polymers

Review
A Review on Properties and Application of Bio-Based
Poly(Butylene Succinate)
S. Ayu Rafiqah 1 , Abdan Khalina 1, *, Ahmad Saffian Harmaen 1 , Intan Amin Tawakkal 2 , Khairul Zaman 3 ,
M. Asim 1, *, M.N. Nurrazi 4 and Ching Hao Lee 1, *

1 Laboratory of Biocomposite Technology, Institute of Tropical Forestry and Tropical Products,

Universiti Putra Malaysia, Selangor 43400, Malaysia; [email protected] (S.A.R.);
[email protected] (A.S.H.)
2 Engineering Faculty, Universiti Putra Malaysia, Serdang 43400, Malaysia; [email protected]
3 Polycomposite Sdn Bhd, 75-2 Jalan TKS 1, Taman Kajang Sentral, Kajang 43000, Malaysia;
[email protected]
4 Center for Defence Foundation Studies, National Defence University of Malaysia, Kem Sungai Besi,
Kuala Lumpur 57000, Malaysia; [email protected]
* Correspondence: [email protected] (A.K.); [email protected] (M.A.);
[email protected] (C.H.L.)

Abstract: Researchers and companies have increasingly been drawn to biodegradable polymers
and composites because of their environmental resilience, eco-friendliness, and suitability for a
range of applications. For various uses, biodegradable fabrics use biodegradable polymers or
natural fibers as reinforcement. Many approaches have been taken to achieve better compatibility
for tailored and improved material properties. In this article, PBS (polybutylene succinate) was





 chosen as the main topic due to its excellent properties and intensive interest among industrial
and researchers. PBS is an environmentally safe biopolymer that has some special properties,
Citation: Rafiqah, S.A.; Khalina, A.;
such as good clarity and processability, a shiny look, and flexibility, but it also has some drawbacks,
Harmaen, A.S.; Tawakkal, I.A.;
Zaman, K.; Asim, M.; Nurrazi, M.N.;
such as brittleness. PBS-based natural fiber composites are completely biodegradable and have
Lee, C.H. A Review on Properties and strong physical properties. Several research studies on PBS-based composites have been published,
Application of Bio-Based including physical, mechanical, and thermal assessments of the properties and its ability to replace
Poly(Butylene Succinate). Polymers petroleum-based materials, but no systematic analysis of up-to-date research evidence is currently
2021, 13, 1436. https://doi.org/ available in the literature. The aim of this analysis is to highlight recent developments in PBS research
10.3390/polym13091436 and production, as well as its natural fiber composites. The current research efforts focus on the
synthesis, copolymers and biodegradability for its properties, trends, challenges and prospects in the
Academic Editor: Dilip Depan field of PBS and its composites also reviewed in this paper.

Received: 28 February 2021

Keywords: poly butylene succinate; copolymers; biodegradability; mechanical; physical properties
Accepted: 7 April 2021
Published: 29 April 2021

Publisher’s Note: MDPI stays neutral

1. Introduction
with regard to jurisdictional claims in
published maps and institutional affil- The expansion of industry produced not only many products for human activities
iations. but also a large amount of plastic waste to the environment, because used products are
discharged after human activities. Plastics are polymers that are chemically synthesized
from petroleum products that contain long chains of monomer. The plastics industry
has been around for 60–70 years. Plastics have excellent properties in terms of flexibility,
Copyright: © 2021 by the authors.
longevity, light weight, and low cost [1]. Plastic was invented in the 1860s, but it was
Licensee MDPI, Basel, Switzerland.
not until the 1920s that it was produced for commercial use. In the 1940s, its production
This article is an open access article
exploded, making it one of the world’s fastest-growing industries. Plastics expanded at an
distributed under the terms and annual rate of 8.7% on average from 1950 to 2012, from 1.7 million tons to nearly 300 million
conditions of the Creative Commons tons today. In 2015, the world plastic increased to 8.3 billion tons and produced up to 76%
Attribution (CC BY) license (https:// plastic waste [2,3]. In 2018, it was showed that the annual growth rate of 8.4% of plastic
creativecommons.org/licenses/by/ production was about 360 million tons. It is estimated to reach 500 million tons in 2025.
4.0/). From this total production, 60% entered the environment as plastic waste [4].

Polymers 2021, 13, 1436. https://doi.org/10.3390/polym13091436 https://www.mdpi.com/journal/polymers

Polymers 2021, 13, 1436 2 of 28

Recent data revealed that the increased use of plastic materials in domestic and in-
dustrial sectors have exceeded their global production by up to 400 Mt/year, which poses
serious concerns, mainly for their disposal, environmental contamination, toxicity to the
ecosystem and human health [5]. Synthetic plastics produced a large fraction of submerged
waste in the natural habitat and are considered as emerging pollutants with a significant
impact on the environment owing to their large concentration, widespread distribution,
and non-biodegradable property. There is significant evidence of plastic pollution in the
aquatic ecosystem, including plastic islands and micro plastics [6]. Polymer has begun
to replace advanced materials in recent years due to its superior properties. However,
disposable materials account for more than a third of plastics production, resulting in
waste and leading to plastic emissions [7]. The use of non-biodegradable polyethylene (PE)
mulch films in greenery fields or soil has created serious problems in Southeast Asia [8].
Non-biodegradable polymers, i.e., polyethylene (PE), polypropylene (PP), ethylene vinyl
alcohol, poly(ethylene terephthalate), polystyrene, expanded polystyrene, polyamides,
polyurethane, and poly(vinyl chloride), have dominated in the packaging application
because of their good physical and mechanical properties The disposal of synthetic plas-
tics makes an additional contribution to the carbon dioxide emissions in the atmosphere,
which contributes to global warming. The most obvious form of pollution associated with
plastic packaging is waste plastic sent to landfills. Plastics are very durable and therefore
remain in the atmosphere for a long time after they have been discarded, particularly if
they are sheltered from direct sunlight by being buried in landfills [9]. In response to these
problems associated with plastic waste, this article used PBS as the main biodegradable
polymer to be discussed, due to the fact that there is rarely research on these materials for
commercial application. The melting point for PBS is 115 ◦ C, which is lower compared with
polylactic acid (PLA). These properties could save on industrial processing as it takes a
shorter time to melt and blends with other material. PBS is also easy to process and handle
while mixing it with other materials. In terms of brittleness, PBS is more rigid but slightly
brittle due to the fact that it is produced from petroleum-based materials. PBS also has
good thermal stability and excellent mechanical properties [10]. Other bio plastic such as
polyhydroxyalkanoates (PHAs) and polyhydroxybutyrate (PHB) also possess great prop-
erties. This bio plastic production contributes to between 25% to 30% of the total plastics
market worldwide [11]. The biodegradability of PBS is an attractive attribute for single-use
food packaging since it is able to degrade at high rates over short periods of time and has
also been listed as being certified as compostable according to the Biodegradable Products
Institute, and is available in direct food contact grades [12]. In 2003, Mitsubishi Chemicals
built a 3000 tons/year capacity plant and launched to the market a PBS named GS Pla
(Green and Sustainable Plastic). This polymer has high molar masses without the use of a
chain extender. Since then, several PBS producers such as Hexing Chemical (Anhui, China),
Xinfu Pharmaceutical (Hangzhou, China) or IRe Chemical (South Korea) appeared on the
market. In 2010, Hexing Chemical became China’s first large-scale PBS enterprise, with the
annual capacity of 10,000 tons. The same year, Xinfu Pharmaceutical announced the con-
struction of the world’s largest continuous PBS production line, with an annual capacity of
20,000 tons [13]. Figure 1 shows increasing trends of bio-based polymer production in the
year 2011 to 2020.
Mulching films occupy more than 8000 km2 of agricultural land, resulting in many
negative effects but still preserving horticulture [15]. As a result of increased understanding
of environmental contamination, people have been searching for polymers that can replace
petroleum-based plastics [16]. As a result, biodegradable plastics have been produced to
substitute non-biodegradable plastic in order to resolve the environmental problem [17].
The production of bio-plastic has made a major contribution to the mitigation of global
warming [18]. The initiative to develop new biodegradable polymers has been made using
renewable resources as the raw material. This is due to the rapid depletion of fossil fuels
and the vast amount of non-biodegradable plastics in use. Green polymers, in particu-
lar, are an important alternative as a new eco-friendly material for growing the plastic
Polymers 2021, 13, 1436 3 of 28

waste material that is accumulated every day on Earth [16]. The growing market for
biodegradable polymers such as polylactic acid, cellulose-based thermoplastics, and other
polysaccharide-based plastics aids in the reduction of pollution [17,19]. Biopolymer prices
are rising every year. Business Communication Company (BCC) published a research
report in 2014, estimating global bio plastic demand at more than 1400 kt (metric kilo
tonnes). Nonetheless, it is estimated that demand will increase to around 6000 kt in 2019.
Due to increased demand, global production is projected to hit more than 7.8 million
tons in 2019 [19]. Many biodegradable polymers have recently been launched. These in-
clude polysaccharide polymers (cellulose, chitosan, chitin, and starch), protein-based
polymers (gluten, ovalbumin, soy protein, casein, and others), and bacterial polymers such
as poly(3-hydroxybutyrate) or (3-hydroxybutyrate-co-3-hydroxyvalerate) [20]. Biodegrad-
able polymers have a lot of promise in biomedical and environmental applications. As a
result, fundamental science and technology have centered on it. Poly(butylene succinate)
or PBS has greater biodegradability, thermal properties, melt processability, and chemical
resistance than other aliphatic polyesters. With these properties, it is a promising plastic
material in the industry. Injection molded items, fibers, and films have all been made from
it [21–23].

Figure 1. Bio-based polymers production capacities from 2011 to 2020 [14]. PLA: polylactic acid;
PHA: polyhydroxyalkanoate; PA: polyamide; PBAT: poly(butylene-adipate-co-terephthalate); PBS:
poly(butylene succinate); PET: polyethylene terephthalate; CA: Cellulose acetate; PU: polyurethane.
Adapted with permission from Aeschelmann and Carus (2015).

Since the price of PBS is expensive, many researchers have used other materials to
substitute a partial percentage of PBS, such as using natural fibers. Oil palm fiber and
tapioca starch are used as reinforcing materials to minimize the amount of PBS used
and the cost of production in PBS-based products. Reinforcement products also assist
in improving the material’s strength. Furthermore, the combination of biodegradable
Polymers 2021, 13, 1436 4 of 28

polymers reduces the total cost of the material while also changing the desired properties
and degradation rates. In terms of the matter, as opposed to the copolymerization process
with biodegradable polymer blending, the latter was found to be a much simpler and faster
method of achieving the desired properties [24]. PBS brittleness can be strengthened via
the copolymerization process. The presence of a compatibilizer or additive will increase
the miscibility of a blend composite, which increases impact strength. The use of urethane
composite as a compatibilizer is an example [25]. Meanwhile, natural fibers such as oil
palm, flax, and jute can be combined to create a biodegradable composite that is both
environmentally sustainable and recyclable. In addition, natural fibers involve the use of a
compatibilizer or reinforcement to cross link the community, resulting in good properties
for potential use [26].
However, some of its drawbacks, such as slow crystallization rate, low melt viscosity,
and softness, have limited its processing capabilities and applications, especially in injection
molding. PBS strength properties deteriorate due to a rapid crystallization reaction when
combined with other materials [27,28]. The rheological properties of PBS have a major effect
on its processability. Its viscosity will decrease as the sheer rate increases. The low melt
viscosity makes PBS production more difficult. The lack of accessibility is a shortcoming
of PBS, which used to hinder its extension. To boost its properties for different purposes,
PBS must be modified and treated [29].
Thus, the objective of this contribution is to collect, analyze and compare the results
collected by research on the use of PBS concerning its copolymer, physical, mechanical prop-
erties and its applications.

2. Poly(Butylene Succinate)
Poly(butylene succinate) has seen a rise in demand in recent years as a result of its
promising sustainability and biodegradability. It was discovered that the production of bio-
based plastics was 4.2 million tons in 2016, and that it is projected to rise by 45 percent by
2021 [30]. PBS (poly(butylene succinate)) was first used in 1993 as a biodegradable polymer
and is still commonly used in industry. Mulching films, compostable bags, nonwoven
sheets and garments, catering goods, and foams are only a few of the applications [31].
PBS was also listed as a bio plastic, raising general awareness of environmental problems
caused by non-biodegradable and non-renewable plastics, as well as the rapid loss of
fossil fuel supplies. There are biodegradable polymers manufactured from petroleum-
based materials that are also known as green polymeric matrices [32]. 1,4 butanediol (BD)
is a compound that is widely present in fossil fuels and available on the market. It is
worth noting that succinic acid and BD can be derived not just from oil, but also by the
fermentation method.
Few microorganisms have been studied to generate succinic acid using biotechnologi-
cal processes in recent years, and these processes have shown good yields [33]. PBS de-
grades faster in soil than petrochemical plastic and may not be toxic to the environment.
The involvement of microorganisms such as Fusarium solani may cause it to degrade. It has
been documented that 39 bacterial strains from the Firmicutes and Proteobacteria classes
can degrade polyhydroxybutyrate (PHB), polycaprolactone (PCL), and PBS.
Plastics’ biodegradability is closely connected to their substance, and the chemical and
physical properties of plastics affect the biodegradation process. The surface conditions
of polymers play an important role in the biodegradation process, for example, surface
area, hydrophilic and hydrophobic properties [34]. However, the price of PBS is expensive
compared with petrochemical-based plastic such as polystyrene (PS), polyamides (PAs)
polyethylene terephthalate (PET) and polyethylene (PE). The price is higher due to the cost
of processing that involves electrochemical processing and the condensation of succinic
acid and 1,4 butanediol [24]. Table 1 shows several grades and properties of PBS that has
been commercially available.
Polymers 2021, 13, 1436 5 of 28

Table 1. Properties of different grades of PBS. Tm : melting temperature; Tg : glass transition temperature.

Density Tensile Tensile

PBS Grade Company MFI Tg (◦ C) Tm (◦ C) Reference
(g/cm3 ) Strength (MPa) Modulus (MPa)
Molecular Anqing Hexing
- 1.24 −44.3 109 27 - [35]
Weight 80,000 chemical co.ltd
Bionelle Showa Denko 20–34 g/10 min
1.23 59.7 114.1 - 643 [36]
1020 MD (Tokyo, Japan) (at 140 ◦ C and 2.16 kg)
Showa
Bionelle 25 g/10 min at
Highpolymer 1.26 −32 115 33.7 707 [37]
1020 MD (190 ◦ C, 2.16 kg)
(Tokyo, Japan)
PTT Public
5 g/10 min at
FZ91PM Company Limited 1.26 78 115 20 450 [17]
(190 ◦ C, 2.16 kg)
in Thailand.
HKH National
Engineering 5 g/10 min at
Bionelle 1.26 −32 114 32 30 [38]
Research Centre 150 ◦ C, 2 kg
of Plastic

2.1. Structure
PBS is a versatile semi-crystalline polymer with a semi-crystalline structure. PBS is in
high demand in sectors because of these characteristics. PBS has similar physical properties
to polyethylene terephthalate [39]. PBS has strong elongation properties and can be used in
a number of applications [40]. PBS has an ester group in its chemical structure, which de-
grades into low molecular weight polymers when exposed to water. As the temperature
rises, the rate of PBS depletion rises as well [41]. The chemical structure of the repeat unit is
–[O–(CH2 )m –O–CO–(CH2 )n –CO]N , as shown in Figure 2. The values of m and n were found
to be 4 and 2, respectively [39]. PBS has α or β crystal polymorphs. The β structure can be
found when the material is under strain [42]. However, softness and gas barrier properties
are lacking, necessitating the use of PBS blended with other materials such as fillers to
satisfy application specifications [43]. PBS provides a wide range of workability; the glass
transition temperature should be below room temperature to allow for manufacturing in a
variety of ways, including extrusion, injection molding, and thermoforming [33].

Figure 2. Chemical structure of poly butylene succinate [42]. Adapted with permission from
AKanemura et al. (2012).

2.2. Synthesis
Figure 3 shows that PBS can be synthesized in various ways such as the polyconden-
sation of succinic acid (or dimethyl succinate) and 1,4-butanediol whereby the monomers
can be obtained from fossil-based or renewable resources. The benefit of this synthesis
method is that it increases thermal and mechanical properties, as well as thermoplastic
processability [30]. The most popular method of processing petrochemical succinic acid is
the catalytic hydrogenation of maleic acid or its anhydrite.
Figure 4 illustrates how the hydrolysis of maleic anhydride to succinic acid starts.
Maleic acid is made when one of the single bonds between carbon and oxygen is destroyed.
Furthermore, by adding hydrogen, it splits the carbon–carbon double bond and completes
the reaction to produce succinic acid [44].