very high
biochemical oxygen demand (BOD) i.e. 40,000 mg/kg and
significant amount of organic matter (lactose, protein, miner-
als and water-soluble vitamins), its disposal causes degrada-
tion of environment [96]. Whey majorly consists of globular
proteins like beta-lactoglobulin (β-lg) and alpha-lactalbumin
(α-lb) which have the ability to unfold and interact with each
other to develop a three-dimensional structure on varying
temperature, pH, shear forces or addition of salts and sol-
vents. Solvent casting, physical vapour deposition, spraying,
spin coating and extrusion are some of the methods used
for developing whey-based packaging film both for research
and large scale production. Thermal denaturation of whey
protein is a significant step involved in film development
process which mainly occurs at 78 °C but it still varies with
the composition of whey film forming solution [97]. The
whey films developed under high temperature are more
brittle and highly tensile because of excessive cross-link-
ing. Hydrostatic pressure is also used for developing whey
protein based biodegradable films but as compared to heat
induced films, hydrostatic pressure processed films shows
lower mechanical properties because of weaker interactions
of β-lg gels [98].
Whey protein-based films are generally transparent and
flexible with good barrier properties but have poor mechani-
cal strength. Irradiation treatment like gamma radiation and
ultraviolet (UV) radiation generate cross linkages necessary
for whey protein film formation. Dityrosine bridges induced
by gamma radiations and free radical formations induced
by UV rays are responsible for the same. Other than physi-
cal agents including heat treatment, extrusion, hydrostatic
pressure and ultrasonic treatment, chemical modifications
due to pH changes (alkylation, acetylation, succinylation)

13
 Table 4  Whey based packaging films
Journal of Polymers and the Environment

Ingredients/formulations Method Functional properties/key findings Proposed application References

Poly (3-hydroxybutyrate-co-3-hydroxyvalerate) Nanoprecipitation High mechanical strength than other polymers Plastic replacement [103]
by Bacillus megaterium utilizing Cheese Whey
Permeate
Whey based films incorporated with natamycin and Microfluidization Antioxidant activity and antibacterial activity Active food packaging [104]
nanoemulsion of α-tocopherol against C. albicans, P. chrysogenum, and S. cer-
evisiae
Whey protein films and coatings added with prebi- Film forming Diversification of functional foods in the market Edible films for fruits and vegetables, dairy, meat [105]
otic ingredients and bakery products
Duplex and triplex laminated edible films using Solution casting Composition with Sodium alginate showed best Miscellaneous food and packaging industries [106]
whey protein isolate, gelatin and sodium alginate water vapor and oxygen barrier; also highest
tensile strength and elasticity
Whey protein-based plastic Co-polymerization It is economically feasible to produce plastics from Plastic replacement [107]
whey wastes
Whey protein–gelatin–nanoclay films with orange Solution casting Biodegradable and antibacterial property Food packaging [108]
peel extract and tripolyphosphate
Whey protein isolate/polyaniline Solution casting Semi-conducting properties Smart packaging to monitor electrical properties [109]
of foods
Whey protein film incorporated with green tea Solution casting Higher antioxidant capacity Active packaging; delaying lipid oxidation of fresh [110]
extract salmon

13

and biochemical modifications involving peptidases, hydro-
lysates and transglutaminases enzymes had also been used
for modifying whey protein film properties. Peptidases and
whey protein hydrolysates cleave the peptide bonds thereby
improving the film flexibility and reducing the amount of
plasticizer required for film preparation [99], while transglu-
taminases owing to the formation of ε-(γ-glutamyl) lysine
bond improves the water vapour barrier and mechanical
properties of the films [100]. Low-pressure glow plasma
has shown potential for modifying protein films by surface
ablation or etching, cross-linking, and modification of func-
tional properties [101]. Dielectric barrier discharge plasma
is another novel method of polymer surface modification
technology employed for whey protein concentrate (WPC)/
wheat cross‐linked starch (WCS) composite films with
enhanced mechanical and barrier properties [102]. Table 2
summarizes a latest prior-art on the development of func-
tional whey-based films with their respective applications
[103–110]. Whey protein films offer the opportunities of
recyclability (in case of multilayered laminates) as well as
biodegradability. The rate of biodegradation depends on film
composition and cross-linkages.
In the project WHEYLAYER, the commercialization
and small-scale production of whey based sustainable food
packaging material as a replacement of synthetic polymer
ethylene vinyl alcohol copolymers (EVOH) was evaluated.
The whey coating was applied on a layer of PET at semi-
industrial scale and showed escalated oxygen barrier and
compatibility with ‘buttercheese’ (semi-soft, cow’s milk
German cheese) thus outperforming EVOH. Terg-a-zyme®
detergent removed the whey coating form the multilayered
material within 2 h, making the base layer (PET) suitable for
recycling [111]. Henceforth, huge amount of whey produced
every year and its utilization in pilot scale production of
whey-based packaging materials with biodegradability and
recyclability preferences illustrates the leeway of replacing
synthetic polymers.
Conclusion/Future Prospects
Presently, the market of agro-residues, whey and bagasse
based biodegradable and edible packaging materials is
limited by low techno-commerciality. It is the view of the
authors that sophisticated and expensive chemical pro-
cesses involved in their production process poses a major
limitation in their commercialization. The newly developed
process should be cyclic without any chemical or biologi-
cal imbalance in the ecosystem. The performance proper-
ties (mechanical, barrier and appearance) still need to be
improved with more advanced technological breakthroughs.
The new technologically advanced process should focus on
use of agricultural crop residues and other waste by-products
13
Journal of Polymers and the Environment
with minimal processing in packaging applications instead
of extracting any component and utilizing it. In the following
years, more efforts are required for upscaling of the process
involved in manufacture of sustainable packaging materi-
als. However, at present, persuading the customers to use
eco-friendly packaging materials as a substitute to cheaper
synthetic options is the biggest challenge. A Germany based
firm, BIO-LUTIONS® is purchasing agricultural waste
(wheat straw, pineapple leaves, banana peels and water hya-
cinth plants) from the farmers and using it for producing bio-
degradable disposable dishware, thereby reducing the agro-
waste as well as preventing pollution from plastic tableware
(BIO-LUTIONS, 2019) [112]. Such kind of initiatives needs
to be promoted by the authorities along with better policy
framework for managing the agricultural waste.
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