Review

Electro Fluid Dynamics: A Route to Design Polymers and

Composites for Biomedical and Bio-Sustainable Applications
Nergis Zeynep Renkler, Iriczalli Cruz-Maya, Irene Bonadies and Vincenzo Guarino *

Institute of Polymers, Composites and Biomaterials, National Research Council of Italy,

Mostra d’Oltremare Pad.20, V. le J.F. Kennedy 54, 80125 Naples, Italy
* Correspondence: [email protected]

Abstract: In the last two decades, several processes have been explored for the development of mi-
cro and/or nanostructured substrates by sagely physically and/or chemically manipulating polymer
materials. These processes have to be designed to overcome some of the limitations of the traditional
ones in terms of feasibility, reproducibility, and sustainability. Herein, the primary aim of this work
is to focus on the enormous potential of using a high voltage electric field to manipulate polymers
from synthetic and/or natural sources for the fabrication of different devices based on elementary
units, i.e., fibers or particles, with different characteristic sizes—from micro to nanoscale. Firstly,
basic principles and working mechanisms will be introduced in order to correlate the effect of se-
lected process parameters (i.e., an applied voltage) on the dimensional features of the structures.
Secondly, a comprehensive overview of the recent trends and potential uses of these processes will
be proposed for different biomedical and bio-sustainable application areas.

Keywords: electrospinning; electrospraying; nanofibers; microgels; nanoparticles; biomaterials

Citation: Renkler, N.Z.; Cruz-Maya,

I.; Bonadies, I.; Guarino, V. Electro 1. Introduction
Fluid Dynamics: A Route to Design
Nowadays, a wide range of biomaterials—from various synthetic or natural
Polymers and Composites for
sources—are continuously processed with an ever-increasing control of the structural fea-
Biomedical and Bio-Sustainable
tures in order to create 3D platforms suitable for tissue engineering applications and var-
Applications. Polymers 2022, 14,
ious therapeutic applications. Over the relevance of constituent materials and their phys-
4249. https://doi.org/10.3390/
ical/chemical properties, it is well known that peculiar structural features at different
polym14194249
scales can affect a wide range of final product properties. For instance, several studies
Academic Editor: Huaizhong Xu remarked that nano or microparticles could be more advantageous for injection applica-
Received: 15 September 2022 tions than those with bigger sizes ranging from hundred microns up to millimeters [1].
Accepted: 5 October 2022 Likewise, in the case of fibrous scaffolds used in vitro, it is known that nano-textured
Published: 10 October 2022 surfaces, i.e., fiber diameter at the nanoscale, are able to better influence the behavior of
living cells in terms of biomechanical, biological (i.e., cell adhesion and proliferation) and
Publisher’s Note: MDPI stays neu-
fluid/molecular transport properties rather than micro-surfaces, thus mimicking the typ-
tral with regard to jurisdictional
claims in published maps and institu-
ical architecture of basement lamina membrane, present in all the natural tissues [2].
tional affiliations.
Lastly, for bio-filtering applications, the role of mesh size in nanofibrous membranes is a
determinant to improving separation efficiency, thus meaning a better capacity to remove
bio-contaminants in medical solutions, higher flux in separation, and lower energy for
operation [3]. Therefore, it is crucial to employ the processing techniques available to pre-
Copyright: © 2022 by the authors. Li- serve control of their structural properties at micro- and nano-levels to impart, case by
censee MDPI, Basel, Switzerland. case, morphological and topographical cues tailored for the specific application [4]. In the
This article is an open access article last decade, various cost-effective and reproducible manufacturing techniques have been
distributed under the terms and con- developed to produce micro and nanostructured materials with the desired characteristic
ditions of the Creative Commons At- sizes. In the literature, different methods were described to produce micro-and nano-
tribution (CC BY) license (https://cre- fibers, including interfacial polymerization, self-assembly, and freeze-drying [5]. Among
ativecommons.org/licenses/by/4.0/). them, Electro Fluid Dynamic processes (EFDs) currently identify one of the most versatile

Polymers 2022, 14, 4249. https://doi.org/10.3390/polym14194249 www.mdpi.com/journal/polymers

Polymers 2022, 14, 4249 2 of 25

and cost-effective class of manufacturing technologies for the manipulation of polymers

or composites, generally from melt or solution, by the application of high voltage electric
field, to produce fibers or particles from micro to nanoscale [6,7]. They include two differ-
ent working modes, electrospinning and electrospraying, that allow producing, respec-
tively, non-woven fibers or particles of different sizes and shapes. They are highly tunable
in their characteristic size and shape by accurately selecting the materials/solvents/addi-
tives and finely controlling the process parameters [8]. Moreover, many materials, such as
synthetic and natural polymers, metals, ceramics, composites, and blend systems can be
sagely combined for the fabrication of multicomponent devices suitable in many fields
such as tissue engineering and regenerative medicine [9], drug delivery [10], wound
dressing [11], bioelectronics [12], and biofiltration systems [13].
Despite the recent goals in terms of research outcomes in the biomedical field, up-
scaling EFD technologies for clinical translation and large-scale production is still so far
due to several problems concerning the current biomanufacturing processes, mainly re-
lated to the use of volatile solvents and all the risk factors connected to health and safety
standards during fabrication and product implementation [14].
It is well known that the solvent evaporation mechanism drives conventional elec-
trospinning. Environmental damage associated with using organic solvents with low boil-
ing points—namely Trifluoroethanol (TFE) and dichloromethane (DCM)—may not be
thoroughly recommended by the U.S. Food and Drug Administration for the fabrication
of electrospun fibers for pharmaceutical applications. Moreover, solvent traces may be
entrapped into the fiber body after resting treatments, thus restricting their use for biolog-
ical use that requires direct contact with the cells [15].
In this review, an overview of the different EFD processes was proposed. In the first
part, working principles were introduced, highlighting some recently explored insights
to minimize the manufacturing impact on the environment (i.e., melt electrospinning,
green electrospinning). In the second part, a wide range of blends or composite devices
based on fibers or particles with different size scales were systematically discussed ac-
cording to their application in the biomedical and environmental fields.

2. Electro Fluid Dynamics: Classification and Working Principles

In the last two decades, a large variety of technologies based on “bottom-up” or “top-
down” manufacturing techniques was investigated, highlighting relevant benefits and
some drawbacks. In contrast to the top-down approach, bottom-up methods first attempt
to produce micro-scale structures that can be put together to develop complex structures.
They are described as a two-stage fabrication process that includes the final assembly of
these structures after they are created [16,17]. This bottom-up approach is essential to pro-
cessing and manipulating small-scale biomaterials using specific technologies such as mi-
crofluidic techniques [18]. Among them, EFDs can be considered a class of “bottom-up”
technologies that use high-voltage electric forces on viscoelastic polymers at the melt state
or in solution form. It includes two main processing modes: electrically assisted spinning
and spraying—suitable to synthesize micro- and nanostructures in the form of particles
or fibers [6]. Their popularity is mainly due to the high reliability and versatility of these
processes that allow fabricating a plethora of smart devices with controlled sizes from
micro- to submicrometric scale and multiple functionalities as a function of the specific
experimental configuration used.
The most elementary configuration is straightforward and includes three compo-
nents: a high-voltage power supply, a pump system where a syringe/cartridge is ar-
ranged, and a ground collector (Figure 1a). Polymer comes out of the needle tip at a con-
stant rate with the support of pumping forces until a droplet is formed [19].
Polymers 2022, 14, 4249 3 of 25

Figure 1. (a) Scheme of the basic electrospinning setup and influence of solution parameters: (b)
Polymer concentration (SEM images of PCL fibers at different concentrations from [20]) and (c) sol-
vent boiling point (SEM images and diameter size distribution of poly(trimethylene carbonate-co-
ϵ-caprolactone) [P(TMC-CL)] nanofibers from [21]—spinning parameters: (d) applied voltage (SEM
images of PVP/Cellulose Acetate/Garlic nanofibers(scale bar 5 μm-int 1 μm) from [22].

Two opposite forces contribute to forming the droplet: the electrostatic force acting
on this droplet shape and the opposite force, the surface tension force, that tends to pre-
serve the droplet’s spherical shape. At the point that the two forces have equilibrium, it is
expressed by the following equation:
1 𝑄𝑄2
. = 8𝑝𝑝σs𝑅𝑅
8𝑝𝑝εo 𝑅𝑅2
where Q is the charge located on the droplet surface, R is the droplet radius, εo is the
vacuum permeability, and σs is the surface tension coefficient. The charge increases by
increasing the strength of the electric field, and the value of this electrostatic field force
can be controlled by varying the voltage at a fixed distance between the two electrodes
[23]. Up to a critical point where the electrostatic force overcomes the surface tension, the
droplet is then disrupted into smaller droplets in electrospraying [5]. The solution will
become a conical droplet, a Taylor cone, when using a higher molecular weight polymer.
Due to sufficient chain entanglement structure, hydrophobic interactions, and hydrogen
bonds of the polymer lead to a stable, continuous fiber formation instead of droplets.
When the electrostatic force overcomes the surface tension, it stretches the jet stream caus-
ing it to elongate as a filament. This filament solidifies and is eventually deposited on a
grounded collector, these ultrafine fibers will form, and this process is then called electro-
spinning [24].
In the electrospinning process, many parameters determine spinnability and the final
product’s morphology and uniformity of nanofibers. Different nanofibers with different
morphologies can be fabricated by sagely dosing and combining these parameters in un-
countable ways. Solution-dependent parameters (i.e., viscosity, polymer concentration,
solvent type, surface tension, electrical conductivity, and molecular weight) (Figure 1b,c)
and environmental conditions, such as humidity and temperature, directly affect spinna-
bility. The set up parameters can be adjusted during processing. For instance, spinning
distance, applied voltage, flow rate, and collector type also affect spinnability and the final
product morphology [25,26]. It is known that the polymer concentration affects the fiber
diameter from micro- to nano-size by changing the viscosity, and together with surface
tension, it is directly proportional to fiber diameter. As the viscosity increases, the fiber
diameters also increase. In addition, the fiber diameter can be affected by adjusting the
distance, voltage, and flow rate during the process [27,28]. Especially the applied voltage
Polymers 2022, 14, 4249 4 of 25

is a critical factor because the formation of fibers only occurs when the applied voltage
exceeds the threshold voltage [29]. Additionally, it directly affects fiber morphology, as
an increase in applied voltage leads to an increase in the electrostatic force of the polymer
solution and a decrease in fiber diameter with the stretching of the jet (Figure 1d) [22].
However, it should be noted that these parameters do not affect the fiber morphology
alone; for example, the effect of voltage on the fiber diameter will vary according to the
polymer solution concentration and the distance between the tip and the collector [30].
Numerous and varied polymers can be processed by electrospinning but often re-
quires the use of toxic organic solvents. The awareness of the disadvantages associated
with the use of toxic solvents has increased interest in using non-toxic (benign) solvents
for electrospinning. However, many benign solvents are not directly suitable for electro-
spinning, and longer and more accurate process optimization is required to obtain fibers
with suitable morphology [20]. For instance, it has been reported that PCL, a polymer
frequently used in biomedical applications, applies to electrospinning using less harmful
solvents, including formic acid/acetic acid. Moreover, Van der Schueren et al. showed that
increasing the formic acid in the solution decreases the mean fiber diameter [31].
EFDTs also represent useful tools of current materials science and processing to fab-
ricate micro- and nanoparticles made of polymers from the natural or synthetic origin,
overcoming some limitations of other consolidated technologies in this area, i.e., micro-
emulsification, self-assembly, and solvent evaporation. They can be classified into two
different groups: electrospraying (ES) and electro hydrodynamic atomization (EDA) (Fig-
ure 2) [32]. Both technologies are based on applying an electric field to nebulize a highly
dilute polymer solution into droplets with highly controlled and uniform diameters. In
particular, ES is a continuous process where the mechanism of polymer jet deformation
and disruption into small particles is due to the Coulombic repulsion onto the surface of
highly charged droplets against cohesive forces among polymer chains [33]. The solvent
evaporation can be controlled by varying the distance between the tip-nozzle and collec-
tor to ensure the formation of spherical and solvent-free nanoparticles [34,35]. Contrari-
wise, EDA is a non-continuous mode, or dripping mode, where the gravity forces—due
to the drop density and weight—and electric forces compete to overcome the surface ten-
sion at the needle tip. However, they are strongly counteracted by the peculiar properties
of the used solvent (i.e., permittivity, boiling point) that drastically limit the capability of
droplets to surface overcharge [36]. In this case, solvent removal can be obtained by col-
lecting droplets into a bath via chemical or physical ways (i.e., gelation, solvent/non-sol-
vent extraction) that allow freezing the particle sizes into a dimensional range from tens
to hundreds of micrometers. The chance to minimize chemical additives, working at am-
bient temperature/humidity conditions, means that they are a sustainable choice to pro-
cess biologically derived and biodegradable materials for different bio-inspired applica-
tions. Moreover, numerous versatility of the process setups, i.e., coaxial-ES/EDA, co-
ES/EDA, and sequential ES/EDA, allows for a mix of different materials for the fabrication
of multi-component systems that may combine particles and/or fibers for countless uses
[37,38].
Polymers 2022, 14, 4249 5 of 25

Figure 2. Fabrication of particles based on biomedical/bio-sustainable polymers from macro to na-

noscale switching between EDA to ES mode. EDA process is mainly dedicated to the fabrication of
balloons made of polysaccharides (i.e., chitosan, alginate) and/or glycosaminoglycans (i.e., hyalu-
ronic Acid [39]) in water solution. EDS process is mainly devoted to the fabrication of nanovectors—
i.e., nanoparticles with sub-micrometric or nanometric diameters—using highly volatile solvents
(i.e., acetic acid, ethyl acetate). Specific modification of the experimental process setup can impart
different sizes and shapes to final particles (i.e., snakes, Rings) [40].

3. Melt Polymers vs. Polymer Solution

3.1. Fibers from Melt Polymers
Melt electrospinning is a simple method to produce polymeric fibers without using
organic solvents. This environmentally friendly approach offers several advantages in fi-
ber manufacturing, including avoiding the use of solvents to dissolve the polymers, as in
the case of solution electrospinning.
The basic apparatus generally consists of a high-voltage power source, a needle, a
heating device (heating oven, heat guns, laser melting devices, and electric heating), a
melted polymer, and a collector. Similar to polymer solution electrospinning, larger di-
ameter nanofibers are obtained using polymers with higher molecular weight in the melt
electrospinning system. The electrospun melt mats generally consist of fibers both on the
nanometer and micrometer scales [5]. Basically, in a melt electrospinning system, the melt
polymer forms a cone at the tip of the capillary when the voltage is applied. After a critical
voltage, electrostatic forces cause the surface tension of the melt polymer and produce the
fiber [41].
As previously discussed, in nanofiber production from solution and melt polymer,
voltage is the main factor affecting spinnability and fiber morphology. It is possible to
reduce the diameter of the polymer fibers by applying higher electric field strengths by
causing further stretching of the jet. Additionally, increasing the electric field strength is
possible by increasing the supplied voltage or decreasing the needle tip-collector distance
[42]. Qin et al. [43] investigated the effect of collector distance on fiber diameter, and the
fiber diameter first decreased and then increased. The reason for this can be that the fiber
stretching time is first prolonged in the electric field, and then the electrostatic pulling
force weakens in the case of a large spinning distance. Although the surface tension of the
low viscous polymer melt is almost close to that of the polymeric solution system, the
viscosity of the polymer melt is higher than the viscosity of the polymer solution; there-
fore, more charge is required for melt electrospinning to initiate the jet than the solution
electrospinning voltage [44]. In addition, because of the high viscosity and the rapid heat
Polymers 2022, 14, 4249 6 of 25

loss of the jet, larger fiber diameters are obtained in melt electrospinning. For instance,
Sarwar et al. [45] investigated the effects of applied voltage, distance, and flow rate on
fiber morphology while producing melt and solution from PEBA polymers. They showed
that increasing voltage decreased fiber diameter from 7 to 5 μm. In both types of spinning
techniques, the effect of process parameters on fiber diameter was found that similar re-
sults. The fibers’ minimum average diameters obtained by melt electrospinning were
larger than solution electrospinning fibers. Additionally, Hao et al. studied the influence
of temperature and voltage on the diameter of the melt-spinning polypropylene fibers.
They found that with the 70–80 kV spinning voltage, they obtained good quality fibers
with smooth surfaces and diameters smaller than 10 microns [23]. Morikawa et al. [46]
showed that they could produce fibers with a diameter much closer to the fibers produced
by solution electrospinning by developing a wire-based method based on the variation of
the electrostatic fields around the spinneret instead of the needle-based method often used
in melt electrospinning. In some cases, sub-micrometric fibers can be obtained because of
the branching of larger fibers during the spinning of molten polymers. Because the jet may
not solidify immediately after being ejected, it is subjected to stronger field forces as it
moves towards the electric field. As a result, if the molecular weight of the polymer is low
enough, side jets may form, leading to fibers with a smaller diameter than the molten jet
[47].
The absence of solvents in melt spinning makes it a safer, greener, and completely
automated method to produce fibers for various applications in the case of all the poly-
mers, easily processed under controlled temperatures but requiring the use of highly toxic
solvents to be dissolved[41]. However, it has complex pieces of equipment, ends up with
a larger fiber diameter, and deficiency of suitable materials are a few problems.

3.2. Fibers from Polymer Solution

This method is based on fabricating an electrospun mesh from the polymer dissolved
in a moderately volatile solvent, delivered to a spinneret, and exposed to a voltage poten-
tial (between the spinneret and a collecting surface) [48]. Any lower or higher applied
voltage will result in beaded morphologies and inhibit polymer jet initiation. As the ap-
plied voltage rises above a critical value, the nanofiber diameter initially shrinks and in-
creases after a certain point. This initial reduction in fiber diameter is due to the increase
in voltage with increasing charges in the jet repelling each other and a high jet stretch. It
is mainly reported that, with the increased applied voltage, the instability and stretching
of the polymer jet also increase and generally lead to smaller fiber diameters [49]. Shao
and co-workers investigated pullulan-CMC nanofibers modulated through process pa-
rameters (i.e., Polymer solution concentration, applied voltage, and feed rate) as a fruit
packaging material. They showed that increasing the applied voltage from 19 to 21 kV
and the feed rate from 0.36 to 0.6 mL/h leads to a reduction in mean fiber diameter from
0.187 to 0.092 µm [50]. In a previous study of the same group, the effect of applied voltage
on the morphology of PVDF nanofiber mats was investigated, and the average fiber di-
ameter decreased from 630 nm to 284 nm by increasing the voltage from 9 kV to 15 kV
[51].
In a study, Herrero-Herrero and co-workers [52] investigated PLA/PCL fibers diam-
eter as drug delivery systems and obtained under- and above-micron-sized fibers with
the influence of majorly solvents ratio (chloroform/methanol and dichloromethane/dime-
thylformamide) and voltage. They showed that as the voltage increases, the diameter of
the fibers decreases because of the stretching in the polymer jet associated with the charge
repulsion.
In a different study, Nasouri and co-workers [53] aimed to model and optimize elec-
trospun PAN nanofiber diameter using response surface methodology. They confirmed
with the RSM analysis that polymer concentration and applied voltage were the main fac-
tors affecting the average nanofiber diameters. An increase in the applied voltage beyond
the critical value will result in the formation of beads or beaded nanofibers. Increases in
Polymers 2022, 14, 4249 7 of 25

the diameter and formation of beads or beaded nanofibers with an increase in the applied
voltage are attributed to the decrease in the size of the Taylor cone and the increase in the
jet velocity for the same flow rate [54].
The preparation process for producing membranes with electrospinning from poly-
meric solutions frequently involves using unfriendly solvents for the environment and
humans. In addition, final product electrospun fibers may contain traces of solvent after
production. Generally, in this method, a polymer is dissolved in volatile solvents, namely
trifluoroethanol (TFE), dimethylformamide (DMF), or dichloromethane (DCM) [55]. Con-
sidering the environmental risks and ecological damage they cause, the green production
process in electrospinning is becoming widespread to produce biomaterials based on en-
vironmentally friendly resources. Accordingly, using green solvents with slow volatility
may contribute to forming a fibrous network with a minimal effect on health and the en-
vironment. Recently, several studies have focused on using aqueous polymer solutions
for electrospinning applications [56–58]. Alternatively, biologically benign solvents, such
as formic acid or acetic acid, can be used alone or in combination as green solvent candi-
dates. For instance, a recent study provided a comparative study on the fabrication of
nanofibers from a PLGA and PCL solution in DMF: DCM and acetic acid, observing no
significant difference in fiber morphologies and diameters in terms of using acetic acid
[55].
A disadvantage of the green fabrication process is that the fibers present low physical
stability, so a crosslinking strategy is required. In this case, green agents (e.g., citric acid)
can be used in the place of other toxic chemicals (glutaraldehyde) for fiber crosslinking
[59]. This approach is promising for processing eco-friendly sources, thus concurring to
limit the destructive impact of petroleum-based products and relevant benefits in terms
of environmental protection. For this purpose, the electrospinning technique is an optimal
way to process biopolymers from natural sources such as chitin, chitosan, and pectin—to
functional nanofibrous membranes [58]. For instance, in one study, a bio-based blend was
successfully electrospun by combining small amounts of PEO with chitin propionate and
green solvents, ethanol, and water [60]. This way, the electrospinning process is environ-
mentally and human-friendly, fulfilling all basic sustainability principles better than other
techniques. This process is summarized in Table 1, where a comparative analysis of the
benefits/limitations of processing techniques based on using a solution or polymer melt
to produce bulk or micro/nanofibrous films was reported.

Table 1. Comparative analysis of fiber manufacturing via melt and solution processes.

Poly-
mer HV Size Main Benefits Limitations Refs.
State
-Time-consuming to build.
10 µm -High structural control at the mi--Few polymers to test (thermal
Melt + to 100 croscale; stability required) [61]
µm -No solvent use; -High equipment costs
-Hard to reach the nanoscale
-Highly customizable setup; -High solvent volatility is re-
<100
Solu- -Low costs; quired (few green solvent)
+ nm to [55]
tion -Suitable for many polymers; -Low control of structural order
10 µm
-Sub-micrometric scale (no direct writing)
50 µm -High mass production -High production cost
Melt - to 500 -Weaving tech combination -No diameter homogeneity [62]
µm -Large-scale applicability -No nanometric scale
500 nm -Thermally unstable polymer use; -Solvent removal
Solu-
- to 50 -Several configurations -Lack in morphological order [63]
tion
µm -Industrial use (high defect occurrence)
Polymers 2022, 14, 4249 8 of 25

4. Blended and Composite Fibers towards Bio-Sustainability

A polymer blend is a single-phase substance obtained by mixing two or more poly-
mers, generally without strong chemical bonds. Polymeric composites are a multi-phase,
multi-component system that combines polymeric and/or non-polymeric materials to im-
prove their native properties by creating physical/chemical bonds. Especially in recent
years, interest in polymers obtained from renewable resources has increased; thus, natural
polymers, synthetic polymers from natural monomers, and polymers from microbial fer-
mentation are frequently investigated. Similar to other petroleum-based polymers, poly-
mers from renewable resources are rarely used alone, and many of their properties can be
enhanced through blending and composite formation [64]. Micro- and nano-scale poly-
meric fibers have many advantages, such as large surface area and high porosity for use
in biomedical applications [65], environmental filtrations [3], and textile products [66].

4.1. Biomedical Applications

In recent years, materials based on multi-component systems have been frequently
investigated for the fabrication of nanomaterials with advanced mechanical and chemical
properties [67] for biomedical use. Polymers with two or more synthetic or natural addi-
tives are generally used to obtain better properties. This way, desired chemical properties
such as biocompatibility and biodegradability can be obtained, especially for functional
tissue scaffolding [68,69]. Electrospinning enables the formation of nanofibers from a wide
variety of materials, for example, polysaccharides, proteins, composite metals, metal ox-
ides, ceramics, and carbon-containing biomaterials. Natural polymers (collagen, elastin,
hyaluronic acid, and fibrinogen) commonly found in the native tissue extracellular matrix
or derivative components obtained from natural sources such as gelatin, chitosan, silk fi-
broin, or vegetable oils are able to facilitate cell attachment, growth, and differentiation.
Moreover, they are biodegradable and biocompatible.
Due to environmental needs, the development of bio-based fibers is becoming an in-
creasingly hot topic and makes them interesting materials for environmental applications
[67]. Despite the desirable properties, utilizing only natural polymers shows low spinna-
bility. Additionally, one of the main disadvantages is their fast degradation rates due to
their hydrophilic character and, in some cases, their poor mechanical properties, espe-
cially in wet environments [64]. To increase the spinnability of natural polymers, combin-
ing different polymers to formulate an electrospinning solution is a considerable strategy.
Additionally, it is possible to integrate the desirable properties of natural and synthetic
polymers into a single platform and fabricate various scaffolds with adjusted structural
and chemical properties, depending on the intended application.
Synthetic polymers, for example, PCL, PLLA, PGA, and PLGA, remain important
candidates for scaffold production because they have high mechanical strength and are
structurally stable, easing tailoring the degradation rate. However, they are limited, espe-
cially in biomedical applications, when utilized alone because they lack functional parts
and need modifications. Aliphatic polyesters, such as PLA, are known for their biodegra-
dability and susceptibility to hydrolytic degradation. They have attracted much attention
among commercial polymers as they are produced from renewable resources, are com-
postable, and have high mechanical performance [64]. Natural materials are mainly uti-
lized effectively to achieve the desired biological properties (biocompatibility and bioac-
tivity) lacking in other synthetic polymers. However, they must be stabilized by cross-
linking or other methods in order to yield a stable material that can maintain its integrity
[70,71]. In this case, polymer blending can enable the combination of complementary
properties of different synthetic and natural polymers or can be used as a one-step surface
modification technique to alter the wettability of electrospun mats [72].
It is already known that nanofiber diameter, surface morphology, and pore size dis-
tribution of the mats obtained in electrospinning can be affected by electrospinning pa-
rameters. For instance, the type of polymer melt or solution, needle size, working distance,
Polymers 2022, 14, 4249 9 of 25

applied voltage, flow rate, and working environment could influence the final product’s
properties [25]. The use of blends in the electrospinning system rather than a single poly-
mer melt or solution system can affect the morphology and the chemical properties of the
obtained mat. This effect is shown in a study to investigate the possibility of mixing PAN
with different water-soluble polymers to change the morphology of the electrospun nan-
ofibers. It was found that the nanofibers’ diameter was increased in the PAN/gelatin blend
[73]. In another study, the fiber diameters of collagen–chitosan-TPU nanofiber scaffolds
were found to be in the range of 256 ± 145 nm in the aligned fibers and lower than the
fiber diameters in the random fibers, respectively. This is thought to be due to the stretch-
ing and weakening of the fibers with a high rotational speed. More importantly, many
fine-diameter fibers (diameter ≤ 100 nm) were also seen in the scaffolds, which is ex-
plained by the positive charges carried by the chitosan in the blend. In other words, it is
thought that the solution conductivity also increases with increasing loads, and the repul-
sive forces increase with the loads on the electrospinning jet, leading to further stretching
of the fibers [74]. The choice of blend materials is also essential in electrospun membranes
in tissue engineering applications because, in this way, fiber morphologies can be fabri-
cated more suitable for tissue needs. In a study investigating the use of one- or two-com-
ponent nanofiber channels in nerve tissue applications, the properties of nanofibers pro-
duced from the blend obtained by adding gelatin to the PCL polymer were compared
with those produced using only PCL. The average (0.59 ± 0.15) μm diameter of the two-
component fibrous channels obtained by adding gelatin solutions was in the submicron
range. At the same time, PCL has been shown to consist of microfibers with an average
diameter of (5.61 ± 0.8) μm [71,75]. Recently, it has been shown in the literature that toxic
or hazardous solvents have been replaced with green solvents because of the effect of the
chemicals on health and the environment. In addition, since solvents such as TFE are
known to cause denaturation in the collagen structure, it has been shown that collagen
and PCL-based nanofiber membranes can be successfully obtained by electrospinning by
dissolving them in an aqueous solution of acetic acid (Figure 3) [76].
Polymers 2022, 14, 4249 10 of 25

Figure 3. Composite (A–C) and blended (D) PCL-based fibers via green solvent electrospinning: (A)
qualitative morphological analysis via SEM, (B) quantification of 1:1 and 1:2 PCL/Collagen blended
nanofibers, and (C) FTIR analysis; (D) SEM and EDS spectra with element mapping of PCL/BG nan-
ofibers [20,76]. (images from [20,76] with free license).

In a study aiming to examine the physicochemical properties of fibers consisting of

collagen type I, collagen III, elastin, and polycaprolactone (PCL), when a 10% collagen and
elastin blend is added to PCL, the fiber diameters obtained are thicker (310 nm), and
where thick and flimsy fibers were observed this could be the reason of strong intermo-
lecular bonds between proteins and forming bundle fibers and thus observing rounded
surfaces instead of flat ones. When the polymer ratio is increased to 36%, thick and flimsy
fibers are the majority (397 nm). When the effect of elastin and collagen was analyzed
separately, the fiber diameters were obtained as 322 nm and 293 nm, respectively, in the
case of 36% elastin and collagen added to PCL [77].
Polymers 2022, 14, 4249 11 of 25

More recently, the use of water solution to mix bioactive proteins with either syn-
thetic or natural polymers was investigated to design more sustainable scaffolds able to
improve cell interactions in vitro and in vivo. Ramirez et al. investigated the contribution
of benign solvents in combination with additional polymers to address the properties of
wool keratin nanofibers for drug delivery and wound healing applications (Figure 4). It is
well known that solvent interactions can modify the spatial organization of macromolec-
ular chains, playing an essential role in forming supramolecular structures and altering
the electrospun fibers’ chemical and physical properties. They demonstrated that by
blending keratin with hydrogel-like polymers, such as polyethylene oxide (PEO) (Figure
4a) [78] or polyvinyl alcohol (PVA) (Figure 4b) [79], the in vitro activity of cells can im-
prove due to the local conditions of fluid and molecular transport that concur to form a
better-recognized interface in terms of chemical stability and wettability features.

Figure 4. Keratin-based fibers processed via aqueous solvent electrospinning by adding hydrogel-
like polymers: (a) PEO [78] and (b) PVA [79]: Fiber morphology via SEM and diameter distribution.
(adapted from [78,79]).

Alternatively, Vineis et al. [80] proposed the fabrication of protein-based nanofibers

by dissolving a mix of three different proteins—gelatin, wool keratin, and sericin from
silk fibroin—in an aqueous solution to validate their use for in vitro interaction studies.
They investigated the combined effects of keratin and sericin on gelatin-based nanofibers’
chemical and physical properties, highlighting a correlation between physical/chemical
interactions among proteins, i.e., a decrease in the hydrogen bonds of the N–H groups,
and in vitro stability and cell response of nanofibers.
Polymer matrix reinforcement using fillers is commonly used in the production and
processing of polymeric materials [64]. The fillers may geometries continuous (i.e., fi-
brous) or discontinuous geometries, such as short fibers, cubes, and blocks embedded in
the polymers. They are used in a large volume concentration in polymers (>5 vol.%) [81].
Nanocomposite materials, in which the fillers are homogeneously dispersed in the poly-
mer matrix and nanometric in sizes smaller than 100 nm (nanoparticles), differ from micro
composites due to their unique properties and have great potential for advanced applica-
tions [82]. The properties of polymer micro/nanocomposites are affected by the nature,
size, and shape of the polymer matrix and filler, the distribution of particles within the
polymer matrix, and the thickness of the filler. Nanocomposites are one of the most re-
searched areas in nanoscience, and currently, nano carbons, carbon nanotubes, graphene,
nanodiamonds, and nanodots can be added to many electrospun functional polymers. It
Polymers 2022, 14, 4249 12 of 25

is widely used as a polymer matrix phase because it offers advantages in terms of pro-
cessability compared to others, and it is known that nano carbons increase the functional-
ity of electrospun polymeric fibers, enhance physical and mechanical properties and pro-
vide advantageous properties. For this purpose, it can be used to provide bio functionality
as a scaffold in tissue engineering and sensors. Using this technique, composite electro-
spinning can form different polymers, such as PLA, PLGA, PCL, and PU, into different
nanostructured materials. The choice of polymer for tissue engineering and biomedical
applications is critical to achieving the target function [83–85].
It is known that the final product obtained with composite materials can also affect
the nanofiber morphology. For example, it can be concluded that carbon nanotubes added
to the polymeric matrix can cause an increase in solution viscosity, increasing fiber diam-
eter. In one study, it was observed that electrospun nanofibers obtained from PAN poly-
mer exhibited a smooth surface with a diameter of 200–400 nm. In contrast, no significant
difference was observed in fiber diameters for PAN/CoFe2O4 fibers. The fibers obtained
from the composite structure formed with CNTs had an increased diameter (400–700 nm).
On the other hand, in PAN/CNT-CoFe2O4 fibers produced by electrospinning, the larger
diameter approaching the microscale (approximately 700–1000 nm) suggests that it may
be the result of a further increase in viscosity when CNTs and CoFe2O4 nanoparticles are
added to the electrospinning solution [86].
In summary, it is possible to conclude that combining two or more materials with
different physicochemical properties and phases—including polymers, ceramic, and/or
metallic components—allows for fabricating composite materials with enhanced func-
tional properties at the micro- and nanoscale. In this context, the definition of tailored
setups can be relevant in producing composite and blending nanofibers from benign sol-
vents. For instance, multi-needle electrospinning systems have a multi-needle setup to
produce composite fibers from polymers that are not easily soluble in common solvents.
Likewise, coaxial needles allow for the design of core–shell fibers in which a polymer so-
lution (shell) and a compound solution (core) or two different polymer solutions (core–
shell) can be assembled by controlling the spatial distribution of each phase, thus specify-
ing the properties of the final device.

4.2. Environmental Applications: Contaminants Adsorption in Water and Their Sensing

Natural fibers are receiving growing interest due to their functionalization capabili-
ties and relevant advantages in weight and fiber–matrix adhesion, especially in combina-
tion with polar matrix materials. They can be successfully used in waste management due
to their biodegradability and much lower ash production after burning and post-pro-
cessing. In this context, nano-based filler compounds, such as cellulose nanofibers, can
also improve mechanical, physical, and gas-inhibitory properties. For instance, cellulose
nanofibers were combined with starch to prepare nanocomposites acting as filters with
high efficiency and accurate control of fiber mesh for particle separation [87]. Bates et al.
[88] used electrospun chitosan–polyethylene oxide-oxidized cellulose composites to fab-
ricate ultrafine membranes for wastewater applications with surface pore diameters less
than 0.1 µm and uniform diameter distribution. Cellulose nanofibers are essential in the
food industry as food packaging to match functional properties serving as gas or moisture
absorbers, specific gas barriers, antimicrobial properties, and antioxidant activity [89].
In this frame, it is reported that the preparation of a novel cellulose-based nano-
fibrous membrane for separation of oil/water emulsions starts from an aqueous system
coated with polydopamine (PDA), followed by grafting with polyethyleneimine (PEI).
The as-prepared super-hydrophilic and underwater super-oleophobic membrane showed
excellent separation performance for all different emulsions under broad pH range envi-
ronments with separation efficiency above 99.1%. The membrane also exhibited good an-
tifouling properties due to the development of a hydration layer underwater on the mem-
brane surface. The reusability study indicated no noticeable decline in the permeation flux
and separation efficiency even after 20 cycles [90].
Polymers 2022, 14, 4249 13 of 25

Multicomponent membranes based on polyvinyl alcohol (PVA)/alginate/chitosan

composite nanofibers containing nanomagnetic ZnO were studied for the removal of phe-
nolic compounds from aqueous solutions. The composite nanofiber dosage and phenol
solution temperature positively impact the phenol adsorption process. The thermody-
namic parameters confirmed the endothermic and spontaneous nature of the phenol de-
contamination process onto the polymeric composite nanofibers. The fabricated compo-
site nanofiber also revealed its capability for reuse after three cycles of regeneration [91].
In air filtration, electro fluid dynamic processes can be successfully used to design
fibrous membranes with peculiar features in terms of morphology and composition and
different structural order (Figure 5).

Figure 5. Scheme of a waterproof membrane suitable for air filtration/bio-filtration thanks to its
structural features. Examples of structures and morphologies obtained by Electro Fluid Dynamic
techniques: bead-on-string, porous and core/shell nanofibers.

For instance, combining commercialized cellulose paper towels with zein electro-
spun fibers was realized for biodegradable composite filters, as the solvent selected was
the well-known mixture of ethanol/water that led to both round and flat ribbon zein fibers.
The results reveal that the filtration efficiency of the flat zein fiber air filter is 99% for
PM0.3 removals and a low-pressure drop of 109 Pa, and it is much higher than that of the
round zein fiber filer. These properties were also confirmed after 40 repeated filtration
tests, and, more importantly, the developed filter was completely degraded after 42 h in
cellulase solution [92].
For the same application, konjac glucomannan (KGM)/polyvinyl alcohol (PVA) elec-
trospun membranes, loaded with ZnO nanoparticles, using water as a solvent and eco-
friendly thermal cross-linking via citric acid and temperature were also realized (Figure
6). The obtained fibrous membranes show a filtration efficiency for ultrafine particles (300
nm) higher than 99.99%, superior to commercial HEPA filters [93].
Polymers 2022, 14, 4249 14 of 25

Figure 6. Schematic summary of processing routes based on EFDTs for the fabrication of active par-
ticles loaded systems via thermal crosslinking and examples of nanoparticle loaded membranes ap-
plications for environmental remediation, i.e., bacteriostasis, air filtration, photocatalysis (adapted
from [93]).

Additionally, concerning petroleum-based polymers, the current trend is to realize a

green electrospinning process, replacing toxic solvents for different applications.
Environmentally friendly PU nanofibrous waterproof and breathable membranes
useful for broad-band applications such as in medical hygiene, wearable electronics, and
outdoor clothing were realized via solvent emulsion electrospinning technique combined
with heating treatment. A small amount of polyethylene oxide (PEO) was used as the
template polymer, whereas trimethylolpropane tris (2-methyl-1-aziridine propionate)
(TTMA) was selected as the crosslinking agent. Moreover, eco-friendly short perfluoroal-
kyl segments were introduced into the spinning emulsion to impart the hydrophobic char-
acter. The resultant water-processed nanofibrous membranes exhibit good waterproof-
ness, impressive air permeability, outstanding water vapor transmission rate, and high
elasticity [94].
Degradable and environmentally friendly polylactic acid (PLA) bead-on-string mem-
branes to be used as air filtration masks were realized as well by green electrospinning
using a mixture of relatively green solvents, ethyl acetate (EA)/N, N-dimethylformamide
(DMF). Optimizing the solvent composition and polymer concentration made it possible
to obtain the bead-on-sting morphology that led to an outstanding removal efficiency of
over 98% for aerosol particles and an extremely low-pressure drop of 29.3 Pa. Further-
more, compared to commercial masks, the prepared PLA bead-on-string membrane
shows higher filtration efficiency also in a real hazy environment, which results in a rela-
tively safer PM index value [95].
As a membrane for seawater desalination, environmentally friendly alcohol-based
polyamide mats were realized via one-step green solvent/non-solvent electrospinning by
directly incorporating the fluorinated chemical into spinning solutions. The resultant pol-
yamide nanofiber membranes exhibited high vapor permeation, good tensile strength,
and elongation, thus permitting robust seawater desalination performance with remark-
able salt rejection (99.97%) [96].
Lastly, petroleum-free polymers can be successfully used to fabricate membranes for
an oil spill that is currently one of the major sources of water contamination. Generally,
Polymers 2022, 14, 4249 15 of 25

industrial or oil transport accidents can generate the uncontrolled release of crude oils into
the oceans with relevant problems for environmental safety. This is imposed on develop-
ing cost-effective technology to reduce the environmental impacts caused by oil spills,
overcoming the limitations of conventional strategies (i.e., mechanical recovery and chem-
ical treatment) [97]. In this context, the electrospinning technique is a low-cost and highly
versatile methodology that allows control over the fiber diameter. For instance, Zhu et al.
reported the use of electrospun polyvinyl chloride/polystyrene nanofibers as sorbent for
oil removal, with relevant benefits compared with commercial Polypropylene based
nonwoven fabrics [98]. The peculiar sorption capacities of these fibers allow for the im-
provement of the performances of motor oil and diesel (i.e., 146 and 38 g/g, respectively)
several times with respect to commercial sorbent fibers. Similar studies were conducted
by Alnaqbi et al. that proposed the fabrication of recycled polystyrene micro-scaled fibers
with a sorption capacity as high as 95 g/g of crude oil spills [99]. All of the previous works
confirmed a relevant effect of process parameters (i.e., solvent type, voltage, flow rate,
electrode distance, humidity degree) on the properties of fibrous sorbents to be used to
minimize the damages related to crude oil spills in the sea. In this context, a step-by-step
optimization of the process conditions is mandatory to improve the final performance of
the fibrous sorbents for the definition of innovative and efficacious treatment of polluted
seawater.

5. Monocomponent/Multicomponent Particles
5.1. Biomedical Applications
The production of micro- and nanosized particles represents an advantage for differ-
ent applications in tissue engineering and drug delivery systems. For instance, micropar-
ticles can transport cells and display a longer retention time of molecules, while nanopar-
ticles can easily penetrate barriers (i.e., brain–blood barriers) and cellular membranes
[100,101]. In recent years, many studies have focused on the fabrication of polymer-based
devices by EFDTs, particularly to encapsulate biomolecules to be used in drug delivery
systems (antimicrobial and anticancer agents), theranostics, and tissue engineering [102].
EFDTs were originally used to fabricate particles to encapsulate hydrophobic and
hydrophilic drugs for their attitude to high encapsulation efficiency and control of size in
the range of micro- and nanoscale. For instance, cisplatin, an anticancer agent, was encap-
sulated into spherical and smooth PLGA nanoparticles via ES; Different formulations and
process parameters, i.e., voltage and flow rates, were tested to optimize the final shape
and size of nanoparticles. Further studies were performed to investigate the drug release,
characterized by an initial burst release followed by a sustained release. For the higher
content of cisplatin (10 wt.% with respect to PLA), the smallest burst release was recorded
[103]. The initial burst release was attributed to the drug amount onto the particle surface,
while the sustained part was mainly related to the peculiar properties of the polymer ma-
trix (i.e., swelling, diffusion, degradation rate) [104]. PCL and PLGA microparticles have
been fabricated to investigate in vitro the delivery of anticancer drugs. The release of
paclitaxel was faster for loaded-PLGA than loaded-PCL microparticles in more than 30-
day in vitro release [105]. The higher retention of drugs in PCL materials is related to its
hydrophobic and slow degradation rate. For particular applications such as orthopedic
grafts, the slow rate of degradation of PCL can be an advantage. For instance, melatonin
has been encapsulated into PCL microparticles to inhibit osteoclastic activity and support
bone remodeling [106].
Recently, the increased interest in using sustainable materials has also led to the use
of materials from waste biomass and marine origin for biomedical applications [107].
Among them, chitosan is a non-toxic and biodegradable polymer that has become mostly
used for the fabrication via ES of nanovectors loaded with different drugs (i.e., antibiotics
[100], anti-inflammatory [108], and chemotherapeutics [109]). Moreover, other natural
polymers, for example, alginate, chitosan, cellulose, collagen, gelatin, and hyaluronic acid,
Polymers 2022, 14, 4249 16 of 25

are currently being investigated, alone or blended in solution, to form mono- or multi-
component particles (Figure 7).

Figure 7. EFDTs for the fabrication of micro- and nano-devices. (a) electrospraying (ES): diclofenac-
loaded (DS) erythrocyte-like nanoparticles—effect of DS on particle morphology and release profile
(adapted from [110]); nanoparticle decorated fibers via co-electrospinning (i.e., simultaneous or se-
quential mode) for the development of fibrous platforms with different release of antibiotics from
chitosan nanoparticles (adapted from [111]). (b) Electrodynamic technique (EDA): drug-loaded cel-
lulose carriers with different compositions—i.e., mono-component (MC) or bi-component (BC) and
effects on morphology and release profiles (adapted from [112]; alginate microgels for cell car-
rier/encapsulation—effect of polymer concentration on morphology and in vitro cell response
(adapted from [113]).

Traditionally, an accredited approach involved the modification of natural and syn-

thetic polymers to improve their chemical and physical properties. For instance, cellulose
was grafted with PCL (cell-g-PCL) for the obtention of an amphiphilic polymer to design
smart nanoparticles via ES for drug delivery applications using as drug model sodium
diclofenac (DS) [110]. In this case, nanoparticles with an erythrocyte-like shape were ob-
tained due to the intercalation of DS molecules between hydrophobic PCL branches
grafted along the cellulose backbone, inducing an alteration of the entanglement density
at the equilibrium. It was demonstrated that this interaction generates an initial burst re-
lease followed by a sustained release related to the cellulose phase and PCL, respectively.
More recently, different strategies were explored to fabricate multi-component par-
ticles via ES with increasing structural complexity in order to refine the drug release mech-
anisms for therapeutic applications. For example, multi-component PCL/silk fibroin par-
ticles loaded with anti-inflammatory and osteogenic factors were fabricated via monoax-
ial electrospraying [114]. The incorporation of silk fibroin overcomes the lack of surface
functional groups and hydrophobicity of PCL, improving cell adhesion and growth.
Moreover, the additional bioactivity conferred by dexamethasone and ascorbic acid in-
duced the osteogenic differentiation of human adipose-derived stem cells and minerali-
zation for bone tissue engineering. Gelatin methacryloyl (GelMA) microparticles were
used as carriers of cells and growth factors for the treatment of degenerative disc disease
Polymers 2022, 14, 4249 17 of 25

Gelatin methacryloyl (GelMA) [115]. However, they present some drawbacks for oral ad-
ministration related to limited targeting ability, short retention time in the gastrointestinal
(GI) tract, and low bioavailability [116].
In order to better protect the active compounds, more complex experimental setups
were optimized for the fabrication of drug carriers with core–shell architectures. For in-
stance, cellulose acetate and chitosan have encapsulated and protected ketoprofen
lysinate (KL) in the acid microenvironment [117]. In this case, the presence of the chitosan
shell as a protective layer enables starting a progressive dissolution in the acid microen-
vironment, which eventually exposes the KL-cellulose core that retained the drug at gas-
tric pH.
Additionally, one of the main issues in drug delivery is overcoming side effects due
to inadequate drug concentration at the site of interest of systemic administration. In this
regard, hierarchically structured composite systems can be fabricated for the local deliv-
ery of drugs [118,119]. For instance, it is preferred to avoid the formation of biofilms after
chirurgical treatments in the periodontal pocket. Accordingly, the fabrication of amoxicil-
lin-loaded chitosan nanoparticles entrapped into PCL nanofibrous networks was opti-
mized by innovative processing routes based on a sequential or simultaneous deposition.
A faster release of antibiotics was observed when the multi-component systems were pre-
pared by sequential mode because the nanoparticles are especially dislocated onto the
surface, with respect to simultaneous one, involving a more efficient entrapment of parti-
cles among the fibers, with major benefits in terms of release control and in vitro antibac-
terial response, for potential use in periodontal disease treatments [111]. A similar ap-
proach was followed to fabricate multi-component scaffolds of curcumin-loaded PLA par-
ticles into PCL/gelatin fibers for skin regeneration [120].
An alternative strategy involves using EFDTs to fabricate microgels, namely hydro-
gels at a micrometric size scale, which are suitable for drug and cell delivery. Recently,
new experimental setups have been customized to process biopolymer solutions to fabri-
cate different kinds of microgels. In particular, low-cost biopolymers from renewable re-
sources, such as polysaccharides, are receiving particular attention due to their tunable
properties (i.e., water adsorption, mechanical properties) that EFDTs processes can finely
adjust for the fabrication of different devices [121].
For instance, alginates were widely processed via EHDA to produce mono-compo-
nent microgels for cell carriers [122]. Alginate solution was atomized directly into a bath
containing a crosslinking agent (i.e., BaCl2, CaCl2, FeCl3) [123] to fix size and shape. Fur-
ther post-treatments are generally required to protect the encapsulated molecules or to
functionalize the surface for cell adhesion. The fabrication of alginate microgels loaded
with caffeine can be mentioned as a model for low molecular compound encapsulation.
In this case, microgels were coated with chitosan to enhance caffeine retention [124].
As for a 3D in vitro model for cells, recent approaches have moved towards develop-
ing 3D culture into microgels with tailored properties to provide chemical and mechanical
signals similar to the microenvironment of cells. In this regard, alginate microgels’ com-
position and process conditions were recently optimized to deeply investigate in vitro
interaction with human mesenchymal stem cells (hMSCs) [113]. In order to include more
efficient bioactive signals (i.e., adhesive or proliferative cues), mono-component microgels
can be modified by adding proteins or growth factors to form multicomponent devices
able to stimulate specific cell activities [125]. Chitosan was also proposed in combination
with alginate to modulate the mechanical stiffness of the matrix to support and stimulate
neuronal cultures [126]. Bio-inspired particles made of poly-D-lysine/alginate were used
to encapsulate MSCs in order to protect them from immune cells, maintaining their im-
mune-modulating functions suitable for systemic lupus erythematosus treatment [127].

5.2. Other Green Applications

EFDTs with different configurations permit to attachment/decorate different sub-
strates with micro/nanoparticles with controlled shapes/sizes for various applications
Polymers 2022, 14, 4249 18 of 25

such as separation membranes, antifouling sensors, active packaging, and innovative tex-
tiles (Figure 8).

Figure 8. Scheme of experimental setup modifications of EFDTs for the fabrication of nanoparticles
and thin films as sustainable coatings (images adapted from [128]). In comparison with the conven-
tional setup used for the fabrication of electrospun fibers, the use of polymer solution with lower
concentration/low molecular weight enables particles suitable for micro-nanostructured coatings.
Likewise, a significant modification of fluid dynamic parameters (i.e., increase in flow rate) may
also allow creation of a homogeneous and thin coating of porous substrates and textiles.

In particular, ES is an easy and low-cost technique with the potential to create uni-
form multilayer thin coatings that can be scalable and manageable more quickly than a
spin coating or dip coating [129]. Based on that, non-conventional EFDTs were also intro-
duced—using electrostatic forces to polymer/composite solutions—to fabricate homoge-
neous coatings with tailored functionalities by a one-step process [128].
Different papers reported the use of electrosprayed interfacial polymerization (EIP)
for fabricating polyamide-based membranes for nanofiltration. EIP simulates an additive
manufacturing process with reciprocating scans of monomer spray; in this way, it is pos-
sible to control the thickness and facilitate the dissipation of reaction heat. Many strategies
have been developed by tuning the surface structure, surface chemistry, and polyamide
layer thickness to enhance separation performance. A polyamide composite nanofiltration
membrane was realized starting from solutions of piperazine, benzenetricarbonyl trichlo-
ride, and Span 80 intercalation was used to coat a commercial membrane via EIP. The
reduced thickness, surface roughness, and additional lamellar spacing nanochannels are
responsible for good flux performance. Thanks to Span 80, high interfacial stability (pol-
yamide layer and support layer), anti-backwashing ability, and 97.8% bisphenol A rejec-
tion are obtained [130].
ES can also be used to realize thickness-controllable selective layers of self-assem-
bling materials onto commercial membranes via non-solvent-induced phase precipitation.
Zwitterionic copolymers are able to self-assemble, thus creating domains that could be
used to provide molecular-scale separation. The Zwitterionic and the non-solvent (isopro-
panol) solutions were deposited on the PAN400 ultrafiltration membrane to realize the
copolymer layer. The results reveal that the ES printing technique enables the fabrication
of a selective layer with a controllable thickness below 50 nm, high water permeability,
and the complete rejection of chlorophyllin dye [131].
Another paper reports a similar procedure to realize ultrathin zwitterionic copoly-
mer coatings onto an ion-selective membrane (ISM) used as the sensing layer of the ion-
Polymers 2022, 14, 4249 19 of 25

selective electrodes sensor (S-ISE). The copolymer and non-solvent solution were co-elec-
trosprayed in order to induce copolymer precipitation. The coated membrane utilizes the
microphase separation of the zwitterionic copolymer to form hydrophilic nanochannels
acting as pores to mitigate biofouling without compromising the diffusion of primary ions
(e.g., NH4+ for NH4+ S-ISE sensors) throughout the ISM matrix and augment the long-
term accuracy and stability of the S-ISE sensors in wastewater [132].
A thin electrosprayed coating can also be realized on fabrics to obtain specific surface
properties. A hydrophobic/superhydrophobic layer onto viscose fabric was obtained
starting from a solution of Poly(tetrafluoroethylene) (PTFE), a synthetic fluoropolymer.
First, the PTFE dispersion was electrosprayed, and then the sintering process was realized
via a thermal treatment to activate the hydrophobicity and stabilize the PTFE-coated vis-
cose fabric. The physical formation and adhesion of particles to the fibers were analyzed
as a function of the sintering temperature. The fabric’s final properties were assessed in
terms of self-cleaning property, anti-fouling property, and air and water vapor permea-
bility. Coated fabrics increase their hydrophobicity by keeping breathability and water
moisture transfer because of the difference between the PTFE-coated and uncoated sides
[133].
ES has also been optimized to realize edible films and coatings acting as a reinforce-
ment of the outer protective layer of foods (peel) and as a barrier to reduce the quality
deterioration process. In particular, the feasibility of producing electrosprayed films with
low and high-methoxyl pectin (LM and HM, respectively) added with recovered sun-
flower wax starting from water emulsion is reported. The results reveal that the addition
of sunflower waxes to pectin films decreased molecular mobility and water molecule ac-
cessibility, reducing the rate of water vapor transmission. The films obtained with HM
pectin resulted in more resistance, less flexibility, and greater stiffness than those from
LM pectin [134].
Recently, A combination of electrospraying and spinning has been proposed to fab-
ricate integrated Lithium-ion batteries (LIB). Thanks to the processes’ low cost, a wide
range of raw materials, good process controllability, and high throughput, electrospin-
ning and electrospraying technologies should be outstanding battery-manufacturing
methods compared to spin coating, doctor blading, and paste coating. In particular, elec-
trospinning was used to realize the polyacrylonitrile (PAN) separator, which was to pre-
vent direct contact between the cathode and anode in case of a short battery circuit, to
allow the fast transportation of Li+ ions and guarantee thermal stability and good me-
chanical properties. Then, the lithium iron phosphate (LiFePO4) cathode and commercial
graphite anode are sprayed separately on both sides of the separator. The coated separator
was then used to realize the LiFePO4||graphite full cell by electrolyte-injecting and pack-
aging processes. The as-prepared full cell could light up a red light-emitting diode and
provide high Coulombic efficiency of 97% and great cycling stability (capacity retention
is 80.3%) [135].

6. Conclusions and Future Perspectives

In agreement with recent trends and political issues for environmental safety, sus-
tainability is emerging as an essential criterion for developing innovative products suita-
ble for biomedical and bio-environmental applications. For instance, a strong demand
concerns the use of green technologies properly adapted to face the compelling need to
‘manufacture” biomaterials in combination with biological matter, i.e., cells, extracellular
matrix (ECM), to produce even more complex living/not living products able to mimic the
chemical and structural features of natural tissues.
Nowadays, substantial efforts are currently underway to synthesize new chemical
and/or physical formulations to reach, within a few years, the definition of a new class of
bio-sustainable materials that might combine the basic features of renewable natural re-
sources and those of conventional biomaterials. In this view, significant attention should
be focused on designing green processing routes with a lower energetic impact that
Polymers 2022, 14, 4249 20 of 25

should be progressively used by slowly replacing the traditional ones. Considering the
different classes of biomaterials, from resorbable polymers such as polysaccharides and
the proteins extracted from natural sources (i.e., plants and animals) to bioactive ones with
solid interaction with living tissues can be successfully used in combination with fully
sustainable and non-hazardous solvents, EFDTs are currently ready to face the challenge,
allowing them to manipulate polymeric materials and their composites from renewable
sources soluble in aqueous solutions, thus limiting the use of fossil-fuel-based products
during product manufacturing. Meanwhile, new ideas to process via EFDs are under con-
stant development due to their immense versatility and the high customization of the ex-
perimental setups. To date, more significant trends are mainly addressed to green manu-
facturing conditions involving the optimization of cross-linking reactions in a green envi-
ronment to improve final devices’ structural and functional complexity.
In this perspective, a growing interest is emerging for the use of marine biopolymers
to be efficiently used in the biomedical (i.e., cell scaffolds, bio-adhesives, molecular re-
lease, wound healing) and environmental application (i.e., water remediation). In this
view, several works are suggesting the use of combinations of marine polymers (i.e., car-
rageenans, ulvans, fucoidans, laminarins)—usually characterized by low processability
due to the absence of chains entanglements—with other biopolymers to obtain new for-
mulations (i.e., blends, emulsions) with improved spinnability, suitable for the fabrication
of nonwovens membranes by via co-electrospinning. This approach may contribute to
overcoming some of the intrinsic limitations due to the poor mechanical properties and
fast degradation of these materials in aqueous media. Meanwhile, the use of novel cross-
linking methodologies based on the use of green compounds can offer the opportunity to
modulate the mechanical properties in order to optimize polymer stability as a function
of the required longevity in aqueous media, without significant decay of the main prop-
erties (i.e., hydrophilicity, stiffness). This approach could pave the way for the develop-
ment of novel hybrid nanofibrous scaffolds with fascinating properties toward the more
sustainable use of biomaterials.
Author Contributions: Conceptualization, V.G.; Draft preparation, N.Z.R., I.C.-M., I.B. and V.G.;
Writing—review and editing, N.Z.R., I.C.-M., I.B. and V.G.; Funding, V.G. All authors have read
and agreed to the published version of the manuscript.
Funding: AFOSR 3DNEUROGLIA FA9550-18-1-0255, MSCA-ITN-2020-ASTROTECH (GA956325).
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable
Data Availability Statement: Not applicable.
Conflicts of Interest: The authors declare no conflicts of interest

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