Dyes and Pigments 201 (2022) 110214

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Dyes and Pigments

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

Review

Melanin pigment derived from marine organisms and its

industrial applications
Khadijeh Ghattavi a, Ahmad Homaei b, *, Ehsan Kamrani a, Se-Kwon Kim c
a
Fisheries Department, Faculty of Marine Science and Technology, University of Hormozgan, Bandar Abbas, Iran
b
Department of Marine Biology, Faculty of Marine Science and Technology, University of Hormozgan, Bandar Abbas, Iran
c
Department of Marine Sciences and Convergent Technology, Hanyang University, Ansan, Seoul 426-791, Republic of Korea

A R T I C L E I N F O A B S T R A C T

Keywords: Melanin is a complex group of natural pigment substance, and it shows excellent biological and biomedical
Biotechnological applications applications which is commonly present in algae, fungi, bacteria, cephalopoda, and sea cucumber. From the past
Melanin few decades, great attention has been given to melanin and its derivative for the product development in the area
Marine organism
of medical, industrial, food and cosmetic industries. In addition, melanin plays an important in pharmaceutical
Melanin production
product development in antioxidant, anti-inflammatory, immunomodulatory, radioprotective, and gastrointes­
tinal benefits. In this review, we focus on melanin production from various marine species, summarized Puri­
fication and extraction strategies of various marine melanin with their analyzes and also their application in
medical and industries.

1. Introduction Allomelanins are the oxidation product of caffeic acid, 4-hydroxyphe­

Melanin is the broad term used to refer to a group of natural, dark-
colored pigments [1] and it is a simple and cheaply accessible
biopolymer that can be found in living organisms [2]. The meaning of
melanin is black which is derived from Greek melanos [3–7]. Melanins
are group of complex pigments [8–10]. Melanin is produced by the or­
ganisms in a process called melanogenesis, which includes the oxidation
of the amino acid tyrosine followed by polymerization. Eumelanin,
allomelanin, pheomelanin, and pyomelanin are the principal forms of
melanin [11–14]. Eumelanin, which is one of the most common types of
melanin, due to its functional groups and similarities in structures has
various properties of physiochemical with Polydopamine [15,16].
Eumelanin has a broad absorption spectrum that includes 400–700 nm
(visible wavelengths) and 100–400 nm (ultraviolet) [17]. The brown or
black pigment of eumelanin is the most common melanin product; it is
the oxidation product of the L-tyrosine and/or L-dihydroxyphenylalanine
(L-DOPA) amino acid [18–24]. Eumelanin serves important bio­
functional roles in a variety of living organisms [8,25]. Allomelanin is a
nitrogen-free pigment [26], which is also known as catechol-melanin
because it is derived from catechol [27,28]. they are known to be pro­
duced by phenoloxidase enzymes from phenolic compounds [29,30] and
nylacetic acid, dihydroxynaphthalene (DHN), catechols, γ-gluta­
minyl-4-hydroxybenzene, protocatechualdehyde, or tetrahydroxy
naphthalene [11]. Allomelanin presence is essential for increasing the
protection of organisms against environmental damage [26]. The
red-yellow pigment pheomelanin is formed from the combination of
L-tyrosine and/or L-DOPA with L-cysteine [11,21,31–33] and degrada­
tion studies and intermediate analysis show that it contains benzothia­
zine subunits [34,35] and also because pheomelanin is phototoxic and
produces a key intracellular antioxidant, it may be costly [36]. Neuro­
melanin is a dark brown, intracellular insoluble pigment [37,38] that is
present in brain and neural cells. It and it is made up of metal ions,
proteins, lipids, and melanin [39,40] that their pigment accumulates in
autophagic organelles [41–43]. Pyomelanin is a brown form of melanin
[44,45] that is created by homogentisic acid (HGA) oxidation [45–48].
Its molecular structure is similar to that of eumelanin [27,28]. pyome­
lanin pigment has the potential to be used in a variety of fields, including
cosmetics, medicine and pharmacology [49]. Fig. 1 summarizes these
different melanins and their biosynthesis.
Different enzymes play a role in producing melanin, but tyrosinase is
the most important and most frequent enzyme involved in melanin
synthesis [50–54]. It is responsible for catalyzing the oxidation of

* Corresponding author. Department of Marine Biology, Faculty of Marine Science and Technology, University of Hormozgan, Bandar Abbas, P.O. Box 3995, Iran.
Tel.: +98 76 33711000 11; fax: +98 76 33670716.
E-mail addresses: a.homaei@gmail.com, a.homaei@hormozgan.ac.ir (A. Homaei).

https://doi.org/10.1016/j.dyepig.2022.110214
Received 5 February 2022; Received in revised form 23 February 2022; Accepted 24 February 2022
Available online 2 March 2022
0143-7208/© 2022 Elsevier Ltd. All rights reserved.
K. Ghattavi et al. Dyes and Pigments 201 (2022) 110214

L-tyrosine to dihydroxyphenyl-L-alanine (L-dopa), and also the oxidation 3. Melanin analysis

of L-dopa to melanin [55–57]. Tyrosinases are mono-oxygenases with a
dinuclear copper site responsible for catalysis [11,58,59]. The reaction The commonly used analytical techniques for the structural identi­
pathways for the biosynthesis of the different melanins and their pre­ fication of melanin are Fourier transform infrared spectroscopy (FT-IR),
cursors are shown in Fig. 2. Nuclear Magnetic Resonance Spectroscopy (NMR), Mass spectroscopy
In general, melanin performs important physiological functions [60, (MS) combined with high pressure liquid chromatography (HPLC),
61]. In the biosystem, melanins have a significant range of roles [62,63] Thermal properties, Scanning electron microscopy (SEM), Transmission
in the field of biomedicine and biological functions [64,65] and also it is electron microscopy (TEM), Electron spin resonance (ESR), and pyrol­
a very hopeful drug due to its good biocompatibility and biodegrad­ ysis gas chromatography coupled with mass spectrometry detection (py-
ability [27]. Melanin is recognized eco-friendly and biocompatible since GC-MS) (Fig. 4). The list of sources and techniques used for melanin
it is normally synthesized by most species. Melanin has recently analysis is given in Table 2.
emerged as a practical additive that can significantly increase the effi­
ciency of traditional materials for a variety of purposes in materials
3.1. FTIR
science and green technology [66]. In this review, we discuss melanin
production by various marine species, summarize the various extraction
Wang and Rhim used FTIR (Fourier Transform Infrared Spectrom­
and purification strategies of marine melanins, discuss the different
etry) to characterize melanin isolated from the sepia ink. The broad peak
analytical methods to detect melanin, and, finally, highlight applica­
observed around 3100–3300 cm− 1 and a peak at ~2920 cm− 1 can be
tions of marine melanin in medicine and industry.
assigned to OH and aliphatic C–H groups stretching vibrations, respec­
tively [86]. The peaks related to the stretching vibrations of O–H and
2. Extraction and purification strategies to obtain marine
N–H groups, available in the extracted melanin structure as the amine,
melanin
amide or carboxylic acid, phenolic and aromatic amino functions,
appear in the range of 3600–2800 cm− 1. The characteristic strong band
The extraction and purification of melanin is highly dependent on
at ~1710 cm− 1 is attributed to C– – O stretching, and the ~1650 cm− 1
the melanin source (algae, fungi, bacteria, sea cucumber, etc). Since
band represents the vibrations of aromatic ring C–– C of amide I, and the
melanin is tightly bound to other cellular components, it can be a
symmetric stretching of COO- groups [92,123]. The appearance of the
challenging task to isolate pure melanin [67]. In an alkaline environ­
peaks at 1514 cm− 1 is related to the C–N stretching (amide II band) and
ment, melanin extraction is mostly achieved by a reflux method in a
N–H deformation, indicating that the pigment contains the typical
water bath or autoclave [68]. Table 1 and Fig. 3 illustrate the various
indole component of melanin. The aliphatic C–H groups of melanin
extraction and purification steps suggested for different forms of
appear around 1400–1500 cm− 1 [81]. Phenolic C–OH stretching is at
melanin.
~1200 cm− 1. The peak based at 1021 cm− 1 is the aliphatic structure

Fig. 1. Structure of different forms of melanin, and the substrates for their biosynthesis: Eumelanin (a), Pheomelanin (b), Allomelanin (c), Pyomelanin (d), and
Neuromelanin (e).

2
K. Ghattavi et al.
Fig. 2. The reaction pathway of melanin production.
indicator of the C–H in-plane, which is also a characteristic melanin
pigment peak. The peak observed at 950-750 cm− 1 is related to the ar­
omatic C–H group’s out-of-plane bending. The alkene C–H substitution
in the melanin pigment is due to bands below 700 cm− 1 [86,124].
3.2. NMR analysis
Sun et al. confirmed the molecular structure of melanin from
Auricularia auricula, by one- and two-dimensional NMR spectroscopy.
The results of their study showed that the melanin isolated from
A. auricula is a eumelanin, a macromolecular polymer of 5,6-dihydrox­
yindole and 5,6-dihydroxyindole-2-carboxylic acid. In the one-
dimensional 1H NMR spectrum of melanin, peaks were observed in
both aliphatic and aromatic regions. The peaks observed in the aliphatic
region at δH 0.5 ppm–2.5 ppm can be assigned to CH3, and CH2 alkyl
fragment groups. Carbons belonging to these groups appear in the 13C
NMR spectrum in the range of δC 15 ppm–40 ppm [96,125,126]. In
addition, the peaks appearing in the regions of δH 3.5–4.5 ppm can be
attributed to protons on electronegative atoms, oxygen and nitrogen,
attached to the carbon atom. The peaks appear in the aromatic region at
δH 8.29 (s) ppm and δH 7.02 and 6.73 ppm belong to the proton on the
pyrrole and benzene rings, respectively. Moreover, two-dimensional
1
H–1H correlation spectroscopy (COSY) was used to support the struc­
ture of melanin [126].
3.3. Mass spectrometry
Araujo et al. used mass spectrometry to identify the melanin
biopolymer of marine sponges. The result of their study showed that
there were significant differences between melanin from sponges from
various locations by the absence of peaks assigned to unique melanin
structures and also 5,6-dihydroxyindole (DHI) was found in the F, B and
G melanin mass spectra, but not in the commercial sample. In general,
results from mass spectra show that the different chemical compositions
evidenced by the respective melanin samples can be explained by
sponges belonging to different species and environmental factors must
also be identified to explain structural differences [98].
Palumbo also used mass spectrometry to prove the structure of Sepia
melanin. The result of their study showed that a mixture of strongly
cross-linked, irregular polymers like pyrrolecarboxylic acids, 5, 6-dihy­
droxyindole (DHI), 5,6-dihydroxyindole-2-carboxylic acid (DHICA)
3
Dyes and Pigments 201 (2022) 110214
exists of sepia melanin and at different states of oxidation and fairly
randomly, leucodopachrome and uncyclized dopa units connected to
each other and analysis of carboxyl content, consumption of ferricya­
nide, pyrrole-3, pyrrole-2,3,5-tricarboxylic acid and adsorption spectra
showed that the Sepia pigment is a combination of oligomeric structures
that included 20% of DHI derived units and over 75% of DHICA derived
units are included that it occurs mainly as pyrrolecarboxylic acids in an
irreversibly degraded form, probably [127,128].
This section is not sufficient data for melanin chemical character­
ization using Mass spectroscopy. Mass spectra provides sufficient in­
formation on molecular weight of the melanin. I suggest to add some
more sentences; how molecular weight is changing from one species to
another species using mass spectral data.
3.4. ESR spectroscopy
Another helpful technique for detecting melanin is electron spin
resonance (ESR), which provides information about melanin’s magnetic
properties [129]. Melanins are typically insoluble in a variety of organic
solvents and most of what we know today about melanin ESR spectra
comes from research of aqueous suspensions or dried powders [130]. In
the case of aqueous suspensions, the pH has a strong influence on the
signals. An intense and relatively sharp ESR resonant line is observed at
neutral and high pH. The ESR spectrum can be changed to higher
magnetic fields by lowering the pH of the solution, in addition to signal
broadening and intensity reduction which is due to changes in the
chemical balance of the systems’ paramagnetic centers [131,132].
3.5. py-GC-MS
Melanin pigments have been thoroughly investigated using py-GC-
MS (pyrolysis gas chromatography coupled with mass spectrometry
detection) due to their polymer-like structure [133–135] and, in gen­
eral, it can provide new information about the melanin structure [136].
By heating macromolecules to high enough temperatures to cause bond
breaking, this method analyzes the produced fragments. The degrada­
tion is repeatable and reproducible, and the pyrograms generated are
specific for the original analyte [67,137,138].
K. Ghattavi et al.
Table 1
Purification and extraction strategies to obtain marine melanins.
Source of Purification and extraction
melanin
a Algae 1 • A 5-liter algae culture was grown in LBSM
supplemented with 2 g of tyrosine for 12
days
• Production of pigments began at 72 h and
continued to increase until day 12
• The cell supernatant was acidified with 6
N HCl to a pH of ˂ 2.0 for partial
purification of the melanin, and, during 4
h, the melanin was permitted to
precipitate at 20 ◦ C
• The concentrated melanin was
transferred to a 8-kDa dialysis tube and
dialyzed in distilled H2O for 24 h with
four water changes during this period
• The dialyzed melanin was dried at 60 ◦ C
and then powdered
2 • Seaweed collection
• Microorganism isolation and strain
identification
• Optimization of production process and
growth kinetics
• 1 mol l 1 NaOH was used to extract the
cell-free supernatant (1 L)
• Autoclaved at 120 ◦ C for 20 min
• Centrifuged at 5000 g for 5 min
• To precipitate the melanin, the alkaline
colored supernatant was acidified with 1
N HCl to pH 2
• Centrifuged at 12000 g for 20 min
b Fungi 1 • The fungal disks were cut from the
margins of the colonies, boiled in 5 mL of
distilled water for 5 min and centrifuged
for 5 min (5000 g)
• By autoclaving the pellet with 3 mL 1 M
NaOH for 20 min at 120 ◦ C, the pigment
was extracted
• The of alkaline melanin extract was
acidified with concentrated HCl at pH 2.0
in order to precipitate melanin
• The precipitate was washed with three
times distilled water changes, and then
dried overnight at 20 ◦ C in a
dehumidified atmosphere
• The melanin was further purified by acid
hydrolysis (5 mL of 7 M HCl) for 2 h at
100 ◦ C in a sealed glass vial
• 3 mL of borate buffer (pH 8.0) was
applied to the supernatant after cooling
and centrifugation
• The absorbance was measured at 540 nm
using an UV/Vis spectrophotometer.
• The amount of melanin produced by
treated cultures of fungi was estimated
using the extracted melanin.
2 • Prepared spore suspension
• The inoculated cultures were incubated
for 14 days at 27 ◦ C with agitation at 150
rpm on an orbital shaker
• Fungal biomass centrifugation at 12,000
rpm for 20 min and then filtering (0.45-
μm, Whatman,)
• After adjusting the pH of the culture
filtrate to pH 2.0 with 6 M HCl, it was
statically incubated.
• After precipitating the melanin present in
the culture filtrate, the pellet was
separated by centrifugation at 12,000
rpm for 20 min
• To remove the unessential components,
the pellet was then acid-hydrolyzed in 6
M HCl at 100 ◦ C for 4 h
• The melanin pellet was re-collected by
centrifugation at 12,000 rpm for 20 min
Dyes and Pigments 201 (2022) 110214
Table 1 (continued )
Source of Purification and extraction Reference
Reference melanin
3 • Removal of culture biomass by [77,78]
[69,70] centrifuging it for 10 min at 5000 g
• Extraction of the resulting supernatant
with 1 M NaOH
• Autoclaving for 20 min at 120 ◦ C
• The supernatant was collected by
centrifuging the solution at 5000 g for 5
min.
• To precipitate the melanin, the alkaline
supernatant was acidified to pH 2
• Centrifugation at 12000g for 20 min
• The melanin was rinsed with 3 ml of
deionized water
4 • Fungal cells suspended in 1 M sorbitol- [79]
0.1 M sodium citrate (pH 5.5)
• Lysis using Trichoderma harzarium
enzymes followed by overnight
[71,72] incubation at 30 ◦ C
• Denaturation, protoplast collection,
centrifugation with 4 M guanidine
thiocyanate, at room temperature
• Centrifugation with proteinase K
• Particle boiling with 6 M HCl for 1 h
• Phosphate buffered saline and deionized
water were used to wash the resulting
material and to dry it at 65 ◦ C
c Bacteria 1 • Bacteria collected from the coastal area of [80,81]
the sea were spread on agar plates at pH 7
• These agar plates were incubated at 25 ◦ C
for 48 h with media and inoculum, and
[73,74] the black pigment was marked on the
agar plates
• In 250 mL flasks, about 10 μL (108 CFU/
mL) culture suspension was added to 50
mL of marine broth
• Placement of this medium at 25 ◦ C on a
rotating rotary shaker moving at 200 rpm
was incubated for 48–72 h until the
colored liquid medium was dark and
almost opaque
• After incubation, the medium was
centrifuged at 8000 rpm for 15 min to
separate broth and cells
• To collect supernatants, the cells were
centrifuged again.
2 • The Streptomyces sp. strain was inoculated [82]
in 250 mL Erlenmeyer flasks at 160 rpm,
30 ◦ C for 7 days.
• For 15 min, the broth was centrifuged at
5000 rpm, 4 ◦ C.
• The residue was mixed at a 1:5 (w/v)
ratio with 0.5 N NH4OH
• The mixture was centrifuged at 5000 rpm,
4 ◦ C for 15 min after being lysed with an
ultrasonic cell disrupter system at 800 W
[75,76] for 10 min.
• The supernatant was stored.
• The supernatant was adjusted to pH 2,
and centrifuged at 10 000 rpm 4 ◦ C for 15
min yielding crude melanin
3 • The marine bacterium was inoculated in a [83,84]
nutrient broth medium to produce
melanin.
• orbital shaking at 150 rpm for 48 h at
37 ◦ C
• Melanin was separated by centrifugation
(5000 rpm, 10 min)
• The medium was acidified to pH 2 for
precipitate out of melanin
4 • A 6-day culture was centrifuged, and the [85]
cell-free supernatant was acidified with 1
N HCl.
• Storage in dark place at 25 ◦ c for 1 week
• Boiling for 1 h, then cooling and
centrifugation
(continued on next page)
4
K. Ghattavi et al.
Table 1 (continued )
Source of Purification and extraction Reference
melanin
• 0.1 N HCl and double distilled water were
used to clean the pellets.
• pellets were washed in ethanol for 10 min
at 100 ◦ C
• Storage at room temperature for 24 h
• wash ethanol residue
d Sepia ink 1 • The ink was combined with a 5000 rpm [86,87]
homogenizer for 5 min and 5 times prior
to rinsing.
• The melanin was then extracted at 10000
rpm for 30 min using a centrifuge (This
process is repeated 3 times)
• the samples drying in oven at 40 ◦ C for
24h.
2 • The ink is washed 20 times with distilled [88,89]
water while on a stirring at 4 ◦ C.
• Centrifuging the ink (15 min, 10000 g,
4 ◦ C, n = 6)
• Melanin was derived through hydrolysis
and vacuum freeze-drying.
3 • Centrifuging the ink at 6000 rpm for 15 [90]
min
• To solubilize the pigment, the
supernatant was adjusted to pH 13 (10 M
NaOH), then to pH 2 (5 M HCl)
• Centrifuging melanin at 12,000 rpm for
30 min
• The precipitate was dissolved in a
solution of 10 M NaOH.
• the pigment precipitated (at pH 2)
• The melanin was washed with methanol,
then with 70% ethanol, and air-dried.
e Sea 1 • The dried sea cucumber 1:10 (W/V) ratio [91]
cucumber of 20 g of soaked sea cucumber was
homogenized with deionized water
• The pH of the protease was adjusted to
the optimum
• At 360 U/mL, three separate protease
forms, Trypsin, pancreatin, and pepsin,
were added respectively.
• The hydrolysis solution was centrifuged
at 8,000 rpm for 15 min after enzymatic
hydrolysis at the optimal temperature for
10 h, and the precipitate was dissolved
with 0.1 g/L NaOH.
• The pH of the supernatant was set to
approximately 2.0 for 30 min to fully
precipitate the melanin
• By centrifugation and vacuum drying,
crude melanin was obtained.
3.6. Thermal properties
One of the properties of microbial melanin that distinguishes it from
other natural polymers is its thermal stability, which can be attributed to
the polymer’s graphite-like structure [139]. According to Gomez-Marin
and Sanchez and also Sajjan et al., melanin displays a distinct pattern of
peaks [139,140]. In general, the endothermal peak (250 ◦ C) is related to
water vapor, the exothermic peak (350 ◦ C) is related to CO2 evaporation,
and melanin decomposition has been observed at temperatures greater
than 500 ◦ C [63,141,142].
3.7. Morphology of the surface
Microscopic techniques (SEM, TEM) are being used to determine the
morphological characteristics and particle size distribution of microbial
melanin. SEM is a useful technique for morphological characterization
and particle size distribution of various kinds of melanin [117]. Ac­
cording to surveys that Pralea et al. did, the granule morphology and the
size ranges from 30 to 1000 nm depending on the source of the melanin
5
Dyes and Pigments 201 (2022) 110214
[67]. One of the most important cellular biology technologies is the
TEM. It helps the investigation of the best high-resolution cell structures
with a resolution of 20 nm [121,143].
4. Marine resources of melanin
In recent decades, significant attention has been paid to natural
pigments from marine animals and organisms [144–146]. Marine or­
ganisms are rich in melanin which are very diverse in applications and
presented in Fig. 3 and Table 3.
Marine algae are eukaryotic species that are found in coastal areas
[147,148]. Based on pigments, marine algae are divided into three
groups such as Phaeophytes (brown algae), Rhodophytes (red algae),
and Chlorophytes (green algae), [147–152]. Marine algae produce sec­
ondary metabolites to survive in the environment [153–155], and the
important secondary metabolites are organic compounds, proteins, fatty
acids, lipids, pigments etc. [156–158]. These marine algae secondary
metabolites are extensively studied for different biological and
biomedical applications [159]. Melanins from marine macroalgae have
the ability to protect against UV rays [44,69,71].
Melanin pigments from fungi are an important resource from marine
organisms [7]. [74]. Marine fungi contain different forms of melanins
(black or dark brown), pheomelanins (yellow or red), and the most
heterogeneous group of alumlanins, including soluble pyomelanins and
melanin composed of dihydroxynaphthalene (DHN) compounds. Marine
fungi are adaptable to extreme salinity and can adopt to any environ­
mental condition [1,160,161]. It has been reported that melanin in fungi
is involved in a variety of virulence-associated functions [7,162–164].
Antarctic fungi can produce pigments, which include melanin and ca­
rotenoids [165].
Bacteria are widely available and distributed in all marine environ­
ments [166]. Bacteria produce a variety of enzymes, vitamins and
anti-tumor substances and etc [167,168]. More than a century ago, the
production of black pigments in bacteria was discovered and linked to
the metabolism of tyrosine [169]. Several forms of melanins including
phaeomelanins, pyomelanins, allomelanins and eumelanins, have been
identified in bacteria [170,171]. However, complex biological functions
and the regulation of melanin synthesis are recently explored and
investigated [169].
Cephalopoda is a class of molluscs which appeared around 500
million years ago and in many different oceanic ecosystems [172,173].
It includes cuttlefish, octopus and squid [174,175]. However, they are
underexplored marine products for commercial applications [172,176].
All the Coleoidea orders have ink sacks and they can produce ink.
Cephalopod ink is made of two-gland secretions. The ink sac produces a
black ink that contains melanin with its ink gland [172]. Melanin is
~15% of the total wet ink in its body weight [177,178]. The ink present
in cephalopods is Eumelanin [119,179], which has a dark brown color
[180–183]. From scientific studies, squid inks have several uses in
different pharmaceutical applications [172].
Sea cucumbers are invertebrates that belong to the phylum Echino­
dermata and belong to the Holothuroidea family [184–186]. Most sea
cucumbers feed on sediments and play an important role in the aqua­
culture system and act as environmental cleaners [184,187]. Sea cu­
cumbers produce many active substances and bioactive compounds [91,
188,189]. One of them is melanin, on which only few studies have been
performed [91]. In the body wall of marine cucumbers, five biological
pigments were found; among them, melanin plays a key role, since
increased secretion and melanin production contributes to better de­
fense and growth of sea cucumbers. Studies have shown that
deeper-colored sea cucumbers include more melanin [190].
5. Application of melanin
The number of applications of marine melanins in pharmacy and
biotechnology is substantial. Some of the important uses of melanin are
K. Ghattavi et al. Dyes and Pigments 201 (2022) 110214

Fig. 3. Schematic Purification and extraction strategies of various marine melanins: Algae (a), Fungi (b), Bacteria (c), Sepia ink (d) and Sea cucumber (e).

6
K. Ghattavi et al. Dyes and Pigments 201 (2022) 110214

Fig. 4. Different analysis for identification of melanin.

summarized in Fig. 5.
Table 2
List of sources and techniques used for melanin analysis.
6. Applications of melanin
Source Technique Reference

Sepia ink FTIR, SEM, Thermal properties [86] 6.1. Antioxidant activity, biomedical and packaging applications of
Sepia melanin FTIR [92] melanin
Squid Ommastrephes bartrami Mass spectrometry, NMR, py-GC- [93–95]
MS
Sepia ink FTIR, NMR [96] An ingenuous, emerging application of melanin is antioxidant-active
vibrio alginolyticus NMR [97] packaging, which is a packaging method that contains antioxidants that
Sponge melanin FTIR, Mass spectrometry, SEM [98] can provide a sustained release of antioxidant during storage.
Aspergillus nidulans sp FTIR, Mass spectrometry, NMR [99]
Antioxidant-active packaging can delay lipid oxidation, thereby
Azotobacter chroococcum FTIR, NMR [100]
Sepia melanin FTIR [101] extending the shelf life of food products [238]. Increasing the usage of
Sepia ink FTIR [102] melanin in biotechnological and food sectors due to non-toxic, and
Shewanella algae BrY FTIR [69] important physiochemical properties [239]. Melanin prevents food
Sepia officinalis NMR [103] spoilage due to its antimicrobial properties, and melanin used as a food
Shewanella colwelliana D. Mass spectrometry, NMR [104]
Streptomyces rochei Mass spectrometry, NMR [105]
coloring agent [109,216,225,228,229]. Melanin is a powerful antioxi­
Thalassotalea sp. PP2-459 NMR [106] dant because of its intramolecular non-covalent electrons, which easily
Bacterium Bacillus sp. Mass spectrometry, NMR [107] interact with reactive species and free radicals [86,240]. Wang and
Marine macroalgae-associated FTIR, Mass spectrometry, NMR [108] Rhim and also Shankar, reported that melanin can be used to enhance
heterotrophic bacteria
and improve the stability of oxidation-sensitive products by incorpo­
Marine bacteria FTIR [109]
Aglaophenia latirostris FTIR, Mass spectrometry [110] rating melanin into packaging films and as food additive. Melanin, in
Pseudomonas stutzeri FTIR [111] general, has the ability to prevent and protect against damage or loss
Nocardiopsis Sps FTIR [112] caused by reactive oxygen species [86,241]. Furthermore, melanin has
Providencia Rettgeri Strain FTIR, NMR [113] been shown to significantly increase the activity of antioxidant enzymes
BTKKS1
that could reduce the amount of lipofuscin in the nervous system and
Ornamental fish FTIR [114]
Pseudomonas stutzeri BTCZ10 FTIR, NMR [115] brain, preventing aging [242,243].
Eurotium rubrum Mass spectrometry, NMR [116]
Microbial melanin py-GC-MS, NMR, FTIR [63]
Sepia ink SEM, TEM [117–120] 6.2. Antimicrobal activity
Pseudomonas sp. Mass spectrometry, Thermal [80]
properties
Bacterial and fungal pathogens have a negative impact on food
Sepia officinalis SEM, TEM [121]
Fungi, plants, and animal sources ESR, py-GC-MS, Thermal [122]
storage facilities and medical equipment, as well as having a negative
properties, SEM, TEM, FTIR effect on the body of humans [242]. Marine melanin has antimicrobial
and antifungal properties 175,181. Shankar and Liu, as well as their col­
leagues, identified melanin as a significant antimicrobial agent against

7
K. Ghattavi et al. Dyes and Pigments 201 (2022) 110214

Table 3 Table 3 (continued )

Marine resources of melanin and their applications. NO. Species Applications References
NO. Species Applications References
Absorption of heavy
1 Algae Gelidium spinosum Photoprotective [191] metals
Wound healing 8 Thalassotalea sp Cosmetics, [106,166,
2 Sehwanella algae UV resistant [69, Pseudomonas sp depigmentation 222]
BrY 192–195] properties
3 Chlorogloeopsis spp Prevention of [196] 9 Vibrio natriegens Protection of UV [223]
damage from UVA irradiation
and UVB radiation 10 Bacillus spp. Anti-inflammatory [224]
4 Himanthalia Anti-microbial [197] BTCZ31 and ntioxidant
elongata 11 Actinoalloteichus sp. Antioxidant activity [225]
5 Isochrysis galbana Antibacterial [166,198] MA-32 and antibacterial
Chlorella marina activity
Nannochloropsis 12 Vibrio alginolyticus Antibiofilm and [97]
oculata anti-inflammatory
Dunaliella salina 13 Streptomyces sp. Antibacterial [114]
Pavlova lutheri MVCS13 activity
6 U. pinnatifida Antioxidant activity [199] 14 Pseudomonas Anti-biofilm [224]
stutzeri BTCZ10
1 Fungi Antarctomyces Colorant [200] 15 Pseudoalteromonas Anti-biofilm [226]
pellizariae tunicata
2 Schizophyllum Antibacterial and [201]
commune antifungal activity 1 Cephalopoda Illex argentinus Antitumor activity [227]
3 Aspergillus nidulans Anti-inflammatory [99,202] 2 Arroz negro Food coloring in [228,229]
activity, UVB txipirones en su tinta food industry,
protection ikasumi jiru antimicrobial
4 Hortaea werneckii Antibacterial [203,204] activity
activity 3 Sepiella maindroni Anticancer activity [230,231]
5 Crypotoccus Sunscreens, [204–206] 4 Sepia officinalis Antibiofilm activity [64]
neoformans melanoma, 5 Octopus vulgaris antiulcer activity [232]
Aspergillus cosmetic, Ommastrephes
fumigatus Radioactive waste bartrami
Colletotrichum immobilisation,
1 Sea Stichopus japonicus Antioxidant [184,
lagenarium such as uranium
cucumbers activity, anti- 233–235]
Paracoccidioides
melanogenic
brasiliensis
activity
Magnaporthe grisea
2 Apostichopus Antioxidant activity [190]
Sporothrix schenckii
japonicus
6 Streptomyces Antioxidant activity [207]
3 Stichopus Wound healing [236,237]
glaucescens NEAE-H and anticancer
chloronotus
activity
7 Yarrowia lipolytica Antibiofilm and [208,209]
additives to color
with antifungal
both gram-positive and gram-negative bacteria [241,244] and also
effects Mackintosh and coworkers reported that melanin has been shown to
8 Aspergillus Antifungal [210] have antimicrobial properties, inhibiting and preventing the growth of
fumigatus fungi, bacteria, and other parasites of the dermis and epidermis [245].
Aspergillus flavus
Aspergillus niger,
Aspergillus tamarii 6.3. Anticancer activity
9 Dichotomomyces Antivirus [211]
cejpii F31-1
10 Periconia abyssa Anticancer [212,213]
Artificial pigments endanger human health and increase the risk of
11 Eurotium rubrum ———— [214] liver, bladder, and skin cancer. Moreover, the components used, as well
Talaromyces as the waste produced during the manufacturing process, are harmful for
albobiverticillius the environment. Bio-pigments, such as melanin, are both environ­
12 Aspergillus nidulans Antioxidant activity [99]
mentally friendly and constitute an effective treatment option for can­
sp and UVB protection
cer. According to the results of Russo and coworkers, purified tyrosine
1 bacteria Colwelliana As colorant in food [215,216] from the ink’s melanin-free fraction is toxic to transformed human cell
alteromonas and anticancer
Nigrifaciens properties
lines [246]. Studies and researches on mice showed that sepia ink helps
cellulophaga to prevent or stop cancer by helping to promote the activity of killer cells
2 Pseudoalteromonas Anti-biofouling [217] [247].
lipolytica activity
3 Vibrio cholerae Anti-biofouling [218]
activity 6.4. Sunscreen
4 Bacillus anthracis, UV protection [219]
5 Pseudomonas Resistant to [220]
One of the most damaging factors to human skin is direct sunlight
aeruginosa photodynamic
oxidative stress
exposure [60]. Therefore, sunscreen should be used to prevent skin
6 Legionella Increasing [221] damage. Most sunscreens are chemical and have the ability to penetrate
pneumophila bioavailability of the skin that causes DNA damage [248,249]. By filtering ultraviolet rays
iron (heavy metal) and absorbing reactive oxygen species (ROS), melanin reduces UV ra­
7 Pseudomonas Used in commercial [83,115,
diation damage in the body, thus protecting the cell nucleus and DNA
stutzeri sunscreens, 169]
damage [250,251]. Kurian and Coworkers examined the biological
properties of melanin and use it in healthcare. The results of their study
showed that melanin has anti-inflammatory properties and can increase

8
K. Ghattavi et al.
Fig. 5. Source and various applications of marine melanins (a), applications of marine melanins (b), antibacterial activity (c) and UV protection (c).
the effects of ultraviolet absorbent effects of sunscreen [115].
6.5. Wound healing properties
Biologically active compounds derived from marine sources cause
wound healing and tissue regeneration because they have skin-
compatible molecules [252]. Poulose et al. used spongy bacterial
melanin and seaweed concentrate and examined the method of wound
healing and the results of their research showed that melanin-seaweed
cream has a very effective role in wound healing [191].
6.6. Melanin as a heavy metal remover
Today, heavy metals are a significant human concern because of
their bioaccumulation, and toxicity [253]. The use of melanin for the
removal of heavy metals is in its early stage [254] and because of mel­
anin’s ability to interact with metals, it can be used in bioremediation of
contaminated water or for the recovery and identification of valuable
and useful heavy metals from solutions [31,111]. Thaira et al. extracted
melanin from marine bacteria and studied it to investigate the removal
of heavy metals. They showed that, from very low initial concentrations,
melanin nanoparticles could adsorb various heavy metals such as
chromium, selenium, and lead [77] and also Manirethan et al. derived
melanin nanoparticles from the marine bacterium Pseudomonas stutzeri
to investigate the removal properties of heavy metals, their result indi­
cate that even at low concentrations, melanin has a strong potential for
removing heavy metals from the aqueous system and has a tremendous
potential to be used in large-scale continuous mode activities [77].
9
Dyes and Pigments 201 (2022) 110214
6.7. Melanin as a battery
Young Jo Kim extracted melanin electrodes with PTFE from Sepia
officinalis, and showed that nanoparticles of melanin act as sodium-ion
energy storage devices and according to structural stability of melanin in
water and the substantially high density of catechol groups were pro­
posed for use of eumelanin half-cell of reversible Mg2+ ion charge-
discharge [255,256]. Melanin has also been suggested to be used as
sensors, batteries [27] and that it can act as an electron acceptor [192,
193,195].
6.8. Melanin as a solar-thermal system
In modern renewable energy science, high-efficiency solar harvest­
ing and solar-thermal conversion have been targeted for broad useful
uses. To enhance the solar thermal effect of bio-melanins, Zong et al.
showed that alginate, an abundant marine polysaccharide of brown
algae, could be used as a structural guide to modulate polydopamine
nanostructures from nanospheres to nanofibers. These biological nano­
fibrils promise great potential for high-efficiency solar energy consid­
ering their sustainability, biocompatibility, easy-availability and low
prices [98,257].
7. Potential use of melanin
Melanin is a multipurpose biological pigment that is widely used
[258,259]. One of the potential uses of melanin is to increase the visi­
bility of structural colors, which a black background is used to improve
K. Ghattavi et al.
the visibility of structural colors and also It is used in the fabrication of
spherical photonic materials, with a three-dimensional structure made
of colloidal particles using the membrane emulsification method [76,
260]. Melanin is used in fluorescent probes and photothermal therapy
due to its high biocompatibility and non-toxicity [261]. The results of
d’Ischia research in 2014 showed that eumelanin is used as a useful tool
for evaluating structural models in computational modeling techniques
in the design and optimization of optical properties [262]. Melanin plays
a very important role in protecting against photo and ionizing radiation.
In general, different melanin community offer distinct chemical prop­
erties that lead to new discoveries based on innovative materials [263].
8. Conclusions and future perspectives
The present review shows that melanin is widely used due to its
excellent biocompatibility and biodegradability, and that it is a good
candidate for environment. Melanin has a broad range of applications in
the medical science such as antioxidant activity, wound healing, anti­
microbial activity, anticancer activity, antibiofilm activity, anticancer
activity and sunscreen and also it has been used in industry as heavy
metal remover, battery, solar-thermal system, sensor, electron acceptor
and also food coloring in food industry and packaging. Melanin as a
pigment has attracted significant attention because it can be manufac­
tured on a large scale and at low cost, and is generally commercially
viable. Clinical and preclinical evaluation of melanin is required for
commercial product development in pharmaceutical applications. Based
on the scientific findings on melanin in industrial applications, there will
be a huge demand for melanin products. A better understanding of the
chemical structure of marine melanin will allow for a more complete
definition of the basic structures, as well as their intrinsic physico­
chemical characteristics, in order to get the most out of their prospective
applications, so it is suggest that melanin chemical structures should be
further examined and also optimization extraction procedures of marine
melanin, as well as short-term and long-term toxicity assays it should be
done and evaluate. Therefore, we hope that this review will be helpful
and promote researches on melanin, in particular from marine
organisms.
Ethics approval and consent to participate
Not applicable.
Consent for publication
Not applicable.
Availability of data and materials
All data were included in the manuscript.
Funding
This work has not been funded in the form of grant.
Authors’ contributions
This manuscript was written through contributions of all authors
listed.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
10
Dyes and Pigments 201 (2022) 110214
Acknowledgement
The authors express their gratitude to the research council of the
University of Hormozgan for financial support during the course of this
project.
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