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sustainability

Article
Contribution of Plant Transfer Printing to Sustainable Fashion
Irena Šabarić, Ana Sutlović * , Jana Filipčić and Franka Karin

Faculty of Textile Technology, University of Zagreb, Prilaz baruna Filipovića 28a, 10000 Zagreb, Croatia;
irena.sabaric@ttf.unizg.hr (I.Š.)
* Correspondence: ana.sutlovic@ttf.unizg.hr; Tel.: +385-1-4877-354

Abstract: Nowadays, there is a growing awareness of environmental protection, new findings in


the field of sustainable chemistry, the use of biodegradable materials, and the increased use of eco-
friendly textile products. For this reason, natural dyes are being used more and more frequently,
giving rise to a new way of decorating textiles, namely, plant transfer printing, popularly known
as “eco-printing”, in which the shape and/or pigment of a plant is transferred to the textile. In
addition, the great interest of the young generation in the application and research into the use of
natural dyes can create incentives for cultural and social sustainability through the preservation of
national heritage. Plant transfer printing is a method that combines scientific technology and artistic
design with corresponding benefits for the eco system. The very fact that the patterns are unique
and unpredictable brings out the notion of artistic freedom. In the work, plant transfer printing was
carried out on undyed cotton material and on material dyed with pomegranate peels, walnut leaves,
coffee, and aleppo pine bark. The influence of the pH value and the capillarity of the fabric, as well
as the treatment of the leaves with iron(II) sulphate heptahydrate solution, on the aesthetics of the
print and the colour fastness during washing was investigated. Based on the optimised parameters
and a sustainable fabric design, the clothing collection “Hamadryad”, inspired by Greek mythology,
was realised.

Keywords: plant transfer printing; eco-printing; natural dyes; sustainable fashion

1. Introduction
Citation: Šabarić, I.; Sutlović, A.; Since the dawn of the human species, man has achieved colourful effects on textiles
Filipčić, J.; Karin, F. Contribution of with natural dyes derived from mineral, vegetable, and animal sources. Natural dyes
Plant Transfer Printing to Sustainable have been the only type of dye for a long series of years and humans have perfected their
Fashion. Sustainability 2024, 16, 4361. use and passed on traditional knowledge over generations. The production and use of
https://doi.org/10.3390/su16114361 synthetic dyes gradually replaced natural dyes, and, today, they have almost no commercial
Academic Editor: Humberto Varum significance in the textile industry [1–7]. The modern textile industry faces the problem
where it is both one of the world’s most strategically important industries and one with the
Received: 22 March 2024 greatest negative impact on the environment. On a global scale, the textile and clothing
Revised: 16 May 2024
industry is one of the largest, but, unfortunately, also one of the most environmentally
Accepted: 17 May 2024
damaging industries. Environmental problems are usually related to the consumption
Published: 22 May 2024
of energy, water, and chemicals, direct CO2 emissions, and solid waste [8–10]. However,
with the growing awareness of global warming, climate change, the limitation of water
resources, and the problem of chemical waste disposal, dyeing with natural dyes [1–7] and
Copyright: © 2024 by the authors.
plant transfer printing can be seen as a good solution and a step in the right direction in
Licensee MDPI, Basel, Switzerland. terms of environmental protection and the preservation of our planet [8–13].
This article is an open access article One of the health-acceptable methods of textile dyeing, and certainly with a great
distributed under the terms and contribution to human well-being, is the application of the plant transfer printing method
conditions of the Creative Commons on textile material with the aim of producing eco-friendly textile products. Plant transfer
Attribution (CC BY) license (https:// printing, i.e., eco-printing, has recently been developed mainly by boosting the creativity of
creativecommons.org/licenses/by/ fashion designers who are concerned with sustainable fashion. By promoting the idea of
4.0/). “eco-design”, they want to help raise awareness of the harmful effects of the fast fashion and

Sustainability 2024, 16, 4361. https://doi.org/10.3390/su16114361 https://www.mdpi.com/journal/sustainability


Sustainability 2024, 16, 4361 2 of 13

textile industries on environmental pollution and global warming. Eco-printing represents


an improved, more environmentally friendly way of dyeing textiles by using natural plant
dyes in the production process and, on the other hand, achieving very interesting, non-
uniform prints that appeal to the artistic side of textile design. Natural materials from
all parts of plants are used, i.e., roots, leaves, flowers, fruits, and bark. They serve as
templates to achieve interesting colour shades and patterns on textiles [1–4]. In addition to
the colour, the textiles processed in this way have multifunctional properties. This applies,
in particular, to the benefits for human health. They offer good protection against UV
radiation and have anti-fungal properties, and less unpleasant odours have been observed
precisely because of their antibacterial and bacteriostatic properties [14–20].
Precisely because the natural plant dyes mainly belong to the group of flavonoid acid
mordant dyes, they have been used throughout history mainly for protein materials. The
author Ismal points out that plant transfer printing is suitable for applying these dyes to
common cellulosic materials such as cotton, viscose, and Tencel, as well as their blends
with polyester [9].
Sahu emphasises that the application of this method has an impact on the propor-
tion of the positive consumer attitude according to their impact on the environment [10].
Manuja and colleagues have demonstrated good colour fastness using this technique and
emphasise the importance of using natural dyes given their multifunctional properties [11].
Authors Tri and Nooryan [12] contribute to the combination of proven screen printing and
vegetable transfer printing and to the subjective assessment of fastness. Considering the
impossibility of spectrophotometric measurements, Nurmasitah [12] and team have taken a
commendable step by evaluating the clarity of the subject, colour sharpness, uniformity of
colour, and colour absorption based on the scores of 40 observers. However, this evaluation
method also needs to be extended due to the statistical acceptability.
Despite its name, plant transfer printing belongs to the group of contact dyeing and
can be carried out according to different principles. There is a physical (mechanical)
method, popularly known as the Hapa-Zome technique, in which mechanical forces are
used to imprint the plant material into the textiles, and another chemical method, in which
natural mordant dyes and metal salts are used together. By using water vapour with
natural materials such as flower petals or different leaves, very fascinating and unique
patterns can be achieved. Plant transfer printing combines the chemical aspect of dyeing
with the artistic freedom of designing plant prints, creating unique and very interesting
designs. The term plant transfer printing refers to the direct use of plants in this process
without extracting their natural substances. As the material is not uniform, the end result
will certainly vary and it is not possible to achieve absolute repeatability of patterns, but
each one will be unique [8–13]. However, to achieve an “eco” premise, both technical
and chemical knowledge is required. By using the optimal chemicals and adjusting the
process parameters, the print will look as clear and sharp as possible. In addition, the term
“eco-printing” must emphasise the use of renewable and sustainable plant materials and
the exploitation of invasive species. No protected plant species should be used or plant
habitats jeopardised when using this technique. The modern application of natural plant
dyes makes it imperative to use waste from other industries, easily renewable plants, and
invasive species while caring for the preservation of biological diversity [21–26].
The principle for achieving colour effects with the plant transfer printing process
is based on the fact that most natural plant dyes belong to the group of flavonoid acid
mordant [1–5]. The use of acid mordant dyes is based on the treatment of textiles with metal
salts (mordants), which influence the colour hue and colour fastness achieved. If the goal is
to achieve lighter colours, aluminium salt is used as a dye. Plant transfer printing, however,
emphasises the contrasting structure of the leaves and the textile substrate and usually uses
iron salt, giving darker shades [1–7]. The chemical bonding of the dye molecules in the fibre
structure takes place during fixation, and this is where colour fastness is achieved. During
fixation, depending on the composition of the raw material, a reaction occurs between the
imide, carbonyl, or hydroxyl groups of the textile material, metal ions from the mordant,
usually uses iron salt, giving darker shades [1–7]. The chemical bonding of th
molecules in the fibre structure takes place during fixation, and this is where
Sustainability 2024, 16, 4361
fastness is achieved. During fixation, depending on the composition of the raw m
3 of 13
a reaction occurs between the imide, carbonyl, or hydroxyl groups of the textile m
metal ions from the mordant, and hydroxyl or carbonyl groups of the natural dye
andcomplexes
hydroxyl orwith different
carbonyl groupscolours are formed;
of the natural i.e.,complexes
dye. Metal the colours
withobtained and their pro
different colours
areare the result
formed; i.e., theof the formation
colours of ligands:
obtained and fibre–metal
their properties ion–natural
are the result dye (Figure
of the formation of 1) [2
ligands: fibre–metal ion–natural dye (Figure 1) [2–4,21].

(a) (b)
Figure
Figure 1. Treatment
1. Treatment of textiles
of textiles withmordant
with natural natural dyes:
mordant dyes: (a)
(a) cellulosic cellulosic
material; material;
and (b) protein and (b)
material
material [4,21].
[4,21].

Plant transfer
Plant printing
transfer is alsoisassociated
printing with the
also associated notion
with theof a sustainable
notion method metho
of a sustainable
that seeks to minimise the negative impact of the textile industry on the environment.
seeks to minimise the negative impact of the textile industry on the environment. T
The use of natural dyes can be considered a sustainable method of processing, mainly
of natural
because dyes
it results can
in the be considered
production of a smalla number
sustainable method
of garments thatofareprocessing,
both unique mainly
and bec
notresults in the production
mass-produced, so that thereof a small
is no numberforofraw
large demand garments
materials.that arepromotes
It also both unique a
mass-produced, so that there is no large demand for raw materials. It
healthy and safe working conditions without health risks, as no harmful chemicals arealso pro
used. Among
healthy other
and things,
safe the amount
working of waste
conditions is reduced,
without and, risks,
health as leaves, flowers,
as no harmfulbark, chemic
and twigs are the main raw materials, it is possible to recycle/reuse them. As no strong
used. Among other things, the amount of waste is reduced, and, as leaves, flowers
chemicals are used, there is also no risk of polluting the soil, air, and water. At the same
and twigs are the main raw materials, it is possible to recycle/reuse them. As no
time, printing on plants can be a very effective way of reusing old clothes, giving old clothes
chemicalsnew
a completely areoutfit
used,instead
thereofisbuying
also no risk
new of polluting
clothes. According thetosoil, air, and
statistical water. At th
estimates,
thetime, printing
consumption on plants
of clothing will can be abyvery
increase 63% by effective
2030 andway of reusing
the amount old textile
of annual clothes, givi
waste will reach 102 million tonnes. If the goal is to preserve
clothes a completely new outfit instead of buying new clothes. According the environment and not to sta
neglect future generations, sustainable fashion is a big step in the right
estimates, the consumption of clothing will increase by 63% by 2030 and the amo direction [19,20].
By analysing the process parameters that affect the aesthetics and fastness of the
annual textile waste will reach 102 million tonnes. If the goal is to preser
colouration and the realisation of the finished garment, this research represents a contribu-
tionenvironment
to sustainableand notand
fashion neglect future
is a bold generations,
step towards sustainable
the possibility fashion
of moving fromis the
a big step
right direction [19,20].
laboratory scientific testing of samples to the creation of a clothing collection. In view of
By analysing
the exceptional colouringthe process parameters
heterogeneity and colourfulnessthatofaffect the aesthetics
the samples obtained byand plantfastness
transfer printing, the success of the process presented in the paper
colouration and the realisation of the finished garment, this research repres is based on the author’s
many years of experience
contribution in the usefashion
to sustainable of natural
anddyesis for dyeing
a bold andtowards
step textile printing.
the possibility of m
from theand
2. Materials laboratory
Methodsscientific testing of samples to the creation of a clothing collect
2.1.view
Textileof the exceptional colouring heterogeneity and colourfulness of the sa
Material
obtained
We used by plant
100% transferbleached
chemically printing, the success
cotton fabric inof the weave
plain process presented
from producer,in the p
based
Čateks on Čakovec,
d.o.o., the author’s many
Croatia. years
Textile hasof
theexperience in the use
following structural of natural weight
characteristics: dyes for dyei
191.45 2 , density in warp direction 26 cm , and density in weft direction 25 cm−1 .
g/mprinting.
textile − 1

2.2. Plant Selection for Transfer Printnig


2. Materials and Methods
For the plant transfer printing, the plants available in the surrounding area, i.e., in
the2.1. Textile
centre of theMaterial
city of Zagreb, Croatia, were selected, which, according to the literature,
could beWeusedused
for this purpose
100% [1–4]. These
chemically were the cotton
bleached leaves offabric
various
inmaple
plainspecies
weave (e.g.,
from pro
silver-leaf maple, honeydew maple, and chub maple), walnut, birch, and red-leaved plum.
Čateks d.o.o., Čakovec, Croatia. Textile has the following structural characteristics:
2.3.191.45 g/m2, density
Plant Selection inProcess
for Dyeing warp direction 26 cm−1, and density in weft direction 25 cm
The textile material was dyed with plant extracts from pomegranate bark, walnut
2.2. aleppo
leaves, Plant Selection for Transfer
pine collected Printnig
in Croatia, and coffee grounds bought in a local shop.
For the plant transfer printing, the plants available in the surrounding area,
the centre of the city of Zagreb, Croatia, were selected, which, according to the lite
Sustainability 2024, 16, 4361 4 of 13

2.4. Plant Transfer Printing on Uncoloured Fabric


The plant transfer printing on uncoloured fabric was tested with the following parameters:
• Influence of fabric pH—printing was performed in an acidic medium (pH 4 adjusted
with tartaric acid, C4 H6 O6 , Kemika, Zagreb, Croatia), a neutral medium, and an
alkaline medium (pH 8 adjusted with Na2 CO3 , Kemika, Zagreb, Croatia);
• Influence of capillarity—printing was performed under neutral conditions in all com-
binations of dry and wet fabric and leaves;
• Influence of leaf mordanting—leaves were treated for 10, 30, 60, and 120 min in a solu-
tion of 10 g/L iron(II) sulphate heptahydrate, FeSO4 ·7H2 O (Kemika, Zagreb, Croatia);
• The influence of leaf positioning—the front and back of the leaves were used (neutral
conditions, and dry substances)

2.5. Plant Transfer Printing on Pre-Dyed Fabric


Plant transfer printing was carried out on fabrics pre-dyed with natural plant dyes
according to the following steps:
• Extraction of the dye was performed in soft water containing 100 g/L of plant raw
material. The extraction was performed in a bath ratio of 1:40 (considering the mass
of the plant matter) at 100 ◦ C for 60 min. The bath was then cooled for 12 h and the
extract was decanted.
• The dyeing process was performed in the prepared solution at a bath ratio of 1:30 bath
ratio (considering the mass of the textile) at 100 ◦ C for 60 min.
• The plant transfer printing was carried out on dry pre-dyed fabric with dry leaves
immersed for 30 min in a solution of 10 g/L FeSO4 ·7H2 O.

2.6. Fixation
Fixation was carried out with steam at the same time as the printing process. Leaves
treated with iron salts were placed on the fabric. Aluminium foil is placed on top; every-
thing is wrapped around a wooden roll, wrapped again with aluminium foil, and tied with
string. The fabric prepared in this way is placed in a pot of hot water for 90 min, and then
wrapped and cooled for 60 min.

2.7. Wash Fastness


The wash fastness of cotton fabrics was tested in a laboratory apparatus for wet and
dyeing processes—Polycolor, Mathis, Basel, Switzerland. The test was performed according
to the standard ISO 105-C06:2010 (A2S) Textiles-Colour fastness tests-Part C06: Colour
fastness in domestic and commercial laundry [26] using 2 g/L standard detergent (James
Heal ECE A, without optical brighteners and without phosphates), with a bath ratio of 1:20
(considering the mass of the textile), a temperature of 40 ◦ C, and a soaking time of 30 min.
The alkalinity of the solution was pH 8.
Considering the appearance of the colourful pattern on the textile and the purpose of
the test, the evaluation was based on the designer’s subjective assessment.

2.8. Applying the Recipe—Creating a Clothing Collection


In the final phase, the clothing collection “Hamadryad”, inspired by Greek mythology,
i.e., Greek nymphs who were born and died together with the tree they were connected to,
was realised from the created patterned textiles. In realising the collection, the inspiration
of the designer and the freedom to use plant transfer printing to achieve the desired unique
design were respected.

3. Results and Discussion


The results shown vary considerably depending on the process parameters: the pH
value, use of the mordant, capillarity of the fabric, and properties of the plant material. The
adjustment of these parameters is the result of the knowledge and experience of a textile
chemist and has a considerable influence on the intensity and sharpness of the print, as
Sustainability 2024, 16, 4361 5 of 13

well as on the washing fastness. However, the choice of the “best” result certainly depends
on the designer’s attitude and the market’s requirements for the aesthetics and purpose of
the textile material.

3.1. Printing on Uncoloured Fabric


3.1.1. Effect of the pH Value of the Fabric
inability 2024, 16, x FOR PEER REVIEW Figure 2 shows the effect of the pH value of the fabric on the quality of the plant transfer
printing. The research was carried out by pre-treating the fabrics in acidic, neutral, and
alkaline media. The leaves were pre-treated for 45 min in a solution of 10 g/L FeSO4 ·7H2 O.
It was found that the palest and dullest samples are obtained in an acidic medium, and
sharper contours the
In addition, are more visible in a neutral
non-uniformity ofmedium, while the
colouration andsamples are most intense
the specific shading as w
in an alkaline medium. The transition of plant pigments into textiles is also the best in an
presence
alkaline of different
medium, shades
and brown of the
and green shadessame hue are
are obtained, whilevisible,
grey tonesdue to which, a
are obtained
mentioned,
in an acidicthe colouration
medium, obtained
which is due could
to the use of ironnot bethe
salt as objectively
mordant. analysed.

10 cm 10 cm 10 cm
(a) (b) (c)
Figure 3. Effect
Figure ofofthe
2. Effect the pH valueofof
pH value thethe fabric
fabric on plant
on plant transfertransfer
printing: printing:
(a) pH 4; (b)(a)
pHpH 4; (b) pH
7; and
pH 8.
(c) pH 8.

It is important to note that it was not possible to objectify the colouristic analysis,
3.1.2. Influence
since ofcolouration
the specific the Capillarity of thebyFabric
is characterised a multitude of shaded transitions and the
simultaneous presence of different shades of a single hue. Therefore, the colouristic analysis
The investigations into the influence of the capillarity of the cotton fabric a
was carried out on the basis of the theoretical guidelines for harmonic and contrasting
are shown in Figure
relationships between4.colours.
Combinations of dry or wet fabric and dry or wet leaves a
The research was carried
When the pH value out
shifts to in a neutral
alkaline, medium
an increase using
in colour chromairon salt as aThe
is observed. mordant
grey to grey-green hues seen in Figure 2a change to colours of the yellow-orange and
observed that the best contact and, therefore, the sharpest print is achieved
yellow-green spectrum, in an alkaline medium (Figure 2c). The intensity of the colouration,
textiles
whichand dryfrom
results leaves. Any ratio
the specific source of moisture
of saturation disturbs
(chroma) this relationship
and lightness, is also more and
blurring of the
pronounced in sample. Depending
the same samples, and the on the colour
specific design idea, it is
characteristic of possible
the natural to create a
plant
dyes is more pronounced. In terms of the harmonious and contrasting relationship between
varying sharpness by combining wet and dry leaves.
the colours, in Figure 2c, the relationship of analogous colours can be observed, i.e., of
different colours but in a spectral sequence, which is exactly characteristic of the harmony
of natural colours.
In addition, the non-uniformity of colouration and the specific shading as well as the
presence of different shades of the same hue are visible, due to which, as already mentioned,
the colouration obtained could not be objectively analysed.

3.1.2. Influence of the Capillarity of the Fabric


The investigations into the influence of the capillarity of the cotton fabric and leaves
are shown in Figure 3. Combinations of dry or wet fabric and dry or wet leaves are shown.
The research was carried out in a neutral medium using iron salt as a mordant. It can be
observed that the best contact and, therefore, the sharpest print is achieved with dry textiles

10 cm 10 cm 10 cm 10 cm
(a) (b) (c) (d)
Figure 4. Influence of the capillarity of the fabric on plant transfer printing: (a) dry textile–
3.1.2. Influence of the Capillarity of the Fabric
The investigations into the influence of the capillarity of the cotton fabric and leaves
are shown in Figure 4. Combinations of dry or wet fabric and dry or wet leaves are shown.
Sustainability 2024, 16, 4361 6 of 13
The research was carried out in a neutral medium using iron salt as a mordant. It can be
observed that the best contact and, therefore, the sharpest print is achieved with dry
textiles and dry leaves. Any source of moisture disturbs this relationship and leads to a
and dry leaves. Any source of moisture disturbs this relationship and leads to a blurring
blurring of the sample. Depending on the design idea, it is possible to create a pattern of
of the sample. Depending on the design idea, it is possible to create a pattern of varying
varying sharpness by combining wet and dry leaves.
sharpness by combining wet and dry leaves.

10 cm 10 cm 10 cm 10 cm
(a) (b) (c) (d)
Figure
Figure 4. Influence
3. Influence of the
of the capillarity
capillarity of the
of the fabric
fabric on plant
on plant transfer
transfer printing:
printing: (a) (a)
drydry textile–dry
textile–dry leaves;
leaves;
(b) dry textile–wet leaves; (c) wet textile–dry leaves; and (d) wet textile–wet leaves.
(b) dry textile–wet leaves; (c) wet textile–dry leaves; and (d) wet textile–wet leaves.

Figure
Figure 4a shows
3a shows thethe print
print created
created by the
by the useuse of dry
of dry fabric
fabric andanddrydry leaves.
leaves. A sharp
A sharp
contour of the leaf and the leaf veins can be recognised. When
contour of the leaf and the leaf veins can be recognised. When using wet leaves on the sameusing wet leaves on the
dry fabric (Figure 3b), the pattern is still clearly visible, but the inner structure is destroyed. is
same dry fabric (Figure 4b), the pattern is still clearly visible, but the inner structure
Thisdestroyed.
phenomenon This is
phenomenon
logical and to is logical and todue
be expected be toexpected due tomovement
the capillary the capillary of movement
the dye
of the dye on a wet surface. If the goal is greater sharpness, a contribution
on a wet surface. If the goal is greater sharpness, a contribution to this can be expected to this can
if be
expected if a larger-diameter
a larger-diameter roller is used for roller is used
fixing, which forhelps
fixing,towhich
reducehelps to reduce
the number the number
of layers of
of layers
fabric and theofpassage
fabric and the passage
of moisture of moisture
through the layers. through
When thewetlayers.
(3c) or When
dry (3d) wet (4c) or
leaves aredry
used(4d)
onleaves are used
a wet fabric, on a wetinfabric,
a reduction coloura intensity
reductionisin colourInintensity
visible. is visible. Inthe
these combinations, these
contour is pale and barely visible; i.e., the effect of the print pattern is lost. The evaluation is
combinations, the contour is pale and barely visible; i.e., the effect of the print pattern
lost. The
of these evaluation
patterns of theseorpatterns
as satisfactory as satisfactory
unsatisfactory dependsor onunsatisfactory
the designer’sdepends
ideas for onthethe
designer’s
realisation ideas
of the for design
textile the realisation
and clothing of the textileFrom
design. design
the and
aspect clothing
of colour design.
analysis,From
thethe
aspect
colour of colour
of the alreadyanalysis,
mentioned theyellow-green
colour of thetoalready mentioned
yellow-orange yellow-green
spectrum to yellow-
can be observed
orange spectrum
in addition to grey. No can be observed
sample can be saidin addition to grey. intense,
to be completely No sample as thecan be said to be
characteristic
completely
colour obtainedintense,
with plant as the characteristic
pigments, although colour obtainediswith
harmonious, plant of
generally pigments, although
lower intensity.
However, a comparison of Figure 3a–d shows that the colour is more pronounced when
the textile or textile web I is wet, although the sharpness of the contour is lost.

3.1.3. Influence of Time Mordanting of Leaves


Leaves treated in a solution of 10 g/L FeSO4 ·7H2 O were placed on a pH-neutral dry
fabric for the following periods: 10, 30, 60, and 120 min. The results shown in Figure 4
indicate that extending the mordanting time does not have a good effect on the print. After
a longer treatment of the leaves in the metal solution, dark spots can be observed on the
sample, which may indicate iron deposits. An excess of iron on the textile material can
have a negative effect on the quality of the textile; i.e., damage can occur over time. If the
designer wants to create a garment, iron deposits can have negative effects on the skin and
cause allergic reactions. This negative phenomenon can be avoided by optimising the metal
salt concentration. For the reasons mentioned above, metal salts should be used in the
lowest possible concentration. It is also necessary to use containers adapted to the selection
of plants.

3.1.4. The Influence of Leaf Positioning—Front/Back


Figure 5 shows that the choice of leaf side, i.e., front or back, can influence the appear-
ance of the sample obtained. By using the front side of the leaves, patterns with a more
accentuated colouration will be obtained, and, with the reverse side, the structure of the
leaf itself (veins and petiole) will be expressed. In addition to a more intensive pigment
deposition, the positioning of the front of the leaves on the textile led to a higher colour
a longer treatment of the leaves in the metal solution, dark spots can be observed on the
sample, which may indicate iron deposits. An excess of iron on the textile material can
have a negative effect on the quality of the textile; i.e., damage can occur over time. If the
designer wants to create a garment, iron deposits can have negative effects on the skin and
Sustainability 2024, 16, 4361 7 ofthe
13
cause allergic reactions. This negative phenomenon can be avoided by optimising
metal salt concentration. For the reasons mentioned above, metal salts should be used in
the lowest possible concentration. It is also necessary to use containers adapted to the
Chroma,
selectionwhich is reflected in the more intensely perceptible yellow-orange colouration of
of plants.
the sample in Figure 5a compared to Figure 5b.
10 cm 10 cm 10 cm 10 cm
(a) (b) (c) (d)
Figure 5. Influence of time mordanting of leaves on plant transfer printing: (a) 10 min; (b) 30 min
(c) 60 min; and (d) 120 min.

3.1.4. The Influence of Leaf Positioning—Front/Back


Figure 6 shows that the choice of leaf side, i.e., front or back, can influence th
appearance of the sample obtained. By using the front side of the leaves, patterns with
10 cm more accentuated
10 cm colouration will be10obtained,cm and, with the reverse
10 cm side, the structure o
(a) the leaf itself(b)
(veins and petiole) will be(c) expressed. In addition to a(d) more intensive pigmen
deposition, the positioning of the front of the leaves on the textile led to a higher colou
Figure4.5.Influence
Influenceofof timemordanting
mordantingof
ofleaves
leaves onplant
planttransfer
transferprinting:
printing: (a)
(a) 10
10 min;
min; (b)
(b) 30
30min;
min;
Figure
Chroma, which istimereflected in the
(c) 60 min; and (d) 120 min.
more on intensely perceptible yellow-orange colouration
(c)
of60 min;
the and (d)in
sample 120 min. 6a compared to Figure 6b.
Figure
3.1.4. The Influence of Leaf Positioning—Front/Back
Figure 6 shows that the choice of leaf side, i.e., front or back, can influence the
appearance of the sample obtained. By using the front side of the leaves, patterns with a
more accentuated colouration will be obtained, and, with the reverse side, the structure of
the leaf itself (veins and petiole) will be expressed. In addition to a more intensive pigment
deposition, the positioning of the front of the leaves on the textile led to a higher colour
Chroma, which is reflected in the more intensely perceptible yellow-orange colouration
of the sample in Figure 6a compared to Figure 6b.

10 cm 10 cm
(a) (b)
Figure5.6.The
Figure Theinfluence
influenceofof leaf
leaf positioning
positioning on on plan
plan transfer
transfer printing:
printing: (a) front
(a) front of theofleaves;
the leaves;
and and (b
back of the leaves.
(b) back of the leaves.

3.2. Plant Transfer Printing on Pre-Dyed Fabric


Sustainable textile design was also realised through a combination of plant transfer
printing and 10 pre-dyeing
cm 10 cm(Figure 6). Based on previous results, plant
of the textile material
(a)
transfer printing was performed with dry dyed fabric (b)and dry leaves pre-treated in a
solution
Figure 6.of 10influence
The g/L FeSO ·7Hpositioning
of4leaf 2 O for 30 min. Depending
on plan on the choice
transfer printing: ofofplants,
(a) front a different
the leaves; and (b)
colour
back ofisthe
obtained,
leaves. i.e., a chromatic yellow fabric from pomegranate bark, a reddish one
from Aleppo pine bark, and soft pastel achromatic colours without an accentuated tone
from walnut and coffee leaves. With such combinations, a sustainable designer can choose
an accentuated contrast or a subtle pattern.
The colours obtained are the result of the chemical structure of the dyes obtained
by extraction (Figure 7) and their reaction with iron ions, as shown in Figure 1 [2,3]. The
peel of the pomegranate (Punica granatum L.) contains 28% of the tannins punicalagin and
punicalin, which are responsible for the yellow colour (Figure 7a). Walnut leaves (Juglans
regia L.) contain the brown pigment juglone (Figure 7b) as a glycoside. The most common
chemical compound in coffee is caffeine (Figure 7c), an alkaloid from the xanitol group,
which is responsible for the brown colour. Procyanidin (Figure 7d) from the flavonoid
class is responsible for the red colour extracted from the bark of the aleppo pine [2,3]. The
final colour of the fabric depends on three parameters: the raw material composition of the
textile material, the chemical structure of the natural dye, and the choice of metal. Their
interaction creates a metal complex with a specific colour. If one of these three parameters
Sustainable textile design was also realised through a combination of plant trans
printing and pre-dyeing of the textile material (Figure 7). Based on previous results, pl
transfer printing was performed with dry dyed fabric and dry leaves pre-treated i
Sustainability 2024, 16, 4361 solution of 10 g/L FeSO4·7H2O for 30 min. Depending on the choice of plants, 8 of 13
a differ
colour is obtained, i.e., a chromatic yellow fabric from pomegranate bark, a reddish o
from Aleppo pine bark, and soft pastel achromatic colours without an accentuated to
from walnut
changes, and coffee
the colour of the leaves. With such
textile changes. It is combinations,
also known that a sustainable
dark colours aredesigner
achievedcan cho
by combining natural dyes and iron salts
an accentuated contrast or a subtle pattern. [1–7].

10 cm 10 cm
(a) (b)

10 cm 10 cm
(c) (d)
Figure
Figure 7. Samplesofofplant
6. Samples plant transfer
transfer printing
printing on pre-dyed
on pre-dyed textiles:textiles: (a) pomegranate
(a) pomegranate peels; (b) wal
peels; (b) walnut
leaves; (c) coffee; and (d) aleppo pine
leaves; (c) coffee; and (d) aleppo pine bark. bark.

The strongest
The colour contrast
colours obtained are thewasresult
achieved when
of the printingstructure
chemical on a substrate
of thedyed with
dyes obtained
a natural dye from pomegranate peels. The colours of the yellow spectrum with their
extraction (Figure 8) and their reaction with iron ions, as shown in Figure 1 [2,3]. The p
brilliance and high level of lightness, as well as their medium to high Chroma, have the
ofproperty
the pomegranate (Punica granatum L.) contains 28% of the tannins punicalagin a
of highlighting the printed pattern and placing it visually in the foreground
punicalin,
(Figure 6a).which are responsible
It is, therefore, not only afor the of
matter yellow
contrastcolour
due to(Figure 8a). Walnut
the different leaves
intensities of (Jugl
regia L.) contain
black-brown the brown
and yellow pigment
colours, but alsojuglone (Figure
this specific 8b) as
property of a glycoside.
the The most comm
colour yellow.
Evencompound
chemical the achromatic colour is
in coffee of caffeine
the background
(Figurewith
8c),aan
high lightness
alkaloid fromin Figure 6c
the xanitol gro
has a pronounced difference in intensity with the printed pattern of
which is responsible for the brown colour. Procyanidin (Figure 8d) from the flavon very low lightness
and Chroma, but does not lead to such a strong contrast visually. In the case of example
class is responsible for the red colour extracted from the bark of the aleppo pine [2,3]. T
6d, if the effect achieved is considered from a colouristic point of view, a complementary
final colour between
relationship of the fabric depends
the reddish on three
background andparameters: the raw
the greenish print withmaterial composition
a low lightness
the
can textile material,
be defined, the chemical
which brings structure of
the entire composition the
into natural
balance dye,however,
without, and thecreating
choice of me
Their interaction
an accentuated creates a metal complex with a specific colour. If one of these th
contrast.
parameters changes, the colour of the textile changes. It is also known that dark colo
3.3. Wash Fastness Test
are achieved by combining natural dyes and iron salts [1–7].
The fastness to washing test (Figures 8 and 9) is an important parameter for the
colouring of textiles intended for the manufacture of clothing. The samples are found to
have a satisfactory stability. After washing, the samples become even more intense, which
may be due to the chemical reactions on metal salts and plant substances (Figure 1). In an
alkaline detergent solution, the ionisation of the molecule can occur (Figure 7), which can
lead to a change in the colour obtained [4,5,17,18].
ainability 2024, 16, x FOR PEER REVIEW 9 of
Sustainability 2024, 16, 4361 9 of 13

(a) (b)

(c) (d)
Figure
Sustainability 2024, 16, x FOR 8. Chemical
PEERFigure
REVIEW structures:
7. Chemical (a)punicalin
structures: (a) punicalin (4,6-gallagyl-D-glucose);
(4,6-gallagyl-D-glucose); (b) juglone (b) juglone (5-hydroxy-1,
(5-hydroxy-1,4- naph-
10 of 14
thoquinone); (c) caffeine
naphthoquinone); (1,3,7-trimethylxanthine);
(c) caffeine and (d) procyanidinand
(1,3,7-trimethylxanthine); (2-(3,4-Dihydroxyphenyl)-2-
(d) procyanidin (2-(3
((2- (3,4-dihydroxyphenyl)-5,7-dihydroxychroman-3-yl)oxy)chroman-3,4,5,7-tetraol).
Dihydroxyphenyl)-2-((2-(3,4-dihydroxyphenyl)-5,7-dihydroxychroman-3-yl)oxy)chroman-3,4,5,7
tetraol).

The strongest colour contrast was achieved when printing on a substrate dyed wi
a natural dye from pomegranate peels. The colours of the yellow spectrum with the
brilliance and high level of lightness, as well as their medium to high Chroma, have th
property of highlighting the printed pattern and placing it visually in the foregroun
(Figure 7a). It is, therefore, not only a matter of contrast due to the different intensities
black-brown and yellow colours, but also this specific property of the colour yellow.
10 cm 10 cm
Even the achromatic colour of the background with a high lightness in Figure 7c h
(a) (b)
a pronounced difference in intensity with the printed pattern of very low lightness an
Chroma, but does not lead to such a strong contrast visually. In the case of example 7d,
the effect achieved is considered from a colouristic point of view, a complementa
relationship between the reddish background and the greenish print with a low lightne
can be defined, which brings the entire composition into balance without, howeve
creating an accentuated contrast.

3.3. Wash Fastness Test


10 cm The fastness to washing test (Figures109cm and 10) is an important parameter for th
(c) (d)
colouring of textiles intended for the manufacture of clothing. The samples are found
Figure 9. Colour fastness to washing of undyed samples: (a)before
and (c) before washing process; and
after(b) whic
have aFigure
satisfactory
8. Colour stability.
fastness Afterofwashing,
to washing
and (d) after washing process.
undyed the samples
samples: (a,c) become
washing even more
process; and intense,
(b,d)
may be washing
due to process.
the chemical reactions on metal salts and plant substances (Figure 1). In a
alkaline detergent solution, the ionisation of the molecule can occur (Figure 8), which ca
lead to a change in the colour obtained [4,5,17,18].
It can also be seen from the chemical structures shown in Figure 8 that, in addition
the colour, these compounds also have hydroxyl or carbonyl groups in favourab
positions for the formation of metal complexes with trivalent iron ions. It is precisely f
this reason that dark-coloured imprints of plant structures were obtained. In addition, th
m 10 cm
(c) (d)
Sustainability 2024, 16,
Figure 9. 4361
Colour
fastness to washing of undyed samples: (a) and (c) before washing process; and (b)
10 of 13
and (d) after washing process.

10 cm
Figure 10. Colour fastness
Figure 9.toColour
washing of pre-dyed
fastness to washingsamples before
of pre-dyed washing
samples before process / after washing
washing process/after washing
process. process.

It can also be seen from the chemical structures shown in Figure 7 that, in addition to
3.4. “Hamadryad” Clothing Collection
the colour, these compounds also have hydroxyl or carbonyl groups in favourable positions
Based on theforresults of the
the formation textile
of metal design with
complexes obtained
trivalentby
ironcombining technological
ions. It is precisely for this reason
that dark-coloured imprints of plant structures were obtained.
parameters, fabrics with transfer printing on undyed fabrics and fabrics dyed In addition, the iron
inions
form co-ordination bonds with the textile material, which ensure good colour fastness.

3.4. “Hamadryad” Clothing Collection


Based on the results of the textile design obtained by combining technological parame-
ters, fabrics with transfer printing on undyed fabrics and fabrics dyed in pomegranate bark
were selected for the realisation of the collection. Plant transfer printing was performed in
an alkaline medium with dry dyed fabric and wet and dry leaves pre-treated in a solution
of 10 g/L FeSO4 ·7H2 O for 30 min. This choice emphasises the pattern of leaves, which is in
line with the creations of the clothing collection (Figure 10a) inspired by Greek nymphs,
i.e., the trees they were associated with.
The realisation of the “Hamadryad” collection (Figure 10b) is a true example of
sustainable textile design. The collection consists of classic garments such as skirts, shirts,
jackets, and trousers, with interventions in cuts that attempt to imitate trees. The garments
from the collection are easy to mix and match and can be an interesting detail in combination
with everyday clothing.
tainable textile design. The collection consists of classic garments such as skirts, shirts,
jackets, and trousers, with interventions in cuts that attempt to imitate trees. The garments
from the collection are easy to mix and match and can be an interesting detail in combi-
nation with everyday clothing.
Sustainability 2024, 16, 4361 11 of 13

Sustainability 2024, 16, x FOR PEER REVIEW 12 of 14


100 cm

(a) (b)

100 cm

(c) (d)
Figure 11. Selection from the “Hamadryad” clothing collection: (a) and (c) fashion illustrations; and
Figure 10. Selection from the “Hamadryad” clothing collection: (a,c) fashion illustrations; and
(b) and (d) realisations.
(b,d) realisations.

4. Conclusions
The result of plant transfer printing is based on chemical and technological
knowledge about the application of natural plant dyes. By varying the process parameters,
Sustainability 2024, 16, 4361 12 of 13

When applying the plant transfer printing technique in the realisation of textile design
and clothing collections, it is important to emphasise the co-operation between sustainable
textile chemistry and design. From a technological point of view, it would be logical to
choose methods that achieve sharp contours and visible motifs. However, designers often
opt for the technique of plant transfer printing, which gives them blurred contours and
indistinct motifs. It is important that the process is carried out in such a way as to obtain
a final product that satisfies the market with all its characteristics in terms of aesthetics,
functionality, and colour fastness. It is precisely for this reason that the impossibility of
carrying out measurements commonly used in colour analysis, such as spectrophotometric
measurements, becomes a less important problem.

4. Conclusions
The result of plant transfer printing is based on chemical and technological knowledge
about the application of natural plant dyes. By varying the process parameters, different
colours and effects can be achieved, the choice of which depends on the attitude of the
sustainable designer.
By using iron(II) sulphate heptahydrate as a mordant, it has been confirmed that the
reaction of natural mordant dyes and the use of iron(II) ions produce dark colours, i.e.,
high-contrast prints. This contrast can be further enhanced by the choice of plants for
pre-dyeing the textile material. For sharper contours in textile printing, it is also necessary
to prepare dry material and dry herbs that have previously been treated with metal salts.
The “Hamadryad” clothing collection was realised through the synergy of textile
chemistry and sustainable design. Considering the fact that it is inspired by Greek mythol-
ogy, i.e., Greek nymphs who were born and died together with the tree they were connected
to, the contribution to sustainable design was confirmed by the choice of cutting and plant
printing technique. Clothing produced in this way can help to raise the market’s awareness
of its impact on environmental protection.
This research is a direct contribution to the imperative of understanding this connec-
tion, to understand and target natural colourants and to develop branding techniques to
achieve effects with natural colourants in the context of sustainable fashion, as well as
textile and clothing production.

Author Contributions: Conceptualisation, A.S. and I.Š.; methodology, A.S. and J.F.; investigation,
J.F. and F.K.; writing—original draft preparation, A.S., J.F., and I.Š; writing—review and editing,
A.S.; visualisation, F.K.; supervision, A.S. and I.Š. All authors have read and agreed to the published
version of the manuscript.
Funding: This work has been founded by University of Zagreb grants, TP17/22, University of Zagreb,
Faculty of Textile Technology.
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: The data presented in this study are available upon request from the
corresponding author.
Conflicts of Interest: The authors declare no conflicts of interest.

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