CHEMArts Summer School | Report

LIGNIN BIOCOMPOSITE
From classic bioplastic recipe to a potential lignin biocomposite

Nhung Pham – Master of Science in Architecture

1. INTRODUCTION

Biomaterials have gained significant attention in various fields such as product design, tex-
tiles, and interior design due to their unique properties. However, their applications in the
architecture and construction industry, particularly as exposed materials like building skins,
structures, or canopies, remain relatively limited. This is primarily due to considerations of
degradation and stability.

Throughout history, building materials were sourced from the natural environment, with
indigenous communities constructing their homes using materials such as branches, tim-
ber, rocks, and soil, mimicking the way animals build their nests. Nevertheless, the rapid
advancement of technology and the prevalence of synthetic materials in the construction
industry have shifted the focus away from natural biomaterials. Considering this context, it
becomes evident that there is a compelling need to investigate the potential of biomaterials
in earnest for architectural and construction applications.

Building upon the starting points, this study represents my initial venture into the field of
biomaterials, as I humbly strive to explore the potential of lignin composites as a viable bio-
material for building design. Lignin, a byproduct of the paper industry, serves as the primary
focus of this investigation, with a specific emphasis on examining its characteristics in rela-
tion to porosity, aesthetic surface quality, and stability performance.

2. EXPERIMENT PROCESS AND RESULTS

To begin the experimentation phase, several recipes from the CHEMArts Cookbook were
employed to assess their viability for practical application. The objective was to identify a
suitable material capable of fulfilling the desired attributes of hardness, flexibility, smooth-
ness, and waterproofness, thereby serving as a potential substitute for plastic in constructing
building facades.

Initially, the Bio-based plastic recipe from the cookbook seemed promising. However, it was
discovered that the inclusion of Cellulose diacetate powder (CDA), a key ingredient, was not
advisable. Consequently, additional research was conducted to explore alternative bio-plas-
tic recipes commonly employed by researchers such as Dunne (2018) and Bogers (2020).
Ultimately, one of these alternative recipes was chosen as the starting point for the study.

2
 AGAR AGAR - BASED BIOPLASTIC: (AP)

INGREDIENTS

· Agar agar (polymizer) 4gr

· Glycerol (plasticizer) 1ml
· Water 100ml

METHOD:

1. Begin by measuring the required amount of water and placing it in a beaker. Heat the
beaker on a magnetic hot plate stirrer, maintaining a temperature of 60°C while stirring.
2. Measure the Agar agar and gradually add it to the heated water, ensuring a steady and
controlled addition.
3. Introduce glycerol into the mixture and continue stirring for a minimum of 40 minutes,
ensuring thorough incorporation.
4. Allow the mixture to cool down slightly and then carefully pour it into pre-prepare
molds.
5. Allow the molds to sit undisturbed for 15-20 minutes until the mixture solidifies to a firm
yet delicate consistency. Gently remove the samples from the molds.
6. Place the samples on a metal mesh and transfer them to an oven set at 50°C. Allow the
samples to dry overnight in the oven.

RESULT:

In contrast to the guided tutorial for the recipe, which suggests a “ Wait and Dry, typically
2-4 days” (Ribeaux, 2023), I opted to place the samples in an oven at 50°C overnight. The
outcome was a hard, flexible plastic, albeit with some distortion (see Image 1).

3
Image 1: Agar-agar based bioplastic
 6
9

10
8

11

Image 2: Experiment 1 results

EXPERIMENT 1 INGREDIENTS

1
In this very first experiment, I ex- · agar agar based bioplastic 100ml
perimented with mixing the origi- · willow inner bark 10gr
nal agar agar recipe using various 2
bio ingredients, including willow · agar agar based bioplastic 100ml
inner barks, coffee powder, lignin, · wood dust 8gr
wood saw, and more, to observe 3
the resulting effects. In the follow- · agar agar based bioplastic 100ml
ing sections, I will describe the · lignin 8gr
ingredients used, the methods 4
employed, and the outcomes · agar agar based bioplastic 100ml
obtained from these experiments. · coffee powder 8gr
(Images 2, 3)

4
 2

Image 3: Experiment 1 results

5 9
· agar agar based bioplastic 100ml · agar agar based bioplastic 100ml
· hemp fiber 10g · willow inner bark 10gr
6 · nanofibrillar cellulose DMC 2% 50gr
· agar agar based bioplastic 100ml 10
· paper pulp 8gr · agar agar based bioplastic 100ml
7 · birch chips 100ml
· agar agar based bioplastic 100ml · CMC 1% 50ml
· red cotton 4gr 11
8 · Potato starch (polymizer) 4gr
· agar agar based bioplastic 100ml · Glycerol (plasticizer): 1ml
· paper pulp 6gr · Water: 100ml
· red cotton 2gr · Nanofibrillar cellulose DMC 2% 50gr

5
METHOD:

1. Start by accurately measuring the required amount of AP and place it in a beaker.

2. If the second ingredient is in the form of powder or liquid, add it to the beaker and mix
thoroughly until well combined. However, if the second ingredient consists of fibers,
carefully place them into the molds and fill the molds with the AP mixture.If the second
ingredients is fibers, then put them into the molds, and fill with the AP mixture
3. Allow the molds to sit undisturbed for 15-20 minutes until the mixture solidifies to a firm
yet delicate consistency. Gently remove the samples from the molds.
4. Place the samples on a metal mesh and transfer them to an oven set at 50ºC. Allow the
samples to dry overnight in the oven.

RESULT

When using an agar agar-based polymer in a 50ºC oven, it has been observed that the
polymer tends to shrink unevenly, particularly when fibers are present as part of the studied
ingredients. Although the addition of powder helps the mixtures to solidify, the resulting
polymer still suffers from significant uneven shrinkage.

However, incorporating lignin into the mixture has shown to be beneficial in creating a more
uniform shrinkage process. Lignin helps to enhance the structural integrity of the polymer,
leading to a more consistent and even shrinkage during the drying process.

Furthermore, the intriguing characteristics exhibited by lignin samples have prompted a

change in the direction of my study. Instead of solely pursuing a waterproof combination,
my interest has shifted towards investigating the porous characteristics of the AP mixed with
powder, with a particular emphasis on lignin. As a result, I have decided to redirect my focus
towards exploring the combination of agar agar and lignin from this point forward.

Image 4: agar agar - water - glycerol - lignin

hard . uniform shrinkage . smooth surface

6
EXPERIMENT 2

With a basic background in wood, I had a hypothesis that lignin, along with hemicellulose and
cellulose, the components that make up wood, possesses unique properties. Lignin provides
stiffness to wood, acts as a barrier against water penetration (as it does not dissolve in water),
and exhibits exceptional weather resistance. Research suggests that only a few fungi can
break down lignin, making it a durable material in various environmental conditions.

In the next phase of my study, I aimed to mix lignin with cellulose to investigate if they would
exhibit a recombination similar to that found in wood, where lignin and cellulose microfibrils
interact. In the laboratory, there are several innovative materials available in the industry, such
as microfibrillated cellulose and nanofibrillated cellulose. I hoped that agar agar and glycerol
could substitute for the role of hemicellulose in binding lignin and cellulose (Images 5, 6).

INGREDIENTS METHOD

12 · Begin by measuring the required amount

· agar agar based bioplastic 100ml of AP mixture and placing it in a beaker.
· lignin & dish washing liquid 8gr Heat the beaker on a magnetic hot plate
· nanofibrillated cellulose 2% 50gr stirrer, maintaining a temperature of
13 60°C while stirring.
· agar agar based bioplastic 100ml For samples no. 12, 13, 14, 16:
· lignin & dish washing liquid 8gr 1. Slowly add lignin and the third ingredi-
· methy cellulose 3% 50ml ent into the mixture and continue stirring
14 for a minimum of 40 minutes, ensuring
· agar agar based bioplastic 100ml thorough incorporation.
· lignin & dish washing liquid 8gr 2. Allow the mixture to cool down slightly
· microfibrillated cellulose 50gr and then carefully pour it into pre-pre-
15 pared molds.
· agar agar based bioplastic 100ml 3. Allow the molds to sit undisturbed for
· lignin & dish washing liquid 8gr 15-20 minutes until the mixture solidifies
· potato starch 8gr to a firm yet delicate consistency. Gently
16 remove the samples from the molds.
· agar agar based bioplastic 100ml 4. Place the samples on a metal mesh and
· lignin & dish washing liquid 8gr transfer them to an oven set at 50ºC.
· methy cellulose powder 3gr Allow the samples to dry overnight in
17 the oven.
· agar agar based bioplastic 100ml For samples no. 17, 18:
· lignin & dish washing liquid 8gr 1. Slowly add lignin and continue stirring
· methy cellulose 3% 50ml for a minimum of 40 minutes, ensuring
18 thorough incorporation. Let the mixture
· agar agar based bioplastic 100ml cool down.
· lignin & dish washing liquid 8gr 2. Mix the mixture with the third ingredient
· methy cellulose 3% 50ml with hand blender.
3. Pour the mixture into molds.
4. Put the sample no.17 to an oven set at
80ºC and no. 18 to an oven set at 50ºC.
Allow the samples to dry overnight in
the oven.

7
Image 7, 8: Lignin biocomposite with thin layer sample

12

14
15
8
Image 5: Experiment 2 results
 RESULT

The results were far from successful — quite the opposite with my intention! I created samples
(12, 14,15) using MFC, NFC, and potato flour. Initially, all the samples showed promising re-
sults: they shrank uniformly, had smooth surfaces, and appeared a comfortable black surface.
Unfortunately, after being left at room temperature for just one day, the samples started to
become moist again and failed to dry, even after more than two days in the oven. It is clear
that my initial assumption was unreasonable

The samples incorporating MC (methyl cellulose) exhibited improved performance, display-

ing even shrinkage, dryness, and stability (13, 16). Additionally, when these samples were
mixed using a hand blender to create foam materials, the resulting materials proved to be
durable, tenacious, and resistant to tearing.

Furthermore, during the second round of testing with a thinner layer, the original lignin com-
posite recipe (4) lost its characteristic of even shrinking. However, despite this uneven shrink-
age, the surface of the final sample retained favorable attributes: it remained smooth, hard,
slightly flexible, and exhibited a porous structure. (Images 7, 8)

13 16

17
Image 6: Experiment 2 results

18

9
EXPERIMENT 3 INGREDIENTS

19
Based on the results from experiment 2, the · agar agar based bioplastic 100ml
third and final experiment will involve mixing · lignin & dish washing liquid 4gr
lignin with a combination of dry ingredients. · sawdust 4gr
These dry ingredients will include coffee 20
powder, sawdust, birch pulp, peanut powder, · agar agar based bioplastic 100ml
and fiber. (Image 9) · lignin & dish washing liquid 4gr
· fiber 4gr
21
· agar agar based bioplastic 100ml
· lignin & dish washing liquid 4gr
· coffee powder 4gr
22
· agar agar based bioplastic 100ml
· lignin & dish washing liquid 4gr
· peanut powder 4gr
23
· agar agar based bioplastic 100ml
· lignin & dish washing liquid 4gr
· birch pulp 4gr

20

19

10
Image 9: Experiment 3 results
 METHOD RESULT

1. Begin by measuring the required amount The combination of agar agar and lignin
of AP mixture and placing it in a beaker. composites, when mixed with coffee pow-
Heat the beaker on a magnetic hot plate der, peanut powder, and sawdust, yielded
stirrer, maintaining a temperature of favorable results with even shrinkage and
60°C while stirring. hardness. Furthermore, the mixture of coffee
2. Slowly add lignin and the third ingredi- and lignin resulted in a homogeneous color
ent into the mixture and continue stirring throughout the samples.
for a minimum of 40 minutes, ensuring
thorough incorporation. However, when agar agar and lignin were
3. Allow the mixture to cool down slightly mixed with fiber and pulp, the balanced
and then carefully pour it into pre-pre- shrinkage process was disrupted, leading to
pared molds. distorted shapes in the samples.
4. Allow the molds to sit undisturbed for
15-20 minutes until the mixture solidifies Overall, the samples exhibited a rough,
to a firm yet delicate consistency. Gently rubber-like texture and emitted a light odor
remove the samples from the molds. (which was lighter compared to the original
5. Place the samples on a metal mesh and lignin).
transfer them to an oven set at 50ºC.
Allow the samples to dry overnight in
the oven.

22

21 23

11
3. DISCUSSION & CONCLUSION

The experimental results shed light on the behavior and properties of agar agar-based poly-
mers mixed with various ingredients, with a specific focus on the impact of lignin and other
components. In Experiment 1, the addition of lignin was found to significantly improve the
uniform shrinkage of the polymer, enhancing its structural integrity during the drying process.
This observation highlights the crucial role of lignin in achieving consistent and even shrink-
age, which is essential for the stability and performance of the composite material. Conse-
quently, the study’s direction was redirected towards exploring the porous characteristics of
agar agar-lignin combinations.

Experiment 2 provided valuable insights into the performance of different ingredients in the
composite. While samples incorporating microfibrillated cellulose (MFC), nanofibrillated cel-
lulose (NFC), and potato flour initially displayed promising results, they exhibited a lack of
long-term stability and dryness. In contrast, samples containing methyl cellulose (MC) showed
improved properties, including even shrinkage, enhanced dryness, and greater stability. The
successful incorporation of MC in the composite suggests its role in improving the overall per-
formance and durability of the material. Additionally, the use of a hand blender to create foam
materials demonstrated the potential for achieving desirable characteristics such as durability
and tenacity in the composite structure.

In Experiment 3, the combination of agar agar-lignin composites with coffee powder, peanut
powder, and sawdust showcased favorable outcomes, including even shrinkage and increased
hardness. This indicates the potential for utilizing these combinations in applications where
uniformity and strength are desired. However, the inclusion of fiber and pulp disrupted the
balanced shrinkage process, resulting in distorted shapes in the samples. This finding under-
scores the importance of ingredient selection and compatibility in achieving desired material
properties and shapes. The samples exhibited a rough, rubber-like texture, suggesting the
need for further optimization to improve the overall surface characteristics.

In conclusion, these experiments provided valuable analytical insights into the behavior and
properties of agar agar-based polymers when mixed with various ingredients, with a spe-
cific emphasis on the influence of lignin. The findings emphasize the critical role of lignin in
achieving uniform shrinkage and enhancing the structural integrity of the composite material.
Furthermore, the study highlights the varying performance of different ingredients, with MC
demonstrating improved properties such as even shrinkage, enhanced dryness, and stability.
These results open up avenues for further research and optimization to enhance the stability,
durability, and desired characteristics of agar agar-lignin composites for potential applica-
tions in biomaterials and architectural design. The analytical examination of the experimental
outcomes provides a foundation for future studies in this field, aiming to advance the under-
standing and application of lignin-based biomaterials.

12
Image 10: Lignin biocomposite 13
4. REFLECTION

Throughout this course, I embarked on a journey into the realm of biomaterials, with a specific
focus on exploring the potential of lignin composites as a viable biomaterial for architectural
design. This study marked my initial foray into this field, and I approached it with humility and
a desire to delve into the characteristics of lignin, particularly in terms of degradation, stability,
and porousity performance.

At the outset, biomaterials were a completely new concept to me. However, with the guid-
ance of teachers and teaching assistants, as well as the freedom to explore and experiment,
I found myself inspired and gained a wealth of knowledge. The learning process was not
without challenges, but the support and resources provided paved the way for my growth and
understanding in this fascinating subject.

Undertaking this research, I aspired to make a meaningful contribution to the existing body
of knowledge in the field of biomaterials. My aim was to establish a foundation for future ad-
vancements in utilizing lignin within architectural design. However, I am aware that there is still
much more to be explored and refined in this exciting and rapidly evolving field.

In conclusion, this course has provided me with valuable insights, inspired me, and ignited my
passion for further exploration in this field. I am eager to continue expanding my knowledge
and pushing the boundaries of what can be achieved with lignin in architectural design.

5. REFFERENCES

· Ribeaux, Tiare. Accessed July 10, 2023. “Agar Agar”. Bioplastic Cookbook for Ritual Heal-
ing from Petrochemical Landscapes. https://bioplastic-cookbook.schloss-post.com/agar-
agar.html
· Dunne, Margaret. 2018. “Agar Agar Plant Based Bioplastic”. Bioplastic Cook Book. Fab
Textiles. https://issuu.com/nat_arc/docs/bioplastic_cook_book_3
· Bogers, Loes. 2020. “Agar foil”. Loes’ Fabricademy Journey. https://class.textile-acade-
my.org/2020/loes.bogers/

14
Image 11 Experiment 1’s samples before putting into oven 15
 Thank you.

July 11, 2023 | Espoo, Finland

16