Biomass Conversion and Biorefinery

https://doi.org/10.1007/s13399-022-03642-3

REVIEW ARTICLE

Paper bottles: potential to replace conventional packaging for liquid

products
Arihant Ahuja1 · Pieter Samyn2 · Vibhore Kumar Rastogi1 

Received: 13 September 2022 / Revised: 14 November 2022 / Accepted: 5 December 2022

© The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature 2022

Abstract
Packaging for liquid products is mainly made from petroleum-based polymers, either rigid or flexible. The multilayer
packaging provides small and handy packs available for the common masses. However, an alternative bio-sourced material
for liquid products is urgently needed due to the limitation of fossil fuel, restrictions from environmental regulations, and
its non-biodegradable nature. Paper is used as a packaging material that mainly provides structural strength to the package
with some barrier properties if required after suitable surface treatment. Here we review the use of lignocellulosic pulp to
produce paper-based sachets and paper bottles for liquid product packaging, emphasizing the detailed manufacturing pro-
cess. The barrier properties of various conventional polymers and barriers required by a specific liquid product package are
also discussed and detailed, as a barrier is required to increase further or maintain the product’s shelf-life. Current research
and new product development at an industrial scale and their materials are critically discussed. Suitable coating materials
on paper sheets and paper bottles are detailed, as paper alone cannot be used for liquid products due to wettability in the
hydrophilic region and poor barrier properties. The potential of biopolymers like polylactic acid, polyhydroxyalkanoates,
and their nanocomposites are further explored to ensure the package’s sustainability compared to conventional polymers.
Moreover, the emerging biomaterial such as cellulose fatty ester, cellulose nanopaper, waterborne acrylic emulsion, and
natural wax-based dispersion for coating on paper packaging is detailed. Furthermore, the barrier, mechanical properties,
and finally, recyclability are a concept taken into account from the design phase onwards.

Keywords  Paper-based sachets · Paper bottle · Liquid packaging · Biopolymers · Sustainability

1 Introduction same [2]. In past years, we have seen environmental activ-

A need to shift from conventional to sustainable packag-
ing is inevitable. Worldwide, packaging has played a keen
role in creating waste, usually landfilled. In 2015, the global
plastic waste generation was highest for the packaging sec-
tor, amounting to nearly 141 million tons of waste (Fig. 1)
[1]. Packaging accounts for about 50% of all plastic wastage.
Also, the high consumption of crude oil in the fast pacing
world has led to a shortage of crude oil and is expected to
deplete within 43 years if the consumption pace remains the
* Vibhore Kumar Rastogi
vibhore.rastogi@pt.iitr.ac.in
1
Department of Paper Technology, Indian Institute
of Technology Roorkee, Roorkee, Uttarakhand 247667,
India
2
SIRRIS - Smart Coatings Lab, Wetenschapspark 3,
B‑3590 Diepenbeek, Belgium
ists debating reducing plastic wastage. Measures are being
taken worldwide to phase out single-use plastics, including
plastic cutlery, plastic bags, sachets, pouch, and certain Sty-
rofoam. However, these single-use packaging materials are
the most consumed and thus make up most of the wastage.
Phasing out might not help the consumer, as the demand for
small sachets, pouches, cutlery, and paper cups is the highest
due to the low cost. Therefore, shifting from conventional
packaging to more sustainable packaging is inevitable, not
sourced from petroleum-based crude oil but preferably from
bio-based natural or renewable sources.
Most liquid products such as water, syrup, curry, ketchup,
oil, sanitizer, and soap solution possess many challenges
for sustainably sourced packaging materials compared to
solid products due to their wettability concern. Traditionally,
liquid products like water, milk, and liquid beverages were
packaged in glass bottles or ceramic pots. Glass being heavy
adds weight to the transportation and thus increases the

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 Biomass Conversion and Biorefinery

[7]. Today, the paper’s primary purpose in packaging is to

Fig. 1  Global plastic waste generation [1]
transporting cost. Also, the brittle nature of glass held them
back, and soon after the advent of plastic, polymers replaced
glass packaging due to the tailored properties and low cost
of production. It was also noted that plastic bottles like Poly-
ethylene terephthalate (PET) and High-density polyethylene
(HDPE) have a lower carbon footprint when compared to
glass bottles [3]. Glass and ceramic being the ­1st generation
of liquid packaging, petroleum-based plastic being the 2­ nd
generation, now a requirement of 3­ rd generation material
is necessary. This 3­ rd generational material should be bio-
sourced and biodegradable to overcome the limitations of
the previous materials concerning environmental pollution
and hence sustainably. The most abundant naturally sourced
material is cellulose [4], obtained from plant sources that
can be wood and non-wood based. In addition, cellulose
can also be sourced from bacteria as a more sustainable way
of production, avoiding deforestation. Currently, cellulosic
material in paper, paperboard, and molded pulp is used in
packaging products. The most common example is Tetra Pak
for juices [5], molded pulp for trays [6], and multilayer lami-
nate with another polymer as flexible packaging material
provide structural support to the inner packaging material
and make the complete package sturdy and easy to handle.
To package liquid products, the cellulose-based mate-
rial possesses problems like the hygroscopic nature of cel-
lulose [8], poor moisture, and gas barrier properties [9].
Hence, cellulose is not used alone as a packaging material
for liquid. Wax coating is currently used to provide hydro-
phobicity and aluminum to provide the required barrier
properties to the paper-based package [7]. Moreover, paper
is not a sealable material, so using a heat seal polymer like
polyethylene (PE) is a common practice [10]. A layer of
PE also provides a barrier against moisture to the paper
structure. Table 1 shows the characteristics of packaging
material required to pack different types of liquid products
[11, 12]. For example, ketchup and most beverages are
acidic, while milk or soap solutions are alkaline. There-
fore, the packaging material should resist acid or alkali
for different liquid products. In the case of milk, apart
from being alkaline, UV resistance plays a keen role in
the shelf life of milk to avoid the loss of nutrients. Most
oil products (vegetable, motor oil) or curries that contain
vegetable oil require oil-resistant packaging that does not
migrate when it comes into contact with the oil product.
Moreover, alcoholic beverages or hand sanitizers contain
volatile alcohols and may migrate outside if the package
does not have a high barrier and resistant to alcohols. On
the other hand, oxygen and moisture barrier are required
by most products to extend the shelf life. The oxygen bar-
rier helps deaccelerate the oxidation of foods or products,
whereas the water barrier helps to maintain the retain the
water content of the liquid products. Besides ensuring the
required functional packaging properties, the recyclability
of valuable fiber fractions is a more preferred end-of-life
scenario than landfill, incineration or biodegradation.

Table 1  Properties of packaging material required by different liquid products [11, 12]

Product Properties required
Moisture Gas barrier UV barrier Oil resistant Acid resistant Alkali resistant Alcohol
barrier resist-
ant

Water ✓
Ketchup ✓ ✓ ✓
Milk ✓ ✓ ✓
Oil ✓ ✓ ✓
Beverage ✓ ✓ ✓
Alcoholic beverage ✓ ✓ ✓ ✓ ✓
Carbonated alcoholic beverage ✓ ✓ ✓ ✓ ✓ ✓
Soap solution ✓ ✓ ✓
Hand sanitizer ✓ ✓ ✓
Curry ✓ ✓ ✓ ✓

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Biomass Conversion and Biorefinery
This review provides a detailed study of utilizing the
lignocellulosic pulp for liquid packaging products with the
potential biopolymers as a protective coating for the pack-
age. The current scenario of liquid packaging and the shift
from rigid to flexible packaging has been discussed, fol-
lowed by the challenges for lignocellulosic pulp as a pack-
aging material. Moreover, the recent developments in paper
sachets and paper bottles worldwide have been evaluated,
followed by the manufacturing process. Later the potential
biopolymers for coating applications are critically reviewed
in parallel with their user properties and recycling options.
This paper attempts to provide the potential of the lignocel-
lulosic pulp as a sustainable packaging material for liquid
products.
2 Current scenario in polymer‑based
packaging
Most liquids are packed in either bottle (glass, plastic) or
multilayer laminate. The plastic bottles are made up of
either polyethylene (PE), polypropylene (PP), or polyethyl-
ene terephthalate (PET) made by the blow molding process.
These polymers replaced heavy tin cans and glass jars due
to lightweight and low manufacturing costs and better shelf
visibility [13]. These rigid plastic packages are robust and
can bear heavy loads. The rigid packaging mainly includes
cartons, bottles, cans, clamshells, or canisters. But later,
rigid packaging slowly started to fade away from shelves
due to the introduction of flexible packaging. These flexible
packages have replaced rigid packaging due to advantages
such as lightweight, tailored barrier, less raw material for
the same volume, low energy requirement than rigid packag-
ing, highly aesthetic, and many more [13–15]. These flexible
packaging in the form of pouches are usually made up of
three layers, where the ­1st layer (outermost) is used for print-
ing. The middle layer is traditionally metalized by aluminum
to provide a barrier against moisture and oxygen. Lastly,
the ­3rd layer (innermost) is a sealant layer directly in direct
contact with food, as shown in Fig. 2.
The first layer of the multilayer laminate package is used
for printing purposes. The most common printing layer is
PET which is biaxially oriented and provides good gloss,
transparency, and a thickness of around 12 μm. On the other
hand, PP is the second most preferred choice for printing.
However, these PET and PP films are generally oriented
films made by the tenter frame process [16], providing
strength, stiffness, improved optical properties, and dimen-
sional stability [17–19]. Also, the stiffness gives structural
support to the package [18]. PP is only used in those appli-
cations in which the sealing temperature of the pouch is not
too high or where the high seal strength is not important,
such as peelable pouches. But if a high sealing temperature
Fig. 2  Cross-section of a typical multilayer polymer-based laminate
package
is required to seal the packages, where seal integrity is a
matter of importance to avoid any kind of leakages, PET is
preferred over PP due to polyester’s higher glass transition
temperature [17]. In some cases, paper is also used as the
outermost layer for printing purposes. Still, printing on paper
requires an additional layer of primer (ethylene acrylic acid
or polyethylene imide) to be coated on paper for better adhe-
sion of inks to the substrate [20].
The middle layer is mainly used as a barrier layer. In some
cases, when barrier is not required but structural strength is
major concern, then paper is used as a sandwich layer. The
standard barrier properties of the sandwich layer are shown
in Table 2. Aluminum foil is used when the barrier required
for the product to be packed is too high, obtaining the high-
est barrier [11]. Metallized films are used when the barrier
requirement is high but can be compromised because zero
permeation is unnecessary. The metallization can be done
on PET or PP. If a nominal barrier is required, PET alone
can provide a moderate oxygen barrier, and PP can be used
as a good water vapor barrier layer [19]. PET is highly crys-
talline, providing a good oxygen barrier (measured as oxy-
gen transmission rate, OTR) than PP, but PET being polar,
has a poor barrier towards water vapor (measured as water
vapor transmission rate, WVTR) compared to PP, which
is non-polar. Also, the oriented PP has a higher barrier
(WVTR = 3.9–6 gm/m2-day) than cast PP (WVTR = 8–12
gm/m2-day) due to the high crystallization density in ori-
ented films [17]. Apart from metalized films, transparent
barriers are also used. The high barrier transparent mate-
rial is a modified metalized polymer film in such a way that
during metallization, oxygen is introduced, and aluminum
is oxidized [21]. Nylon (PA) and ethylene vinyl alcohol
(EVOH) are also transparent oxygen barrier materials [11].
PA and EVOH are highly polar and hygroscopic; they absorb
water readily and then lose their oxygen barrier property due
to the plasticization effect. PA and EVOH are sandwiched or
coextruded between polyethylene (PE) to provide a moisture
barrier to these polymers [22]. According to the demand of
the product, the barrier layer is chosen and applied.
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 Biomass Conversion and Biorefinery

Table 2  Barrier properties of Polymer OTR @ 23 °C, 0% RH WVTR @ 38 °C, References

conventional polymers (25 µm) (mL/m2-day) 90% RH
(gm/m2-day)

Cast PP (CPP) 2300–4200 8–12 [11, 23–25]

Biaxially Oriented PP (BOPP) 1500–2500 3.9–6 [11, 23, 24, 26]
Biaxially Oriented PET (BOPET) 31–93 16–25 [11, 23, 24, 27]
Biaxially Oriented Nylon (BOPA) 18.6–60 155–310 [11, 23]
EVOH 0.08–1.2 22–124 [11, 23, 24]
Low density PE (LDPE) 6000–8500 12–23 [11, 23, 24]
High density PE (HDPE) 1600–3100 4–12 [11, 23, 24]
Metallized Films
Metalized BOPET 0.16–1.1 0.4–1 [11, 23, 28]
Metalized CPP 20–150 0.4–1.5 [29]
Metalized BOPP 25–160  < 1 [11, 23]
Aluminum 0.06571 0.00873 [30]

The third layer, or a sealant layer, is in contact with the
product, usually PE or CPP, and can be BOPP if seal integ-
rity is not required. BOPP has low seal integrity than CPP,
due to the inherent higher stiffness of BOPP, the seal breaks
easily. The sealing property is the inherent characteristic of
most thermoplastic polyolefins [31]. Also, this 3­ rd layer can
also be avoided by using a variety of heat seal coatings.
The third layer should have good heat seal properties and be
chemically inert when used for liquid products to prevent
interaction between the product and packaging material. PE
is inert to most chemicals as it is non-polar. Most polyolefins
are susceptible to most chemicals and acid/alkali attack [32],
so it is the most suitable polymer for the innermost layer as
it is ideal for food contact applications [33]. In some multi-
layer laminate, two layers are used instead of three, where
a low barrier or non-intact seal (peelable lids) is required
that can be achieved by heat sealable metalized CPP films.
Table 3 summarizes the conventional packaging material
and respective barrier properties required by different liq-
uid products. Most liquid products are packed in multilayer
flexible packaging and a few in rigid packages. Ketchup and
carbonated alcoholic beverages are packed in glass bottles,
whereas vegetable oils are packed in tin due to the require-
ment of high barrier and bulk packaging. In terms of flexible
packages, aluminum is sometimes used as a middle layer
for the barrier, as for ketchup (stand-up pouch), beverages
(tetra-pak) and curries (retort pouch) due to the requirement
of high barrier, which leads to higher shelf life. Moreover, it
can be observed from Table 3 that the small sachets contain
metalized films rather than aluminum, as these sachets are
required only for one-time use and are readily consumed.
PE is common as a sealable layer in all the packages due to
its high seal strength and its susceptibility towards the food
products except for curries that have PP as a sealant layer
due to high retorting temperature.
From the above overview, it is clear that a paper-based
package should have a barrier and sealability to mimic all
the required properties, which can only be fulfilled by using
a coating material on the inner side. The coating material for
the package must be a biopolymer to maintain the sustain-
ability of the whole package. This biopolymer should also
resist the packed liquid material, which can be tested by
migrating biopolymer to the product or vice versa. On the
outer side, the paper or pulp must be hydrophobic to sustain
water vapor or moisture in the environment.
Many industries have initiated projects to replace con-
ventional petroleum-based polymers for liquid packag-
ing. The main concern is to mimic the traditional polymer
properties in processing and barrier (air/water/oil). Bio-
PE is a drop-in biopolymer that resembles traditional PE
obtained from natural and renewable sources. This bio-PE
is obtained from bio-ethanol [34, 35], sourced from sug-
arcane, as shown in Fig. 3a. The fermentation of sugar-
cane results in bio-ethanol, which is then dehydrated to
form ethylene. This ethylene is then polymerized to form
polyethylene. Apart from natural sources, polyethylene has
been manufactured from black liquor (spent liquid of wood
pulping). UPM produced naphtha from crude tall oil [36]
(Fig. 3b) obtained during alkaline pulping in the paper-
making process. The tall oil soap is decantated from the
black liquor and converted to produce crude tall oil. This
crude tall oil is concentrated with the help of an evapora-
tor and purified by a distillation column. Afterward, it is
hydrotreated in the presence of hydrogen and dehydrated
to remove the excess water, and the fractionation results
in naphtha and biodiesel. Further, the naphtha is converted
to bio-PE by Dow Chemicals [37]. Moreover, this bio-
PE, when applied to pulp-based containers, the packaging
was said to be 100% wood-based beverage carton [37].
Like bio-PE, other drop-in polymers came further, such as

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Biomass Conversion and Biorefinery

Table 3  Barrier properties required by different packages containing liquid products [data gathered from Indian Industries]
Liquid Products Package Type Package Material WVTR @ 38 °C, OTR @
90% RH 23 °C, 0%
(gm/m2-day) RH
(mL/
m2-day)

Ketchup Bottle Glass - -

Stand-up Pouch PET/Foil/PE  < 0.1  < 0.1
Sachet PET/Met-PET/PE  < 1  < 1
Oil Can Tin - -
Pouch PE-Nylon-PE  < 10  < 50
Soap Solution Multilayer Pouch PET/PE  < 5  < 120
Milk Tetra Pak PE/Paper/PE/Foil/PE/PE  < 0.1  < 0.1
UHT Pouch PE-EVOH-PE  < 10  < 1
Pouch PE-PE  < 10  < 2500
Shampoo Sachet PET/Met-PET/PE  < 1  < 1
Hand Sanitizer Sachet PET/Met-PET/PE  < 1  < 1
Beverage Tetra Pak PE/Paper/PE/Foil/PE/PE  < 0.1  < 0.1
Stand-up Pouch PET/Foil/Nylon/PE  < 0.1  < 0.1
Alcoholic Beverage Bottle Glass - -
Stand-up Pouch PET/PET/PE  < 8  < 80
Carbonated Alcoholic Beverage Bottle Glass - -
Curry Retort Pouch PET/Foil/Nylon/PP  < 0.1  < 0.1
Transparent Retort Pouch AlOx-PET/Nylon/PP  < 0.1  < 0.1

Fig. 3  a Bio-PE production from Sugarcane [34, 35]. b Production of Naphtha from Black Liquor [36]

bio-PP and bio-PET. These drop-in polymers are sustain- the package. Therefore, drop-in polymers may replace con-
ably sourced but are not degradable due to the same struc- ventional packaging as they mimic the required proper-
ture as their counter petroleum-based polymer. The main ties of packaging material, but it is still not a sustainable
concern here is the biodegradability or compostability of solution.

13

3 Recent developments in paper‑based
packaging
3.1 Paper pouches & sachet
Flexible pouches and sachets comprise multilayer laminate
which are sealed with the help of heat. In most cases of
paper sachets, the printing layer is made up of paper, and
the sealant layer is a polymeric film. This laminate can have
a barrier polymer, an aluminum foil, or a barrier coating as
a sandwich layer. Application of paper pouches that involve
aluminum foil as a barrier layer is limited to juices (tetra-
pack). There have been recent developments in paper sachets
and pouches, but many of them are made for the packaging
of solid products. In terms of liquid products, the applica-
tion is limited to lamitubes for facial creams, cosmetics, and
toothpaste. Uflex [38], BillerudKorsnäs [39] and Toppan
[40] introduced lamitubes for different emulsified products
such as hand wash, toothpaste, and cosmetics products, as
shown in Fig. 4. The type of coating or polymer used on the
paper is not disclosed.
Apart from these paper lamitubes, other packaging for-
mats such as stand-up pouches are made by laminating the
base paper with an appropriate polymer film and then heat
sealing it to form a pouch shape. However, these stand-up
paper pouches have an inner layer of PE or PP as a sealant
layer, making them a non-degradable package, and creating
waste.
3.2 Paper bottles
Water bottles are made up of polyethylene terephthalate
and polypropylene. Most of them are only for single-use
Fig. 4  Paper lamitubes manufactured by a) Uflex [38], b) BillerudKorsnäs [39], c) Toppan [40], and d) an illustration of a paper-based stand-up
pouch
13
Biomass Conversion and Biorefinery
purposes, thus creating a massive amount of waste world-
wide. Apart from water, bottles pack other liquids such as
milk, shampoo, liquid soap, beverages (alcoholic, non, alco-
holic, or carbonated), syrups (retail or pharma), and much
more. A shift in packaging is necessary to move on to a more
sustainable approach to reducing plastic waste; hence many
industries have started to work on paper bottles. The idea of
paper bottles originated as early as 1908. It was discussed
that the paper bottle could reduce the delivery cost of milk
and reduce the spreading of communicable diseases [41].
Later, the paper beverage carton in tetra pack was adopted
worldwide using aluminum and polyethylene for barrier and
inner liner, respectively [42]. Now, the concept of paper
bottle is increasing to replace conventional bottles. Of all
the paper bottle projects by industries worldwide, shown
in Table 4, the outer layer of all the paper bottles is either
from recycled pulp or pulp sourced from Forest Steward-
ship Council (FSC) regulated forest. The inner layers in all
the bottles are different, broadly conventional polymer, bio-
sourced polymers, and degradable biobased polymers, and
some used their undisclosed propriety coatings. These inner
liners are food grade but lack barriers or specific applica-
tions like hot fill, alcohol resistance, or carbon dioxide bar-
rier. Most of the projects are in the development phase and
are expected to end by 2025.
Eco.Bottle (USA) is a pulp-based water bottle in which
the outer shell is made of pulp (Fig. 5a) sourced from recy-
cled cardboard or newspaper that can be recycled again and
meets the composability standard of ASTM D6868 [37].
The inner shell is made from conventional recycled plas-
tic (Fig. 5b). Both layers are not laminated; therefore, these
inner and outer shells can be easily separated and sent to
separate recyclable streams. The outer shell is made in two
parts, covering the inner polymer liner (Fig. 5c) [43] by a
Biomass Conversion and Biorefinery

Table 4  Market scenario of paper bottles.

Product
Image Company Outer Layer Inner Layer Reference
Name
Pulp HDPE
Ecologic (Recycled (80% PCR, 20%
Eco.Bottle (Acquired by cardboard Virgin) [43]
Jabil) and or PET (100%
newspaper) recycled)

Paper Water
Eco1green Pulp Enso Restore PET [44]
Bottle

Frugal
Frugalpac Pulp PE/Met-PET [45, 46]
Bottle

The Paper Bottle

Company Pulp Recycled PET
Paboco (Pioneer Owner - (FSC or polyethylene [47]
Billerudkorsnas, certified) furanoate (PEF)
Alpla) & Others
Pulp
Pulpex
(Sustainably
Pulpex (Diageo and Pilot Proprietary Coating [48]
Sourced -
Lite) & Others
FSC)

Kagzi - a
Recycled
Kagzi subsidiary of Proprietary Coating [49]
Pulp
TableBandi LLP

patented process [37]. The use of pulp in the bottle reduces
the thickness of conventional polymer to reduce the poly-
mer usage and thus uses up to 60% less polymer material.
Although easily detachable bottles make them recyclable,
recycling is not practiced in most countries, which would
not improve the wastage problem. The sustainable use of
recycled polymer is subjective to the adaptability towards
the recycling process.
Paper Water Bottle by Eco1green (USA) made a sus-
tainable bottle made from pulp (65%) and PET (35%) [44]
by a patented process [45]. This PET layer is Enso Restore
PET, an additive made by Enso Plastics; when added to
normal PET, it accelerates the natural degradation of PET.
The degradation occurs only when landfilled due to natural
microbial activity and can take 1–15 years to degrade. The
claim made by Eco1Green bottle is that their bottle is 100%
recyclable, 98% landfill biodegradable, and 65% composta-
ble (pulp). And further, the target is to achieve 100% com-
postable bottles [46].
Frugal Bottle (England) also uses paper as an outer shell
but uses metalized laminate as an inner barrier liner [47].
This laminate comprises two layers: a metalized PET and
PE, where metalized layers give a barrier, and PE is for food
contact and sealing. The shell is designed in a way that both
the layers get separated easily by pressing at a particular
location (Fig. 6a) for ease of recyclability (Fig. 6b). It is

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 Biomass Conversion and Biorefinery

Fig. 5  A) Outer shell, b) inner shell, c) two-halves outer shell integrating with inner shell [43]

Fig. 6  A) Press to split the lay-

ers, b) separated layers ready to
recycle [48]

claimed that it uses 77% less plastic than a typical bottle, is
five times lighter than a glass bottle, and has six times less
carbon footprint than a glass bottle. Cantina Goccia was the
first wine to be packed in a frugal bottle [48].
Paboco, “Paper Bottle Company” (Denmark), is a com-
pany started by Billerudkorsnas and Alpla. They have
partnered with Teknos, Grow, Recycl3R, and Avantium for
making paper bottles with the barrier. They have also part-
nered with other brands like Carlsberg, The Absolut Com-
pany, Loreal, Coca-Cola (Europe), and P&G [49]. They used
pulp with a thin barrier liner of recycled PET or PEF. PEF
is a polymer developed by Avantium (Netherlands), which

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Biomass Conversion and Biorefinery
is biobased and made of 2,5-furandicarboxylic acid (FDCA)
[50] shown in Fig. 7. This setup was shown to have proper-
ties required by alcoholic-carbonated drinks. PEF had pre-
viously been portrayed as a replacement for conventional
PET bottles, with a better barrier than PET [51]. PEF, when
compared to PET, has twice the C ­ O2 and moisture barrier
and six times the oxygen barrier.
Pulpex (England) is a bottling company started by Dia-
geo and Pilot Lite. They began to make pulp-based alcohol
bottles (Johny Walker) with an inner propriety coating [52].
Currently, the coating can hold regular liquid and works on
bottles that take carbonated products and hot filling [53].
Further, they had partnered with Pepsico [54], GSK Health-
care [55], BASF [56], Castrol [57], Uniliver [58], Stora Enso
[59], and Solenis [60] to develop, scale up the paper bottle,
and provide a barrier for various applications.
Kagzi (India) is a subsidiary of TableBandi LLC and
makes paper bottles coated with a propriety material and
claimed plastic-free bottles [61, 62]. The pulp is made up
of recycled paper and paperboards and then shaped into
two halves of a bottle. The uncoated bottle (Fig. 8a) is then
finally spray coated (Fig. 8b) and glued together to form a
Fig. 7  Monomer of PEF; 2,5-furandicarboxylic acid (FDCA)
Fig. 8  The two halves of Kagzi
bottle shown as a) uncoated and
b) spray coated [63]
bottle. The inner layer is said to be 100% compostable and
disintegrate into the soil within months [63].
4 Manufacturing of paper sachet
Paper pouches are conventionally made by laminating
the base paper with the sealant polymer with or with-
out the barrier layer and then heat sealing them to form
a sachet. The paper is made from the lignocellulosic
material extracted from wood or non-wood sources via
a pulping process. The details regarding the effect of fib-
ers is determined elsewhere [64]. Major components of
lignocellulosic materials are cellulose, hemicellulose
and lignin. Pulping is done to remove the lignin from the
lignocellulosic material to form paper. Alkaline pulping
process is the most used method as it removes lignin from
the middle lamella from the lignocellulose material and
separates the fibers [65]. The pulp obtained after pulping
is converted into a slurry by disintegrating the fibers in
the water medium. The pulp slurry is then passed over
a screen where the water is evacuated and a thick fiber
sheet is formed over the screen. The fiber sheet is further
pressed to enhance the density of the paper, this process
also removes the unbound water present in fibers. Further,
the sheets are dried at elevated temperatures to remove
the bound water. Paper produced is laminated with the
polymer possessing heat sealing property such as PE. This
lamination can be done using adhesive (solvent or solvent-
based) or by direct melt-extrusion method [66]. The lami-
nated or coated paper is sealed with the help of heat sealer
to form a paper-based pouch.
13

5 Manufacturing of paper bottle
5.1 Mold design
The paper bottle is based on the thermoforming of pulp
[67, 68], which is conventionally done to make trays for
eggs, take-away containers in many restaurants, fruit trays
or baskets, and pulp-based disposable food trays [69–71].
For pulp thermoforming, a porous molding die is required
to provide the initial shape to the pulp product [72]. This
mold is usually made from aluminum or steel. The shape
of the mold gives the paper bottles its unique shape. The
porous dies are connected to a vacuum source which when
immersed in a pulp suspension pulls out the water and
deposit the pulp onto the die. The molding die can be made
porous using micro channels or a solid material drilled
with holes. In a study, researchers created micro chan-
nels for water evacuation with pore size of 300 µm. A
CAD model was made as shown in Fig. 9a, this was 3D
printed to make a porous mold as shown in Fig. 9b. These
micro-channels were tapered at 2° and manufactured at an
equivalent depth of 3 mm [73]. In another approach, when
the mold die is a solid material drilled with holes, a thin
wire mesh is present inside the mold. This thin wire mesh
restricts the flow of fibers and allows water evacuation
during the paper bottle manufacturing process.
Fig. 9  Design of mold die for
paper bottle, a) CAD diagram
of micro features, b) 3D printed
die mold [73] (Reprinted from
Elsevier, Vol 58, P. Saxena
et al., Mold design and fabrica-
tion for production of thermo-
formed paper-based packaging
products, 411–421, Copyright
(2020), with permission from
Elsevier)
13
Biomass Conversion and Biorefinery
During forming, water is evacuated from the system
through the holes drilled in the solid mold die or via the
micro channels present in the porous mold die, known as
evacuation channel. The water is released in the evacuation
channel in the outward direction. The water in pulp is present
in two forms: bound and unbound water. The unbound water
is not absorbed by the cellulose fibers and is in excess, which
can be removed with the help of vacuum suction and press-
ing. On the other hand, bound water is the water absorbed
by the pulp fibers, and the removal of bound water requires
heating mechanism [74]. Thus, the molding of paper bottles
involves two significant steps: forming and drying process,
which ensures the removal of unbound and bound water,
respectively [75].
5.2 Forming process
Forming is a shaping process that involves the use of mold
die. These molded dies are made in two halves, clamped
together to form a hollow cavity. These molded dies are
drilled with holes to remove the water, and a wire mesh is
kept inside to ensure the passage of water but restrict the
movement of fiber to form the shape. The molded dies are
immersed in the pulp suspension made in water. This pulp
is then sucked into the molded dies with the help of the vac-
uum pump [76]. The unbound water is removed via vacuum
radially outwards (Fig. 10a), creating a pressure differential
Biomass Conversion and Biorefinery
Fig. 10  A) Forming of the paper bottle, b) impulse drying of paper bottle
at the wall. After opening the molded dies, the wet bottle is
removed for further drying [77].
5.3 Impulse drying process
Conventionally, molded pulps are dried in hot ovens or even
sun-dried to remove bound water [76]. Molded pulp prod-
ucts such as egg trays are dried in sun where shape precision
is unnecessary. These are usually bulkier. However, for paper
bottles, the shape plays a crucial role; hence, initial pulp
preforms are hot-pressed between the porous molding die
during the drying process. This process creates nice, sharp-
edged, and denser molded products. In this process, heat and
pressure are responsible for removing bound water from the
fibers and thus making the surface smooth and dense, which
can be seen in the case of the manufacturing of pulp plates.
This phenomenon is called the impulse drying process and
is applied to paper bottles in some patents [78, 79]. In the
drying section also, the molded die is a porous material [75,
77]. This porous tool is made of porous alloy powder filled
in a die, which is pressed and then sintered.
During drying of paper bottle, the porous molded die is
first preheated up to 140 °C, and the wet bottle is placed [80]
in the hollow porous molded die. In order to dry the wet bot-
tle, an inflated silicone core is inserted in the bottle cavity
to press the bottle from the inside that removes the water
with the help of pressure and heat; this is known as Muller's
process (Fig. 10b) [73]. This inflated core helps compact the
wet fibers, avoid shrinkage, and ease water removal. This is
also called restraint drying, which ensures the precise shape
of the bottle. The mold is opened after the drying process
to obtain the paper bottle. But the major problem with this
process is that the fibers are unevenly compacted from the
curvature of the bottle [77]. This is one of the design prob-
lems with the paper bottle. In addition, fibers get clogged in
the pores of a molding die as they are not straight and have
a high degree of tortuosity, thus having a longer cycle time
[75]. These problems can be solved if forming and drying
are carried in a single molding die. Recently the dryness of
molded fiber was also studied by numerical modeling for
water removal and was able to predict the dryness efficiency
with the difference of 0.3% when the process time was 15 s
[81].
5.4 Challenges in a paper bottle
In the concept of the paper bottle, the primary challenge is
to design a closure for the bottle. A screw cap is the most
common closure used in conventional petroleum-based plas-
tic bottles. The screw-type cap can be formed on the bottle
via molding, but capping the mouth of the paper bottle can
distort the bottle shape over time and lose the integrity of the
package. Thus, the strength of the paper bottle at the neck
is of utmost importance. The paper bottles discussed in the
previous section with the inner liner of PET or HDPE use
the inner liner in closure itself; therefore, the integrity is not
lost. The "360 paper bottle" offers an innovative approach
for closure, which involves peeling off the cap and then plug
fitting from the other side at the mouth (Fig. 11) [82]. But in
the case of the coated paper bottle, a different type of closure
such as flip-top or cork closure can be adopted to make the
bottle spill proof without losing the barrier property.
Besides the design aspect, the critical challenge for the
paper bottle is to fulfill the high demand for Fast-moving
13

Fig. 11  Closure of “360 Paper Bottle”
consumer goods (FMCG). The FMCG sector requires pack-
aging to package their products which are primarily used for
one time. Therefore, the high demand can only be fulfilled
by a high production rate of paper bottles. Production rate
however can be controlled by variables such as vacuum time,
temperature, contact time, and pressure. In previous studies
it was concluded that the dewatering of the molded pulp was
highly affected by the mold's temperature and the duration of
the suction via vacuum rather than contact time and pressure
[83]. Other than the production challenge, paper bottles also
face functional challenges such as barriers towards moisture
and oxygen and maintaining a pressure of up to 6 bar inside
the bottle [84], which could be done by a protective layer on
the inner side of the paper bottle.
Fig. 12  Coating of polymer on the paper sachet using a) dip coating, b) solvent casting, and c) bar coating, and d) spray coating
13
Biomass Conversion and Biorefinery
6 Coating processes
Paper sheets or paper bottles alone cannot be used to pack
the liquid products due to poor oxygen and moisture bar-
rier, hygroscopic nature, and nonresistant to many liquid
products. Thus, a protective coating on the inner side, i.e.,
an inner liner, is necessary to extend the shelf life of the
packed liquid products. Coating of biopolymer on a cellu-
losic substance such as paper or pulp can be employed to
maintain sustainability. These coatings can be done by vari-
ous techniques, briefly into melt processing and dispersion
coating. Rigid packages of pulp, i.e., paper bottles, can be
coated either by spray coating, which is a type of dispersion
method or by blow molding and rotational molding, which
comes in the category of melt processing. Whereas, for flex-
ible packaging, the paper can be coated with the help of dip
coating, spray coating, and casting, which comes under the
dispersion coating category, or with compression molding,
melt-extrusion coating, which comes under the category of
melt processing [66].
6.1 Solvent dispersion
Solvent dispersion is used when the desired coating material
is dissolved or dispersed in the solvent, and coated on the
paper substrate. After coating, the solvent evaporates, and
the desired material gets coated on the substrate. Dip coating
is a classical method to coat the material on the substrate,
as shown in Fig. 12a. The paper substrate is dipped in the
coating solution for the desired time and then air dried. The
longer the substrate is immersed in the solution, the higher
the thickness. It is the most effortless process, but the major
disadvantage is that the thickness cannot be controlled effi-
ciently, and both sides are coated, limiting its usage in the
tailoring of the coating on the substrate. Solvent casting can
be used if only one side of the paper needs to be coated. It
is a process in which the coating solution is poured over
the paper substrate and then left to evaporate (Fig. 12b). Its
advantage over the dip coating is that the thickness can be
Biomass Conversion and Biorefinery
controlled by pouring the solution. But the disadvantage of
this process is the low bond strength, as the material to be
coated is in contact with the paper, but due to no pressure
applied, the coating material does not get inside the paper
sheet, and thus delamination is an issue with the obtained
product. Bar coating is the simplest coating method which
involves a threaded bar to maintain the GSM of the coated
material. The bar usually moves towards the other end of
the paper while spreading the coating material and then is
left to dry to evaporate the solvent (Fig. 11c). This method
is like the gravure coating done at an industrial scale for the
surface sizing of paper. In the gravure coating, the paper run-
ning over the cylinder is coated by the cylinder itself, which
is dipped in the reservoir of the coating solution, and the
thickness is maintained by scraping out the excess material
with the help of a doctor's blade. Solvent casting is not easy
to upscale; therefore, bar coating and dip coating are the
most used paper coating method. Spray coating is a modern
technique used to coat both paper and bottles. It is a process
in which high volatile solvents are used as a solubilizing or
dispersing agent. In the case of the paper sheet for sachet
application, a pressure-assisted nozzle is used to spray the
coating substance on the paper from a distance (Fig. 12d),
and the coating weight is increased with time and pressure.
For coating on a paper bottle, coating can be done either
in two halves by spraying (Fig. 13a) and then joining them,
or with the help of a nozzle with upside-down along with
rotation motion (Fig. 13b) to coat the polymer solution on
the single mold bottle. The drying of the spray coating can
Fig. 13  Spray coating on a)
half paper bottle, b) single mold
paper bottle
be done at room temperature and may not require high dry-
ing time, as the solvents used for solubilizing the polymers
are volatile in nature.
6.2 Melt processing
Melt processing is used when the coating substance, gener-
ally a polymer, is melted above the melting point and then
coated on the substrate. It can be easily upscaled in indus-
tries, and its significant advantage over the dispersion coat-
ing is that it requires no solvents. Melt extrusion coating
is a conventional coating method used in many packaging
industries. This melted polymer is dropped from a die on
the running paper to form a continuous layer (Fig. 14a). It's
a swift and accurate process to maintain the thickness of
the coating substrate. Compression molding is a process in
which a polymer sheet or a thick die is kept over the paper
and is pressed over the paper hydraulically at high pres-
sure with the temperature aid to soften or melt it (Fig. 14b)
[66]. In this case, the melted polymer goes inside the paper
structure and provides better bond strength properties [85].
The above two coating processes are limited to coat on
the paper sheet only. Other methods such as rotocasting and
extrusion blow molding can be used for paper bottles. The
rotocasting method can be used for coating the paper bottle.
Although this process is not used to coat the paper bottle
in past, but it has potential in providing unform coating.
The paper bottle containing the polymer in powder form
can be melted and rotated as shown in Fig. 15a and c. The
13

Fig. 14  Coating of polymer on paper sheet via a) melt extrusion, b) compression molding
Fig. 15  Polymer coating on
paper bottle by rotocasting
method a) front view before
molding, b) front view after
molding, c) bottom view before
molding, d) bottom view after
molding
surrounding temperature is set above the polymer’s melt-
ing point, rotated, and then bought at room temperature.
The rotation of the bottle containing the polymer powder
will allow to coat the melted polymer inside as depicted in
Fig. 15b and d. This process is conventionally used to make
water tanks [86].
On the other hand, blow molding is a technique that
uses a blowing of polymer preform coat in the paper
bottle while manufacturing the bottle itself. Convention-
ally, it is used to make plastic bottle. After the form-
ing section, when the paper bottle is sent to the drying
section, then instead of using silicone-based elastomer
to pressurize the pulp, the preform of the polymer that
needs to be coated can be used. When blown at a high
temperature, the preform puts pressure on the inner
13
Biomass Conversion and Biorefinery
part of the paper bottle to assist the drying (Fig. 16).
After drying the paper bottle, the bottle can be bought
at room temperature, which will coat the polymer inside
the paper bottle due to crystallization of the polymer.
But the blow molding has the disadvantage that during
the cooling of coated polymer, the polymer shrinks, and
thus separates from the bottle. This separation might be
due to the absence of pressure during the crystalliza-
tion of the polymer during the cooling of polymer layer.
This disadvantage of the blow molding can be overcome
by maintaining above atmospheric pressure within the
expanded parison (blow molded polymer) while cooling,
rather than cooling at atmospheric pressure. This was
also rectified by conducting a second expansion step of
the polymer coating [87].
Biomass Conversion and Biorefinery

Fig. 16  Blow molding of the

inner liner to coat the paper
bottle

7 Potential biopolymers as coating Table 5  Barrier of commonly used bio-based polymers

for packaging of liquid products Biopolymer Film WVTR OTR (ml/m2.day) References
(gm/
The biopolymer, which is coated on the inner side of the m2.day)
package, must be safe for food contact. The migration limit Polyhydroxybutyrate 13–26 350 [88, 89]
is the significant criterion for finding if the material is safe Polylactic Acid 82–172  > 1000 [88, 89]
for food contact. Over time, the migration of packaging Polybutylene adipate 135 1200 [89]
material is studied at varying temperatures and times with terephthalate
specified food simulants. Overall Migration limit (OML) Polycaprolactone 177 175 [88, 90]
helps to determine the food contact application of packag- Cellulose Acetate 2920 1800 [88, 91]
ing material. The maximum acceptable value of OML has PBS 192 63 [88, 92]
been set by Regulation (EU) No 10/2011 on Plastic Mate-
rials and Articles. This limit is restricted to the maximum
value of 10 mg/dm2 or 60 mg/kg 198 . The polymers to be in water. Hence, the potential biopolymers are limited to
kept in food contact should adhere to the maximum OML these two bio-based polymers.
values for food simulants. Major food simulant used for
OML are ethanol (aqueous, alcoholic or fatty food), acetic 7.1 Polylactic acid (PLA)
acid (acidic pH), octane or hexane (fatty foods).
Many bio-sourced polymers are degradable, such as PLA is made from the condensation of the lactic acid or
starch, pectin, chitosan, polylactic acid, polyhydroxyal- ring-opening polymerization of lactide with a metal catalyst
kanoates, and some non-degradable biobased polymers [93]. It is 100% biobased thermoplastic polymer with good
include bio-PE, bio-PP, and bio-PET. To maintain the sus- mechanical properties and is compostable [94]. The mono-
tainability of the whole package, the polymer to be coated mer of PLA is made from a mixture of two optical isomers
should be biodegradable. Moreover, as the product to be of lactide (L & D). The presence of L-Lactide makes it more
packed is liquid, it narrows down the selection to those crystalline, whereas the D-Lactide makes it amorphous, and
bio-based polymers that are degradable. The packaging in terms of barrier, it has an average moisture barrier but
material should have a sound barrier towards oxygen and a poor gas barrier [66]. Literature shows that PLA and its
water vapor and in the case of bio-based polymers, how- composites have been explored as packaging materials for
ever, many polymers lack high barrier properties. The bar- many liquid products, such as water [95, 96], milk prod-
rier of packaging material is generally tested by OTR and ucts [97–100], plant milk [101], salmon sauce [102], cof-
WVTR. OTR is determined by the ASTM D3985 standard, fee [103], puree [96], and juice [96, 101, 104–107]. There
generally at 23 °C and 0%RH, whereas, WVTR is meas- have been developments in Europe and North America that
ured by the ASTM F1245 standard, generally at 38 °C and have involved the use of PLA-based packaging for super-
90%RH. The inherent barrier data of common industrially market products, such as Biota bottled water, Noble bottled
used bio-based polymers are shown in Table 5. Polyhy- juices and Danno yogurts [104]. To extend the shelf life
droxybutyrate, a type of polyhydroxyalkanoates (PHA), and replace the conventional packaging, the required bar-
and Polylactic Acid (PLA) have the lowest water–vapor rier properties of PLA are much lower when compared to
barrier. Moreover, neither they dissolve in water nor swell the traditional system of packaging, which can be tackled

13
 Biomass Conversion and Biorefinery

using nanomaterials in the polymer bulk or by coating
them with a barrier layer. Nanomaterials in the packaging
material increase the tortuosity, and hence the moisture/air
takes time to travel through it, thus decreasing the WVTR
and OTR. The barrier properties and the migration limit of
nanocomposite of PLA are shown in Table 6. PLA and its
composites with nanocrystalline cellulose (CNC), cellulose
nanofibrils (CNF), cellulose nanosphere (CNS), nanocrystal-
line cellulose-nano silver (CNC-Ag), hydrogenated carbon
(HC), organomodified montmorillonite nanoclay (MMT),
surfactant modified montmorillonite nanoclay (sMMT),
ZnO nanoparticles (ZnO) have helped in decreasing the
OTR and WVTR. The lowest WVTR and OTR is observed
in the PLA-HC nanocomposite. This must be due to smaller
and uniform diameter of HC when compared to CNF or
CNC. Moreover, Ag and ZnO have antimicrobial properties
that can increase the shelf life by protecting from microbial
attack. In terms of overall migration limit, all the nanocom-
posites of PLA were in the permissible limit, except for ZnO
as per the EU regulation.
PLA has been coated on different paper sheets such as
filter paper [115], semi-chemical paperboard [116], solid
bleached sulfate paperboard [117], coated paperboard
[118], handsheets [119], writing & printing paper [120],
pineapple leaf fiber [120], paper cup [103], virgin kraft
paper [121], and bleached kraft paper [122, 123]. The heat
sealing of PLA coated paper starts with the 1% w/v con-
centration of PLA. The heat seal strength increased with
the coating thickness up to 4% w/v and then leveled off.
Also, the bond strength was good enough to result in fiber
tear [117]. Moreover, when coated to paper, plasticized
PLA did not peel off during microwave for 3 min at 750 W
[103]; this coated paper was further used for coffee cups.
As the WVTR of PLA is relatively high, the addition of
grafted CNF in the PLA coated paper resulted in a drastic
decrease of WVTR value to 34 g/m2-day for the coated
paper [119] Apart from CNF, when the paper was coated
with surface modified nanoclay-PLA composite, then a
maximum of 74% decrease in WVTR was achieved (26 g/
m 2-day) [120]. But the main issue with PLA is that its
glass transition temperature is much higher when com-
pared to petroleum-based polymers (PP and PE), which
leads to less flexibility at lower temperatures and could
result in seal failure. These issues are for its film form-
ing capability. When considering packaging application,
PLA having low heat distortion temperature (HDT) [124]
which is not suitable for hot filling application such as hot
beverages (tea or coffee). Other than thermal behavior, the
barrier of neat PLA is not high enough, however, incorpo-
ration of nanoparticles has shown good barrier properties.

Table 6  Oxygen barrier, water vapor barrier, and overall migration values of PLA nanocomposite (OTR and WVTR are normalized with respect
to unit for comparison; N.M. not mentioned)
Polymer OTR WVTR Simulant Time & Temperature OML (mg/Kg) OML (mg/dm2)
(cm3.mm/ (gm.mm/m2.day.bar)
m2.day.bar)

PLA [108–112] 18.8–65 89.9–186 Isooctane 2 Days, 20 °C  < 0.02 -

Ethanol (10%) 10 Days, 40 °C  < 0.09 -
Acetic Acid (3%) 10 Days, 40 °C - 1.84
Ethanol (95%) 10 Days, 40 °C - 2.39
Ethanol (50%) 10 Days, 40 °C - 0.5
PLA/CNC-Ag [113] 18.6 47.5 Isooctane 2 Days, 20 °C  < 0.25 -
Ethanol (10%) 10 Days, 40 °C  < 0.25 -
PLA/HC [114] 15.8 41.5 Isooctane 2 Days, 20 °C  < 0.1 -
Ethanol (10%) 10 Days, 40 °C  < 0.4 -
PLA/sMMT [109] 23.34 - Acetic Acid (3%) 10 Days, 40 °C - 1.98
Ethanol (95%) 10 Days, 40 °C - 2.54
PLA/CNC [108, 112] 15.8 38.9–76.0 Isooctane N.M 0.0242 -
Ethanol (10%) N.M 0.0157 -
PLA/CNS [112] - 44.1 Isooctane N.M 0.0262 -
Ethanol (10%) N.M 0.0242 -
PLA/CNF [112] - 62.2 Isooctane N.M 0.274 -
Ethanol (10%) N.M 0.289 -
PLA/MMT [110] 7.3 - Acetic Acid (3%) 10 Days, 40 °C - 0.7
Ethanol (50%) 10 Days, 40 °C - 0.5
PLA/ZnO [111] 45 108 Ethanol (10%) 10 Days, 40 °C  > 60 -
Isooctane 2 Days, 20 °C  > 60 -

13
Biomass Conversion and Biorefinery

7.2 Polyhydroxyalkanoates (PHA)
PHA's are a family of biopolymer with the polyester group,
which is made intercellularly by various microorganisms
and accumulated for energy and carbon reserves [125]. The
most common type of PHA is Polyhydroxybutyrate (PHB),
having the simplest homopolymer and highest crystallinity.
The main disadvantage of PHB for packaging use is that it's
highly brittle [66] and lacks flexible film forming capabili-
ties. To increase the flexibility and film forming capabilities,
side chains of alkyls groups like hydroxybutyrate, hydroxy-
valerate, or hydroxyhexanoate are added to form PHB-HB,
PHB-HV, or PHB-HH, respectively [66]. These are all short
chain length PHA's, whereas a medium chain length PHA,
such as polyhydroxyoctanoate (PHO) and polyhydroxynona-
noate (PHN), have some elastomeric properties in a minimal
temperature range [126].
Literature on PHA with direct liquid products is only lim-
ited to sour cream [127], which was used as a juice simulant,
and further has been tested with stimulants such as etha-
nol, acetic acid & isooctane. PHAs have shown the overall
migration under the limit for these food simulants, as shown
in Table 7, which concludes that PHA is a food contact poly-
meric material and can be used with beverages, fatty acids,
and alcoholic beverages. And in a simulation, PHB and
graphene showed a four-fold increase in the shelf life of milk
products [128]. But to replace the conventional petroleum-
based polymers, other properties such as water vapor barrier,
oxygen barrier, seal strength, and bond strength are required.
The addition of ZnO nanoparticles, and MMT increases the
barrier, thus decreasing WVTR and OTR without deteriorat-
ing the overall migration, as shown in Table 7. The Addi-
tion of ZnO nanoparticles increased the barrier towards the
oxygen and water vapor than MMT. The OML of all the
nanoparticles was within the permissible limit as defined
by the EU Regulation, but it was very near to Ag. Moreo-
ver, when we compare the PHB nanocomposite with ZnO
nanoparticles, to that of PLA, the overall migration of PHA
is lesser due to the uniform dispersion ZnO nanoparticles
and strong adhesion with the matrix.
PHB has been used as a coating material on paper sourced
from pineapple leaf [135], cellulose paperboard of sisal,
[136, 137] and filter paper [115, 138]. PHB-HV being more
flexible, has been coated on Machine finished paper [85,
139], unglazed paper [139], kraft paper [139], supercalen-
dered paper [139–141], and PHB-HB on kraft paper [142,
143]. The main issue with the PHB-HV extrusion coated
paper is the poor bond strength [85], and the addition of
plasticizer did not have any effect. In both cases, the bond
strength was insufficient to give a fiber tear, although the

Table 7  Oxygen and water vapor barrier and overall migration values of PHA nanocomposite (OTR and WVTR are normalized with respect to
unit for comparison)
Polymer OTR WVTR Simulant Time & Temperature OML (mg/Kg) OML (mg/dm2)
(cm3.mm/ (gm.mm/
m2.day.bar) m2.day.bar)

PHB [129] 7.56 79.9 Ethanol (10%) 10 days, 40 °C  < 8 -

Isooctane 2 days, 20 °C  < 5 -
PHB/ZnO [129] 3.67 47.5 Ethanol (10%) 10 days, 40 °C  < 4 -
Isooctane 2 days, 20 °C  < 3 -
PHB/NCC-Ag [130] - - Ethanol 1 Day, 37 °C 50.9489 -
Acetic Acid (3%) 1 Day, 37 °C 38.1315 -
n-Hexane 1 Day, 37 °C 30.5344 -
PHB-HH [131] - - Ethanol (10%) 10 days, 20 °C 17 -
Ethanol (95%) 10 Days, 60 °C 5.4 -
Acetic Acid (3%) 10 Days, 60 °C 3 -
Isooctane 10 Days, 60 °C 41 -
PHB-HV [132–134]  ~ 5.8  ~ 160 Ethanol (10%) 10 days, 40 °C  < 25 -
Ethanol (95%) 10 days, 40 °C -  < 0.6
Acetic Acid (3%) 10 days, 40 °C  < 0.8
Isooctane 2 days, 20 °C  < 15
Isooctane 10 days, 40 °C -  < 0.8
PHB-HV/ZnO [134]  ~ 3.8  ~ 86.4 Ethanol 10 days, 40 °C  < 7 -
Isooctane 2 days, 20 °C  < 6  < 0.2
PHB-HV/MMT [133] - - Ethanol (95%) 10 days, 40 °C -  < 1.0
Acetic Acid (3%) 10 days, 40 °C -  < 0.2
Isooctane 10 days, 40 °C -  < 0.2

13

elongation at break increased due to the plasticizing effect
[144]. PHA's in the inner side of the package can be used
as a sealant. Compared to LDPE, the sealing temperature
and hot tack temperature of PHB-HV are much higher due
to its high melting point [139], limiting the use of PHB-
HV in the fast sealing application. Apart from the inherent
properties of the PHA, the properties also change due to the
coating process. Melting point and crystallization are higher
for compression molded samples than solution cast on paper,
and the compression molded samples had higher tensile and
modulus due to high smoothness [136]. In the case of PHB
compression molded on paper, the bond strength was good
enough to give fiber tear, and the plasticizer also increased
the bond strength, contrary to the PHBV extrusion coated
paper [137].
The inherent drawback of PHB is the narrow thermal pro-
cessing window, however it has shown that narrow control of
processing conditions provides flexible films for some PHA
copolymers [145]. The thermal degradation studies of PHB
and its copolymers have shown that degradation appears
near the melting temperature of the respective polymer,
mainly due to random chain scission processes. However,
the thermal stability of the polymer can be improved by add-
ing additives or blending with some other polymers [66].
Nevertheless, there is lack of literature on coating different
PHA’s on paper sachets or paper bottles. Apart from draw-
backs, as PHA’s have varied properties, mixing or blending
the PHA’s can give tailored properties for coating applica-
tion. For example: for coating purposes, a less rigid polymer
is required, which can be done with the help of branched
PHA such as PHB-HB, PHB-HV, or PHB-HH. Other than
flexibility, if the pouch requirement is to have a high burst
or good drop strength, then the use of medium chain length
PHA such as PHN or PHO can be utilized either as a sin-
gle polymer or as a blended form as these PHA’s have high
elastomeric properties.
7.3 Emerging materials
Nanocomposites of PLA and PHA’s have proven themselves
suitable for packaging materials in terms of barrier and
migration. Still, the need for more sustainable solutions to
the environment is being researched [146]. The use of cel-
lulose fatty esters (CFE), CNF, and waterborne dispersion
such as acrylic emulsion and the natural wax emulsion is
being thoroughly studied as a coating material on paper for
packaging application. CFE are derivates of cellulose made
by esterification with either fatty carboxylic acid or fatty acid
chlorides such as palmitic acid [147], hexanoic acid [147],
undecanoyl chloride [148], stearoyl chloride [149, 150],
oleic acids [151–153], and various short or long-chain fatty
acids [154–156]. CFE are thermoplastic and have a melting
point unlike cellulose, which creates a whole new range of
13
Biomass Conversion and Biorefinery
biopolymers with good processibility and solubility in sol-
vents. In terms of barrier, the OTR of CFE increases with the
chain length of the fatty ester, whereas a decrease in WVTR
is observed [154]. The increase of fatty groups in the CFE
leads to an increase in WVTR, whereas the OTR decreases
as the chain length increases because the fatty ester also acts
as a plasticizer. Hence, CFE can be used as a barrier polymer
for packaging applications. The CFE has been extensively
studied as a stand-alone polymer for packaging and coating
material for packaging applications. CFE’s has been coated
using bar coater when dissolved in chloroform which pro-
duced water contact angle in the range of 90°to 120° [147].
Further, a dual coating (Dip coating + spray coating) of CFE
was employed on the paper to make it superhydrophobic
with a contact angle of around 150°.149 CFE being thermo-
plastic when coated on paper, was able to form a pouch for
packaging application [156].
CNF is the term used for micro-fibrillated cellulose, the
smallest unit of plant fiber. These can be made by fibrilla-
tion of cellulosic fiber using high-energy disk grinder [157],
TEMPO oxidation [158, 159], or ultrasonication [160].
Nowadays, CNF is being used to make cellulose nanopaper
or nanosheets via a filtration process followed by hot press-
ing or drying at high temperatures [161]. The nanosheets
possess high oxygen and water vapor barrier property. OTR
of nanosheets is as low as 0.001 ml-mm/m2-day-bar when
tested at 0% RH and 6.6–8.7, ml-mm/m2-day-bar when
tested at 80% RH [158]. The OTR is as low as an aluminum
foil at low RH and has values near most bio-nano composite
at high RH. In contrast, the WVTR of nanosheets was found
to be nearly 213 gm-mm/m2-day-bar, which is above the
most biopolymers mentioned but still better than bio-based
materials [162]. The high barrier nanopaper had proven
themselves as a good potential for paper coatings material.
The CNF had been previously coated on paperboards [163],
writing & printing paper [164], kraft paper [165], grease-
proof paper [166], and recycled paper [167]. The coating of
CNF on the paper reduced the OTR by 260 and reduced the
WVTR by 20 to 30% [165]. The spray-coated CNF on paper
also reduced the WVTR by 21% [164]. The main challenge
for bar coating of CNF suspension is difficulty applying the
coating on paper due to high viscosity [168], whereas, in
spray coating, hornification is observed, which produces a
rough surface [169]. Therefore, CNF-coated materials need
to be studied more for industrial applications.
Water-based dispersion coating, such as acrylic and wax-
based dispersion, is now highlighted due to their environ-
ment friendly and the possibility of better recyclability of
coated paper. Acrylic-based coatings may contain polysty-
rene, butyl acrylate, ethyl acrylate, methyl methacrylate,
and acrylic acid. These acrylic-based coatings are generally
water-borne emulsion or dispersion, which can be used as a
coating material on paper. Many modifications of acrylate
Biomass Conversion and Biorefinery
coatings have been researched for better coating adhesion.
Oxidized starch [170], enzymatic degraded starch, [171],
and hydrolyzed starch [172] grafted acrylate emulsion have
been studied for paper sizing and showed an increase of
36.6% in wet tensile strength. When modified by the sili-
cone, the acrylate emulsion decreased the cobb value by 40%
and increased the contact angle from 44.5° to 97°. This was
possible due to the formation of the close-knitted surface
film due to silicone-modified acrylate [173]. When hydrox-
yethyl methacrylate-based acrylic monomer was used for
acrylic coating, it resulted in better coating formation. Still,
it increased the hydrophilicity, decreasing the water contact
angle and decreasing ink absorption [174]. In terms of bar-
rier, the WVTR of acrylated epoxidized soyabean oil and
CNC coated paper was reduced to 1392 from 1926 gm/m2-
day [175]. The WVTR is reduced, but it is not low enough
to that required by most packaging materials. Therefore, the
high barrier in the acrylate-based coatings remains the main
problem.
Besides water-borne acrylic emulsion, the wax emulsion
is now used for coating paper. PE wax emulsions were con-
ventionally used in paper industries. Other natural sourced
wax such as beeswax, candelilla wax, carnauba wax, and
other oil-based wax is being studied to replace the PE wax.
The mixture of beeswax and carnauba wax-based water-
borne emulsion with the help of a cationic emulsifier made
superhydrophobic paper after coating on the paper [176].
The annealing of coatings further increased the contact angle
above 150° and the sliding angle below 10°. This was due to
the melting of beeswax and nano structuring caused by car-
nauba wax. Further carnauba wax micro and nano-emulsion
with ammonium and dimethylpolysiloxane were coated on
paper sheets by dip method, resulting in a contact angle of
50° to 75°. It further reduces WVTR by a 3.55 factor [177].
These emerging materials have proven themselves as reliable
coating solution. Still, they have many challenges ahead,
such as poor barriers and lack of study on the overall migra-
tion of the coatings to the food simulant.
8 Criteria for selection of package
Packaging of the liquid products such as beverages, oils, or
alcohol is dependent on various factors such as moisture
gain or loss, oxidation, temperature deterioration, loss of
nutrients due to UV, and many more, so the packaging of
the produces is done to extend the shelf life by protecting
them. The shelf life of the products is measured by many
qualitative techniques, which are unique for the products.
But the shelf life can also be estimated from various factors
such as water vapor transmission rate, oxygen transmission
rate, heat transfer, or light transfer. The criteria selection
depends upon the deterioration factor of the food to pack.
This determines whether a material can be used to pack the
product or not. The shelf life can be estimated by using equa-
tions involving barrier properties. This can also work on the
other way around, i.e., if we know the requirement of shelf
life, we can calculate the required barrier, hence choosing
the proper bio-nanocomposite for coating application on
paper-based packaging.
8.1 Water vapor transfer
If a product's shelf life is deteriorated by the amount of water
it can gain or lose, the degree of protection is used. This
explains the maximum amount of water/air that a product
can accumulate at a temperature. The shelf life (∅) for the
products that deteriorate by gaining and losing moisture is
calculated using Eqs. 1 and 2, respectively [12].
me − mi P ∗ A ∗ po
ln =( )∗∅ (1)
me − mt X∗ b ∗ W s
mi − me P ∗ A ∗ po
ln =( )∗∅ (2)
mt − me X∗ b ∗ W s
where, ­me = Equilibrium moisture (%), ­Mi = initial moisture
(%), ­Mt = moisture at time “t” (%), P = water vapor transmis-
sion rate (g/m2-day), X = driving force (cm Hg), A = surface
Area of package ­(m2), Po = vapor pressure of water at stor-
age temperature “T” (cm Hg), ­Ws = weight of product to be
packed (gm) and b = slope of moisture sorption isotherm (g
­H2O/g solids/unit ­aw).
The equations mentioned above have been extensively
used for predicting the shelf life and have been able to find
excellent predictions for weight gain or loss. These equations
can also be used if the external conditions of temperature or
humidity are changed as the permeability of the material can
be tested at any temperature and humidity and used in the
equation to estimate shelf life.
A more straightforward shelf-life estimation can be done
using the maximum allowable moisture, as shown in Eq. 3
[178]. This equation takes into an assumption of worst-case
scenario for the food to be packed. Therefore, instead of
WVTR at any condition, WVTR value used for calculating
shelf life is tested at 38 °C and 90% RH and applied in the
Eq. 3.
H2 Omax
∅= (3)
WVTR
where ­H2O max is the maximum allowable moisture (g/m2)
and WVTR is the Water vapor transmission rate (g/m2-day).
Generally, the ∅ is calculated based on the WVTR. But, if
we use ∅ a predefined value, i.e., the required shelf life,
we can calculate the WVTR required by the package. The
13

required WVTR can help us to identify the bio-nanocom-
posite required for the coating application.
8.2 Gas transmission
Many products get oxidized and deteriorate qualitatively,
and thus oxygen barrier is provided by the package to pro-
tect the food. Apart from oxygen, many products have their
aroma, which, if lost, denotes the end of the shelf life; there-
fore, packages also play a crucial role in the aroma barrier.
To estimate the shelf life based on maximum oxygen to per-
meate, Eq. 4 is used to calculate shelf life [12].
Q∗X
∅= (4)
P ∗ A ∗ Δp
where, Q = Max ­O2 permissible (ml), X = thickness of pack-
age (cm), P = permeability (­ barrer10), A = surface area (­ cm2)
and ∆p = Environment vapor pressure of ­O2 (cm Hg).
This is similar to the Eqs. 1 and 2 of the WVTR. There-
fore, to check the shelf life at any temperature or humidity
the permeability values at those condition can be used in
the Eq. 4
And as similar to water vapor, a simple equation can also
be used for shelf life, as shown in Eq. 5 [178].
O2max
∅= (5)
OTR
O2max is the Maximum allowable oxygen gain by the prod-
uct (gm/m2), and OTR is the oxygen transmission rate (gm/
m2-day). As depicted in WVTR section, the OTR required
can also be calculated with the help of the required shelf life
to choose the bio-nanocomposite for coating application.
8.3 Mechanical properties
Many products when packed require different types of
strength properties until it reaches the end consumer. Most
oil products are packed in PE coextruded with nylon or
nylon can be laminated with the PE [12]. Nylon is present
in packaging to provide good puncture resistance [165]. The
puncture resistance in paper coated pouches would be a chal-
lenge. In a similar way, large standup pouches do not burst in
drop test. This is due to the higher elongation and high seal
strength provided by the polyethylene [18, 179]. Therefore,
the coating on paper should produce a good sealability and
also provide good elasticity. Currently, some researchers are
creating a stretchable pouch by micro-shrinking the paper in
both machine and cross direction [180]. These stretchable
pouch with good elastic coating may provide better strength
during drop test. On the other hand, paper bottles can face
a lot of challenges and criticism regarding the structural
strength of pulp due to its ease in deformation. Moreover,
13
Biomass Conversion and Biorefinery
the filling of alcoholic beverages at high pressure may chal-
lenge the structural strength of paper bottle. Therefore, the
use of strength additives will be required. Replacing plastic
bottle with paper may require new methods to test the bottle.
8.4 Recyclability
Following a holistic approach for barrier-coated packaging
papers within the circular economy, the bio-based origin and
end-of-life options should be considered from the design
phase onwards [181]. Besides incineration, biodegradation
or composting, the recovery of a valuable fiber fraction
and their reintegration in novel paper products is the most
responsible alternative. The recyclability of paper products
has been defined as the capacity of a material or product to
be processed effectively from a technological and economic
point of view in order to recover the cellulose fibers it con-
tains and to produce new paper and board, employing the
technologies predominantly used today in the paper industry
[182]. As a first criterion, the repulpability of coated paper
feedstock is assessed through evaluation of fiber yield and
morphology after the repulping process [183]. The recycla-
bility of paper fibers is further evaluated after introduction
of a recovered fiber fraction in combination with virgin pulp
into new paper materials [184]. Although the field relies
on long tradition of experimental research and test meth-
ods to simulate standard stock preparation, advances have
long been hampered through the lack of unified standards
for evaluation. The voluntary testing method of Aticelpa
MC 501–13, internal standard of PTS-RH 021/97 (1997)
and its transformation into INGEDE 11/12 (2012), EcoPa-
perLoop Method 1 (2014) have been accepted as a guid-
ance to assess the repulpability and recyclability next to the
European Standard EN 13430 (2004), but no general agree-
ment existed on standard methods. Only recently (December
2020), Cepi published a harmonized European laboratory
test method to produce parameters enabling the assessment
of the recyclability of paper and board products in standard
paper and board recycling mills. In general, the methods
include pulping and pulp dilution, screening for separation
of coarse rejects and colloidal solids (< 10 µm), measure-
ment of adhesiveness (macrostickies) and optical homogene-
ity testing of produced handsheets.
The recycling of PE-laminated papers is problematic due
to the strong bonding and penetration of the PE polymer film
within the paper fibers [181]. Moreover, general procedures
of mechanical grinding and pulping with consequent sepa-
ration of the polymer film is water demanding and results
in pollutant microplastics [185]. The alternative extrusion
coatings of PLA biopolymers were evaluated and give same
problems owing to the hydrophobicity and strong film form-
ing properties of the thermoplastic layer, while alternatively
the pulping yield of the more hydrophilic polyacrylate-based
Biomass Conversion and Biorefinery
coatings was higher [186]. On the other hand, the remain-
ing polyacrylate flakes must be mechanically fragmented
in addition as they could not be removed by screening and
flotation due to its softness, while the original flakes have
negative effect on the recycled paper properties. The water-
based dispersion coatings based on synthetic polymers are
generally classified as recyclable; however, repulpability
also highly depends on the coating thickness, presence of
a base coating layer, concentrations of hydrophobic com-
ponents, in combination with the temperature and pH of
repulping [187]. The addition of inorganic minerals in the
coating improves the repulpability as they may result in the
formation of smaller particles during the repulping process
[188], or act as an adsorbent for the agglomeration of sticky
latex particles. Alternatively, the repulpability of bio-based
dispersion barrier coatings including hydroxypropylated
starch and hydroxypropylated cellulose relatively poor com-
pared with traditional styrene-butadiene latex coatings, in
parallel with high affinity of biopolymers to the cellulose fib-
ers [189]. The binding of the biopolymer coating fragments
with talc in combination with vast control on solubility of
the coating fragments depending on repulping temperature
was able limit negative effects on sheets of recycled fibers.
In particular, the physico-chemical properties (e.g., zetapo-
tential) of the rejects should be closely controlled in parallel
with the wet-end paper chemistry [190]. However, industrial
concern remains that the separation of large PE flakes dur-
ing repulping is technically more feasible than the separa-
tion of small polymer fragments resulting from water borne
dispersion coatings, depending on the use of appropriate
surfactants and chemical pulping additives. Different meth-
ods for removal of macrostickies originating from adhesives
were evaluated based on enzymatic control [191–193].
Recent approaches have considered delamination mecha-
nisms through enzymatic hydrolysis of the coating layer. The
hydrolysis of a zein-wax coating in presence of proteases
such as pepsin or chymotrypsin resulted in clear separation
from the paper substrate under mild temperatures and neu-
tral pH [194, 195]. The delamination of plastic-coated paper
was also effectuated through the action of enzymes extracted
from fungi, where the paper part partly dissolves through
decomposition of the lignin constituents [196]. As such, a
recyclable alternative for wax-coated packaging papers with
similar performance could be offered. The further advances
in nanotechnology enable the formation of an intermediate
release layer of CNF: the layer improves mechanical proper-
ties and barrier resistance under dry conditions, but starts
to swell and loose strength in the wet state [197]. The for-
mation of a dense cellulose surface layer also hinders the
penetration of a polymer coating into the paper substrate,
but the adhesion of the outer polymer coating onto the inter-
mediate CNF release layer should be further tuned through
the use of additives of surface treatments. However, the role
of nanoparticles in the paper recycling process needs to be
critically assessed in a broader environmental context, as it
has been proven that around 90% of inorganic nanoparti-
cles originally present in the coating end up in the rejected
material stream, while 7 to 16% ends up in the accepted
fiber stream [122]. There were no significant effects on
the strength of handsheets from recycled pulp, while leak-
age into the wastewater streams could not be ruled out and
require safe handling of nanomaterials.
9 Conclusion
Literature shows that petroleum-based packaging may be
replaced with a sustainable solution due to environmental
pollution and the depletion of crude oil. Cellulose, the most
abundant biomaterial, can replace the current rigid and flex-
ible packages in the form of paper bottles and paper sachets
or pouches, respectively. An appropriate combination of
paper and a coating of biopolymer nanocomposite has the
potential to provide fully biobased packaging material and
replace the conventional multilayer flexile sachets or con-
ventional bottles.
Paper sachets and pouches are a commonly used package
that can replace the flexible packaging in the world with
the help of a biodegradable polymer to provide sealabil-
ity, barrier in terms of oxygen, water vapor, and oil. But to
replace the rigid packages, such as containers or bottles, the
concept of the paper bottle is yet to be explored. Although
many industries have initiated the paper bottle project based
on molded fiber technology, the main concern with paper
bottles lies with the closure, barrier (moisture, oxygen) and
resistivity towards alkali or acid attack. Moreover, the pro-
duction speed of paper bottles is a significant concern in a
fast-moving world. An inner liner of biopolymer for food
contact application on the paper bottle has previously been
created, which can be easily removed after use, so that the
paper and polymer may proceed in their respective recycle
streams. The role of biopolymer coating on the paper bot-
tle to increase the product's barrier, eventually increasing
the liquid product's shelf life has been extensively explored.
However, lower bond strength is a critical matter which is an
undervalued property and is yet to be increased to maintain
the package integrity. PLA and PHA nanocomposite have
shown their potential as biodegradable coating on paper
sachets or paper bottle, that can be used as a food safe mate-
rial with a high barrier for the liquid products due to their
inherent hydrophobicity and lower migration values. Fur-
ther, the nanomaterials such as hydrogenated carbon and
nano cellulose (crystal, fiber or sphere) have shown their
ability to improve the barrier property without interfering
with the migration values. Besides these, some emerging
materials such as cellulose fatty ester, CNF and waterborne
13

emulsion of acrylates or waxes have shown their potential
for the coating on paper packaging. But the main issues lie
on the ack of literature on the migration values for different
food simulant and at various environment condition. Besides
tuning appropriate functional properties, the coating com-
position highly imparts recyclability of the paper-based
packaging.
In conclusion, paper sachets or pouches and paper bot-
tles, along with bio-nano composite coatings, are the future
material that can replace conventional petroleum-based
packaging by maintain the combination of hydrophobicity,
degradability, high oxygen and water barrier and permissible
migration limit.
Author contribution  Arihant Ahuja: Investigation, Formal analysis,
Visualization, Writing—Original Draft. Pieter Samyn: Writing, For-
mal Analysis, Manuscript Editing. Vibhore Kumar Rastogi: Con-
ceptualization, Investigation, Resources, Formal analysis, Manuscript
editing and review, Supervision.
Funding  Author Arihant Ahuja would like to thank the Indian Insti-
tute of Technology Roorkee and Prime Minister Research Fellowship
(PMRF), Govt of India for providing online resources and support to
carry out this review study during his Ph.D.
Author Peiter Samyn acknowledges financial support in frame of the
VLAIO-TETRA-CORNET project RePac 2 (2022–2023).
Data availability  Not applicable.
Declarations  org/​10.​1016/​B978-0-​323-​24273-8.​00004-6
Ethical approval  Not applicable.
Competing interests  The authors declare no competing interests.
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