INTRODUCTION

These days nanotechnology may be a fast-growing field with its applications in

inquire about. Nanoparticles having measure ranges from 1 to 100 nm have
found different approaches completely different regions like mechanical [1, 2],
natural [3], biomedical [4], agribusiness [5] and nourishment [6–8] since of their
special and predominant basic physical and chemical properties such as higher
outward zone, mechanical quality, optical dynamic and chemical receptive [9,
10]. The most important use of nanoparticles in the industrial area is their ability
to protect metals against corrosion in a variety of conditions [11, 12]. Metals are
employed as a basic material or raw material in industries and other fields
because of their appealing properties such as electrical and thermal conductivity,
higher melting and boiling points, greater tensile strength, high mass-to-volume
ratio, and ductility.

Corrosion is a natural process that causes a variety of losses, especially in the

sector of industry, owing to the deterioration of metal structures and machinery
[13]. Corrosion is a slow, nondemolished process that affects most metals found
on Earth, such as aluminium, mild steel, and copper, which have a wide range of
applications in industries, automobiles, home construction, and shipping,
resulting in significant economic and resource losses in various sectors by
affecting their tensile strength and physical and chemical properties [14,15].

Organic coatings are the most widely used corrosion protection technology, and
their cost can account for up to two-thirds of overall corrosion protection
expense [16]. Traditional organic coatings, on the other hand, are prone to
different sorts of damage during transit and service applications, including
microcracks, pinholes, cavities, mechanical scrapes, and scratches. As a result,
organic coatings frequently require repair and replacement to retain their
protective benefits, especially when utilised in strong corrosive conditions. Self-
healing coatings were initially proposed in the 1980s to minimise the frequency
of repairs and related expenses [17], and they are still a hot issue in corrosion
research today. These coatings function exceptionally well and improve the
long-term corrosion resistance of the materials to which they're applied [18-21].

Self-healing activities in corrosion protective coatings can be performed by

intrinsic or extrinsic healing processes, or both. Intrinsic self-healing is based on
the coatings' unique molecular architecture and so does not necessitate the use of
an external component.

The initial execution of harmed coatings can be recouped by

reversible responses such as the Diels–Alder response [22, 23], disulfide bond
[24], trithiocarbonate reshuffling response [25], hydrogen bond [26, 27],
or energetic urea bond [28] beneath outside jolts such as light, chemicals,
temperature, or mugginess changes.

The capacity of intrinsic self-healing coatings to reestablish barrier qualities, even

after several damage-healing cycles, is one of its main advantages. The needed
reversible processes, on the other hand, are dependent on certain functional
groups, and their synthesis might be prohibitively expensive and difficult for
commercial use. Extrinsic self-healing coatings, on the other hand, may be easily
repaired by releasing conveyed healing ingredients such as polymerizable
polymers and corrosion inhibitors to the damaged area of the coating. The healing
chemicals are mostly kept in micro/nanocarriers or microvascular networks,
which avoid unwanted interactions with the bulk coating and allow for on-demand
and controlled release [29]. Micro/nanocarriers are frequently engineered to
actively recover the coating's protective function by releasing the encapsulated
healing agents in response to environmental changes. Furthermore, as compared
to micro/nanocarriers, penetrating the coating with a microvascular network may
effectively boost the coverage of healing agents. However, this method carries the
danger of developing additional interfacial flaws that act as conduits for water
penetration, lowering the coating matrix's barrier qualities. As a result, this
method is less commonly used for corrosion prevention applications.

Many innovative solutions have been presented as a result of the fast development
of self-healing coating systems [30-35]. The goal of this research is to present an
updated assessment of the latest advances in the diversified micro/nanocarriers
used for self-healing corrosion protection coatings.

Encapsulation
Nanoencapsulation is defined as the packaging of solid, liquid, or gas
nanoparticles (also known as the core or active) into a secondary material (also
known as the matrix or shell) to produce nanocapsules (see Fig. 1) [36]. The
active element (e.g., pharmaceuticals, fragrances, biocides, vitamins, etc., see
Table 1) is contained in the core, while the shell isolates and protects the core
from the outside world. This barrier can be permanent or temporary, in which case
the core is released by diffusion or in reaction to a trigger like as shear, pH, or
enzyme activity, allowing for regulated and timed delivery to a specific location
[37,38]. Nanocapsules can range in size from 1 to 1000 nm and come in a variety
of forms, depending on the materials and procedures used to make them [37]. The
structure of encapsulated components (see Table 1) may be classified into two
basic groups (see Fig. 2): capsules with (a) a core entrapped inside a continuous
network of the matrix material or (b) a core surrounded by a shell of the matrix
material. Capsules with several cores or multilayered capsules are examples of
these morphologies [36]. The most important property of nanocapsules, however,
is their nanoscopic size, which allows for a vast surface area. The capsule
diameter is inversely proportional to the overall surface area. This huge surface
area is ideal for integrating recognition species (peptides, antibodies, organic
polymers, and so on), adsorption and desorption sites, chemical processes, and
light scattering, among other things. Encapsulating matrices can be made of a
variety of materials, which must be chosen based on the crucial qualities required
for each application (see Table 1). Proteins (lecithin, legumin, gelatin, and
albumin) are the most common carriers, followed by polysaccharides (dextrin,
starch, gums, chitosan, and alginates), fats, liposomes [39], biopolymers, co-
polymers (poly(lactic-co-glycolic acid), micelles, organogels, dendrimers, solid
nanoparticles (SLN), polymeric [40]. The primary motivation for
nanoencapsulating species is to guarantee that the encapsulated material reaches
the region of action without being harmed by the external environment.

Technique of microencapsulation

The most appropriate combination of parts and procedures must be chosen when
developing an encapsulation system for a certain application. Some of these
critical parameters have been proposed by Jafari et al. (2015) and Gómez-
Mascaraque et al. (2015).

1. Physical characteristics such as transparency, opacity, colour, and so forth.

2. The proposed structure's rheological characteristics and flow behaviour

3. The product's flavour and mouthfeel.

4. Stability: During storage, the chemical and physical stability of the

encapsulated substances.

5. Biological functionality: upon ingestion at an appropriate place in the

gastrointestinal system, the nanocarrier releases bioactive components.

Furthermore, the properties of the particles used in encapsulation systems are

(Dons et al., 2011; Khayata et al., 2012; McClements and Li, 2010; Sáiz-Abajo et
al., 2013): digestibility, chemical structure of particles, particle size distribution,
charge density, permeability, and resistance to unpleasant conditions such as pH,
temperature, and enzymes. Another factor that determines the amount and pace of
release is the degree of environmental resilience of the biopolymer components
(Chakraborty et al., 2009). Despite the fact that a variety of encapsulation systems
have been produced and documented, there is still a lack of thorough
understanding of the fundamental elements, making efficient system design for
specific applications somewhat of an invention (Fathi et al., 2014). There are still
questions concerning the extent to which exposure to extreme circumstances
might harm some particularly delicate molecules (proteins, enzymes, DNA, and so
on) (Clarke and Jayasinghe, 2008). Droplets from the core are the focus of several
encapsulation systems (in gas, liquid, or powder form). Following that, the
external agent coats the generated droplets through several physicochemical
processes.

Encapsulation of bioactive substances consists of three stages:

1. formation of the host molecule around the core material;

2. ensuring that no unwanted leakage occurs; and

3. ensuring that no unwanted components are integrated into the capsule.

Traditional techniques for microencapsulating food components exist, but none of
them are suitable with the whole core materials or product applications.

As previously said, the microencapsulation method is decided by the application

and criteria such as the desired particle size, physicochemical features of the
exterior and interior phases, release mechanisms, overall cost, and so on (Jafari et
al., 2008; Sobel et al., 2014; Zuidam and Nedovic, 2010). Because the
encapsulated chemicals are generally in a liquid condition, drying methods are
often used to convert the liquid phase to a stable powder form. Spray drying,
spray chilling, spray cooling, extrusion, fluidized bed coating, centrifugal
extrusion, freeze drying, coacervartion, interfacial polymerization, molecular
inclusion, and other processes are widely used to encapsulate active chemicals in
food products and nutraceuticals.

Micro/nanocarriers can be made in a variety of ways, both physically and

chemically. Solvent evaporation, spray drying, centrifugal extrusion, the spinning
disc process, and fluid bed coating are some of the physical procedures. In situ
polymerization, interfacial polymerization, centrifugal force techniques, submerged
nozzle procedures, and phase separation are some of the chemical methodologies
[41]. The structure and characteristics of micro/nanocarriers have a significant
impact on the extrinsic self-healing coatings' performance. In general, as-prepared
micro/nanocarriers should have the following characteristics: (1) chemical and
mechanical stability, (2) high loading capacity, (3) compatibility with the coating
resin, (4) appropriate size and structure, (6) ability to sense damage or corrosion,
and (7) release behaviours tuned in with damage development [42].
Solid micro/nanoencapsulation procedures, such as in situ polymerization,
interfacial polymerization, Pickering emulsion polymerization, sol-
gel response strategy, dissolvable vanishing, and the
other progressed epitome strategies, that can fulfill these execution necessities, are
briefly depicted within the ensuing segments. The included micro/nanocarriers are
categorized as micro/nanocapsules, micro/nanocontainers, or other inhibitor hosts.
Nanoencapsulation techniques: Similarly, an understanding of the physicochemical
properties of the center and variables that control the interfacial
and conglomeration behavior of the framework materials
is vital to select appropriate forms for nanoencapsulation [43]. Active species are
now nanoencapsulated using a variety of ways. Chemical, physicochemical, and
physicomechanical encapsulation methods are the three primary categories of
encapsulating techniques [44]. Chemical and physicochemical procedures refer to
approaches that include chemical reactions in the creation of nanocapsules. In
contrast, no chemical processes are involved in the synthesis of nanocapsules in
physicomechanical procedures, and only shape fabrication is normally done. Some
of the most widely utilised approaches are briefly reviewed here (see Table 2).

Table 2 Several nanoencapsulation techniques and the steps involved in each process
Methods of Nanoencapsulation Process involved
Sol–gel (a) Solution of core and polymer
(b) Formation of Sol phase
(c) Gelation
(d) Solidification
In situ polymerization (a) Preparation of core solution
(b) Addition of droplets of monomer
Coacervation (a) Formation of a three-immiscible chemical phases
(b) Deposition of the coating
(c) Solidification of the coating
Rapid expansion of supercritical (a) Preparation of solution of core and shell materials in CO2
solution (b) Depressurization through a nozzle
Liposome entrapment (a) Microfluidization
(b) Ultrasonication
(c) Reverse-phase evaporation
Inclusion complexes Preparation of complexes by mixing or grinding
Spray-drying (a) Preparation of a dispersion
(b) Homogenization of the dispersion
(c) Atomization of the dispersion
Solvent evaporation (a) Preparation of solution of polymer and core
(b) Solvent evaporation by heating
Electrocoextrusion (a) Preparation of core solution and wall solution
(b) Simultaneous spraying of two solutions from two coaxial
capillaries

Types of nanoencapsulation techniques: Global trends are shifting away from

large-scale food production based on the abundance of natural resources on the
planet to small-scale production based on green processes and novel technologies
to produce and distribute food products to consumers all over the world.
Nanoencapsulation technologies are allowing for the production of more complex
and technologically sophisticated food items in this way. Nanotechnologies are
expected to have an influence on all parts of the food chain, beginning with
production (agricultural, cattle farming, pisciculture), and continuing through all
intermediate processes of processing, packing, storage, distribution, and consumer
sale [45]. It is vital to establish techniques to enhance the functioning of the
selected foods in order to generate new food items. The most popular technique
for doing this is to add natural chemicals with high biological activity and a
 demonstrated positive effect on human health to food items [46]. Various types of
nanoencapsulation methods and nanocarrier systems have been developed in this
regard. Colloidal and non-colloidal systems are two types of nanocarrier
technology.

2.1 Polymerization in situ

The most prevalent process for encapsulating core materials is in situ

polymerization, which has a number of benefits, including ease of operation,
controlled capsule size and shell thickness, cheap cost, and appropriateness for
upscale production. However, as compared to other encapsulating methods, this
method necessitates a longer response time, often several hours. In situ
polymerization of poly(urea-formaldehyde) (PUF) as the shell material, for
example, was used to make microcapsules containing dicyclopentadiene (DCPD)
monomers [47]. Figure 1 illustrates a typical microcapsule preparation method.
The diameters of the microcapsules formed ranged from 10 to 1000 m, and the
shell thickness was regulated at 160–220 nm by adjusting the agitation speed
between 200 and 2000 rpm.

Fig. 1. Schematic representation of the synthesis of microcapsules using in situ

polymerization.

2.1 Interfacial polymerization

Interfacial polymerization is
another broadly utilized strategy to typify mending operators. Amid interfacial
polymerization, the shell prepolymers are broken up within
the center fabric (i.e., mending agent or corrosion inhibitor), and after
that this blend is blended with the watery stage. Another polymerizable monomer
or curing operator is included to the mixed-phase. In this way, the
polymerization response takes put quickly at
the watery or natural interface, subsequently creating micro/nanocapsules with
the recuperating operator or inhibitor as the center. This
capsulation strategy has numerous preferences, such as
(1) mellow response conditions,
(2) quick epitome,
(3) tall embodiment proficiency, and
(4) controllable capsule estimate (3–30 μm) [48, 49]. In any case,
the arranged capsules by and large contain unpolymerized shell monomers, which
may respond with the center fabric, in this manner affecting the execution of the
microcapsule.

2.2 Pickering emulsion polymerization

The term Pickering emulsion was to begin with set up by S.U. Pickering in
1907 [50]. Be that as it may, it was not until 1996 that Velev et al.
[51] illustrated the potential of this strategy as an epitome strategy. For the
most part, the Pickering emulsion polymerization strategy contains two
steps: (1) arrangement of a Pickering emulsion and (2) epitome of
the center fabric. In brief, the colloidal particles are to begin
with collected at the water/oil interface by mechanical activity to
create a steady Pickering emulsion. Another, the colloidal particles are
cross-linked through a chemical response to make a compact shell divider.
In differentiate to conventional surfactant-based emulsions, the Pickering
emulsion has a few alluring highlights, such
as tall soundness (concealment of beads coalescence), moo harmfulness, m
oo fetched, and reusability, making it an amazing candidate for
microencapsulation. In expansion, numerous colloidal particles can be
utilized as shell materials with polymer microspheres and inorganic
micro/nanoparticles. In addition, the mechanical execution of the shell can
be directed by altering the molecule measure and immobilization strategy.
At the same time, it ought to be famous that the penetrability of the
shell divider can too be effectively controlled by altering the measure of
 the voids between the colloidal particles [52], which may propose a
controlled-release instrument for the microcapsules.

2.3 Solvent evaporation

Within the dissolvable vanishing strategy, the shell fabric is to begin with broken

down in a water-insoluble unstable dissolvable, such as dichloromethane.
The center substance is then dispersed or broken up within
the arrangement gotten. Hence, the arrangement is gradually included to
an watery arrangement containing a stabilizer, such as poly(vinyl liquor) (PVA),
and encourage blended to create micro-sized polymer beads containing
the center substance. The method of solidifying of the
shell divider is fulfilled after the expulsion of the unstable dissolvable from the
polymer beads, regularly at elevated temperatures
or beneath decreased weights. Subsequently, as the mixing continues, the
polymer beads continuously solidify to create the
ultimate micro/nanocapsules. Not at all like other epitome strategies,
the dissolvable vanishing strategy includes exceptionally basic and gentle plannin
g conditions [52]. Be that as it
may, amid the dissolvable vanishing handle, numerous parameters (such as
monomer concentration, scattering rate, and core/shell proportion) must be
carefully considered and controlled. A comprehensive understanding of
the related among these parameters is required to absolutely tailor the
capsule estimate, shell thickness, shell compactness, and surrender. In addition,
this method is more doable for strong center materials than for fluids [53].

2.3 Sol-gel reaction

The sol-gel strategy is the most strategy for planning inorganic

micro/nanocarriers beneath gentle conditions. In self-healing materials, sol-
gel chemistry has been primarily utilized to get ready silica-based
micro/nanocontainers, since silica shells can offer
an viable obstruction for keeping up the chemical action of
the mending specialists. In a commonplace sol-gel strategy,
the natural components are to begin with scattered in an fluid stage. At that
point, the emulsified beads are gotten utilizing either
 a energetic disturbance or a reasonable surfactant/emulsion. The
emulsified beads work as a miniaturized scale reactor
and give appropriate conditions for the response of the silicon-based
monomers, in the long run driving to the arrangement of a suspension
containing sol particles. Utilizing the sol-gel strategy, the
oil, watery arrangement and solid-phase particles can all be typified into
the silica holders. In any case, it is worth noticing that miniaturized
scale absconds (pores and splits) may shape on the shell of the holders after
drying. In expansion,
this methodology is ordinarily utilized to plan nanoscale holders,
which enormously limits the stacking capacity (~10 wt%) of
the mending specialist, driving to trouble in repairing huge harms [53]
Based on the sol-gel response, Stöber and his associates proposed
a strategy for planning strong silica microspheres by hydrolytic
condensation of tetraethoxysilane
(TEOS) beneath antacid response conditions [54]. This strategy has
been broadly utilized and altered to manufacture mesoporous silica or other
inorganic (e.g. TiO2) empty circles as micro/nanocontainers.

2.4 Precipitation-based methods

Polymerization-based and solvent evaporation procedures are utilised to make
organic capsules, whilst sol-gel methods are employed to make inorganic silica
micro/nanocarriers. A variety of inorganic micro/nanocarriers can be easily
generated by precipitating them from aqueous or organic solutions, in addition to
these approaches. Layer-double hydroxides (LDHs) and zeolitic imidazole
frameworks (ZIFs) are two forms of inhibitor hosts discussed in this paper.
LDHs are a kind of lamellar ionic compounds made up of emphatically charged
layers isolated by an interlayer containing solvation atoms and charge-
compensating anions [55]. The foremost normal strategy for planning an LDH is
to co-precipitate divalent and trivalent metal salts in
an soluble arrangement containing the target anions in an worthy proportion.
To encourage crystallization, LDH structures are matured at
certain tall temperatures [56]. LDHs can be utilized as anion exchangers
to immobilize anionic inhibitors such as molybdate [57], vanadate [58],
phosphates [59], tungstate anions [60], and other natural anions [61] since to
their huge interlayer dispersing and anion trade capabilities. An
anion trade instrument with chloride particles can effectively discharge these
inhibitors.
Metal-organic frameworks (MOFs) have gotten a lot of press recently due to their
impressive properties, such as a customizable internal structure, a large specific
surface area, and ease of surface functionalization. MOFs are therefore intriguing
options for catalysis [62], sensors [63], gas storage [64], and drug delivery
systems [65]. MOF-based nanoparticles have been used for corrosion prevention
in several recent research [66-70]. Precipitation of a methanol solution containing
zinc cations and 2-methylimidazole, for example, has produced ZIFs having the
same topological structure as zeolites. By using ligand exchange, corrosion
inhibitors like benzotriazole (BTA) may be loaded onto ZIF nanoparticles [71-73].
ZIF nanoparticles outperformed other micro/nanocarriers in terms of thermal
stability, chemical compatibility, and inhibitor loading capacity (65%)[72, 74, 75].

Encapsulated material Shell thickness

Shell

Fig. 1 Scheme of a nanocapsule

Table 1 Core and shell materials more commonly used in different nanoencapsulation applications

Application Materials
Food C: acidulants (acetic, sorbic, lactic), flavoring agents (citrus/mint oils, oleoresin, oregan, menthol),
sweeteners (sugar, aspartame), colorants (b-carotene), lipids (fish oil, linoleic oil, palmitic acid),
vitamins and minerals (vitamin A, D, E and K, folic acid), salts, preservatives (gallic acid),
antimicrobials and antioxidants (terpene, limonene, black pepper, catechins), probiotics (lactobacillus,
bifidobacteria) enzymes and microorganisms (lipase, invertase, penicillium roqueforti)
S: carbohydrates (sucrose, malto- and cyclo-dextrines, chitosan), gums (agar, arabic, gum acacia,
sodium alginate, lipids (oils, paraffin, stearic acid, fats, beeswax, phospholipids, Stealth® liposomes),
celluloses, proteins (albumin, casein, gelatin, gluten, peptides, zein), synthethic elatomers
(polyacrylamide, polyacrylate, polyethylene, polyvinyl alcohol, polyvinyl acetate), synthetic polymers
(acrylonitrile,
polybutadiene, poly(lactide-co-glycolide), silicon dioxide
Pharmaceutics C: hormones (insulin), vaccines, oncologic (doxorubicin, cisplatin) and hematology actives
(anthracyclines), proteins (bovine serum albumin, globulin, myoglobin,), enzymes (glucose oxidase),
antibiotics (amoxicillin), drugs (felodipine, nicardipine, heparin), bacteria (lactobacillus acidophilus)
and hepatocytes
S: carbohydrates (chitosan, alginate, dextran), proteins (polylysine, polyglutamic, albumin,
peptides), synthethic elatomers (poly(alkyl acrylate), poly(ethyleneglycol)), celluloses (ethylcellulose),
synthetic polymers (poly(lactide-co-glycolide, polyethyleneglycol), lipids (phospholipids), carbon
nanotubes,
erythrocytes, gums (alginate), silicon dioxide, phyllosilicate
Agriculture C: Insecticides (endosulfan), herbicides (fenamiphos), pheromones, fertilizers, pesticides,
microbicides S: Polyurea, polyurethane, gelatin, gum Arabic, chitin, chitosan
Textile C: PCM, emollients (aloe vera, vitamin E, lanolin), dyes, fabrics softeners, flame
retardants S: Poly(styrene), urea-formaldehyde, ethylcellulose
Paintings C: Biocide (OIT), pigments, anti-foulant agents, anti-corrosion
agents S: Melamine formaldehyde, gelatine – acacia, silica, zeolite
Personal care C: natural ingredients, essential oils (menthol, lime, lavender), preservatives, vitamins (A, E, C), retinol and
triclosan
S: carbohydrates (sucrose, malto- and cyclo-dextrines, chitosan), cellulose, silicon dioxide

C core, S shell

Thus, the main reasons for encapsulation are: (a) separation of incompatible materials,
(b) conversion of liquids to free-flowing solids [6], (c) increased stability (e.g.,
protection of the encapsulated against oxidation or deactivation due to reaction in the
environment), (d) masking organoleptic properties such as colour, taste, and odour of
substances, (e) safe handling of toxic materials, and (f) controlled and targeted release
of en Furthermore, nanoencapsulation allows for the modification of the release of
encapsulated active materials, such as sustained release (maintaining the right
concentration), long-lasting (and thus improving effects), target release (improving
tissue adhesion, penetration, or recognition), or triggered release (improving adhesion,
penetration, or recognition of tissues and cells) (mainly by environmental changes in
pH, temperature). Encapsulation and release modification (sustained, triggered, or
targeted release) lower dosages and, as a result, the risk of side effects. In medical
applications, this is of particular importance. Furthermore, because the
encapsulated molecule is not in direct touch with the environment, discomfort at
the injection site is usually decreased.

Nanoencapsulation technologies are used in a variety of industries, including the

medical, pharmaceutical, cosmetics, chemical, textile, construction, agricultural,
and food industries, due to their vast range of benefits and features. In reality, this
technology is already widely used in a variety of sectors, although it is estimated
that only around 10% of the potential applications are now being used. The core
substance (e.g., medications, vaccines, etc.) can be targeted and delivered in a
regulated manner and at a specific place, for example, in the case of medicine
delivery (see Fig. 3 Nanocapsules have been proposed in agrochemistry to
regulate the release of insecticides or pesticides, enhance their efficiency, and
reduce the amount of active compounds used in a given application. Durable
textile scents and skin softeners in the form of nanocapsules have also been
created in the textile sector [6].
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Fig. 2 Morphologies of nanocapsules (from left to right): (i) single-core capsule, (ii) dispersed
core in polymer gel, (iii) multi- layer capsule, (iv) dual-core capsule and (v) single-core-
multi-shell capsule