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

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

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 Journal of Polymers and the Environment

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

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

Fig. 2  Average cereal residues

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

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

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 Journal of Polymers and the Environment

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

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

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 Journal of Polymers and the Environment

by-product with approximately 70% starch, which shows the and plasticization effect, thus providing a flexible film fit for
possibility of its incorporation in biodegradable films. Rice food packaging [6, 33].
bran, used as a filler in a blow molded LDPE film at a rate of Alkali treatment of wheat straw nanofibres doubled its
5–10%, using twin screw extruder, showed enhanced tensil- cellulose content due to hydrolysis of lignin and hemicel-
ity as well as biodegradability [28]. However, mechanical lulose impurities from the straw’s internal structure [34].
and barrier attributes decreased for rice bran incorporated The adhesion and mechanical properties of injection molded
films but it was suitable for normal packaging applications wheat straw HDPE (high density polyethylene) composites
and weight loss in films was observed during biodegrada- had also been improved by removing lignin using white-
tion [29]. The use of rice bran in its crude form (i.e. without rot fungus Pleurotus ostreatus. In an effort to improve the
extracting starch) instead of utilizing extracted starch for thermal properties, cellulose extracted from soy hull, a mill-
film preparation, could be a highly cost effective and novel ing by-product of soybean oil production process and wheat
use of rice bran. The similar approach could also be used for straw fibres were used for reinforced polymer manufactur-
other by-products of cereal milling industry. 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
Wheat Straw soy by-product nanofibres improved efficiently i.e. thermal
degradation temperature above 290 °C was obtained [34].
China is a leading producer of wheat, followed by India, Polyhydroxyl-3-butyrate-co-3-valerate (PHBV) is a fully
the United States, and Russia, together which contribute to biodegradable polymer produced by microbial source and
approximately 45% of the total world wheat production. This processed into films using extrusion or injection process.
clearly implies ample generation of wheat straw residues; The fusion of wheat straw fibres in PHBV pellet-based
more than 650 million tons of wheat straw available per year composite affected the mechanical properties adversely i.e.
[30]. The possibilities of wheat straw exploitation as filler in loss of ductility and decrease in elongation at break [35].
composite packaging material has not only aided in signifi- Similarly, Berthet et al. [36] reported an inverse relation-
cant reduction of the cost of the material, but also making ship between wheat straw fibre size (millimeter to microm-
it light weight, thus improving its suitability for food pack- eter) and tensile properties of PHBV-wheat straw compos-
aging applications. Delignification of wheat straw is com- ites obtained after different preparatory (grinding, sifting,
monly done by hydrogen peroxide, alkali (sodium hydrox- impact milling, ball milling and selection sieving) steps.
ide) and acid treatment to produce uniform stable films else Correspondingly, the adverse effects on mechanical proper-
cracked films are obtained [7]. Pretreatments like cutting, ties were overcome by alkali treatment of wheat straw for
drying, milling and sieving are performed to make wheat attaining microfibers and additional mechanical treatment of
straw suitable for mixing with thermoplastic pellets and alkali treated wheat straw microfibers to get nanofibres. In
then co-extruding them to develop bio-composites for food another study, wheat straw’s micro and nanofibres showed
packaging. Advanced techniques like alkali steam explosion significant potential as reinforcing agent for polyvinyl alco-
combined with high shear mixing have also been used for hol based composite material having improved mechanical
producing uniformly dispersed wheat straw nanofibres vary- (tensile modulus increased from 2.1 to 3 Giga pascal) and
ing in size between 10 and 50 nm [31]. However, various thermal properties [37]. Table 2 shows recent developments
research studies on managing wheat straw in bio-composite in packaging material and bio-composite development utiliz-
packaging material development had been reported previ- ing wheat straw [38, 39].
ously [6, 7], but augmentation of their mechanical properties
still remains unanswered. Various coupling agents upgrade
the performance properties of agro-residue based composite Wheat Milling By‑Products (Wheat Bran,
material as they enhance the level of linkages in the inter- Husk and Hull)
nal structure. An intermediate polymerization product of
polyurethane manufacturing process (prepolymer) when Wheat bran is referred to as technological waste of mill-
introduced in recycled wheat straw-LDPE (low density poly- ing process. The particle size and proportion of wheat bran
ethylene) composites boosted its mechanical properties. The is inversely correlated with tensile strain and mechanical
free isocyanate end group in polyurethane prepolymer acted properties of packaging materials [40]. Similarly, amount
as interfacial coupling agent, making it suitable for high load of starch, protein and nature of plasticizer also affects prop-
carrying applications even under humid environment [32]. erties of wheat bran extruded sheets. Sheets with higher
Similarly, citric acid in hemicellulose (extracted from wheat starch content had better tensile strength, water vapour bar-
straw and wheat based by-products) films improved the rier properties and elongation at break. The best results in
water barrier and tensile property because of cross linking terms of mechanical and barrier properties were obtained

13
Journal of Polymers and the Environment

for sorbitol plasticized sheets with higher starch and lower by its extrusion. The extracted arabinoglucuronoxylan
protein [41]. Wheat bran having different particle size (0.4 to and extruded biopolymers based on it had very good ten-
0.8 mm) was studied for its aptness in injection molding of sile strength (76 MPa) and elongation at break (35%). The
LDPE based packaging material without any pro-adhesives. developed material was better than polylactic acid based bio-
The incorporation of wheat bran improved the biodegrada- plymers and use of twin screw extruder instead of solvent
bility and reduced the mechanical properties, thermal deg- casting demonstrated its commerciality [52]. Norashikin and
radation point (160 °C), longitudinal shrinkage and cost. Ibrahim [42], created a biodegradable film using corn husk
In another study, combination of wheat and corn hulls as waste, chitosan and acetic acid which had complete degrada-
reinforcing agent in starch matrix improved the tensile and bility within 7 to 9 months under soil burial test and the film
impact strength but reduced the elongation [42]. 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
Corn Agro‑residues (Cob and Husk) of rice, wheat and corn agro-residues in packaging arena.

Corn is a cereal crop produced across the world and agro-

residues like corn cob, stalk, leaves and husk are left after Barley Straw and Husk
harvesting which are collectively referred as corn stover
[43]. In the year 2018, approximately a billion tons of corn Barley is the fourth major cereal crop with 50 million of
was produced worldwide generating huge amount of corn cultivated area and 150 million tons of grain production
cob and 70 million tons of corn husk [44]. The by-prod- globally. Barley straw has a high carbon/nitrogen ratio
ucts of corn harvest are used for animal feeding, ethanol which causes nitrogen deficiency if left on the fields. Barley
production and also as filler in packaging materials. In the husk, by-product of milling and brewing industry is used for
recent past, corn husk had been used for the evolution of feeding animals. However, substantial amount of cellulose
bio-packaging materials either directly as pulp [45] or after in barley straw and husk brands them for packaging film
extracting cellulose [46] or as reinforcing agent in form of manufacture. Majority of the studies have advocated for the
nanofibres [47]. Pulverized corncobs are used in paper mak- use of barley straw and husk as a reinforcing agent. This
ing as it contains 47% cellulose and 37% hemicellulose, and had been demonstrated by Borjesson et al. [53], that sug-
also as reinforcing agent in polypropylene composites [48]. gests incorporation and transformation of barley husk into
The incorporation of corn cob into the packaging materials new bio-based composites. In addition to this, the cellulose
provides the economic advantage but it reduces the mechani- nanocrystals present in barley straw and husk were extracted
cal properties. The mechanical properties mainly depend by alkaline and enzymatic treatment and studied as reinforc-
on the interaction between two substrates (surface energy, ing agent in polyvinyl alcohol and chitosan biocomposites.
wettability and roughness) and their chemical properties The optical, thermal and mechanical properties were found
(hydrophilicity and chemical sites). The corn cob introduc- to vary depending on the method of extraction, but showed
tion in chitosan bio-composites reduced the tensile property the potential of their introduction in active packaging [54].
and elongation at break while acrylic acid treated corn cob Correspondingly, antimicrobial packaging is also a type of
powder enhanced the mechanical properties due to better active food packaging which interacts with the food product
interfacial bonding [49]. Enhanced protein complexation and extends its shelf-life. Antioxidants derived from barley
with corn polysaccharide in any bio-composite prerequisites husks by acid hydrolysis and delignification, were dispersed
latter to be anionic due to which various chemical modifica- over LDPE for wrapping frozen swordfish. The LDPE film
tions like carboxymethylation, maleiation and succination with sprayed antioxidants prevented the lipid damage and
have been tried. The incorporation of carboxymethylated also increased the oxidative stability of frozen swordfish
corncob in soy protein isolate composite material possessed [55].
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 Miscellaneous Packaging Applications
agent glutaraldehyde upgraded the tensile strength, thermal of Cereal Residues and Milling by‑Products
stability and elongation at break of the corn cob and chitosan (Oat Husk, Oat Hull, Corn Hull) with Other
biocomposite material [50]. Other cross-linking agents like Biodegradable Wastes
epichlorohydrin and adipic acid showed the same effect in
similar biocomposites [51]. Each year approximately 4 million tons of corn hull, the
Another dimension of corn agro-residue utilization in major by-product of corn milling industry is produced in
packaging is extraction of xylan from corn cob followed USA [56]. Oat hulls principally consist of approximately

13
 Journal of Polymers and the Environment

30–35% cellulose and hemicelluloses and 2–10% lignin esters and stearyl (meth) acrylate and glycerol as plasticizers
while corn husk fibres have about 80–87% of cellulose and [65]. Seed coatings, edible films for encapsulating flavour
6–8% of lignin. It has been reported that isolation of cellu- compounds, tough transparent films and several remark-
lose nanofibrils from corn husks and oat hulls by oxidation able applications of hemicelluloses extracted from cereal
and high-pressure homogenization, can generate possibili- milling products had been appraised thoroughly by Hansen
ties of their exploitation in development of nano-packaging and Plackett [68]. However, sophisticated extraction meth-
material from agro-residues [57]. Development of biocom- ods and compromised mechanical properties of arabinoxy-
posites by incorporating oat hulls (hydrolyzed cellulose and lan based films are still the major hurdles in upscaling as
lignin) in biodegradable polymers (polylactic acid and poly- it involves massive investment and technological barriers.
propylene blend) was reported to have improved tensile and Wood plastic composites generally consist of thermoplas-
flexural strength [58]. Yet another process of corn husk’s tic polymer as matrix and cellulosic material as reinforcing
etherification generated food grade carboxymethyl cellulose material. Wood plastic composites consisting of thermoplas-
which may be employed for development of sustainable food tic polymer polypropylene (PP) and rice husk fibres, bagasse
packaging materials in near future [59]. Oxy-biodegradable fibres and Kilka (Clupeonella engrauliformis) waste fish as
linear density polyethylene (LDPE) based packaging mate- reinforcing material were developed using extruder and
rial constituting pulverized husk of four different agricul- evaluated for their biodegradability. As compared to pure
tural crops i.e. wheat, corn, rice and soybean demonstrated PP material, composites containing waste fish were having
good mechanical properties at 50 µm thickness and suitable higher degradation rates under soil burial tests while the
biodegradability (51.5%) [60]. Likewise, introduction of rice husk and bagasse fibres improved the tensile strength,
corn husk fibre in baked starch foam trays after mild pro- elongation at break, impact strength and flexural ability [69].
cessing (cutting, hydrating, homogenizing and sifting) not Extrusion process to fabricate the pellets demonstrated sig-
only reduced the cost but also improved the surface quality, nificant engineering and functional potential of biodegrad-
tensile strength and flexibility [61]. The incorporation of able packaging prospects from agricultural wastes encom-
nanocellulose extracted from oat husk at 5% concentration passing rice husk, rice bran, potato peels, deoiled rice bran,
strengthened the tensile property, young’s modulus, elon- banana peels and cashew nut shell [70].
gation at break, water vapour barrier and opacity of whey Polyhydroxybutyrates (PHBs) are the macromolecules
films [62]. produced during bacterial fermentation and most signifi-
Arabinoxylans are a heterogenous class of hemicelluloses cantly used for bioplastics’ production because of their 100%
found in cereal milling by-products that have complex side biodegradability. However, very high contribution of initial
chains as compared to whole grain, thus making former the raw material in its production cost had forced researchers
best choice for development of biodegradable packaging and to search for alternative substrates for bacterial fermenta-
coatings. Arabinoxylans and other hemicelluloses from most tion. Agricultural residues like sugarcane bagasse, corn cob,
of the cereal milling by-products i.e. corn hull [56], barley banana peel and teff (Eragrostis teff) straw had been utilized
husks [63], wheat bran [64] have good film forming ability as carbon source for PHB producing microorganisms and
which reflect their importance and suitability as a sustain- development of biodegradable plastics. In a study, agro-
able raw material. Arabinoxylan is extracted using water, residues were dried, milled and hydrolyzed by zinc chloride
mechanical (ultrasound, steam explosion, microwave, super- for their use as carbon source resulting sugarcane bagasse as
critical ­CO2), chemical (sodium hydroxide and hydrochloric the cheapest carbon source followed by corn cob. PHB pro-
acid) and enzymatic (endoxylanase) methods [65]. Ultrafil- duction was least (27%) in banana peel inspite of significant
tration and diafiltration process purified the barley husk’s bacterial growth because of relatively less reducing sugar
arabinoxylan, thereby augmenting oxygen barrier property content in pretreated banana peel [71].
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 Sugarcane Processing By‑products (Bagasse
formation of laminar structure [66]. Exceptional mechanical and Sugar Beet Pulp)
strength of films, in terms of puncture resistance, modulus
of elasticity, and tear resistance, made from arabinoxylan An estimated amount of 540 million metric tons of sugarcane
extracts of wheat bran, along with sorbitol as a plasticizer, bagasse (SB) is produced worldwide annually from distiller-
indicate its utility in packaging application where it could be ies and sugar factories. Sugarcane bagasse, at large is used as
used to protect food product from mechanical stress during fuel or burnt down in fields or as an animal feed in develop-
transportation and storage [67]. Arabinoxylan from maize ing countries, and has also been used in various biotechno-
bran is most extensively used for sustainable and edible logical (enzyme extraction) and non-biotechnological (single
packaging material after grafting it with fatty acids, sucro cell protein) applications. The valued 33.5% hemicellulose

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Journal of Polymers and the Environment

present in sugarcane bagasse has been acknowledged as a of better interaction between carboxyl groups of PBSA and
key ingredient in development of biodegradable packag- hydroxyl groups of bagasse cellulose and the material also
ing films and coatings for food industries. Hemicellulose degraded completely in microbial compost within 60 days
is extracted from sugarcane bagasse using alkali treat- [86]. Table 3 shows several recent developments in regard
ment alone, alkali-peroxide treatment, acid hydrolysis [72] to SB nano-cellulose based films and bio-composites, hav-
and enzymatic treatment [73] and films can be developed ing potential to be employed in food packaging applications
using casting or extrusion techniques. The application also [83, 87–91].
expands to production of foam trays by baking process [74, Sugar beet pulp is another by-product of sugar refin-
75], which points out to the fact that these can replace the ing industry having 20% cellulose, 25% hemicellulose and
expanded polystyrene (EPS) based materials. The hemicel- 25–30% pectin. During 2011, the sugar industries of USA
lulose-based films and their characterization have shown the singly threw away 26.7 million tons of sugar beet pulp based
potential for production of biodegradable films for various on dry matter basis. It finds miscellaneous applications in
packaging applications [76]. Some researchers had even the form of energy rich animal feed supplement, fuel source
utilized the hemicellulose of sugarcane bagasse as a plas- and platform chemicals. However, the presence of sugar beet
ticizer in cellulose acetate films developed from acetylated lignocellulose also makes it a suitable alternative for flex-
bagasse cellulose [77]. An all-cellulose nanocomposite film ible and biodegradable packaging films. Different treatments
and sheets i.e. having both fibre and matrix of cellulose was like cryo-crushing, homogenization, alkali extraction and
developed using sugarcane bagasse cellulose nanofibres. bleaching using sodium chlorite are given to the raw sugar
Both films and sheets were not only fully biodegradable but beet pulp for film preparation. Casting and hot press methods
were also found to be suitable for food packaging applica- create self-supported films with good mechanical and optical
tions based on their acceptable water barrier properties and properties (i.e. transparency) [92]. Another dimension of
toughness [78]. Sugarcane bagasse derived nano-cellulose, sugar beet pulp usage in packaging is the use of compression
has been a subject of intense research in recent decades due heating technique for composite materials based on sugar
to their renewability, high strength as well as eco-friendly beet pulp and polylactic acid with high cost effectiveness
nature [79]. Techniques for nano-fibrillation include ultra- as compared to single polylactic acid-based films [93]. An
sonication; homogenization, microfluidization, mechanical equal proportion of sugar beet pulp and polyvinyl alcohol
grinding etc. [80–82]. Sugarcane bagasse fiber cellulose (PVOH) had been reported as the best suitable biodegrad-
nanocrystals have witnessed prevalence and have been able composite film material based on tensile strength, ther-
regarded as the next generation green material for packaging mal and barrier properties [94].
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 Dairy By‑Products
for enhancing the shelf life of perishable food commodities
[83]. A dairy by-product could be defined as the product achieved
The development of advanced bio-composite materials, through the processing/manufacturing of any major dairy
such as, sugarcane bagasse fiber reinforced polymer com- product. Skim milk, buttermilk, whey and ghee residue
posites have also demonstrated excellent specific strength are the major rudimentary by-products of dairy processing
and high modulus, in addition to being environmentally at industry. Skim milk and buttermilk are either used for direct
stages of production, processing as well as disposal [84]. consumption or in other dairy products (yoghurt, cheese,
Nano-composites are also significant in achieving remark- probiotic drinks and ice-cream) to enhance their functional
able barrier properties. Additionally, eco-friendly nano-bio- properties. Ghee residue is a by-product with very high
composite films using 0.5–10% cellulose nanocrystals from nutritive value and has been incorporated in chocolate,
sugarcane bagasse in polyvinyl alcohol/carboxymethyl cel- candy, edible paste and other bakery products at laboratory
lulose blend matrix showed good tensile strength, high water scale. Currently, consequential research and development for
vapour barrier and almost equivalent transparency in com- ghee residue utilization in high worth products is impera-
parison to control films (i.e. without any cellulose nanocrys- tive. Casein-rich water is another plentiful, but underuti-
tals) [85]. Poly-(butylene succinate adipate) (PBSA) is lized protein source which is generated during the clean-
the most vital biodegradable plastic because of its better ing of dairy plants. Ryder et al. [95] suggested the use of
mechanical strength and hydrophobicity but its high produc- casein rich material (referred to as DAF-casein) harvested
tion cost is a barrier in its wide commercialization. Sugar- from dairy wastewater using a dissolved air flotation (DAF)
cane bagasse incorporation in PBSA based composite mate- procedure having potential for the formation of biopolymer
rial had positive effect on mechanical properties because composites, upon inclusion with κ-carrageenan, sodium

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

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

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 Journal of Polymers and the Environment

and biochemical modifications involving peptidases, hydro- with minimal processing in packaging applications instead
lysates and transglutaminases enzymes had also been used of extracting any component and utilizing it. In the following
for modifying whey protein film properties. Peptidases and years, more efforts are required for upscaling of the process
whey protein hydrolysates cleave the peptide bonds thereby involved in manufacture of sustainable packaging materi-
improving the film flexibility and reducing the amount of als. However, at present, persuading the customers to use
plasticizer required for film preparation [99], while transglu- eco-friendly packaging materials as a substitute to cheaper
taminases owing to the formation of ε-(γ-glutamyl) lysine synthetic options is the biggest challenge. A Germany based
bond improves the water vapour barrier and mechanical firm, BIO-LUTIONS® is purchasing agricultural waste
properties of the films [100]. Low-pressure glow plasma (wheat straw, pineapple leaves, banana peels and water hya-
has shown potential for modifying protein films by surface cinth plants) from the farmers and using it for producing bio-
ablation or etching, cross-linking, and modification of func- degradable disposable dishware, thereby reducing the agro-
tional properties [101]. Dielectric barrier discharge plasma waste as well as preventing pollution from plastic tableware
is another novel method of polymer surface modification (BIO-LUTIONS, 2019) [112]. Such kind of initiatives needs
technology employed for whey protein concentrate (WPC)/ to be promoted by the authorities along with better policy
wheat cross‐linked starch (WCS) composite films with framework for managing the agricultural waste.
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 References
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