Journal of Cleaner Production 294 (2021) 126218

Contents lists available at ScienceDirect

Journal of Cleaner Production

journal homepage: www.elsevier.com/locate/jclepro

Review

An overview of non-biodegradable bioplastics

Md Hafizur Rahman, Prakashbhai R. Bhoi*
Department of Mechanical Engineering, Georgia Southern University, Statesboro, GA, 30460, USA

a r t i c l e i n f o a b s t r a c t

Article history: Bioplastics have introduced numerous flexibilities to humankind. However, bioplastics have brought
Received 13 August 2020 newer challenges in waste management. Approximately half of the current bioplastic market is not
Received in revised form biodegradable, and with a larger market volume, its end-of-life allocation will be problematic for the
27 January 2021
governments and policymakers. This study aims to provide an overview of the non-biodegradable bio-
Accepted 29 January 2021
Available online 1 February 2021
plastics market, including their underlined challenges, typical production methods, characterization, and
possible alternative waste utilization perspective. Bioplastic production usually starts from a biological
Handling editor: Prof. Jiri Jaromir Klemes source i.e., biomass and a series of modification techniques such as pretreatment, hydrolysis, and
fermentation are carried out to produce bioethanol. Then, bioethanol is converted to non-biodegradable
Keywords: bioplastics. The major non-biodegradable bioplastics are bio-polyethylene (bio-PE), bio-polypropylene
Bioplastics (bio-PP), bio-polyethylene-terephthalate (bio-PET), bio-polytrimethylene terephthalate (Bio-PTT), and
Energy bio-polyamide (bio-PA). In this review article, an overview of each bioplastic is presented with flow
Fermentation diagrams. Also, the production method of compostable bioplasticsdpolylactic acid (PLA) d is briefly
Gasification
discussed for comparison purpose. Since the chemical structure of bio-based non-biodegradable plastics
Gasoline
is similar to the conventional fossil-based plastics, the characterization and alternative thermochemical
Pyrolysis
utilization techniques of five bioplastic wastes are discussed based on the conventional plastics char-
acterizations. Per ultimate analysis, considering high hydrogen, low oxygen, and low fixed carbon con-
tent, bio-PE and bio-PP are recommended as potential feedstocks for the catalytic pyrolysis process to
produce gasoline and diesel range liquid hydrocarbons. Alternatively, bio-PET, bio-PA, and PLA are rec-
ommended as potential feedstocks for the gasification process, considering their higher oxygen content.
© 2021 Elsevier Ltd. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2. Methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3. Bioplastics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.1. Problems leading to pollution . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.1.1. Misconceptions about bioplastics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.1.2. Marine litter . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.1.3. Microplastics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.2. Non-biodegradable bioplastics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.2.1. Bio polyethylene (Bio-PE) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
3.2.2. Bio polyethylene-terephthalate (Bio-PET) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
3.2.3. Polytrimethylene terephthalate (Bio-PTT) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
3.2.4. Bio polypropylene (Bio-PP) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
3.2.5. Bio-polyamide (Bio-PA) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.3. Compostable bioplastics: bio polylactic acid (Bio-PLA) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8

* Corresponding author. Department of Mechanical Engineering, Georgia

Southern University, Statesboro, GA, 30460, USA.
E-mail addresses: mr07444@georgiasouthern.edu (M.H. Rahman), pbhoi@
georgiasouthern.edu (P.R. Bhoi).

https://doi.org/10.1016/j.jclepro.2021.126218
0959-6526/© 2021 Elsevier Ltd. All rights reserved.
M.H. Rahman and P.R. Bhoi Journal of Cleaner Production 294 (2021) 126218

3.4. Characterization . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.4.1. Ultimate analysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.4.2. Proximate analysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
4. Cost and properties of bioplastics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
5. Challenges and opportunities of bioplastics under circular economy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
6. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
Declaration of competing interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
Acknowledgment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13

1. Introduction resources such as corn, sugarcane, and biomass (European

Bioplastics, 2020). The production process involves pretreatment,
Plastics are a universal part of the modern economy due to their hydrolysis, fermentation and several steps of organic reactions. The
unique functional properties at low-cost. The industrial production conversion of green plants into plastics has an appeal among con-
of plastics has brought enormous ease to human life. Therefore, the sumers. This is one of the key reasons for the growing popularity of
yearly production of plastics is increasing ever since its inception. bioplastics among consumers. As a result, McDonald’s and many
The annual production of plastic was only 15 million metric tons in other companies used bioplastic containers to offer fast food to
1964, which became 360 million metric tons in 2018 (Neufeld et al., their customers (Arikan et al., 2015).
2016; Plastics Europe, 2019). By 2018, approximately 8660 million The popularity of bioplastics was initially backed by the idea
metric tons of virgin plastic have been produced worldwide. This that bioplastics are 100% biodegradable, compostable and
immense production volume has introduced massive garbage. By environment-friendly (Reddy et al., 2013). In recent studies, the
2015, the estimated global plastic waste was around 6300 million popular conceptdbioplastic itself is biodegradabledhas been
metric tons of which only 9% has been recycled, 12% has been rebutted and referred to as misleading due to some limitations
incinerated, and 79% has been dumped in landfills or natural (Iwata, 2015). The first limitation is the substantial quantity of
environment (Geyer et al., 2017). bioplastics, equivalent to that of traditional plastics, such as Poly-
Europe was the first continent to step ahead to recover waste ethylene (PE), polypropylene (PP), polyamide (PA), or polyethylene
plastics. From 2006 to 2018, they reduced 44% of their landfilling terephthalate (PET). Usually, biomass-based plastics are referred as
and the energy recovery and recycling practices from waste plastics bio-PE, bio-PP, bio-PA, or bio-PET. According to the European Bio-
were increased by 77% and 100%, respectively. In 2018, around 29.1 plastic Association, these bioplastics are not biodegradable and
million metric tons of plastic waste were collected from 30 Euro- possess the same threat as traditional plastics (European
pean countries, among which 32.5% was recycled, 42.6% was used Bioplastics, 2020). The second limitation is the requirement of the
for energy recovery, whereas 24.9% was landfilled. Per US EPA, 27 specific composting conditions. The bio-based biodegradable bio-
million metric tons of plastic is received in their landfills that is plastics, which are compostable, such as PLA, require composting
approximately 41% of their annual production of 64.6 million facilities to biodegrade. In these facilities, waste compostable bio-
metric tons (Plastics Europe, 2019; US EPA, 2019). In Asia, there are plastics are degraded at a certain temperature and pressure. As the
limited treatment facilities in most of the countries in response to compostable plastic is a partial fraction of the total plastic usage, in
their 132 million metric tons of plastic production in 2018 (Plastics the USA, they need to be separated from the waste stream and
Europe, 2019). As a result, unattended and landfilled plastics transported to an eligible composting facility. However, most of the
became critical from plastic pollution point of view that drives the consumers are unaware of this requirement, and therefore the
global leaders for developing waste plastic minimization policies. compostable bioplastic waste eventually ends up in landfills with
By virtue, dumped plastics can remain unaffected for a hundred other plastics. As a result, in the last decade, global plastic pollution
to thousands of years (Wang et al., 2016). Even by that time, if it took a new paradigm. Per the World Economic Forum report, more
breaks down, then it creates fragmented micro and nanoparticles. than 8 million tons of plastic is dumped annually into the ocean;
These micro and nano-plastic particles accelerate the problems that is equivalent to discarding one garbage truck per minute
even further by affecting human health (Galloway, 2015). There- (Neufeld et al., 2016). Without necessary actions, this continued
fore, managing plastic waste has become one of the major issues for practice will lead to 4 trucks per minute by 2050. In this way, the
policymakers and researchers. In this regard, international policies approximated plastic-to-fish ratio (by weight) in the ocean will
initiated the reduction of single-use plastics, and many countries become >1:1 compared to 1:5 in 2014 (Neufeld et al., 2016). So, the
banned plastic polybags since 1991 (Xanthos and Walker, 2017). existence of our marine ecosystems will be at an enormous threat.
Scientific investigations have also been carried out in the quest for Due to all these problems, plastic waste became one of the major
suitable substitutes for traditional plastics. One of the potential challenges for the policymakers even after the invention of
substitutes of traditional plastics, which has been introduced so far bioplastics.
into the market with greater hope, is known as “bioplastic”. Bio- As of today, several articles have reported upcoming challenges
plastics are a polymer family whose carbon is usually sourced from of bioplastics from different perspectives. For example, research
biological resources such as biomass (Narayan, 2011). However, insights have been reported on the anaerobic and aerobic digestion
biodegradable bioplastics can be either bio-based or fossil-based. of biodegradable bioplastics (Ruggero et al., 2019). However, non-
Therefore, the term “Bio” before “plastic” refers to its carbon biodegradable bioplastics (which are around 50% of the market)
source or its biodegradability. Interestingly, bio-based bioplastics are excluded from their scope of work. Andreeben et al. (Andreeben
can be non-biodegradable (de Vargas Mores et al., 2018). Currently, and Steinbüchel, 2019) discussed the production process of non-
almost half of the available bio-based bioplastics are non- biodegradable biopolymers, however, the pollution perspective
biodegradable (Fig. 1). was not discussed. Besides, the scenario of chemical characteriza-
Non-biodegradable bioplastics are usually produced from green tion for waste utilization was not addressed. The characterization of
2
M.H. Rahman and P.R. Bhoi
plastic generally offers the critical insights on moisture, fixed car-
bon, volatile, ash content and chemical compositions. These in-
sights are helpful to project plastic’s viability for thermo-chemical-
conversion (TCC) processes. Moreover, some investigations on PLA
production, and possible recycling techniques were reported in
studies (Payne et al., 2019). Overall, many investigations have been
carried out separately on bioplastic production, biodegradation and
challenges within the last two decades (Brodin et al., 2017). How-
ever, in our opinion, there is no article that presents an overview of
non-biodegradable bioplastics market, its challenges, production
methods and evaluates the characterization in terms of its
utilization.
The objective of this study is to provide an overview of bio-
plastics in terms of the market volume, challenges, production
methods, characterization and feasibility for upcycling of bio-
plastics. This paper specifically focuses on the major non-
biodegradable bioplastics, such as bio-PE, bio-PP, bio-PET, bio-PTT
and bio-PA. Besides, compostable bioplastic, such asdPLA is also
addressed for comparison. These bioplastics represent nearly 50%
of the current bioplastic market. In this review analysis, the pro-
duction flowcharts of all these bioplastics have been discussed,
with an insight into the pretreatment, hydrolysis, and fermentation
processes. In addition, characterization of bioplastics is analyzed in
terms of its downstream utilization for fuels and chemicals
production.
2. Methods
An overview of bioplastics is provided in this manuscript, which
is described based on 120 state-of-art research papers in the field of
bioplastics, circular economy, biomass pretreatment, and plastic
characterization. These papers were collected using Web of Science,
Scopus, ScienceDirect, Google Scholar, ResearchGate, Academia,
and Georgia Southern interlibrary loan program, covering Elsevier,
Springer, Taylor & Francis Group, Wiley, Royal Society of Chemistry
(RSC), and similar highly reputed publishers. This manuscript
consists of synthesized information on bioplastics, which is well-
articulated in different phases covering market volume, chal-
lenges, production methods characterization, and its viability as
feedstocks for fuels and chemicals production.
3. Bioplastics
Bioplastics are a family of materials with different properties
and applications. According to European Bioplastics, plastic can be
termed as a bioplastic if it is either biobased, biodegradable, or
consists of both properties (Bioplastics, 2016). If the plastic is
resourced completely or significantly from a biological source, it
can be considered biobased bioplastics. These types of bioplastics
can be either biodegradable or non-biodegradable. Both types of
bioplastics are presented in Fig. 1. The important definitions of
concepts typically related to bioplastics are illustrated below ac-
cording to the international standards.
Biodegradation: Degradation is an irreversible process, creating
a significant change inside the plastic structure, causing it to lose its
properties and leading to fragmentation. Biodegradation is caused
by biological activity, such as enzymatic action, which leads to a
significant change in the plastic’s chemical structure (Pagga, 1998).
Biodegradability: As per EN 14046 test method, biodegradability
is determined by estimating the actual metabolic conversion of
compostable materials into carbon dioxide. According to this
standard, the acceptance level is 90%, which must be reached
within 6 months at 58
C and around 50% controlled humidity. Also,
air circulation is required to maintain an oxygen concentration of at
least 6% (Briassoulis et al., 2010).
3
Journal of Cleaner Production 294 (2021) 126218
Disintegrability: As per EN 14045, disintegrability is measured
by degrading the test material together with organic waste for
three months. After that, the compost is sieved using a 2 mm sieve.
If any residue of the tested plastic stays higher than 2 mm, it is
considered as not disintegrated. The non-disintegrated fraction
must be less than 10%, and then the plastic is considered as
disintegrable.
Compostability: According to European standard EN 13432, the
characteristics that are observed in compostable material are i)
biodegradability, ii) dis-integrability, iii) absence of negative effects
on composting process, iv) absence of negative effects on the
compost quality and low level of heavy metals, and v) fulfillment of
above four requirements simultaneously (Briassoulis et al., 2010).
Bioplastic can be resourced from biological sources such as
biomass. Due to its advantages in terms of fossil fuel savings and
potential biodegradation, the market of bioplastic is emerging
rapidly and replacing traditional plastics. The global production
capacity of bioplastics reported by European Bioplastics Association
is 2.11 million tons in 2020, as shown in Fig. 1 (European Bioplastics,
2020). The bioplastics market will experience an increase of 36%,
and it could reach 2.87 million tons by 2025 (European Bioplastics,
2020). As per Fig. 1, non-biodegradable bio-based bioplastics are
mainly Polyethylene terephthalate (bio-PET), Polyamide (bio-PA),
Polyethylene (bio-PE), Polypropylene (bio-PP), Polytrimethylene
terephthalate (bio-PTT) and Polyethylene furanoate (bio-PEF),
(European Bioplastics, 2020). On the other hand, biodegradable
bio-based bioplastics include mainly Polylactic acid (PLA), Poly-
hydroxy alkanoate (PHA), Polybutylene succinate (PBS), and starch
blend.
Per market data of 2020, the major bioplastics including bio-PE,
bio-PET, bio-PTT, bio-PP, bio-PA, and PLA, cover approximately
59.5% of the current bioplastic market. As per the Plastics Europe,
traditional plastics consisting of PP, PE (both HDPE and LDPE), and
PET cover 56.7% of the traditional plastic market (Plastics Europe,
2019). Due to the similarity of chemical structure, bio-PE, bio-PP,
and bio-PET waste can be treated alike traditional PE, PP, and PET.
3.1. Problems leading to pollution
3.1.1. Misconceptions about bioplastics
It is a fact that the majority of the current world bioplastics have
similar chemical compounds like traditional plastics. Therefore,
most of the bioplastics are prone to exhibit similar problems as
traditional plastics. Consequently, bioplastics need to be recycled or
utilized to avoid plastic pollution. The bioplastics that are com-
postable need well equipped industrial composting facilities to
break down (Niaounakis, 2019). So far, a few cities over the world
have been equipped with industrial composting facilities. There-
fore, a lot of compostable bioplastics fail to meet a composting fa-
cility and goes to the landfill. As per the US EPA, only 29.1% of the
produced PET bottles and 31.2% of the produced HDPE were recy-
cled in 2017 in the US (US EPA, 2019). A similar trend is obvious for
bio-PET, bio-HDPE, and other bioplastics unless a strong notion is
raised against mismanaged plastics waste. Earlier, Pathak et al.
(2014) mentioned that 93% of the worldwide produced plastics
end up in landfills and oceans every year. These practices will
passively entertain stakeholders to mismanage bioplastic wastes
unless alternative solutions are addressed. However, there are
some biodegradable plastics present in the market, such as poly-
hydroxyalkanoate (PHA), Polyvinyl alcohol (PVA); which can be
anaerobically degraded (B atori et al., 2018). They have the potential
to decay with microorganisms, which can decompose them
without producing harmful or noxious residues. It is a matter of fact
that the process of decomposition depends solely on the specific
environmental conditions (Emadian et al., 2017). A few bioplastics
M.H. Rahman and P.R. Bhoi
Fig. 1. Bioplastic market in 2020 as per European Bioplastics data (European Bioplastics, 2020).
require specific atmospheres, such as soil with bacteria or fungi, to
degrade. This condition is usually unavailable at the landfills or
ocean litters (Pathak et al., 2014). Therefore, if anyone leaves these
bioplastics in the trash with a hope that bioplastic will vanish itself
over time, is not going to happen. In order to mitigate this confusion
and misconception regarding biodegradation, biodegradability, and
composability, a BS EN 13432 standard was adopted (British Plastic
Federation, 2009). It is identical to UNI EN13432 standard from
technical perspectives. As per this standard, bio-based plastic is
good to be processed through compostable industrial facilities, if it
complies with prescribed standards (European Bioplastics
Association, 2019). So, any bioplastic package that is certified to
be compostable needs to be composted in the equipped facilities
and should not be left unattended with the belief that it will vanish
over time. Consumers are required to act wisely with bioplastic
waste to recede similar problems as traditional plastics. Specially
for non-biodegradable bioplastics, a unique short terminology,
such as ‘NB-plastic’ can be used, referring to its non-biodegradable
nature.
3.1.2. Marine litter
Researchers addressed about the damages that plastic have
already caused to our ocean environment (Kuhn et al., 2015). The
number of species among all groups of wildlife that have been
affected by either entanglement or ingestion of plastics has been
doubled now since it was in 1997. According to the research data of
2015, 81 out of 123 species of mammals, 203 out of 406 species of
seabirds and 7 out of 7 species of turtles have been already affected
(Kuhn et al., 2015). If the current trend of dumping plastic in the sea
carries forward, there will be more kg of plastic in the sea than fish
by 2050 (Neufeld et al., 2016). Also, the types of plastics in the
marine litter were analyzed and reported in a study. Alarmingly, the
majority of plastics based on the percentage of the global produc-
tion were polyethylene (29.1%), polypropylene (18%), polyethylene
terephthalate (20%) and polyamide (1%) (Andrady, 2015). In the
same study, approximately 1.13 million PE bags, 1 million PP food
wrappers/containers, and 0.88 million PET beverage bottles were
reported in the marine litter which is alarming for the ocean
environment and human health (Kuhn et al., 2015). As per record,
4
Journal of Cleaner Production 294 (2021) 126218
around 12.7 million tons of plastic enter the oceans as marine litter
every year, creating environmental, social, and economic problems
(Jambeck et al., 2015). Bioplastics, which were thought to be a
potential solution since its invention, are now considered as a
similar threat (European Bioplastics, 2016). Therefore, their accu-
mulation in the ocean is going to accelerate the problem in the
coming decades, unless a truly biodegradable bioplastic is invented
or a proper recycling or upcycling of the current bioplastics waste
could be developed.
3.1.3. Microplastics
According to the publication of a joint group of experts on the
scientific aspects of Marine Environmental Protection (GESAMP),
2016; microplastics are small pieces of plastics less than 5 mm in
size with no lower limit established. In 1972, the first plastic
observed in the western North Atlantic consisted of pre-production
pellets and degraded fragments (Barnes et al., 2009). An investi-
gation in the North Pacific, and South Atlantic also revealed the
existence of microplastic fragments in the seawater (Morris, 1980).
These microplastics consumed by aquatic animals like fish are
consumed by humans, which increased harmful plastic accumu-
lation in the human stomach and accelerated the cancer risk and
the other problems In the last decade, scientists clearly understood
the global implications of fragmented plastics traveling long dis-
tances (Yogui and Sericano, 2009). Therefore, not only by eating fish
but inhaling air from the environment also increases the risk of
fatal diseases due to harmful microplastics. It is important to note
that the majority of bioplastic counter-products such as PE, PP, PA,
and PET identified in microplastics have a hazard score of 11, 1, 63-
50 and 4, whereas PVC possessed a hazard score between 10551-
10001 (Galloway, 2015). Therefore, without a proper management
of the bioplastic life cycle, the situation will become more
dangerous in its bigger market dimension (Barboza et al., 2018).
3.2. Non-biodegradable bioplastics
Bioplastics could be produced from lignocellulosic biomass
through a series of conversion processes (Figs. 3e6). The overall
process flow diagram of the biomass to bioplastics production is
M.H. Rahman and P.R. Bhoi
provided in Fig. 2. As shown in Fig. 2, the first step involves the
pretreatment of biomass. The biomass basically constitutes cellu-
lose, hemicellulose, and lignin (Ouedraogo and Bhoi, 2020). The
pretreatment is performed to increase the accessibility of enzyme
to cellulose to increase its degradation (Alvira et al., 2010). In pre-
treatment, biomass breaks down into oligomer subunits, which are
followed by enzymatic hydrolysis to extract sugar. The extracted
sugar is fermented to produce bioethanol.
The pretreatment processes can be categorized as physical,
chemical, biological and thermochemical (Sebayang et al., 2016).
Physical pretreatment is used to increase the pore size and surface
area of the biomass. It reduces the crystallinity and degree of
polymerization at the same time. As a result, enzymatic degrada-
tion is improved. The physical pretreatment can be done through
ball milling or mechanical extrusion processes. Ball milling drops
down the crystallinity index from 4.9% to 74.2%, which is advan-
tageous for the production of fermentable sugar at mild hydrolysis
conditions (Aftab et al., 2019). For instance, oil palm fond fiber
biomass produced 87%, 81.6%, and 85.4% of glucose, xylose, and
total sugar using a ball milling pretreatment process (Zakaria et al.,
2014). However, ball milling is an expensive option in terms of
energy consumption, which is a huge drawback for industrial ap-
plications (Aftab et al., 2019). Physical pretreatment can also be
performed mechanically with a single screw and double screw
extruders. In such a mechanical extrusion, biomass is passed
through a defined cross-section die and comes out with a unique
profile. This process is advantageous because of less product
degradation, high adaptability to modification, and high
throughput. Glucose, xylose, and combined sugar yield in single
screw extruder under physical pretreatment process from soybean
Fig. 2. Process flow diagram of lignocellulosic biomass to bioplastics production (blue
represents stages of the process and green represents products).
5
Journal of Cleaner Production 294 (2021) 126218
hulls, corn stover, and switchgrass were reported in the literature
(Zheng and Rehmann, 2014). The optimum pretreatment condi-
tions of screw speed and barrel temperature of those studies were
60 rpm, 75 rpm, 155 rpm, and 130
C, 125
C, 176
C accordingly
(Karunanithy and Muthukumarappan, 2010; Karuppuchamy and
Muthukumarappan, 2009).
Pretreatment can also be done chemically using organic acid
catalysts such as oxalic acid, acetylsalicylic acid, or salicylic acid
while organic or aqueous organic solvent mixture with hydro-
chloric acid or sulfuric acid is used to break down the internal
bonds of lignin and hemicellulose (Behera et al., 2014). It was re-
ported that acid pretreatment produced glucose, xylose, and other
minor sugar from basam and switchgrass, between 160 and 190
C
and within 4 h using dilute sulfuric acid solvent (Yat et al., 2008).
Concentrated acids are less preferred in this process due to asso-
ciated corrosion and cost. Besides, the formation of microbial in-
hibitors such as furfural and 5-hydroxyl methyl furfural (HMF) from
hemicellulose degradation affects the fermentation process later on
(Karlsson et al., 2012). Relatively, alkali pretreatment of biomass
produced higher sugar yield than acidic pretreatment for switch-
grass and big bluestem (Karunanithy and Muthukumarappan,
2011). Also, alkali pretreatment removed the acetate group from
the hemicellulose, which assists the enzymes in accessing the
carbohydrates more easily (Bochmann, 2019). Apart from acid and
alkali pretreatment, organosolv process is getting popular nowa-
days because of its extensive potential to remove lignin and to
produce high ethanol yield. In this process, internal lignin and
hemicellulose bonds are broken down using a mixture of inorganic
acids (HCl or H2SO4) with organic solvent in the aqueous form
(Behera et al., 2014).
Biological pretreatment uses white rot, soft rot, and brown fungi
to separate lignin from biomass (Han et al., 2013). Brown rot usually
attacks cellulose, while soft rot and white rot target both cellulose
and lignin of the biomass (Aftab et al., 2019). The presence of such
microorganisms made this method more environmentally friendly
and energy-efficient than physical and chemical pretreatment
processes (Wagner et al., 2018). However, it is necessary to inves-
tigate their mode of action for full-scale industrial implementation.
Other pretreatment methods, such as thermochemical pre-
treatment, can be done through steam explosion (STEX), liquid hot
water (LHW), Ammonia fiber explosion (AFEX), wet oxidation
(WO), microwave process (MWP), CO2 explosion pretreatment and
Sulphite pretreatment to overcome the recalcitrance of lignocel-
lulose (SPORL) (Sebayang et al., 2016). More details on biomass
pretreatment procedures are reported elsewhere (Agbor et al.,
2011; Jonsson and Martin, 2016).
As shown in Fig. 2, after the pretreatment, hydrolysis breaks
down lignocellulose into the simplest sugar monomers, such as
xylose and glucose. Hydrolysis can be done chemically or with
enzymes. Through chemical hydrolysis, dilute acid is used to
convert the lignocellulose structure into fermentable sugar
(Sebayang et al., 2016). It was reported that hemicellulose could be
degraded by dilute acid to release 5-carbon monomers like xylose,
whereas cellulose, having a complex structure, requires higher
temperatures to convert into 6-carbon monomers like glucose with
dilute acid-based hydrolysis process (Balat et al., 2008). For a strong
acid (concentration more than 10%) condition, the hydrolysis could
be done at fair temperatures to have rapid degradation of cellulose
and hemicellulose (Balat et al., 2008). However, this process leads
to a higher cost due to the corrosion of instruments. In addition, this
process needs to be carried out with extreme precaution due to the
chances of health hazards (Sebayang et al., 2016). Most importantly,
acid hydrolysis produces inhibitors such as furfural that hinders
bio-ethanol formation in the fermentation process (Aftab et al.,
2019).
M.H. Rahman and P.R. Bhoi
Enzymatic hydrolysis is comparatively advantageous, as the
inhibitor formation can be avoided. The formation of syrupy sugar
helps the anaerobic fermentation process (Bhatt and Shilpa, 2014).
Enzymatic hydrolysis processes involve specific enzymes based on
the type of biomass used. Cellulase and Amylase are two enzymes
that can hydrolyze cellulose and amylose (Sebayang et al., 2016).
These enzymes can be derived from fungi and bacteria (Gusakov
et al., 2007). The cost of cellulase is high, and therefore, recycling
is required to make the process cost-effective. There are ongoing
studies for optimizing the enzymatic hydrolysis process by devel-
oping cheaper enzymes (Sebayang et al., 2016). However, the rate of
enzymatic hydrolysis can be increased 3e10 times with proper
pretreatment as stated earlier (Aftab et al., 2019).
As shown in Fig. 2, the third step is the fermentation process.
Fermentation is a biological technique to produce ethanol from
sugars such as glucose and xylose. It is commonly used to convert
the sugar into bioethanol after biomass pretreatment and hydro-
lysis processes. Fermentation can be done using various kinds of
microorganisms such as bacteria, fungi or yeast. Several saccharo-
myces cerevisiae yeasts have been extensively used for anaerobic
fermentation of C6 sugar (such as glucose). It was reported that
saccharomyces cerevisiae yeast could theoretically convert 90% of
glucose sugar to ethanol (Gabriel and El-Halwagi, 2013). However,
in practice, with higher ethanol production, the activity of saccha-
romyces cerevisiae decreases which hinders the satisfactory indus-
trial production of bio-ethanol (Tsegaye et al., 2019). Therefore,
improvised techniques, such as Separate Hydrolysis and Fermen-
tation (SHF) and Simultaneous Saccharification and Fermentation
(SSF) have been adopted (Sebayang et al., 2016). As reported by
Tsegaye er al., SSF produced 13% higher ethanol yield than SHF
(Tsegaye et al., 2019). SSF is more advantageous when cellulase is
used to break down cellulose into glucose at the hydrolysis stage
(saccharification). The released glucose acts as an inhibitor of the
cellulase enzyme. Therefore, to ferment the produced glucose into
ethanol, yeast, or other microorganisms are implemented. SSF
process provides better rates, yields and ethanol concentration at a
lower temperature than that of optimal for a respective enzyme
(Wyman and Yang, 2009). One of the limitations of sugar fermen-
tation using saccharomyces cerevisiae is that it can barely ferment
C5 sugar (such as as-xylose). Although the fermentation of pentose
sugar has been accomplished using P. stipitis, P. tannophilus and
C. shehatae yeasts, they have not been used in large scale processes
(Martin et al., 2007). Therefore the scope of research is wide open
for developing genetically-modified Saccharomyces Cerevisiae
strain that will ferment pentose sugar for bioethanol production
(Moyse s et al., 2016). Ethanol production is of interest since long
(Strawn, 1995). Typically, the reported ethanol yield is approxi-
mately 32e33% i.e. 0.33 kg of ethanol per kg of biomass (Volynets
et al., 2017). A theoretical value of glucose to ethanol conversion
is 51%, i.e., yield of 0.51 g ethanol/g glucose (Araque et al., 2008).
Other than bioethanol, chemicals such as 1,3 propanediol, iso-
butanol, succinic acid, terpenes, lactic acid, squalene are derived
commercially through the fermentation of glucose that was pre-
viously separated from the fermentable sugars (Rosales-Calderon
and Arantes, 2019). Among them, 1,3 propanediol is used to pro-
duce PTT (section 3.2.2), and lactic acid is used to produce PLA
(Section 3.2.4). On the other hand, bioethanol, produced from the
lignocellulosic biomass-derived glucose, xylose and other sugar
contents, are used to produce bioplastics, such asdbio-PE, bio-PP,
bio-PET, PLA. Alongside, castor oil is used to produce PAd11, one
of the most common polyamides. Therefore, the production route
of bio-PA from castor oil is described in Section 3.2.5. All the pro-
duction routes for these bioplastics are briefly discussed in the
following sections with flow diagrams (Fig. 3dFig. 5).
6
Journal of Cleaner Production 294 (2021) 126218
3.2.1. Bio polyethylene (Bio-PE)
A flow chart of bio-polyethylene (Bio-PE) production is shown in
Fig. 3. Ethylene was mainly produced from ethanol until the earlier
20th century, and later on, it was produced through the steam
cracking of hydrocarbons at 750e950
C. This shift happened due
to the lower price of fossil-derived oil. However, the demand of
fossil fuel based ethylene is decreased due to an adverse impact of
fossil fuel on environment. As a result, companies such as Dow,
Braskem, and Solvay started bioethanol to bio-PE production
(Isikgor and Becer, 2015). The first and most important step of bio-
PE production is the conversion of bioethanol to bio-ethylene. It is
achieved through the dehydration process using solid acid catalysts
such as alumina or silica-alumina at around 400
C (Rose and
Palkovits, 2011). The solid acid catalyst improves the selectivity of
ethylene conversion. Rose and Palkovits reported a selectivity of
99.9% in their process. The polymerization reaction is then carried
out with the ethylene monomers to produce polyethylene. In this
process, П-bond of the ethylene monomer breaks down to establish
a new bond with another similar monomer. Thus, multiple
monomers connected to each other to produce a larger polymer
chain. Hydrogen is supplied in the process to control the chain
length of the polymer. Such polymerization of ethylene requires
high pressure and temperature (Ebringerova et al., 2005). LDPE can
be produced at 1000e3000 atm and 150e300
C in the presence of
oxygen or organic peroxide initiators (Industry, 2017). However, the
process pressure can be reduced by using Ziegler-Natta organo-
metallic catalyst. This is a titanium compound with an aluminum
alkyl. It operates the process at 10e80 atm at around 70e150
C.
Ziegler-Natta is widely used in industries under the slurry process
using a continuous stirred tank reactor (Wang et al., 2018). In this
process, Ziegler-Natta granules are mixed with liquid hydrocarbon
diluents. A mixture of ethene and hydrocarbon is passed into the
slurry under pressure to polymerize ethene into HDPE. The solvent
is evaporated, and polyethylene is extracted from the process. Total
petrochemicals in collaboration with Chevron Phillips Chemical
Company is producing HDPE in a state-of-art advanced double loop
(ADL) reactor technology using the slurry process. This ADL tech-
nology can produce up to 1.1 B lbs (500 KMTA) of polyethylene per
year.
3.2.2. Bio polyethylene-terephthalate (Bio-PET)
A flow chart of the bio polyethylene-terephthalate (Bio-PET)
production is presented in Fig. 3. Initially, bioethylene is converted
into ethylene oxide through oxidation, in the presence of silver-
based catalysts (Yue et al., 2012). Then, ethylene glycol (EG) is
produced by the hydration of ethylene oxide (EO) (Yue et al., 2012).
EG is an important intermediate for bio-PET production. Usually,
around 60% of the globally produced EO is converted to EG (Isikgor
and Becer, 2015) and nearly 40% of the global EG is utilized in the
polymer industry for manufacturing polyethylene terephthalate
(PET) (Yue et al., 2012). In order to produce more than 99% EG with
negligible byproducts, Shell Global Solution has implemented
“OMEGA” technology. In this technology, EO is reacted with CO2 to
produce ethylene carbonate, which is then hydrolyzed to produce
EG and CO2 (Shell.Corporation, 2019). Then, EG is converted to
terephthalic acid through polycondensation, and in the last step,
terephthalic acid (benzene-1,4-dicarboxylic acid) is reacted with an
alcohol (ethane-1,2-diol) to produce PET monomer through dehy-
dration (Isikgor and Becer, 2015). The monomer then produces PET
at a high temperature of 260e300
C (The Essential Chemical
Industry, 2017b). During polycondensation stage, catalyst such as
antimony (III) oxide, is used when the monomer and polymer both
are molten. Finally, ethane-1,2-diol is recycled, and PET polymer is
obtained through this process.
M.H. Rahman and P.R. Bhoi Journal of Cleaner Production 294 (2021) 126218

Fig. 3. A flow chart of production of Bio-PP, Bio-PE, Bio-PTT and Bio-PET (blue represents stages of the process, green and brown represents the intermediate and end products).

3.2.3. Polytrimethylene terephthalate (Bio-PTT) from the fermentation of glucose, sourced from lignocellulosic
Bio-PTT constitutes approximately 9% of the global bioplastics biomass through pretreatment and hydrolysis. DuPont is the main
market in 2019. The process is similar to bio-PET up to the pro- producer of plant-based PTT resin.
duction of terephthalic acid. Then, to produce bio-PTT, trans-
esterification reaction is carried out with terephthalic acid and 1,3
3.2.4. Bio polypropylene (Bio-PP)
propanediol (Rosales-Calderon and Arantes, 2019). As discussed in
A flow chart of bio polypropylene (Bio-PP) production is dis-
Section 3.2, the production of 1,3 propanediol can be carried out
played in Fig. 3. It is reported that bio-based alcohol, such as bio-
7
M.H. Rahman and P.R. Bhoi
ethanol, has a significant potential to be one of the key in-
termediates in bio-PP synthesis (Mathers, 2012). In order to pro-
duce bio-PP, first, bioethanol is converted to ethylene through
dehydration using silica/alumina or alumina catalyst. Further,
ethylene is converted to 1-butene through dimerization (Isikgor
and Becer, 2015). In this step, ethylene is passed over a zeolite
catalyst, impregnated with transition metal complexes such as
rhodium or titanium. The 1-butane is then mixed with ethylene,
heated and passed over the solid catalyst, based on organo-
ruthenium (II) (the Grubbs’ catalysts), molybdenum (IV) or tung-
sten (IV) compounds (the Schrock catalysts) using a fixed bed
reactor to produce propylene (The Essential Chemical Industry,
2017a). Propylene can also be obtained in another way through a
metathesis reaction. For that, 1-butene is isomerized to 2-butene,
which then reacts with ethene to form propene through metathesis
reaction. Then, polypropylene is produced through the polymeri-
zation reaction of propylene in the bulk process using the Ziegler-
Natta catalyst. These catalysts are formed by the interaction of ti-
tanium (IV) chloride and aluminum alkyl, such as triethyl
aluminum. Unlike polyethylene, this process does not need an
organic solvent. The temperature required is around 70e90
C and
pressure of 30e40 atm (The Essential Chemical Industry, 2017a).
According to market report (2019), bio-PP took less than 1% of the
bioplastic market. However, numerous investigations are going on
with bio-PP production because fossil based polypropylene (PP) is
the second most demanded product in the petrochemical industry
(Yao and Tang, 2013).
3.2.5. Bio-polyamide (Bio-PA)
Bio-polyamide (Bio-PA) is another type of bioplastic which is
also known as bio-nylon. It consists of around 12% of the global
bioplastic market in 2019. Polyamide has multiple structural
formulae, each of which has a separate method of production. Each
method constitutes the synthesis of amide monomer from sources
like castor oil or biomass. The amide monomer then goes through
the polymerization process to produce desired polyamides. Based
on the reaction mechanism, PA can be produced through several
routes. In this section, a brief description of widely used bio-PA 11
production from castor oil is reported with a flow diagram.
In this method, castor oil is hydrolyzed to produce Ricinoleic
acid (Fig. 5). Methyl ricinoleate ester is produced from the catalysis
reaction of Ricinoleic acid using methanol. Then, high-temperature
treatment of Methyl ester of Ricinoleic acid provides 11-
undecanelic acid. Bromine peroxide converts it to 11-
bromoundecanoic acid, which further reacts with ammonia to
produce the 11-aminoindecanoic acid, the monomer for producing
PA11 (Gotro, 2013).
The other bio-polyamides are PA5,10; PA6; PA6,6 and PA12
(Bioplastic News, 2016). It is reported that, bio-nylon PA 5,10 can
be produced from edible glucose feedstock through metabolic
engineering of Corynebacterium glutamicum, which initially cre-
ates a diaminopentane (polymer building block) and was fol-
lowed by an integration of biological and chemical approaches
afterward to produce bio-PA (Kawaguchi et al., 2016). In the
recent years, such bio-based PA’s have been used in bioplastics
such as Terryl® (of Cathay Industrial Biotech, Shanghai, China),
Zytel® (of DuPont, Wilmington, Delaware), EcoPaXX® (of DSM)
for manufacturing automotive parts for Ferrari and Mercedes
Benz (Chung et al., 2015). Bio-PA has gained much attention due
to their advantageous physical and chemical properties. They
exhibit higher thermal stability than the other plastics. Their
glass transition temperature is 110
C. Besides, bio-PA offers
properties like impact resistance, abrasion resistance as well as
chemical resistance.
8
Journal of Cleaner Production 294 (2021) 126218
3.3. Compostable bioplastics: bio polylactic acid (Bio-PLA)
Polylactic acid (PLA) is included in this review as a reference of
compostable bioplastics. PLA consists of 13% of the bioplastic
market (Fig. 1) in 2019. Its market volume is projected to exceed
3,47,000 tons by 2023 (Bioplastics, 2016). The demand of PLA is
continuously increasing with its vast application in the 3D printing
industry, besides its existing market at food packaging (Arrieta
et al., 2017; Pei et al., 2015). As discussed in Section 2.2, lactic
acid is produced from the fermentation of sugar. In the polymer
industry, Polylactic acid (PLA) is produced from the lactic acid
monomer basically using two routes. It can be done either by the
well-known polycondensation (DP) route or through the ring-
opening polymerization (ROP) route (Sin et al., 2013). Lactic acid
can be formed through the fermentation of glucose and sucrose by
genetically modified lactic acid bacteria (Isikgor and Becer, 2015).
Lactic acid (LA) is converted to Polylactic acid through poly-
condensation. In this process, Poly-L-lactic acid of high molecular
weight can be produced if condensed water is efficiently removed
from the system without allowing the L-lactide monomer to be
evaporated in equilibrium (Jime nez et al., 2015). The useful condi-
tion for water removal was reported as: 180e200
C temperature,
low pressure of 5 torrs, and a long reaction time with catalyst and
azeotropic solvent (Jime nez et al., 2015). Poly-L-lactide, converted
from the polymerization of L-lactide, exhibits high crystallinity
(37%), its glass transition temperature is between 60 and 65
C, and
a melting temperature is around 175
C (Isikgor and Becer, 2015). In
the second route, Polylactic acid (PLA) is obtained using Ring-
Opening Polymerization (ROP) (Jime nez et al., 2015). Metal cata-
lysts such as Al, Mg, Zn, Ca, Sm, Fe, Lu, Ti, Zr, cationic catalysts (using
strong acids), organic catalysts (4-(dimethylaminopyridine)
(DMAP) and 4-pyrrolidino-pyridines (PPY)) have been used in ring-
opening polymerization reaction (Jime nez et al., 2015). Demand for
metal-free organic catalyst is increasing for the application of PLA
in medical and micro-electronics and research is underway to
optimize the process (Jime nez et al., 2015).
The commercial production of PLA from corn and other raw
materials has been reported. Hitachida leader in the PLA market-
dis producing PLA from lactic acid through both condensation and
ROP. In their process, L-Lactic acid is converted into lactide through
polycondensation. In a second route, Hitachi uses a direct poly-
merization of L- Lactic Acid to produce PLA (Hitachi, 2019).
3.4. Characterization
Ultimate and proximate analyses are important to understand
the chemical constituents, type, and potential of plastics as a
thermochemical conversion (TCC) feedstock (Ouedraogo, 2020).
Ultimate and proximate analyses of plastics are presented in
Table 1. For TCC, biomass has been investigated extensively as a
feedstock (Bhoi et al., 2020). For example, pine biomass has been
successfully used for energy recovery through pyrolysis and gasi-
fication (Gao et al., 2008). Based on the availability of Pine biomass
in Georgia, ultimate and proximate analyses of pine biomass is
added in Table- 1 for comparison. The ultimate or proximate
analysis of bio-PTT or fossil-based PTT is not observed in the liter-
ature, therefore PTT is not included in Table 1. However, the other
five types of bioplastics, which represents around 48% of the cur-
rent market, are discussed based on ultimate and proximate ana-
lyses. Comparative insights about common bioplastics as a
feedstock for the thermochemical conversion processes are dis-
cussed based on ultimate and proximate analyses.
3.4.1. Ultimate analysis
From the ultimate analysis, it is obvious that the carbon content
M.H. Rahman and P.R. Bhoi
Fig. 4. Production route of bio-Polyamide: PA,11 (blue represents stages of the process and green represents products).
is abundant in the considered plastics. As shown in Table 1, PE and
PP possessed the highest carbon content in the range of 82e85%. PA
and PLA have a relatively lower carbon constituent (63 and 50%,
respectively) which is higher than that of pine sawdust biomass
(46.12%). Besides, the hydrogen content is the maximum in PE
(12e15%) and PP (14e15%), significant in PA (8e10%), and relatively
lower in PET (4.2%) and PLA (5.6%). In comparison, the percentage
of hydrogen in pine sawdust is about 6.23%, which is close to some
of the plastics such as PLA and PET and lower than PE, PP, and PA.
On the other hand, the oxygen content is very high in PLA
(30e44%), PET (32e33%), PA (15e26%), and none in PE and PP.
Comparatively, the oxygen content in pine sawdust is higher
(45.46%). Therefore, like pine biomass, bio-based non-biodegrad-
able bioplastics should exhibit some interesting chemical yield
from catalytic pyrolysis (Rahman, 2020). Bio-PE, having no oxygen
content, could be the best candidate for hydrocarbon fuel produc-
tion through catalytic pyrolysis. Similarly, bio-PP is also a good
9
Journal of Cleaner Production 294 (2021) 126218
candidate for the pyrolysis process. On the other hand, PLA, bio-
PET, and bio-PA are less favorable for pyrolysis, considering sig-
nificant oxygen content that will lead to undesired compounds
which negatively impact the pyrolytic oil properties. Instead,
gasification could be a more suitable option to utilize the oxygen-
rich PLA, PET, and PA bioplastics (Santos et al., 2010). However,
some studies were reported on the co-pyrolysis of biomass and PLA
and some investigated PET pyrolysis. The results regarding PA py-
rolysis was barely observed. However, some mixed plastics pyrol-
ysis investigations have been carried out, which showed the
potential aspects to recover useful chemicals from the used plastics
mixtures (Lopez et al., 2010; Sikdar et al., 2020; Syamsiro et al.,
2014).
3.4.2. Proximate analysis
In the proximate analysis, volatile, fixed carbon, moisture, and
ash contents are analyzed. It is known that high volatile content in
M.H. Rahman and P.R. Bhoi Journal of Cleaner Production 294 (2021) 126218

Fig. 5. Bio-PLA production from Lactic Acid (blue represents stages of the process and green represents the products).

Table 1
Ultimate and proximate analysis of plastics and biomass.

Plastics and biomass Basis Ultimate Analysis Proximate Analysis Ref.

%C %H %O %N %S Basis % Fixed Carbon % Moisture % Volatile % Ash

PET Daf 62.93 4.26 32.64 0.04 0.13 Dm 9.47 e 90.44 0.09 Zhou et al. (2014)
e 62.26 4.06 33.69 0.00 0.00 e 5.60 e 94.09 0.31 Zhang et al. (2012)
Dm 62.00 5.20 32.80 e e e e e e 0.12 Lian et al. (2011)
Avg. 62.39 4.50 33.04 0.02 0.06 7.54 e 92.26 0.17

PA Dm 55.38 8.65 26.03 0.95 e Dm 0.69 3.22r 99.78 0.00 Othman et al. (2008)
Dm 62.70 9.70 16.63 10.67 0.00 Dm 0.20 1.10 98.40 0.30 Panagiotis Vounatsos (2012)
Avg. 59.04 9.18 21.33 5.81 0.00 0.45 2.16 99.09 0.15

PLA Dm 49.84 5.63 44.42 0.15 e Dm 1.30 0.00 98.05 0.65 Cornelissen et al. (2008)
Ad 49.86 5.55 44.33 0.26 e Dm 0.53 0.00 98.92 0.55 Gang and Aimin (2008)
e 61.31 8.57 30.12 0.01 0.0005 e e 1.60 95.60 2.80 Miskolczi (2013)
Avg. 53.67 6.58 39.62 0.14 0.0005 0.92 0.53 97.52 1.33

PE Dm 85.81 13.86 0.00 0.12 0.06 Dm 0.00 0.02 99.85 0.15 He et al. (2009)
Ad 85.83 14.38 0.00 0.16 0.07 Ad 0.00 0.02 99.83 0.15 Zheng et al. (2009)
e 75.56 11.98 0.00 0.10 0.10 e 0.00 0.57 92.37 7.05 Faizal et al. (2016)
Avg. 82.4 13.41 0.00 0.13 0.08 0.00 0.20 97.35 2.45

PP Dm 77.54 14.22 7.46 0.10 e Dm 0.00 0.22r 99.44 0.67 Othman et al. (2008)
Daf 83.75 13.98 2.27 0.00 0.00 Dm 0.00 e 99.18 0.82 Zhou et al. (2014)
Daf 84.62 15.23 0.00 0.14 0.01 Dm 0.13 e 99.79 0.08 Zhou et al. (2014)
Avg. 81.97 14.48 3.24 0.08 0.01 0.04 99.47 0.52

Pine sawdust Daf 44.75 6.31 47.21 1.68 0.05 e 18.88 3.93 76.85 0.34 Gao et al. (2008)
e 48.71 5.99 44.2 2.39 0.28 Dm 18.60 18.84 81.03 0.37 Chaula et al. (2014)
Ad 44.90 6.38 44.98 3.74 18.33 Ad 16.28 1.44 80.78 1.50 Zeng et al. (2016)
Avg. 46.12 6.23 45.46 2.60 6.22 17.92 8.07 79.55 0.74

*r for wt % residual content Daf-Dry Ash Free basis Dm-Dry Mass basis Ad-Air Dried.

biomass provides a higher quantity of bio-oil and syngas (Jahirul
et al., 2012). Table 1 shows that plastics have more than 90% of
volatile content, which is, therefore, favorable for the pyrolysis
process. Typically, the fixed carbon governs the production of bio-
char in the pyrolysis process. In Table 1, only PET has around 7.54%
fixed carbon, which is even lower than that of pine biomass
(17.92%). Therefore, alike biomass, PET can also be utilized under
gasification. However, investigations have been carried out to uti-
lize PET under both the pyrolysis and gasification processes
(Artetxe et al., 2010; Lee et al., 2014; Lopez et al., 2012). HDPE, on
the other hand, is hydrophobic and barely contains moisture.
Moreover, the volatile content is high, and the fixed carbon is low.
These properties favor the pyrolysis process, and therefore, several
10
investigations have been carried out using HDPE as a feedstock in
pyrolysis and co-pyrolysis processes (Rahman, 2020). Also, HDPE
has been reported as a feedstock for gasification and co-gasification
to derive hydrogen and syngas (Arena and Di Gregorio, 2014).
Syngas is an important precursor for the Fischer-Tropsch synthesis
process. It can be concluded that bio-PE and bio-PP have enormous
potential to exhibit similar yield. Utilization of bioplastics for fuels
and chemicals production would help to minimize bioplastic waste
while enforcing a circular loop in the biobased plastic economy.
4. Cost and properties of bioplastics
Properties and costs of the abovementioned plastics are
M.H. Rahman and P.R. Bhoi Journal of Cleaner Production 294 (2021) 126218

provided in Table 2. These prices reflect the current price per ki-
logram of plastics available in the online marketplace. They may
differ depending on the time and location. Also, the quantity of
purchase can affect the pricing. From Table 2, it is lucid that the
biobased non-biodegradable plastics are expensive than the con-
ventional plastics with similar mechanical properties. For example,
the price of 1 kg of bio-PE is approximately 30% higher than con-
ventional PE, whereas their chemical and mechanical properties
are identical (Siracusa and Blanco, 2020). However, there are some
novel soy-protein-based biopolymers in the research phase that
can offer improved mechanical properties similar to that of PE at a
cheaper cost (Jime nez-Rosado et al., 2020). Although the prices are
high, non-biodegradable bioplastics are advantageous from envi-
ronment point of view, as they are produced from biomass. They
will reduce the carbon footprint and will develop a positive impact
on our environment, provided that their waste is not mishandled
like traditional plastics (Lamberti et al., 2020). A similar assumption
is applicable for compostable plastics as well.

Table 2
Price, properties and comparisons between bioplastics and traditional counter plastics.

Plastic Price  Properties Comparison References

type ($/kg)

PE 1e1.2  Specific gravity: Bio-PE is sourced from bio-ethanol and helps to reduce carbon footprint. Bio-PE holds similar properties Akay (2012)
Bio-PE 1.3 0.91e0.96 as conventional PE.
e1.8  Young’s modulus,
GPa: 0.2e1.4
 Yield strength, MPa:
0.2 MPa-1.4
 Tensile strength,
MPa: 8-35
 Flexible
 waterproof
PP 1e16  Specific gravity: 0.9 Currently, bio-PP is costlier than conventional PP. However, bio-PP is less than 1% of the current Akay (2012)
Bio-PP ~20 e0.95 bioplastic market. Therefore, a large production of PP will reduce the price in the future.
 Young’s modulus,
GPa: 1.1e1.55
 Yield strength, MPa:
25-38
 Tensile strength,
MPa: 21-43
 Good fatigue
resistance
PET 0.4  Specific gravity: Both PET and bio-PET are recyclable. The cost of recycled products is less than that of virgin PET. As of Akay (2012)
e2.2 1.33e1.48 now, Bio-PET is more expensive than the conventional PET.
Bio- 2.4  Young’s modulus,
PET e3.2 GPa: 2.25e4.14
 Yield strength, MPa:
50 - 59
 Tensile strength,
MPa: 47-72
 Recyclable (1)
 Flexible
 waterproof
PTT e  Specific gravity: Bio-PTT esters have three methyl groups attached to it which is similar to that of conventional PTT. (Chan et al., 2014;
Bio- e 1.35 Therefore, they share similar properties. Supaphol et al., 2004)
PTT  Young’s modulus,
GPa: 2.2
 Tensile strength,
MPa: 58.3
 Flexible
 waterproof
PA 1e3  Specific gravity: The price of bio-PA is more than the conventional PA. However, since they are sourced from biomass, Akay (2012)
Bio-PA e 1.07e1.24 they reduce carbon footprint.
 Young’s modulus,
GPa: 1.4e3.8
 Yield strength, Mpa:
55 - 85
 Tensile strength,
MPa: 70-95
 Good abrasion and
wear resistance
 Good processability
 Good insulation
properties
PLA 4e20  Specific gravity: PLA is a compostable plastic. The challenge of the ongoing R&D is to minimize the cost below $1/kg. The Farah et al. (2016).
1.27 mechanical properties are suitable for biomedical applications
 Young’s modulus,
GPa: 1.28
 Yield strength, MPa:
70
 Tensile strength,
MPa: 59

11
M.H. Rahman and P.R. Bhoi
5. Challenges and opportunities of bioplastics under circular
economy
One of the major challenges of plastic and bioplastic wastes
utilization for energy and fuel recovery is the preparation of the
feedstock because the collection and separation of waste bioplastic
are challenging. Automatic machines such as near-infrared spec-
troscopy have been used for sorting plastic wastes, but they are not
popular due to the cost and technical difficulties (Rujnic-Sokele and
Pilipovic, 2017). Therefore, a proper policy for wastes collection,
handling, and management is needed for enhancing the utilization
of waste plastics by either recycling, reusing or reducing through
conversion technologies such as gasification and pyrolysis pro-
cesses (Barker and Safford, 2009). Nowadays, the focus is on the
upcycling the mixed discarded plastics waste for valuable fuels and
chemicals production.
Bioplastics such as bio-PE, bio-PP, bio-PET, bio-PA inherent
similar chemical compositions of traditional plastics (Table 1).
Parallelly, their waste is as harmful as traditional plastics’ in the
landfills. Therefore, laboratory-based alternative waste utilization
techniques such as pyrolysis and gasification should be carried out
and must be optimized for industrial scale. Besides, a proper
awareness needs to be created regarding the adverse environ-
mental impacts of the bioplastic wastes because the existing hype
in favor of bioplastics is passively influencing consumers to dump
bioplastic products in undesired places rather than designated
dumpsites. Even from the dumpsites, the bioplastics can travel
towards landfill or incineration plants breaching the transportation
chain. Landfill accumulation of waste plastic is a major environ-
mental issue and therefore, many companies such as Google,
Microsoft, Subaru, Sierra Nevada have moved towards Zero Waste
to Landfill (ZWTL) certification.
Moreover, incineration of plastic wastes produces dioxin which
is hazardous for the environment as well as for human health
(Shibamoto et al., 2007). Therefore, fuels and chemicals such as
gasoline, diesel, jet fuel, and BTX, using pyrolysis process or
hydrogen and syngas production through the gasification route
could be an effective solution to minimize the bioplastic wastes. In
addition, rigorous research and experimentation should be carried
out to develop an effective and low-cost catalysts (Kunwar et al.,
2016). This will also help to establish the circular loop in the plas-
tic economy.
The circular economy was initially proposed in the later nine-
teenth century. It is described as a closed-looped system to recreate
the maximum possible value from the end product wastes. Ac-
cording to Yuan et al. (2006), “the core of the Circular Economy is
the circular (closed) flow of materials and the use of raw materials
and energy through multiple phases.” Plastic holds a major interest
in the circular economy due to its extensive usage and consequent
waste accumulation. It was reported that Austria could recover
26 ± 7% of its total waste stream as re-granulated and recovered
40 ± 3% in waste to energy plants (Van Eygen et al., 2018). A similar
trend is observed in many countries in Europe, based on the fact of
fossil fuel depletion and the necessity of waste plastic utilization.
A life cycle of traditional plastic and bioplastics under circular
economy has been depicted in Fig. 6. Plastic and bioplastic are
generally differentiated based on their sources of production or
biodegradability. Both biomass and fossil resources can be used to
produce certain bioplastics such as bio-PE, bio-PP, bio-PET, bio-PA
(Block 1). In recent times, scientists are investigating cheaper
sources to make the other bioplastics (Perez-Puyana et al., 2018).
Some novel bioplastics have been resourced from soy protein
(Perez-Puyana et al., 2018). Also, plasma protein-based green
superabsorbent materials were produced with improved mechan-

ical properties (Alvarez-Castillo et al., 2019). Similarly, shrimp shell
12
Journal of Cleaner Production 294 (2021) 126218
has been used to produce chitosan-based eco-friendly biopolymers
(Mujtaba et al., 2019). Many research expeditions are currently
going on worldwide, and newer bioplastics are coming to the
market to replace fossil-derived plastics. In general, all bioplastics
will be disposed to the dumpsite after usage. Then, these plastics
will be sorted and sent to the composting or recycling facilities. The
remaining wastes are usually accumulated in landfills or inciner-
ated for energy recovery (block 2).
It is observed that most of the plastic wastes go to the landfill
and remain unattended. Bioplastics, with its misconceptions, may
accelerate this problem in the near future. Therefore, instead of
letting them articulate in the existing system, bioplastic wastes
could be considered as a feedstock for pyrolysis and gasification
(block 3). As discussed, several companies such as Choren, TRI,
Syntroleum are working on thermochemical conversion technolo-
gies such as gasification to produce jet fuel, while Envergent (UOP/
Ensys), Dynamotive, KiOR, RTI, GTI are working on the pyrolysis
process for fuel production (Milbrandt et al., 2013). Similar energy
recovery techniques have a scope for investigation for both non-
biodegradable as well as biodegradable bioplastics (Niaounakis,
2013). In 2020, Lambetti et al. (Lamberti et al., 2020) emphasized
that no additional accessory is needed to treat recyclable bioplastics
such as bio-PE in the same equipment where PE can be treated.
Therefore, bioplastic waste should be carefully utilized and not left
unattended. The utilization of recyclable bioplastic waste will help
in minimizing carbon footprint (Lamberti et al., 2020). Overall, the
conversion of PE, PP, PET shows significant prospects to produce
transportation fuel and syngas. These fuels and chemicals will be
converted to CO2 after its utilization, which will be further restored
in plants to preserve the global carbon cycle. This process will help
to close the loop of the circular bio-based plastic economy.
6. Conclusions
Plastic pollution and fossil fuel depletion are the two major
challenges of the globe. Though bioplastics have positive impacts
on reducing greenhouse gases (GHGs) emissions and improving the
economy by conserving fossil fuel resources, the biodegradability of
bio-based plastics at different environmental conditions is still
ambiguous. Moreover, at present, the majority of the recyclable
plastics are not going to the recycling facilities. The same is pre-
dicted for the bioplastics as well. Statistically, 79% of the total waste
plastics is directed towards the landfill, which accelerated the
problems like marine litters and microplastic pollution. Besides, the
incineration of plastics waste is producing dioxins that have
detrimental impacts on the environment and human health.
Therefore, transportation fuel such as gasoline and diesel recovery
through pyrolysis from waste bioplastics has gained attention. The
energy recovery options such as hydrogen and syngas production
through gasification processes is another potential solution to uti-
lize waste bioplastics. These conversions will help to establish new
industries with employment and truly enforce the circular econ-
omy. In this circular chain, biomass is an important resource for
producing bio-based ethanol. Bioethanol is the key intermediate for
the major bioplastics. The overview of the production of bioplastics
involves the pretreatment process, which can be a mechanical,
chemical, or biological process. Then, the hydrolysis process pro-
duces fermentable sugar (C5 and C6). In the next step, fermentation
is carried out using microorganisms that convert the sugars into
ethanol. Then, the polymerization is done in the bulk process to
produce bio-HDPE, bio-LDPE, bio-PP using the Ziegler-Natta cata-
lyst. For PLA, the process involves the production of lactic acid from
the fermentable sugar. Then, LA is converted into lactide using
condensation, which is transformed into PLA using polymerization.
The LA can also be converted into PLA using the direct
M.H. Rahman and P.R. Bhoi
Fig. 6. Role of bioplastics in the circular economy to reduce fossil fuel consumption.
polymerization process. Bio-PA, on the other hand, can be produced
from a series of chemical modifications involving hydrolysis,
catalysis, and other reactions from castor oil. For the characteriza-
tion, the ultimate and proximate analyses were analyzed in this
review. Based on the ultimate analysis, bio-polyethylene and bio-
polypropylene consist primarily of carbon and hydrogen. Overall,
bio-PE and bio-PP are the best candidates for producing gasoline
and diesel range fuels through pyrolysis. On the other hand, Bio-
PET, bio-PA, and PLA have oxygen contents of approximately 33%,
21.2%, and 40%, respectively. Therefore, PLA, bio-PET, and bio-PA are
recommended for the gasification process. In addition, co-pyrolysis
and co-gasification are also potential routes for utilizing bioplastics
waste to extract energy in the form of either hydrogen or syngas.
Syngas is an intermediate for several chemicals and fuels
production.
Declaration of competing interest
The authors declare that they have no known competing
financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
13
Journal of Cleaner Production 294 (2021) 126218
Acknowledgment
We greatly acknowledge the funding and the facilities provided
by the Mechanical Engineering Department at Allen E. Paulson
College of Engineering and Computing at Georgia Southern Uni-
versity, Statesboro, Georgia, USA.
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