Textile industrial application and development of plant dyes

Sun Jieqing 1a, Zhou Huixian 1a, Yang Xiaoli 1b, Zhang Yuanming 1b, Liu Chunguo 2, Han
Guangting 1b, Jiang Wei 1a* (1. Qingdao University a. College of Textile and Clothing; b.
Biopolysaccharide fiber jointly built by the province and the ministry State Key
Laboratory of Forming and Ecological Textiles, Qingdao, Shandong 266071; 2. Shandong
Hengfeng New Yarn and Fabric Innovation Center Co., Ltd., Dezhou, Shandong 253500)

Abstract：Plant dyes have natural and ecological characteristics. In recent years, the
production and demand of plant dyes have been increasing year by year. To review the
recent progress in plant dyeing production technolo gy and provide suggestions for
future textile applications, this article provides a systematic review of the applica tion
and progress of plant dyes in the textile field. It introduces the classification of
commonly used plant dyes and systematically summarizes the extraction methods of
plant dyes, purification processes of plant dyes, dyeing methods of plant dyes,
functional development of plant dyes, and standardization status of plant dyeing
produc tion at home and abroad. It is concluded that the green, harmless, and
sustainable characteristics of plant dyes have enormous potential for future
development. At present, purification of plant dyes, improvement of color fastness, and
standardization of industrial production are key issues that need to be focused on.

Key words: plant dyes; classification; dyeing; textile; industrialization

Vegetable dyeing refers to a method of dyeing materials using dyes extracted from
certain plants. Plants in nature are properly processed to make dyes, and no or very few
chemical additives are used in the dyeing process, so that the products have both
natural artistic style and good ecological compatibility. Dyeing with plant dyes has a long
history and has been the main method of textile printing and dyeing historically. With
the invention of chemical dyes in the mid-19th century, chemical dyes quickly replaced
plant dyes and became the mainstream in the field of textile printing and dyeing due to
their bright colors and ease of industrialization. Plant dyeing has always been mainly
processed in workshops, and this traditional dyeing technique is mostly preserved and
passed down as cultural heritage.

In recent years, with the development of the economy, global industry's requirements
for ecology and greening, and people's demand for green and healthy products, plant
dyeing products with raw materials derived from natural materials have gradually begun
to see market demand, and the industrial production of plant dyes has Research has
also continued to receive attention from the industry. Research on plant dyeing
industrialization technology began in the 1980s, with the United States, Japan, and
Germany as representatives carrying out basic technology research on plant dyeing.
Japan's AIAI applied for patent JP60126388A as early as 1983, which proposed the use
of tea plant dyes to dye fiber products. method 1] . Since the 20th century, research on
plant dyeing industrialization technology has developed rapidly, especially in China,
South Korea, and Japan, where the number of research teams and results has increased
significantly. Japan has specially set up a "vegetable dyeing" research institute to apply
modern technology to research natural plant dyes, and has achieved a series of results
in improving color fastness. The Korean Natural Dyeing Association has conducted in-
depth research on plant dye extraction technology, level dyeing properties and
improving color fastness to sunlight, and has made certain progress. Indian University
Institute of Technology and AMA Company are committed to plant dye extraction
technology and industrial production [2]. my country's Donghua University, Zhejiang
University of Science and Technology, Changzhou University, Qingdao University,
Wuhan Textile University, Changzhou Meisheng Biomaterials Co., Ltd., etc. have also
successively carried out research on plant dyeing, plant dye extraction and other
technologies. The American Allegro Natural Plant Dyes Company and the American PBO
Company can provide more than 100 kinds of natural plant dyes [3]. Especially after
2010, plant dyeing has attracted widespread attention around the world. Dozens of
scientific research institutions and enterprises in more than ten countries have carried
out research on plant dyeing related technologies. China, Japan and South Korea have
become far ahead in scientific and technological research and development results. , the
United States and European countries such as France, Germany, Belgium, and Italy also
have certain research and development results.

However, from the perspective of the printing and dyeing industry, the overall
proportion of plant dyes is still low, mainly due to the following two points: (1) Plant
dyes are natural extracts, and the low purity of their products has always been a
practical problem in their industrial preparation. Its biggest disadvantage compared with
chemical dyes is that it causes a series of problems such as poor dyeing stability and
difficulty in textile production. (2) Plant dyes have low affinity, causing problems such as
low color fastness and incomplete color series. This article intends to review the
research progress in recent years from the aspects of classification, extraction,
purification, dyeing and product development of plant dyes, and provide suggestions for
future development directions.

1 Classification of plant dyes

There are many types of plant pigments in nature, which exhibit various colors and
different physical and chemical properties due to differences in chemical composition.
Vegetable dyes commonly used in textiles can be divided into different types based on
color, chemical composition or dyeing properties, as shown in Table 1

Shown[4-9]

Hue Name Color picking part Dyeing properties main pigment

Red Madder root mordant, Rubiacin
dispersion
safflower flower direct, acidic safflower pigment
Sumu wood wood mordant Hematoxylin,
hematoxylin
Grape peel mordant anthocyanins
Lithospermum root mordant Lithoquinone
Purple Amaranth stems, leaves mordant Amaranth,
betalain
 perilla leaf mordant Perillin, perillin
onion rhizome bark mordant anthocyanins
Impatiens stems, leaves, mordant, anthocyanins
flowers dispersion
orange rouge bark, seeds direct annatto
Saffron flower, stem direct, mordant Crocin
turmeric rhizome direct, mordant curcumin
Sophora japonica flower mordant Rutin
wormwood stems, leaves mordant quincein, luteolin
yellow rhubarb rhizome mordant, emodin
dispersion
Gardenia fruit direct, mordant Gardenia
Huangbo bark Direct, mordant, berberine
positive ion
Green kale leaves reduction Indigo
Polygonum stems, leaves reduction Indigo
Ma Lan stems, leaves reduction Indigo
wood blue leaves reduction Indigo
woad leaves reduction Indigo
oak tree bark, fruit shell direct, mordant Tannin
Buttercups root direct, mordant Tannin

Tea leaf direct, mordant Catechin

Brown Pomegranate peel direct, mordant, punicalagin
acidic
ginkgo bark, fallen leaves direct, mordant Flavonoid
pigments
camphor leaves, bark mordant Rutin, quercetin
chestnut bark, fruit shell direct, mordant Flavonoid
pigments
Oak bark direct, mordant Quercetin

black belang fruit mordant Tannin

 lotus Nutshell direct, mordant Quercetin

gallnut Parasite mordant Tannin

Although there are many types of plant dyes, most of them are limited by the harsh
growth conditions of the plants themselves or their scarce yields, making it difficult to
achieve large-scale production. At present, dyeing plants that can be harvested in large
quantities and are easy to store mainly include indigo, hematoxylin, madder, safflower,
gardenia, turmeric, goldenseal, gallnut, etc. [9-12]. Among them, indigo can be
produced by the fermentation of indigo, woad, moxa or malan, and is currently the
plant dye variety with the largest output.

2 Extraction of plant dyes

Plant dyes are generally taken from plant stems, leaves, flowers and other tissues, and
solvent extraction is usually used. Some dyes require fermentation and other methods
to be effectively extracted, such as plant indigo. In recent years, modern extraction
methods have been widely used in the extraction of plant dyes. Ultrasonic-assisted
methods, microwave-assisted methods, biological enzyme methods, and supercritical
CO2 extraction methods all reflect their respective advantages.

2.1 Solvent extraction method

Solvent extraction method is the most commonly used method for extracting plant dyes.
Its principle is to use the difference in solubility of different components in the raw
material in the solvent to select a solvent that has a large solubility for the target
pigment and a small solubility for other components, and uses methods such as dipping
or reflux heating. , extract the required components from the raw material tissue [13].
In terms of solvent selection, water and ethanol are relatively common media. Plants
such as safflower can better extract yellow dyes using water as a solvent at a
temperature of 60°C [14]; while turmeric dyes require ethanol (water / ethanol)
extraction [15]. The pH value has a certain impact on the extraction of plant dyes, and
sometimes better extraction results can be achieved by adjusting the medium
environment. For example, BORUAH et al. found in their study on the extraction of
impatiens and bread tree dyes that when using a weakly alkaline medium for dye
extraction, the intensity of the dye obtained was the highest [16]. KHAN et al. also found
the same result in their study on camphor dye dyeing. conclusion[17]. However, the
extraction rate of pure solvent is low, so many studies have improved the extraction
process to obtain better extraction results. Due to the tight structure of plant tissue,
pretreatment methods such as biological fermentation, mechanical crushing, and acid
presoaking of plant tissue can destroy the plant cell wall structure and improve the
extraction efficiency of dyes. For example, Du Haijuan et al. pre-fermented the Rubia
Rubia dye before extracting it. It was found that after fermentation with pure water for
24 hours, fabrics dyed with madder pigment extracted by pure ethanol can obtain a
higher K/S value [18].

In particular, the dye extraction objects may not be limited to plants themselves. On the
basis of primary extraction, YANG et al. used ethanol to extract the residual dye in the
residual water of madder dyeing. The secondary recovered dye still performed well in
cotton fabric dyeing. This method effectively improved the utilization rate of the dye
[19]. By sealing and pressurizing, plant-dyed fibers can be stripped. For example, Lu
Haixia and others used a low-acidity nitrogen-filled sealing and pressurizing method to
strip and extract yellow barberry and sophora rice-dyed silk fabrics, which improved the
stripping efficiency. It is helpful to carry out detection work [20].

2.2 Ultrasonic-assisted extraction method

Solvent extraction method has low extraction efficiency and low extraction rate, which
is one of the reasons for the high market price of existing plant dyes. New and efficient
plant dye extraction methods have been widely studied, among which ultrasonic
extraction method is A widely used auxiliary extraction method. The ultrasonic-assisted
extraction method is a method that uses the comprehensive effects of cavitation,
vibration, heat, etc. generated by ultrasonic waves to extract effective ingredients by
increasing the movement speed of medium molecules and increasing the penetration of
the medium [21]. Ultrasonic extraction method can improve extraction efficiency and
increase extraction rate. Due to the characteristics of ultrasonic extraction, ultrasonic
extraction methods mainly focus on the effects of power, time and temperature. The
selection of different solvents will also affect the effect of ultrasonic extraction. Yang Fei
showed through response surface experiments that the degree of influence of various
factors in ultrasonic extraction on the extraction rate of safflower yellow pigment is in
order: ultrasonic power > extraction time > extraction temperature [22]. In the study of
ultrasonic extraction of chestnut shell pigments, Dong Cui found that different mixing
ratios of alcohol-water extracts were also important conditions that affected the
extraction rate of chestnut shell pigments [23]. OANCEA et al. used mathematical
models to optimize the ultrasonic-assisted peony flower dyeing process under a high
solvent-to-solid ratio (50/1), and the results were better than the traditional
impregnation method [24]. Compared with the solvent extraction method, the
ultrasonic-assisted extraction method is more efficient, and because of its simple
equipment and easy operation, it has gradually become a more common extraction
method in experimental research.

2.3 Microwave-assisted extraction method

The microwave-assisted extraction method allows certain components in the raw

materials to be selectively heated based on the differences in the absorption of
microwaves by different substances, thereby separating them from the original system
and entering into solvents with relatively poor microwave absorption capabilities to
achieve the purpose of extraction [13] . Lin Li et al. studied the effect of microwave-
assisted extraction process conditions on the extraction effect of water chestnut skin
pigments. Through response surface experiments, they found that the degree of
influence of various factors on the extraction effect is: microwave power > heating time >
liquid-to-material ratio [25]; FERSI et al. In the study of microwave extraction of oak fruit
dyes, it was found that appropriate pH can also improve the pigment extraction effect
[26]. The effect of microwave-assisted extraction is better than that of ultrasonic-
assisted extraction to some extent, but microwave-assisted extraction can be
destructive to plant dyes when the microwave action is not well controlled, so
microwave-assisted extraction requires more precise process control. Liu Xueke et al.
optimized the anthocyanin extraction process from indigo fruit pomace by combining
ultrasound-microwave-assisted extraction. Through research, they found that the dual
effects of ultrasound and microwave can accelerate the dissolution of anthocyanins, but
as the extraction time increases, the anthocyanin structure may will be destroyed and
reduce the extraction rate, so the optimal extraction time is 2 min[27]. In addition, in
the pretreatment of the extract, ATAV et al. used a microwave device to remove the
moisture in the paste-like plant dye, and then grinded it to obtain plant dye powder,
which is easier to store and use [28]. The microwave-assisted extraction method greatly
saves extraction time, but requires higher precision and safety of the extraction
equipment. At present, the microwave-assisted extraction method has not yet been put
into large-scale industrial production, and the extraction mechanism and control
methods need to be further studied.

2.4 Biological enzyme extraction method

Plant dyes are commonly found in plant cells. Due to the tight structure of plant tissues,
using different methods to destroy the plant cell wall structure can greatly improve the
extraction effect of plant dyes. Enzymes have the ability to degrade or destroy cell walls
and cell membranes. The application of enzymes can reduce the resistance of pigment
molecules to diffuse into the extraction medium, facilitate the precipitation of target
components, reduce the amount of solvent required for extraction, and improve the
extractable content to a certain extent. output[29]. BHATTACHARYYA et al. purified
pectinase through four steps of precipitation, dialysis, ion exchange chromatography,
and gel filtration chromatography, and used the purified enzyme to treat grape skin cells.
Microscopic observation showed that the enzyme caused grape skin cells to shrink and a
large amount of pigments to be lost in a short period of time, proving the feasibility of
the purified enzyme in efficiently extracting plant pigments [30]. LOMBARDELLI et al.
proposed a customized solution based on enzyme extraction of target components for
the extraction of pigments from sugar beets. This process uses a mixture of specific
enzymes to ensure pigment recovery even at lower temperatures (25°C). In addition,
low-temperature enzyme-assisted extraction methods can also better preserve the
color attributes of betalain extracts [31]. Biological enzyme extraction method can also
be combined with other extraction methods to obtain more ideal extraction results.
Dong Zijun et al. used an ultrasonic-biological enzyme collaborative extraction method
to extract purple sweet potato pigments, and the absorbance value of the extract
obtained was significantly higher than that of pure ultrasonic-assisted extraction and
biological enzyme extraction products. pH, enzyme dosage, temperature, enzymatic
hydrolysis time, etc. all have a certain impact on the extraction effect [32]. Compared
with non-enzymatic methods, biological enzyme extraction has good ecological
compatibility and lower energy consumption. However, enzymes are specific, and
further improvement of extraction technology requires flexible use of the working
characteristics of various enzymes.

2.5 Supercritical CO2 extraction method

Supercritical extraction is a new separation method that utilizes the special properties of
supercritical fluid near the critical temperature and critical pressure for extraction.
Dissolve a certain component in the mixture, and then reduce the density of the
supercritical fluid or change it into an ordinary gas state by reducing the pressure or
raising the temperature. The dissolved substance will precipitate and can be separated
[21]. CO2 is the most commonly used supercritical fluid in plant dye extraction. NEDRA
et al. studied the extraction effect of supercritical CO2 on pigments from different plants
(Acacia flowers, Tamarix leaves, tomato processing residues, and pepper by-products).
Compared with Soxhlet extraction solvent extraction, the extraction efficiency of
supercritical extraction is significantly higher. Keep improving. The obtained extract was
used for dyeing a variety of fibers, among which wool and nylon fibers showed good
coloring affinity, proving that plant dyes obtained by supercritical CO2 extraction can be
used for textile dyeing [33]. LUDWIG et al. have shown through research and
calculations that due to the high compression work required to reach the critical
pressure, although supercritical extraction consumes twice as much energy as
traditional solvent extraction, overall the extraction cost is 20% lower than that of
solvent extraction [34 ]. Compared with traditional extraction methods, CO2 has the
advantages of being non-toxic, odorless, and non-flammable, and the obtained extract
will not contain residual solvents. The supercritical CO2 extraction method has broad
prospects for industrial extraction of plant dyes.

3 Purification of plant dyes

Plants are rich in complex components such as polyphenols, glucose, pectin and
nitrogen compounds, which are often precipitated together with pigments during the
extraction process and become "impurities" in the extract. Impurities not only affect the
combination of dyes and fibers during dyeing, making it difficult to control the dyeing
process and reduce the color fastness of fabrics; they also affect the stability of
pigments during storage and accelerate the deterioration of dyes. At present, the purity
of commercialized plant dyes is generally less than 30%, which has a great impact on the
quality and stability of subsequent dyeing. In the preparation of plant dyes, simple
extraction methods are difficult to effectively separate impurities, so further purification
of extracts is also an effective means to improve dye quality.

3.1 Membrane separation and purification

Membrane separation technology uses a selective permeable membrane as the

separation medium and pressure as the driving force to intercept various component
substances with different relative molecular masses step by step, thereby achieving the
purpose of separation, concentration, and purification [35]. Membrane separation is a
phase-change-free process that can maintain the original structure and characteristics
of natural ingredients to the greatest extent, and is suitable for the purification of
natural product extracts. Through membrane separation and purification, not only can
the purity of the final plant dye be improved, but the dyeing effect of subsequent
textiles can also be significantly improved. Jin Limei et al. used pressure-driven
membrane technology to further purify water-extracted adzuki bean pigments. The
anthocyanin color value in the pigment freeze-dried powder purified through the
optimized process reached 2.41 times that before purification [36]. NAIDIS et al.
compared the dyeing properties of saffron extract and ultra-filtered saffron extract and
found that due to the elimination of extraction by-products, ultra-filtered saffron
produced a brighter and stronger dyeing effect compared with the original saffron
extract [37]. ABDOU LAYE et al. proposed a cross-flow microfiltration technology
combined with microfiltration and ultrafiltration/nanofiltration for the purification of
betalains. This method can effectively remove insoluble and colloidal components in
cactus pear juice. By adjusting the type of filter membrane and filtration pressure, and
adding appropriate diafiltration steps, the betalain content in the product can be
increased, and even fractionation of different pigments of the same type can be
achieved [38]. Membrane separation technology has considerable development
potential as a solution for low-temperature concentration and purification of extracts. In
order to be better applied to industrial production, further demonstration of the
purification process from an economic perspective is needed.

3.2 Purification by adsorption method

The adsorption method is an energy-saving technology that selectively absorbs target

components from materials to achieve the purpose of separation and purification. As a
new type of organic polymer adsorbent, macroporous resin can selectively adsorb
organic substances from the solution through physical effects, thereby achieving the
purpose of separation and purification [39]. The adsorption method is highly selective
and can significantly improve the purity and quality of the product. Tang Liqin et al.
studied the purification effect of X-5 macroporous resin on the extraction of gardenia
yellow pigment from gardenia fruits, and optimized the separation process conditions.
Compared with the crude extract, the color value of the purified product increased from
48.51 to 243.43, and it had stronger antioxidant activity [40]. TALPUR et al. compared
the separation characteristics of five macroporous resins (AB-8, Sepabeads Sp-700,
C18SPE Cartridge, Sepabeads Sp-207 and AB-80) for extracting anthocyanins from
walnut berries, among which AB-8 resin showed the best performance. Excellent
adsorption capacity [41]. In addition, carbon nanotubes can also be used for the
adsorption and purification of pigments due to their unique layered porous structure.
REN et al. used ethanol aqueous solution to extract betacyanin from Rhodiola rosea peel,
and compared two types of macroporous resins (X-5 and AB-8) and two types of carbon
nanotubes (MWCNT and carboxylated MWCNT). Purification effect as an adsorbent. The
results show that carboxylated multi-walled carbon nanotubes exhibit the highest
adsorption capacity, and under appropriate extraction and purification conditions, the
pigment content of the extracted product can be increased to 46.2 mg/g [42]. However,
adsorption purification has the problems of high cost and low efficiency, and currently
has certain limitations in its application in industrial production.

3.3 Integrated extraction-purification scheme

In the study of high-purity dye extraction, many researchers have also proposed
integrated preparation plans, which can complete the purification of the product during
extraction, greatly improving production efficiency. JESÚ S et al. proposed a step-by-step
purification process for plant pigments that combines multiple methods, and the
preparation path can be flexibly selected according to actual needs: In the first stage,
32.05 mg/mL cyano-3-glucuronidation is used to oxidize the crude extract and undergo
microfiltration. , ultrafiltration and adsorption, and concentrate the filtrate; in the
second stage, the pigments are fully separated through size exclusion chromatography,
reversed-phase vacuum liquid chromatography and semi-preparative chromatography
to obtain higher-purity pigment components. This scheme can increase the pigment
concentration of purple cabbage extract to more than 3 times that of the initial
extraction through only the first stage, and the yield is significantly higher than that of
general extraction methods [43].

3.4 Centrifugal separation and purification

In the current industrial production of plant dyes, the presence of solid particle
impurities is also one of the important reasons that affects subsequent dyeing results. In
order to obtain as much pigment components as possible during the extraction stage, it
is often necessary to crush or grind plant raw materials first, so that solid impurities are
inevitably mixed into the product; dyes such as natural indigo that require secondary
processing (fermentation) are used as The additive lime water will react with the CO2
gas produced during fermentation to generate calcium carbonate, which will adsorb
suspended indigo and accelerate the precipitation of indigo [44]. Currently, indigo dyes
on the vegetable dye market are generally produced using the above method, but this
method The impurity content of inorganic impurities in indigo dye can be as high as
more than 95%. ISHTIAQUE et al. mentioned in their research that cotton fibers dyed
with vegetable dyes are prone to breakage and adhesion to equipment during spinning.
This is due to the deposition of large particle impurities on the fiber surface during the
dyeing process [45]. Centrifugal separation is a very effective method for these solid
particle impurities. The author's team took advantage of the water-soluble
characteristics of indigo dye after reduction during the dyeing process, and centrifuged
the indigo dye solution dissolved in reduced water, which can effectively separate the
micro-nano solid particles in the dye solution, and the impurity removal rate reached
97%, which significantly improved Dyeing effect and product quality; research results
show that centrifugal pretreatment of indigo dye can improve the friction and electrical
properties of dyed fibers, basically solve the problems of fiber breakage and adhesion in
spinning, and significantly improve the production environment [46].

4 Dyeing with vegetable dyes

For most plant dyes, it is difficult to dye by simply soaking in dye liquor. Therefore,
traditional handicraft workshops often use mordant dyeing to produce plant-dyed
products. In modern industrial production practices, industrial mordants are also
commonly used to achieve large-scale production. With the advancement of dyeing
technology research, researchers have begun to focus on other dyeing methods, such as
ultrasonic or microwave dyeing, fiber modification, supercritical dyeing, etc., to obtain
higher color fastness and develop more environmentally friendly dyeing processes.

4.1 Media dyeing method

Plant dyes generally have the shortcomings of lighter hue and poor dye fastness. In
order to improve their dye fastness, the most common method is to use mordants and
plant pigments to form chelates, so that the pigment molecules can be firmly attached
to the fiber. According to the classification of the mordant dyeing process, it can be
divided into pre-mordanting method, co-mording method, and post-mordanting
method. Different mordant components and different dyeing processes have different
dyeing effects for different dyes. DATTA and others found through research that under
the action of different metal ions, lantana plant dyes will show different dyeing effects,
indicating that the hue of the dyed object can be adjusted by selecting different
mordants [47]. There are also many different categories based on the type of mordant.

4.1.1 Metal mordant

In the industrial production of natural plant dyeing, metal mordants are currently the
most widely used. SUDHIR et al. used Soxhlet extraction method to extract brown dye
from banyan leaves. In a pre-mordant process, aluminum, copper sulfate, ferric sulfate
and stannous chloride were used as mordants for dyeing cotton fabrics. By optimizing
dyeing conditions, the color intensity and color fastness of dyed fabrics can be improved
[48]. YILMAZ et al. used K3Al(SO4)2, CuSO4 and FeSO4 mordants to study the dyeing
characteristics of 16 local plants on wool fibers. The results show that hues such as
brown, gray, khaki, and beige are easily achieved through plant dyes [49]. However, as
far as traditional mordant dyeing methods are concerned, certain metal ions are not
good for human health, and if the dyeing sewage cannot be properly treated, it will have
an adverse impact on the ecological environment, which is contrary to the original
intention of green production. In response to this problem, Qi Di et al. first complexed
catechins with metal ions to prepare metal complex plant dyes, and then dyed the
textiles. The dyed silk fabrics obtained had good color fastness [50]. In addition, the
development of environmentally friendly mordants has become a hot topic in plant
dyeing research.

4.1.2 Natural plant mordants

Certain components in natural plants can act as mordants. Common types include plant
tannin mordants, plant acid mordants, plant alkaline mordants, plant metal mordants,
etc. [51]. ZHANG et al. used banana leaf extract as a mordant for dyeing wool fabrics
with purslane dye. The dyed fabric obtained had a K/S value of up to 23.53 and had
good UV protection and antibacterial properties [52]. Based on historical records, Qiao
Xinxin restored and optimized the plant ash mordant silk fabric process using cotinus
dye, and verified the feasibility of the plant alkaline mordant dyeing method [53].
Ö ZOMAY et al. used high tannin content Quercus japonica extract as a mordant for plant
dyeing of silk and achieved good results [54]. HOSSEINNEZHAD et al. used pumpkin
extract rich in metal ions to complete the mordant dyeing of wool fabrics with
goldenrod and madder [55]. ANKIT et al. used extracts from the pumpkin tree to replace
traditional metal mordants for the dyeing of wool fabrics with myrobalan dyes [55]. 56],
both dyed fabrics have bright colors and good color fastness, and the entire dyeing
process rarely produces polluting wastewater. YAN et al. compared the effects of
different mordants on hemp plants dyed with Buddleia japonica and found that fabrics
enzymatically dyed with rosin, plant ash, KAl(SO4)2 and papaya extract were light to
dark yellow, and compared to KAl(SO4 )2, the other three plant mordants can make
plants obtain better color fastness [57]. Natural plant mordant materials come from a
wide range of sources, but are limited by the influence of the natural environment and
the content of their active ingredients is unstable. Further research is needed on how to
improve the reproducibility of application.

4.1.3 Natural mineral mordants

Minerals in nature contain a variety of metal ions, which can be used as mordants to aid
dyeing. Compared with synthetic metal mordants, natural minerals do not pollute the
environment and have the advantages of high efficiency, non-toxicity and
environmental protection. HOSSEINNEZHAD et al. used a combination of natural alum
and tannin extracted from sumac as a mordant to dye silk fabrics with madder and
mignonette dyes. The dyed fabric has bright color and good color fastness to washing
and light. The process is suitable for producing blankets with ethnic characteristics [58].
WU et al. used the rare earth mordant neodymium oxide to plant-dye silk. Under
appropriate process parameters, good dyeing depth and fastness can be obtained [59].
BARANI et al. used surfactant-modified bentonite to pretreat wool fabrics, causing the
bentonite particles to disperse and settle on the surface of wool fibers to bind more
madder dye molecules. The color fastness to washing of dyed fabrics reaches level 4 or
above, and it has good water absorption properties [60].

4.2 Synergistic dyeing promotion method

4.2.1 Ultrasound to promote dyeing

The use of ultrasonic effect in the dye bath can prevent the agglomeration of dye
molecules and promote the release of air inside the fiber, making it easier for the dye
molecules to contact the fiber, thus improving the dyeing effect. AMUTHA et al. used an
ultrasonic bath to carry out alum/ferrous sulfate mordant dyeing on cotton fabrics and
silk fabrics, and terminalia tree fruit dye dyeing. Compared with the traditional water
bath dyeing method, the utilization rate of dyes under ultrasonic wave dyeing is higher,
which greatly improves the dye utilization rate. Reduce energy consumption [61].
Through research, GUIZHEN et al. found that the dyeing intensity of cotton fabrics dyed
with dense flower dye under ultrasonic conditions was higher than that under
conventional conditions [62]. ZHANG et al. used soybean protein as a mordant and used
mugwort dye to dye cotton fabrics under the action of an ultrasonic bath. They proved
that ultrasonic mordant dyeing can make the fabric obtain a higher K/S value. Moreover,
the action of ultrasonic waves reduces the weight of the fiber and makes the fabric feel
softer [63]. In addition to the single ultrasonic effect, the synergistic effect of ultrasonic
waves of different frequencies has been proven to be more effective in improving the
dyeing effect and reducing the dyeing time [64]. In addition, there are often residues on
the fiber surface after dyeing with vegetable dyes, and ultrasonic waves can also be
used to treat the dyed fibers. For plant-dyed loose fiber materials, Li Yang et al. used
ultrasonic treatment to remove residual particles on the surface of modal fibers after
dyeing with madder dye. Through electron microscopy, they observed that the surface
of the treated fibers was smooth and clean, which effectively improved the spinnability
[65]. In the traditional dyeing process, supplemented by the promotion effect of
ultrasound, it can be regarded as an effective means of energy saving and efficiency
improvement.

4.2.2 Microwave dyeing promotion

Microwave radiation energy can penetrate deeply into fibers and dyes quickly and
evenly, thereby making up for the deficiencies in heat transfer and color fixation of
traditional dyeing methods, greatly shortening dyeing time and saving energy
consumption. ARAIN et al. discussed the dyeing effect of impatiens dye on polyester
under the action of microwave. The results showed that microwave heating is more
than 3 times the dye absorption of conventional heating, and the dyeing time can be
reduced by 60-65% [66]. DAYIOGLU et al. combined plasma pretreatment and
microwave dyeing technology to study the effects of various factors on silk fabrics dyed
with mulberry fruit dye. According to the experimental results, the K/S value of the
sample increases with the increase of plasma pretreatment time. In addition, microwave
heating increases the fixation rate of the dye in the fabric, and the color intensity of the
sample also increases with the increase of microwave intensity. However, in terms of
color fixation performance, the effect of plasma and microwave is not obvious [67].

4.3 Fiber modified dyeing method

Modifying fibers through certain methods, such as changing fiber surface properties and
introducing new active groups, can strengthen the connection between dyes and fibers
to achieve the effects of increasing dye uptake and improving color fastness. Traditional
chemical modification methods often have the disadvantage of serious pollution.
Current research on fiber modification is also developing in a more environmentally
friendly, energy-saving, and efficient direction.

4.3.1 Modification of synthetic materials

In most cases, cellulose fibers carry negative charges in aqueous solutions, causing
electrostatic repulsion between the dye and the fiber and hindering the binding of
molecules. Therefore, cationic modifiers are used to modify cellulose fibers to make the
fibers positively charged, which is beneficial to improving the dye uptake rate of fabrics
[68]. This dyeing method is also suitable for vegetable dyes. CORAK et al. took ferrous
sulfate mordant and cochineal dyed cotton fabrics as examples to study the influence of
cationization on dyeing of fabrics during the mercerization process. Experiments show
that cationized cotton fabrics can absorb more dyes, and the color fastness of the
product also reaches general clothing standards [69]. REHMAN et al. found through
research that cationized cotton fabrics have higher color intensity and color fastness
after dyeing with red mulberry. This treatment method has development potential in
the additive-free dyeing of plant dyes [70]. There are also many studies on the use of
inorganic nanoparticles for fiber modification, which can also achieve the purpose of
improving the dyeing performance of fabrics. EL-KHATIB et al. synthesized extremely
small TiO2 nanoparticles with an octahedral structure through microwaves and used
them to modify silk and wool fabrics. TiO2 with high specific surface area and small
particles shows better affinity for plant dyes, the K/S value of the treated sample is
higher, and it shows excellent antibacterial and self-cleaning properties [71].

4.3.2 Modification of natural macromolecules

Natural macromolecules are used to introduce active groups into the fiber to enhance
the adsorption and connection ability of dye molecules. Common modified materials
include chitosan, cyclodextrin, biological enzymes, etc. Natural macromolecules are
inherently degradable and can also introduce new functional properties to fabrics. Using
cotton fabric as raw material, KE et al. compared the effects of hydrogen peroxide
oxidation and chitosan modification on carmine dyeing properties. They found that
chitosan evenly attached to the surface of cotton fibers improved the dye adsorption
performance, making the fabric more durable. The dye uptake rate [72]. BRUDZYNSKA
et al. found that pretreating cotton fibers with chitosan before dyeing and adding nettle
extract or shellac can significantly change the properties of cotton fibers and effectively
improve the color stability after ultraviolet irradiation *73+. SALIMPOUR et al. grafted β-
cyclodextrin onto silk fibers and directly dyed them with plant dyes. Compared with
traditional copper salt mordant dyeing, the color intensity was significantly enhanced
[74]. ASSEFI et al. used bio-nanocomposites composed of m-trans-glutaminase, m-
glutamyl transaminase and bentonite nanoclay to pretreat wool fabrics under the action
of ultrasound. The surface of the treated wool fiber is rougher and can absorb more dye
molecules during the madder dyeing process, allowing the dyed fabric to obtain a higher
K/S value and color fastness to washing [75]. ATAV et al. studied the application of
laccase-assisted coloring of textile materials in plant dyeing. In this study, hypericum
and white onion dyes catalyzed by laccase were used to dye cotton fabrics, and the
fabrics obtained had a deeper hue and excellent color fastness than conventional dyeing
methods [76].

4.3.3 Physical modification

Physical methods such as plasma treatment and ultraviolet irradiation can change the
surface state or surface characteristics of the fiber, thereby improving the dyeing
performance of the fiber. The main advantage of physical modification is that no
additional chemical additives are used, and the production process is clean and
pollution-free. VANKAR et al. used plasma to modify polyester and found that the
wettability of the modified fiber was enhanced, and after being dyed with vegetable
dyes, its tinting strength (K/S) value and fastness performance were far better than
those of untreated samples. [77]. SADEGHI-KIAKHANI et al. used ultraviolet irradiated
wool yarn for direct dyeing of carmine dye. Research showed that wool scales degraded
under the action of ultraviolet rays into scales deposited on the fiber surface, promoting
the absorption of water and dye. The author believes that UV modification equipment is
simple and cheap, and has certain development potential in industrial applications of
fiber modification [78].

4.4 Supercritical CO2 staining method

Supercritical CO2 can not only be used for the extraction of plant dyes, but also has a lot
of research on its application in dyeing. Supercritical CO2 dyeing technology uses CO2
dyeing as a solvating medium to completely replace the use of water, overcoming the
shortcomings of high water consumption in traditional textile dyeing. PET is the most
suitable substrate for supercritical CO2 dyeing and has also been well used in plant dye
dyeing. KABIR et al. used the supercritical CO2 method to extract curcumin and dye PET
in the same dye bath. The color performance of the dyed fabric obtained was far better
than that of the high-temperature dip dyeing method, and the strength was hardly
affected [79]. MOLLA et al. used a simple supercritical CO2 dyeing process to dye
polyester fabrics with the natural pigment curcumin without using mordants and
pretreatment agents. With this method, higher color intensity (K/S value higher than 17)
can be obtained using a lower curcumin concentration (about 0.75%owf), and the color
fastness to washing and rubbing can meet the general requirements [80- 81]. On the
other hand, research on supercritical CO2 dyeing of natural fibers has also achieved
certain results. Wu et al. grafted natural madder pigments with alkyl and hydroxyalkyl
groups, and dyed wool fabrics with supercritical CO2, solving the problems of low color
intensity and poor fastness of natural fibers dyed with plant dyes [82].

5 Development of functional plant-dyed textiles

In addition to the most basic coloring properties, a variety of natural ingredients also
introduce various functional properties to vegetable dyes. Compared with synthetic
functional finishing agents, active ingredients derived from natural plants have higher
bioaffinity and can avoid potential damage to the human body. With the rise of
functional textiles in the consumer market, functional research on plant dyes has also
begun to receive attention.

5.1 Antibacterial plant-dyed textiles

Chinese herbal medicine is a unique medicine used in traditional Chinese medicine to

prevent and treat diseases. Modern medical research has also proved that the
flavonoids, tannins, polyphenols and other ingredients contained in natural plants have
antibacterial and anti-inflammatory effects. While vegetable dyes are dyeing, their
active ingredients also give the fabric antibacterial cleaning functions. SABYRKHANOVA
et al. prepared four kinds of agricultural waste (walnut shells, onion skins) and
wildflower (tansy, hypericum) dyed fabrics and found that they had excellent resistance
to Escherichia coli, Staphylococcus aureus and Candida albicans[83] . MIRNEZHAD et al.
extracted natural pigments from redbud bark for wool dyeing, and the prepared dyed
yarn has antibacterial and antioxidant properties [84]. SADEGHI-K et al. used chitosan-
polyaminoamine dendrimer hybrid to pretreat wool yarn, and the coloring rate of the
obtained yarn for carmine and madder dyes was improved. More importantly, under
the dual effects of plant dyes and chitosan, the dyed samples achieved more than 99%
of excellent antibacterial and antioxidant properties [85]. The author also added AgNO3
to the dye bath while using malva dye to dye cotton fibers. Through the reduction of
malva dye, AgNO3 was converted into silver nanoparticles (AgNPs) and bound to the
fiber surface. While ensuring a certain color fastness, the presence of AgNPs greatly
improves the antibacterial performance of the fabric, and its antibacterial efficiency
remains above 95% after 10 times of washing [86].

5.2 Anti-UV plant-dyed textiles

Excessive exposure to ultraviolet rays is one of the causes of skin lesions. More and
more people are paying attention to daily sun protection. Natural plant-dyed fabrics
have good UV-blocking properties, which is mainly attributed to the absorption of UV
rays by plant dyes. JIANG et al. tested several properties of camphor leaf-dyed silk fabric
and found that the fabric was very effective in blocking UVA and UVB radiation [87].
SHAHIDI et al. compared the UV protection properties of cotton fabrics dyed with
saffron, cinnamon and turmeric dyes. The results showed that all three had different
degrees of UV shielding capabilities, with saffron being the most significant. The author
believes that this is due to the complex macromolecular structure of saffron pigments
which effectively reduces the transmission of ultraviolet rays in textiles [88]. WANG et al.
comprehensively investigated the possibility of dyeing and UV-resistant finishing of silk
fabrics with blood-vine extract dyes. The samples prepared under optimized conditions
can still maintain excellent UV-resistant properties after 10 times of washing [89]. For
plant-dyed linen fabrics, DAN IELE et al. characterized the UPF values of fabrics dyed
with madder, chestnut, onion, inula and luomu under different dye bath concentrations.
The author believes that plant dyeing can provide functional added value to ordinary
fabrics and can meet today's expanding environmentally friendly consumer demands
[90]. Plant dyes may open up new avenues in the development of sun-protective
clothing.

5.3 Environmentally responsive plant-dyed textiles

Some plant dyes have environmentally responsive properties such as acid-base and
temperature indication. This feature can be used to prepare environmentally responsive
plant-dyed textiles. Common chemical synthesis indicators such as phenolphthalein and
methyl orange have certain toxicity, and long-term exposure will cause adverse effects
on the human body. Therefore, low-cost, easy-to-prepare, and environmentally friendly
plant pigment indicators have begun to arouse the interest of researchers. Zhou Peijian
extracted anthocyanins from purple cabbage and purple sweet potatoes and combined
them with silk fabrics to obtain textile products with acid-base indicating functions.
Compared with general acid-base test paper, acid-base indicating fabric can be used
repeatedly for a long time and can be used in medical and protective fields [91]. Zheng
Hui et al. based on the pH response performance of red cabbage anthocyanin and
curcumin mixed pigments, prepared an indicator label for pork freshness detection. The
product has the advantages of being sensitive, accurate, safe and non-toxic [92]. ABBAS
et al. found in their research on dyeing zucchini leaves that the dye would change color
with changes in temperature. In addition, the dye itself has good antioxidant and
antibacterial properties, and it has certain prospects in the application of medical
materials in the future [93].

6 Conclusion
The naturalness, ecology and functionality of plant dyes are in line with the direction of
industrial development and consumer demand, and have broad development prospects.
But at present, although plant dyes have a lot of research and technology accumulation
in dye preparation, dye purification, dyeing technology and product development;
however, there are still many deficiencies in the industrial implementation of plant dye
dyeing, and it is necessary to focus on dye extraction. With purification, dyeing
technology improvement and color fastness improvement, standardization research and
other directions. (1) Various extraction methods of plant dyes have been perfected.
However, due to the influence of growth environment, maturity and other factors, the
content of active ingredients in the plant itself often fluctuates significantly. In addition,
the plant itself has complex components and high purification costs. How to Obtaining
high-purity, stable-quality dyes at low cost through industrial means still requires
further research. (2) Industrialized plant dye dyeing uses conventional methods such as
mordant dyeing and redox dyeing. The above methods still have deficiencies in leveling
and color fastness when applied to plant dye dyeing. New methods such as synergistic
dyeing methods and fiber modification methods The industrial implementation of
dyeing methods urgently needs to be promoted. (3) At present, plant dyes and their
products have not been included in my country’s national standard system, and this gap
needs to be filled. On the basis of the current research on the extraction and application
of plant dyes, attention should also be paid to the implementation of standardization,
especially the development and formulation of plant dye identification method
standards and related product standards. This is to promote the quality control and
unification of plant dye industrialization and help plant dyeing. Necessary work for
product marketing.

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