J Mater Sci (2024) 59:6206–6244

Review

A review on polyaniline and its composites:

from synthesis to properties and progressive
applications
Navdeep Sharma1,* , Anoop Singh2, Naveen Kumar3, Ashish Tiwari4, Madan Lal5, and
Sandeep Arya2

1
Department of Physics, School of Basic Sciences, Abhilashi University, Chailchowk, Teh. Chachyot, Mandi, Himachal Pradesh 175045,
India
2
Department of Physics, University of Jammu, 180006, Jammu, Jammu and Kashmir, India
3
Department of Physics, Chandigarh University, Gharuan, Mohali 140413, India
4
Faculty of Biomedical Engineering, University of Delaware, Newark, DE 19713, USA
5
Department of Allied Sciences (Physics), Graphic Era (Deemed to Be University), Dehradun, Uttarakhand 248002, India

Received: 13 December 2023 ABSTRACT

Accepted: 4 March 2024 Polyaniline (PAni) is a widely studied conductive polymer that has unique
Published online: properties such as high conductivity and stability. However, poor solubility and
10 April 2024 mechanical properties limit its prospective applications. To overcome these limi-
tations, different synthesis methods have been developed and studied. One of
© The Author(s), under these methods is to make the composites of PAni which displayed prominent
exclusive licence to Springer results not only in addressing poor stability but also in achieving high mechani-
Science+Business Media, LLC, cal properties. This review summarizes various synthesis methods, properties,
part of Springer Nature, 2024 and applications of PAni composites that have been incorporated with differ-
ent materials such as carbon, carbon nanotube, graphite, graphene oxide, metal
and metal oxides, metal–organic framework, bio-molecules, silica, and many
more to enhance their potential applications. The most important applications
of the PAni composite are briefly revealed at the end of this review and discussed
appropriately.

Introduction innovation enabled the possibility to apprehend the

nature of polymers. Polymers can be categorized on
Today’s era is not only constrained by the limited various roots such as source, structure, polymeriza-
use of polymers because polymers were considered tion process, and their conducting properties [1].
as an electronically insulating material but with time Shirakawa et al. in 1977 successfully synthesized

Handling Editor: Annela M. Seddon.

Address correspondence to E-mail: sharmanavdeep1@gmail.com

E-mail Addresses: aschib1111@gmail.com; naveensethi99@gmail.com; atiwari@udel.edu; ashish.larpm@gmail.com;
madan.physics26@gmail.com; snp09arya@gmail.com

https://doi.org/10.1007/s10853-024-09562-z

Vol:.(1234567890)
J Mater Sci (2024) 59:6206–6244 6207

poly-acetylene and reported their electrical conduct- semiconductors [11]. Electrical conducting polymers
ing properties, which presented an innovation of a exhibit deep interest because of their potential appli-
novel class of polymer called conducting polymers cations in sensors [12], LEDs [13], electrochromic
(CPs). MacDiarmid, Shirkawa, and A. Heeger were devices [14], charge storage devices [15], electronic
bestowed with the Nobel Prize in 2000 for the innova- devices [16], etc. Figure 2 shows the overview of the
tion and improvement of conducting polymers [2, 3]. broad conductivity of conducting polymers and their
Poly-pyrrole, poly-thiophene, polyaniline, etc., were composites ranging from insulator to metallic state.
remarked as conducting polymers due to the exist- Conducting polymers (CPs) can facilitate the
ence of conjugated 𝜋–electrons in the backbone of the reversible change in electrical properties over the
polymer chain because it provides an easy path for entire range, from that of an insulator to that of a
the frequent motion of charge carriers by delocaliza- metallic conductor. However, CPs struggle with
tion through the whole polymer chain and exhibits major drawbacks such as un-processability and
electronic properties. Alan Heeger also suggested a intractability which put them in a more difficult state
doping scheme to enhance the conductivity of the to obtain the desired forms. Among ICPs: polyani-
polymer. Chain symmetry and doping are prime fac- line (PAni) is the most studied polymer, due to easy
tors contributing to conductivity in polymers [4–6]. synthesis, low-cost monomer, better environmental
The most investigated conducting polymers, so-called stability, and tunable properties [17]. In many appli-
4th-generation polymeric materials, are polyaniline, cations, solid-state PAni is found to be least useful
poly-phenylene sulfide, poly-pyrrole, poly-thiophene, in technological aspects, because of its poor solubil-
poly-para phenylene, poly-phenylene vinylene, and so ity in common organic solvents and subsequent loss
on [7–10]. Figure 1 displays the structure of some of of mechanical strength at higher temperatures [18].
the conductive polymers. To improve the versatility of polyaniline’s applica-
Intrinsic conducting polymers (ICPs) are a new tions in various technological fields, it is essential
class of organic polymers that conduct electricity to improve quality and effectiveness by overcom-
and are called synthetic metals. ICPs are very ver- ing limitations such as poor processability, weak
satile because of their unique properties electri- mechanical properties, poor solubility, and instabil-
cal, magnetic, and optically similar to metals and ity at ambient conditions [19–21].

Figure 1  Conducting poly-

mers and their structures.
6208 J Mater Sci (2024) 59:6206–6244

Figure 2  Conductivity in
PAni and PAni composites.

However, several successful attempts have been by incorporating < 1 wt% of graphene nanosheets. The
made by the researchers to overcome these limita- binary doping process and graphene combination also
tions to make the multidisciplinary approach of poly- improved the thermal stability of PAni. These PAni/
aniline. Many researchers have sought to overcome graphene nanocomposites exhibit favorable morpho-
PAni constraints in many ways including the develop- logical, electrical, and thermal properties, suggesting
ment of PAni derivatives; Sathyanarayana et al. [22] their potential for diverse biomedical applications,
synthesized an ortho-substituted poly-ethoxy aniline including tissue engineering, biosensors, controlled
(POEAni) by electrochemical and chemical methods. drug delivery, and surface coating [25]. Further,
Results showed excellent solubility and corrosion inhi- Li et al. demonstrated the in situ polymerization of
bition of iron in the presence of acid chloride. Fur- aniline with amine-functionalized carbon nanotubes
ther, Hendi et al. demonstrated that electrodeposited (A-CNT) composites. The results reveal high con-
polyaniline on carbon nanotube fiber (PAni/CNTF) ductivity and Seebeck coefficient. The unique inter-
succeeded in replacing platinum (Pt) electrodes in layer PAni formed through strong π–π interactions
fibrous solar cells. The results showed enhanced elec- facilitated effective charge transfer between PAni and
trical and mechanical properties. This modification A-CNT. This resulted in PAni serving as conductive
improves triiodide ion reduction in dye-sensitized bridges, connecting A-CNT bundles, and enhanc-
solar cells, significantly boosting photovoltaic and ing charge transport. Empirically with fine-tuning of
electrochemical performance compared to unmodified the doping level, the composite with 94 wt% A-CNT
fiber [23]. Saadattalab et al. demonstrated enhanced achieved a power factor of 401 µW ­m−1 ­K−2, surpass-
thermal stability in PAni-CNT nanocomposites com- ing most PAni composites and superior to most of the
pared to pure PAni and PAni-ZnO. The study revealed reported organic composite materials. These findings
that increasing the nanoparticle content in the matrix highlight the potential application of the materials for
improved thermal stability. The electrical conduc- thermoelectric power conversion [26]. Hence, it esca-
tivity of PAni/CNT surpassed that of pure PAni, lates their efficacy and more exploration curiosity of
attributed to the formation of a continuous conduc- the researcher in distinct fields.
tion path. The incorporation of ZnO and CNTs in a Several attempts have been made using different
polyaniline matrix yielded nanocomposites with sig- methods to improve these properties. In this review,
nificantly improved mechanical properties, making we have focused on the prominence of conducting
them suitable for applications in solar cells and other composites polyaniline and their specific applica-
energy-related devices [24]. Baniasadi et al. reported tions. This review is divided into four parts: (1) poly-
enhanced electrical conductivity (2–7 ­Scm−1) in PAni aniline, (2) synthesis methods, (3) composite polyani-
line, and (4) applications, respectively.
J Mater Sci (2024) 59:6206–6244 6209

Polyaniline (PAni) be converted between emeraldine salt and base state

via protonation/deprotonation using acid or base [32,
The discovery of polyaniline (PAni) opened a new 33]. The beauty of the different states of PAni belongs
horizon in the field of conducting polymers. It is the to their specific color’s occurrence. For example, Leu-
second most studied conducting polymer due to its coemeraldine is colorless or clear and the Emeraldine
structural chemical form and ability to switch between state shows blue and green color in base and salt form,
conductive and resistive states via the doping process respectively, while Pernigraniline displays blue or vio-
and vice versa. The history of PAni is old somewhere let color [34]. This color transformation property of
between ~ 1816 and 1876. Henry Letheby in 1862 repre- PAni due to various oxidation states played a vital role
sented polyaniline as aniline (Ani) black, which can be in sensor, electro-chromic device, and digital image
easily synthesized via oxidative polymerization using colorimetry (DIC) applications [35–37]. Figures 3 and 4
chemical or electrochemical methods and achieved represent the different oxidation states and inter-con-
in powder as well as film, respectively [27–29]. The version/switching behavior of the emeraldine state of
different states of polyaniline were proposed by Mac PAni from insulator to conducting material and vice
Diarmid in 1991. PAni contained three different forms versa [27].
depending upon their oxidation level: Leucoemeral- The presence of both quinoid and benzenoid rings
dine (fully reduced state), Emeraldine base (half oxi- in the polymer backbone had significantly different
dized state), and Pernigraniline (fully oxidized state) ratios and caused to produced three oxidized states,
[30, 31]. Emeraldine salt is the only oxidation state namely the fully reduced Leucoemeraldine state has
of PAni occurred in conducting form and was stable a quinoid state, the fully oxidized Pernigraniline state
at room temperature, while the rest showed insulat- has a benzoined state and the stable conducting form
ing behavior and were unstable because they can be entails benzenoid and quinoid rings in the equal ratio.
oxidized or decomposed in air. However, the Emer- The chemical properties of PAni do not change with
aldine base is one intermediate form of PAni that can the dopant because it will not create any bond with the

Figure 3  Different structural forms of polyaniline.

6210 J Mater Sci (2024) 59:6206–6244

Figure 4  Formation of the conducting state of PAni by oxidation and protonation bases.

main polymer chain; however, the dopant only lies in reactants are required for the chemical synthesis: a
the vicinity of the polymer chain to facilitate carrier monomer, an acidic medium (which can be either
mobility [38]. Hence, the doped conducting practices aqueous or organic), and an oxidant [40]. After the
of PAni enable the engineering of electromagnetic polymerization of the monomer in aqueous media
shielding antistatic coatings, and so on [39]. using oxidizing agents, prettification was observed
and could be seen by a visible change in the color of
the polymerization solution during the preparation
Synthesis of polyaniline and polyaniline of polyaniline. The color change provides signifi-
composites cant information on a primary basis. After a definite
time, the initial colorless solution turns to blue and
Conductive polymer: diverse synthesis routes then to dark blue, which indicates the formation of
di and oligomers, and with subsequent time, a dark
Different synthesis methods are being used for the green precipitate of conducting salt state of PAni is
preparation of conducting polymers such as polyani- observed. The autocatalytic behavior during polym-
line and their composites as shown in Fig. 5. erization and the rate of the process depends upon
many variables like the nature of the oxidant used,
dopant, the concentration of reactant, etc. [40, 41]. This
Chemical synthesis method is also utilized for the preparation of com-
posite materials. The most commonly used oxidizing
The classical route used to synthesize conducting agents include hydrogen peroxide ­(H2O2), ammo-
polymers is a chemical oxidation mode, and it is a nium persulfate ((NH4)2S2O8), potassium dichromate
cheap and easiest approach. This method is used to ­(K2Cr2O7), and cerium sulfate (Ce(SO4)2), potassium
produce a large yield of polymers. In this method, ferricyanide ­(K3(Fe(CN)6)), potassium iodate ­(KIO3),
the monomer precursor of the polymer is used and and sodium vanadate ­(NaVO3), etc. [40–42]. The pH
mixed with an oxidizing agent. This method involves of acid dopants causes to affect the conductivity and
the direct oxidation of polymeric material. Three hence the physical parameters. Polyaniline and their
J Mater Sci (2024) 59:6206–6244 6211

Figure 5  Different synthesis

methods presentation.

composites have shown great conductivity when the acid (HCl). Results revealed that increasing the molar
pH level is between 1 and 3 [42–44]. During polymeri- ratio of oxidant to monomer from 0.2 to 1.5, increased
zation the solution temperature also affects the results, the yield of polymerization. Dan et al. [48] also sug-
to avoid the secondary reaction; the temperature must gested that reaction yield and intrinsic viscosity of
be kept between 0 and 4 °C [45]. Schematic representa- polymer depended on synthesis parameters. Erdem
tion demonstrates synthesis of polyaniline by chemical et al. explained the effect of different acids versus
oxidation method as shown in Fig. 6 [46]. oxidants used for the polymerization of PAni. The
Blinova et al. [47] investigated the oxidative polym- results showed that the yield and conductivity of
erization of aniline with ammonium peroxydisulfate PAni were observed to decrease in the following order:
(APS) in an aqueous solution containing hydrochloric oxalic acid > malonic acid > succinic acid > glutaric

Figure 6  Synthesis of polyaniline by chemical oxidation method.

6212 J Mater Sci (2024) 59:6206–6244

acid > adipic acid > phthalic acid, respectively [49]. acid exhibited higher conductivity, as measured by
Stejskal et al. [50]. reported the conductivity of proto- the four-probe technique [58]. Jiang et al. studied the
nated PAni to be 1–10 ­Scm−1 when strong acids were solubility and electrical conductivity of the organic
used. Additionally, Chiang et al. [51] proposed that acid-doped PAni derivatives; poly(o-chloroaniline),
the conductivity of PAni depends primarily on two poly(o-toluidine), and poly(o-anisidine) with cam-
variables, namely the degree of oxidation and proto- phor sulfonic acid (CSA). The electrical conductivity
nation of the polymer, which are both associated with of the prepared film at a molar ratio 1:1 with solvent
its oxidation states. Because polyaniline is customarily m-cresol exhibited higher conductivity due to higher
prepared by the oxidative polymerization of aniline in expanded conformation [59]. Sinha et al. [60] demon-
the aqueous medium [7]. Abdiryim et al. [52] studied strated the synthesis of PAni with different types of
the dopant effect of different organic sulfonic acids dopants, such as DBSA, p-TSA and hydrochloric acid
on PAni. The results showed a distinct effect on the (HCl), lauric acid (LA), and studied that the differ-
physicochemical properties of PAni and found that ent type of dopants and their molecular size played
p-toluene sulfonic acid resulted in higher levels of important roles in the properties of PAni. Bhadra et al.
doping, conductivity, crystallinity, and electrochemi- investigated the impact of aromatic substitution in
cal activity compared to methyl sulfonic acid and Ani on the physicochemical properties of PAni and
dodecyl benzene sulfonic acid. PAni was synthesized other polymers. Results showed that the order of elec-
via in situ chemical polymerization using CSA, p-TSA, trical and thermal conductivity of studied polymers
and DBSA as dopants and found that DBSA-doped was PAni > poly(m-aminophenol) (PMAP) > poly(o-
PAni showed better room temperature conductivity ethylaniline) (POEA) > poly(m-nitroaniline) (PMNA),
compared to the other two [53]. Further, DBSA-doped respectively [61]. Bilal et al. [62] reported that the
PAni synthesized chemically at varying molar ratios, physio-chemical properties of PAni-doped DBSA
exhibited remarkable properties affecting microstruc- changed greatly when synthesized at different tem-
ture, molecular weight, crystallinity, optical proper- peratures. Balcha et al. found that temperature sig-
ties, solubility, and conductivity. However, an increase nificantly affects the molecular structure, morphology
in the aniline to DBSA molar ratio led to a decrease in crystallinity, and electrical conductivity of PAni [63].
the conductivity of resulting PAni [54]. Dominic et al.
[55] revealed an over-oxidation effect with PAni-LiCl
salts. The results showed that an increase in LiCl con- Electrochemical synthesis
centration beyond the optimized monomer-to-oxidant
ratio (~ 1:1.125) significantly decreased the conductiv- The electrochemical synthesis produces highly con-
ity of PAni, primarily due to over-oxidation. Rahim ductive films by emphasizing electrochemistry and
et al. [56] demonstrated the synthesis of sulfonated electrochemical processes. Despite challenges in mate-
oxalic acid-doped polyaniline and showed that sul- rial matching with the synthetic conditions and scal-
fonated polyaniline is hybrid and thermally more sta- ing up the reaction system to laboratory scales, this
ble than pure polyaniline. Polymerization of aniline fast and clean method has numerous applications in
was also conducted at 45 °C under an inert atmos- electronics, energy storage, and sensing [64, 65]. PAni
phere using various substituents and dopants. PAni can be synthesized through three electrochemical
doped with p-TSA exhibited the highest conductivity, methods: galvanostatic, potentiostats, and potentio-
attributed to resonance stabilization. The study dem- dynamic. The process requires a reactor vessel with
onstrated that substituents and dopants had a signifi- a working electrode, a counter electrode (usually
cant impact on the structure–property relationships made of platinum), and a reference electrode (typi-
of PAni [57]. Gok et al. investigated UV–Vis spectra of cally a saturated calomel electrode). Figure 7 displays
emeraldine salt of poly(o-toluidine) and poly(2-chloro- the schematic representation of the electrochemical
aniline) to determine the effect of dopant anions at dif- method [64–66].
ferent pKa values. The study used formic (HCOOH), In addition to traditional electrodes, materials such
acetic ­( CH 3COOH), propionic ­( C 2H 5COOH), and as conducting glass covered by indium-doped tin
boric ­(H3BO3) acids as both dopants that act as anions oxide (ITO) electrodes, iron, copper, gold, graphite,
and synthesis media. The result showed that Poly(o- and stainless steel, etc., can be used to deposit poly-
toluidine) doped with formic, acetic, and propionic aniline film. After the completion of electrochemical
J Mater Sci (2024) 59:6206–6244 6213

Figure 7  Schematic of elec-

trochemical (EC) synthesis
setup.

synthesis, the film could be removed from the elec- between galvanostatic, potentiostatic, and potentiody-
trode surface by immersing it in an acidic solution namic methods. Resistance values were influenced by
[67]. Pharhad et al. synthesized chloride-doped PAni doping/dedoping and the thickness of the PAni film
films using the potentio-dynamic method in an acidic [65]. Jiang et al. [70] prepared a free-standing film of
medium. Cyclic voltammetry study revealed that electrochemically reduced graphene oxide/PAni com-
the doped films were highly hygroscopic. A mono- posites in a single step, which was characterized by
mer concentration of 0.1 M was found significant to various techniques. The resulting film exhibited high
produce high-quality films with smooth surfaces, mechanical stability, flexibility, and conductivity.
good adhesion, and uniform distribution, although Table 1 represents the overall summary of the
the polymerization rate was slow. High concentra- advantages and disadvantages of chemical and elec-
tions (0.15 M) lead to faster polymerization rates but trochemical synthesis methods. In conclusion, both
result in rough, non-uniform, and flaky films with chemical and electrochemical methods have their
poor electrode adhesion [68]. Ozylmaz et al. [69] advantages and disadvantages over one another, and
synthesized polyaniline coatings on stainless steel a choice of technique should be made on the specific
electrodes using two different scan rates, resulting in application.
different morphology and structure in the film with
varying morphology and structure with the variation Advanced synthesis methods
of the first cycle. Mondal et al. used three methods
to prepare PAni films deposited on a stainless steel Recent studies showed that varying the conditions of
substrate for electrochemical impedance analysis and aniline polymerization allows the synthesis of poly-
investigation showed differences in resistance values mer materials with specific structures and properties,

Table 1  Comparative exploration of the chemical and electrochemical synthesis methods of PAni
Synthesis methods of PAni Advantages Disadvantages References

Chemical synthesis Cheap, easy, produce large volumes of con- More risk of chemical hazardous, difficult [59, 60, 68]
ducting polymer in powder form purification, environmental impact, repro-
ducibility issue
Electrochemical synthesis Speedy, easy, and clean method to obtain Expensive, high energy consumption, [65, 66, 68, 71]
highly conducting film which permits a limited scalability, electrode fouling may
superior adhesion of polymer on trans- cause reduced efficiency, complex setup,
ducer surface, no catalyst required safety hazardous, electrolyte limitations,
electrode degradation
6214 J Mater Sci (2024) 59:6206–6244

making polyaniline useful in science, engineering, morphology, specific energy, and specific capaci-
medicine, and industry. Several other methods were tance and become promising candidates to use as a
developed for PAni/PAni composites preparation, to supercapacitor material [75].
mitigate the shortcomings faced in the applicability of
polyaniline. We have discussed prominent routes here.
Sonochemical synthesis
Interfacial polymerization
A sonochemical method is simple and innovative
Interfacial polymerization is a kind of step growth for the fabrication of PAni and its composites. The
method, which is carried out at the interfaces of two method is a part of polymer sonochemistry in which
immiscible solvents as shown in schematic Fig. 8. ultrasound radiation is used as an energy source to
Dallas et al. synthesized polyaniline via interfacial accelerate the reaction in two aspects; (i) by reducing
polymerization of aniline at the interface of water the reaction time, and (ii) by upgrading the yield.
and chloroform, which are immiscible solvents. The The rapid increase in the polymerization process/
process is carried out using an acidic aqueous solu- reaction rate was due to intense collapse effects aris-
tion and oxidizing agents (ammonium peroxydisul- ing due to cavitation formed [76]. Jing et al. demon-
fate and hydrogen peroxide) to initiate the reaction strated the fabrication of polyaniline nanofibers by
at room temperature or any optimized temperature. the drop-wise addition of APS solution into aniline
The synthesis of PAni was carried out in the presence solution and advocated the use of ultrasonic irra-
or absence of surfactants. The end product was sepa- diation instead of mechanical stirring. The polymer
rated through centrifugation [72]. The method used PAni fibers were obtained in the first stage by both
to prepare bulk quantities of polyaniline nanofibers modes i) ultrasonic irradiation and ii) mechanical
without templates, or special devices. A variety of stirring methods. However, over time, mechani-
PAni-nanofibers such as 1-dimensional nanofibers cally stirred synthesized PAni nanofibers turned in
and spherical shaped with different sizes can be to irregular shapes, whereas the growth of irregu-
achieved which also depends on the appropriate lar shapes is prevented in the case of the ultrasonic
reaction conditions and reagents used [72, 73]. Chen irradiation method. It showed that the additional
et al. [74] prepared differently shaped PAni–nanofib- progression and agglomeration of the primary PAni
ers at different ratios such as nanorods (dopant/ fibers are efficiently prevented by the sonochemical
monomer ratio = 1:10), spherical PAni particles method. The advantage of the sonochemical synthe-
(dopant/monomer ratio = 5:10), and bud-like struc- sis method over other template-free synthesis meth-
tures (dopant/monomer ratio = 9:10), respectively. ods is its scalability. Also, PAni nanofibers show
Guan et al. demonstrated the fabrication of the PAni higher solubility and lower conductivity than PAni
nanofibers in the presence of para-phenylenediamine particles compared to irregularly shaped PAni fib-
used as an additive or initiator. Results showed the ers [77].
profound effect of additives or initiators on polymer

Figure 8  Schematic presentation of interfacial polymerization.

J Mater Sci (2024) 59:6206–6244 6215

Plasma polymerization and thickness of the used template. UV–Vis spec-

tra confirmed that photo-catalytic property of PAni/
Plasma polymerization is a method employed to TiO2 micro-tubes was higher than that of simple ­TiO2
fabricate thin film. It is a simple, reliable, and cheap micro-tubes, due to the sensitization of PAni. Figure 9
method because the monomer is polymerized in the shows the schematic presentation of the bilayer PAni/
absence of both oxidant and solvent. In the plasma TiO2 micro-tubes [84].
polymerization of aniline, these two techniques are However, the template synthesis method suf-
required. (1) two parallel electrodes and ultrasoni- fers from some constraints; as polymeric nanotubes/
cally clean glass substrates are placed on the lower nanofibers may be destroyed or possibility to form
stainless-steel electrode for the deposition of polymer undesirable aggregated structures when removed
thin film. (2) Monomer aniline was injected between from the template, further the process requires exten-
the electrodes at monomer vapor pressure (~ 0.2 torrs) sive post-synthesis procedures to eliminate the tem-
and the glow discharge chamber must be evacuated. plates [85, 86].
The electrodes were utilized to generate a discharge
by applying a high voltage (~ 500–800 V) and low
frequency (~ 50 Hz). Polymer thin films were grown Seeding polymerization
under optimum conditions on the substrate [78].
Xing et al. prepared PAni nanofibers by seeding
Nastase et al. [79] also suggested the thermal polymer-
polymerization method, in which conventional
ization method is the best alternative for the prepara-
polymerized PAni powder dissolved in different
tion of PAni nanocomposites in comparison with con-
acid dopants (like dimethyl sulfoxide, DMF, NMP)
ventional methods. Because the deposition parameters
was used as “seed” to induce the polymerization of
can be adjusted to modify the properties of these films
aniline in different acids (HCl, ­H2SO4, ­H3PO4) solu-
following specific requirements such as applied cur-
tion. Results showed that the conductivity and mor-
rent, monomer flow rate, and time of polymerization
phology of resulting samples depend upon various
and pressure. The advantages of this method exhibits
parameters such as acid concentration, reaction time,
chemically inert, clean, thermally stable, and pinhole-
aniline concentration, acids and organic solvents used,
free PAni-film [80].
seed/-dopant amount, and seed/-dopant concentra-
tion, respectively. Based on the preparation condition,
the conductivity of the samples was predominantly
Template (matrix) synthesis influenced by their (i) doping level and (ii) morphol-
ogy. Maximum conductivity reported with PAni/
Templates are one of the effective strategies to syn- DMSO was 34.5 ­Scm−1 due to both higher doping lev-
thesize different nanostructures materials like; zero- els of seed and well-ordered morphology. On the other
dimensional (nanoparticles ranging 10–1000 nm), hand, the concentration of monomer (aniline) was sub-
one-dimensional (geometry belongs nanowires, nano- jected to the increased size of the obtained nanofib-
cables, and nanotubes), and two-dimensional (nano- ers, but reaction time showed less effect. Further,
disks, nanoflakes, and nanosheet) with desired size
and shape and it depends upon the proper selection of
the template [81]. Template synthesis employed both
(1) chemical and (2) electro-chemical polymerization
for the fabrication of conducting polymer nanotubes
[82, 83]. Xiong et al. prepared PAni/TiO2 bilayer micro-
tubes by template synthesis method. Process com-
pleted in two steps (i) firstly PAni micro-tubes were
synthesized by using the anodic aluminum oxide
template and (ii) secondly, ­TiO2 micro-tubes were
synthesized in the channels of the PAni micro-tubes.
The results revealed that the length of the micro-tubes,
and the diameter, were similar to the pore diameter
Figure 9  Schematic diagram of PAni/TiO2 micro-tubes (bilayer).
6216 J Mater Sci (2024) 59:6206–6244

the morphology of obtained samples was not much Metathesis polymerization

affected despite various acids ­(H2SO4, ­H3PO4) used
as reaction medium. Further study revealed that the Metathesis polymerization is a distinctive form of
morphology of resulting PAni was influenced by the polymerization that does not necessitate the use of
choice of organic solvent used to dissolve PAni pow- aniline monomer for the synthesis of PAni. When
der seed, having differences in their alkalinity. Using p-dichlorobenzene along with sodium amide is heated
NMP as a solvent resulted in aggregated PAni, while at 220 °C for 12 h in the presence of benzene, solvo-
DMSO significantly improved the morphology of the thermal metathesis polymerization takes place and
resulting PAni [87]. produces polyaniline. The reaction scheme for the
preparation of polyaniline is shown in Fig. 10 [90].

Enzymatic synthesis

Liu et al. reported the fabrication of water-soluble Hetero‑phase polymerization

conducting PAni by using a unique biological route.
The method is very simple using a single step; polym- Inclusively hetero-phase polymerization technique is
erization is carried out in very mild conditions and a process in which polymerization occurs in two or
function of pH (~ 4.3) and requires nominal separa- more different phases such as aqueous and organic
tion and purification. The polymerization of aniline is phases and can produce high-quality polymer, i.e.,
carried out by using a horseradish peroxidase (HRP) micro-particles or nanoparticles of polymer/inor-
enzyme in the presence of a polyanionic template and ganic hybrid with tailored properties. This technique
sulfonated polystyrene. Cyclic voltammetry studies includes different methods of polymerization as
revealed that PAni/SPS-complex is oxidatively more depicted in Fig. 11 [91, 92].
stable. The conductivity of the pure PAni/SPS was
found to be 0.005 ­Scm−1 and to be enhanced to ~ 0.15
­S cm −1 after additional doping by exposer to HCl
vapor. The advantages of the enzymatic route led to
ease of synthesis, electrical and chemical stability,
good process-ability, and environmental compatibility
[88]. Nabid et al. prepared PAni/TiO2 nanocomposite
by enzymatic polymerization of aniline in the presence
of sulfonated polystyrene (SPS) and ­TiO2 as a tem-
plate and nanoparticle, respectively. In the presence
of hydrogen peroxide, polymerization was supported
by HRP. Hence results showed that strong interaction
at the interface of PAni and nano-TiO2, as evidenced
by the successful deposition of PAni onto the surface
of ­TiO2 nanoparticles, results in a core–shell structure
[89].

Figure 11  Different kinds of hetero-phase polymerization.

Figure 10  Metathesis polymerization.

J Mater Sci (2024) 59:6206–6244 6217

The main features of hetero-phase polymeriza- films at 300 S c­ m−1, compared to 10 ­Scm−1 for pressed
tion in polyaniline are; controlled polymerization, films. Its effectiveness lies in stabilizing doped PAni
improved solubility, enhanced conductivity, improved chains through hydrogen bonds and structural con-
mechanical strength, and dependence on the choice of straining. Additionally, 2-ethylphenol (228 ­Scm−1)
solvent and surfactant [92–94]. Suspension, micro-sus- and hexafluoropropanol (HFP, 60 ­Scm−1) also showed
pension, emulsion, mini-emulsion, and micro-emul- noteworthy conductivity improvements, emphasizing
sion methods of polymerization of polyaniline have the critical role of solvent selection in optimizing PAni-
been differentiated in terms of particle size formed based films for enhanced electrical properties.
and dispersion of polymer particle formed as shown in In recent, Fabio et al. demonstrated the impact of
Table 2. In these polymerization methods, monomers pseudo-doping on PAni/CSA acid, using a novel sol-
should be dissolved in water (aqueous phase), and vent blend of trifluoroethanol (TFE) and hexafluoro-
different dispersing techniques like homogenization, propanol (HFP). This electroconductive polymer has
stirring, etc., enable them to make a controlled-sized shown a vital role in soft electronic devices, suited well
droplet. The use of the stabilizer (surface active agent) with organized chain structures for conductivity. The
helps to stabilize the droplet in the aqueous media. study suggests TFE and HFP mixtures as a cost-effec-
The size of the droplets also depends upon the polym- tive solution to prevent random coil aggregation in
erization method. Based on the size of the droplet, the PAni/CSA without compromising its properties. Vari-
order of polymerization followed; suspension > micro- ous TFE: HFP ratios were systematically compared,
suspension > emulsion > mini-emulsion > micro-emul- representing the easy removal compared to the stand-
sion [95–104]. ard pseudo-doping solvent, m-cresol. Moreover, spin-
The overall conclusion based on different synthe- coating method shown improved electroconductivity
sis methods confirmed that the properties of PAni are value as: σ(TFE) = 61 ­Scm−1, σ(TFE:HFP (50:50 vol)) = 70
predominantly based on the mode of preparation. S ­cm−1) [106]. SEM analysis shown in Fig. 12 revealed
Each synthesis methods have its advantages and dis- diverse morphologies of undoped PAni pellets, influ-
advantages and can be tailored based on the specific enced by solvent choice. In particular, m-Cresol, HFP,
applications. and TH19 induced higher cohesion compared to other
solvents. These observed differences are attributed to
solvent-induced alterations in PAni chain conforma-
Characteristic properties of PAni tion during solution processing, which persist after
solvent removal. Further, Fig. 12 shows the morphol-
Physical properties ogy of PAni/CSA pellets differs from undoped PAni
pellets. Smooth surfaces are observed in HFP and
Morphological impact TH19 samples, while TFE, TH91, TH55, and m-cresol
samples exhibit some aggregates. ­C HCl 3 samples
Cao et al. [105] reported the effectiveness of differ- show predominant aggregate formation, reduced
ent solvents for enhancing polyaniline conductivity, with higher HFP amounts, suggesting conformational
which should have moderate acidity, low dielectric changes in PAni chains in solution [106].
constant, and a relatively large size. m-cresol emerged
as superior, yielding highly conductive PAni/CSA
Color and conductivity

Table 2  Droplet size range fashioned by hetero-phase polymeri- Color and conductivity of PAni are closely related
zation methods because the color of PAni is determined by its oxida-
Polymerization Droplet size References tion state. This is because of the oxidation process that
causes the formation of delocalized electrons, which
Suspension 50–500 µm [95, 96]
affects its conductivity. Different states of PAni; leu-
Micro-suspension 1–10 µm [97, 98]
coemeraldine is color less, emeraldine base is blue,
Emulsion 50–700 nm [99, 100]
emeraldine salt is green, and pernigraniline is blue
Mini emulsion 50–500 nm [101, 102]
and violet, respectively. Among all states, emeraldine
Micro-emulsion 10–100 nm [103, 104]
salt is a conducting polymer [34, 36].
6218 J Mater Sci (2024) 59:6206–6244

Figure 12  Representation of the SEM images of the PAni and PAni/CSA pellets by solvent casting (with two different magnifications).
Source: Reproduced with permission from reference [106], copyright [2024], [Elsevier].

Solubility most solvents such as dimethyl sulfoxide (DMSO),

N-methyl pyrrolidinone (NMP), dimethylformamide
The solubility of the PAni depends upon its oxi- (DMF). Han et al. [107, 108] demonstrated that solu-
dation state and the solvents dissolved. Pure PAni bility parameters affect interactions in doped PAni,
is insoluble in water and acetone but soluble in making it more polar and hydrogen-bonded without
dopant anions.
J Mater Sci (2024) 59:6206–6244 6219

Thermal stability and doping Chemical properties

Thermal stability of PAni is closely related to its dop- Doping

ing level. The thermal stability of the PAni is attributed
to the strong interactions of polymer chains and the The doping of PAni affects its electronic, optical, and
presence of nitrogen atoms in the backbone [53, 109]. magnetic properties and makes it a versatile mate-
Choi et al. [110] reported that enhanced thermal stabil- rial for various applications such as super-capacitors,
ity of PAni at a temperature range of ~ 250–600 °C was solar cells, electrochemical sensors, energy storage, etc.
achieved with polymerizable dopants, i.e., PCDA-tau- Sinha et al. [60] reported that the type and molecular
rine and PCDA-pBzS. Li et al. [111] demonstrated the size of the dopant influenced the properties of doped
consequence of doping-dedoping and redoping on the PAni. Ryu et al. [115] demonstrated that HCl-doped
stability of PAni films in the temperature range from PAni capacitance decreases during ~ 400 cycles but
100 to 200 °C and found that thermal stability stands becomes constant at ~ 40 ­Fg−1; however, with lithium
in the order of PAni-H3PO4 > PAni-p-TSA > PAni- salt (~ L
­ iPF6) it initially showed a specific discharge
H 2SO 4 > PAni-HCl, and PAni-HClO 4 > PAni-CSA, capacitance of ~ 107 ­Fg−1 and 84 ­Fg−1 during ~ 900
respectively. cycles. Xing et al. demonstrated the effect of differ-
ent dopant anions with PAni for super-capacitors and
electrochemical performance. Results showed that
Mechanical properties PAni –ES with dopant anions of ­H2C2O4 exhibits high
specific capacitance and best cycling stability [116].
Mechanical properties of the PAni are central because
The efficiency of dye-sensitized solar cells using PAni
they determine its ability to perform in various appli-
nanofibers was ~ 4% reported by Ammen et al. [117],
cations. The physical features of PAni, including its
while adding sulfuric acid was improved by up to
hardness, resistance to stretching, capacity for stretch-
27%. Lenin et al. revealed that the electrical conduc-
ing, tolerance to repetitive stress, and elastic modulus,
tivity of PAni is tuned well with different dopants and
were investigated under different conditions such as
leads them to electronic and electrical applications.
force, temperature, pressure, and environment. Zhang
Experimental results showed that increasing the dop-
et al. reported that the organogel with its robust and
ing concentration from 0 to 1.0 M HCl resulted in a
conductive properties can show exceptional gauge fac-
significant increase in electrical conductivity, with the
tor and elongation due to the combination of the frag-
conductivity values changing from 1.98 to 10.2 ­Scm−1
ile PAni and the elastic polyacrylate blending layer.
[118]. Ingle et al. investigated the optical properties of
Results showed the gauge factor that stays high even
PAni, doped with protonic acid, i.e., sulfuric acid and
under large strain, reaching up to 2000% and giving
hydrochloric acid. Results showed that doping of PAni
organogel a wide range of sensing capabilities [112].
with HCl results in a notable shift in optical absorption
Valentova et al. [113] studied the mechanical proper-
peak from 440 to 397 nm, with a blue shift of 43 nm.
ties of PAni and showed that Young’s modulus value
This shift can be attributed to the formation of micro-
of PAni hydrochloride pellets was 0.9 ±0.2 GPa and the
fibers within HCl-doped PAni, altering its electronic
value of PAni base was 1.3 ±0.2 GPa and also suggested
structure and thus its absorption spectrum. Con-
that compression pressure value ~ 700 MPa is appropri-
versely, doping PAni with ­H2SO4 leads to a redshift
ate for the preparation of PAni pellets. Wei et al. dem-
in the optical absorption peak, indicating the presence
onstrated the dynamic mechanical analysis method to
of excitons trapped in π–π* transitions of benzenoid
explore the mechanical properties of solution-cast films
rings. These shifts demonstrate the significant impact
of PAni. Results showed that the storage modulus value
of doping on the optical properties of PAni [119]. Long
of PAni thin films was from ~ 200 MPa to − 2 GPa below
et al. studied the magnetic properties of doped PAni
the glass transition temperature and depends on the
and found that its magnetic susceptibility varies with
content of NMP [114].
temperature, magnetic field, doping level, and dopant
type. This affects the ratio of localized spins, mobile
spins, and spinless bipolarons, leading to changes in
the material’s magnetic properties [120].
6220 J Mater Sci (2024) 59:6206–6244

Chemical stability tailored by selecting and combining specific constitu-

ents and by controlling the processing conditions dur-
Chemical stability is a key factor for the properties ing their preparation [125, 126]. However, PAni has
and applications of polyaniline in various fields. The attractive properties but also shows some limitations,
stability of PAni affects its use as a coating material, as which impact its applications. Composites are widely
it must remain stable in various environments and not used in various applications due to their ability to
react with the substrate or surroundings. Blinova et al. combine the desirable properties of their components.
conducted stability tests on polyaniline dispersions We have discussed here different polyaniline compos-
that were stabilized using poly(N-vinylpyrrolidone). ites in detailed as depicted in Fig. 13.
The tests involved subjecting the dispersions to differ-
ent conditions, such as exposure to high temperatures, Carbon, carbon nanotube, graphene,
sonication, and freezing-melting cycles. The chemical and graphite‑based PAni composites
structure was analyzed using UV–visible spectros-
copy, and colloidal stability was determined through PAni composites are attractive because they combine
the measurement of particle size and poly-dispersity. with the properties of other materials. Hybrid elec-
The results showed that the dispersions were stable trically conducting nanocomposites are made of con-
in both chemical and colloidal aspects, regardless of ducting nanoparticles and conducting polymers to
the pH of the medium, and they maintained their sta- exhibit unique properties.
bility even after 10 years of storage [121]. Alam et al.
[122] examined the corrosion–resistance performance
PAni‑carbon composites
of soya oil alkyd with nanopolyaniline against mild
steel to reduce the toxic heavy metals from the pro-
Wu et al. reported PAni-carbon composite films by
tective coatings. Azim et al. revealed and tested the
an electrochemical co-deposition technique with
efficacy of an acrylic-polyaniline paint coating on mag-
improved electro-catalytic activity for methanol oxi-
nesium alloy ZM-21. Results showed that the coating
dation due to better Pt dispersion and better electro-
effectively safeguarded the metal from damage and
chemical surface area and achieved through doping
prevented the dissolution of the base material from
the PAni matrix with carbon black particles (~ Vulcan
exposure to sodium chloride (NaCl) solution even
XC-72). Hence, carbon black was demonstrated as a
after a 75 day [123].
doping material for conducting polymer electrocataly-
Few properties of PAni are discussed here how-
sis [127]. Sun et al. demonstrated a flexible composite
ever, so many applications with improved quality
can be obtained with polyaniline composites because
the properties of PAni composites may be tailored by
varying the material used to make composites and the
most plausible reason to explore composites of PAni.

Polyaniline composites

Composites are materials made by combining two or

more distinct materials to form a new material with
improved or unique properties compared to their com-
ponents. Thus, composites of polyaniline retain the
individual identities of their constituents while work-
ing together to enhance the overall properties, such as
electrical conductivity and mechanical strength [124].
The constituents can be any type of material including
metals/metal oxide, polymers, ceramics, composites,
etc. themselves. The properties of composites can be Figure 13  Representation of different polyaniline composites.
J Mater Sci (2024) 59:6206–6244 6221

electrode made of PAni and flexible graphite (~ car- 407 μW ­m−1 ­K−2. The flexible thermoelectric device
bon) as conducting substrate was developed as a generates a high power of 1.5 μW at ΔT = 50 K, dem-
substitute for expensive Pt counter electrodes in dye- onstrating its potential for energy-harvesting elec-
sensitized solar cells (DSCs). The in situ polymerized tronic devices [132].
emeraldine PAni showed excellent photocurrent den-
sity and higher efficiency compared to pernigraniline.
The composite counter electrode showed comparable
PAni‑SWCNT composites
conversion efficiency (7.36%) to that of a Pt electrode
(7.45%) in a DSC [128]. Li et al. found that PAni-sulfur/
Ramamurthy et al. studied the electrical characteris-
carbon composites showed superior electrochemical
tics of metal–semiconductor devices using polyani-
performance than sulfur/carbon composites due to
line/SWCNT composite and found consistent charge
the unique core/shell structure. This was due to the
transport in a high voltage range, with critical volt-
combined effect of carbon black and conductive PAni,
age varying with SWCNT concentration and temper-
which contain 43.7 wt % sulfur and exhibit high-rate
ature. Improved material quality may enable use in
charge/discharge capability. The improvement in
organic electronic device fabrication with potential
electrochemical performance is attributed to the core/
applications in microelectronics [133]. Gupta et al.
shell structure of PAni-sulfur/carbon composites and
studied the capacitive performance of Polyaniline/
showed their applicability as a cathode material for
SWCNT composites prepared by electrochemical
lithium/sulfur batteries [129]. Zhao et al. reported a
polymerization and found long cyclic stability with
ternary sulfur/PAni-carbon black composite produced
high specific capacitance (~ 485 F/g), specific power
by combining sulfur and PAni-carbon via a two-step
(~ 228 Wh/kg), and specific energy values (~ 2250 W/
thermal treatment. The composite showed improved
kg) for 73 wt% of PAni in SWCNTs. Further, it was
electrochemical performance in lithium-sulfur bat-
suggested as an excellent electrode material for high-
teries due to PAni acting as a bridge between sulfur
performance super-capacitors [134]. Gupta et al.
and carbon and minimizing active material loss. The
[135] investigated the polyaniline/SWCNT compos-
composite cathode showed improved cyclability and
ites by in situ potentiostatic method and showed sta-
rate capability with a retained discharge capacity
ble specific capacitance (5% decrease after 500 cycles,
of ~ 732 mAh ­g−1 after 100 cycles [130].
1% after 1000 cycles) with good cyclic stability and
suggested as a potential material for super-capacitor
applications.
PAni–CNT composites

Li et al. demonstrated that doping level plays a

decisive part in improving the thermoelectric per- PAni‑DWCNT composites
formance of CNTs/polyaniline composites. Results
showed that lowering the doping levels responsible Heiba et al. investigated the functionality of DWCNT/
for compact PAni chains with localized polarons. PAni composites by in situ polymerizations. Results
High CNT loading (~ 69 wt% or more) enhances showed that adding 2.5% of DWCNTs to polyaniline
the power factor (321 ± 24 µW ­m−1 ­K−2) due to the increased its DC conductivity and showed potential
π–π interaction, doping effect, and conductive car- as a tailored conducting material in energy devices
bon nanotube (CNT) network, which facilitates the such as solar cells, sensors, and supercapacitors [136].
carrier transport. Hence, precise tuning of the dop- Fahrettin et al. conducted a study on the electrical,
ing level is an effective strategy to boost the ther- thermoelectrical, and optical properties of PAni-doped
moelectric properties of CNTs/polyaniline compos- boric acid/double-wall carbon nanotube (DWCNT)
ites [131]. Further, Li et al. proposed a method for nanocomposites. The results indicated an increase in
enhancing the thermoelectric properties of CNTs/ electrical conductivity by decreasing the optical band
Polyaniline composite films through consecutive gap with DWCNT doping. These findings highlighted
dedoping–redoping. The redoping practice leads to the potential of using DWCNTs as a means to modify
an improvement in electrical conductivity, result- the properties of PAni-doped boric acid for various
ing in a significantly improved power factor of optoelectronic applications [137].
6222 J Mater Sci (2024) 59:6206–6244

PAni/MWCNT composites tunable conductivity, solute rejection capability, and

hydrophilicity, permeability. These findings showed
Mohajeri et al. developed a ternary nanocomposite its wide applicability for water treatment and bio-
made of PAni/ZnO/MWCNT synthesized through separations technology [143]. An overall view of car-
thermal chemical vapor deposition. Prepared nano- bon and carbon-nanotube–PAni composites, and their
tubes were then modified with ZnO particles via properties and applications are listed in Table 3.
potentiostatic electro-deposition. The experimental
analysis exposed that the ternary nanocomposite Graphite/graphene oxide—PAni composites
exhibited high response time, stability, and repro-
ducibility, making it a potential material for non- Bourdo et al. evaluated the thermal, structural, and
enzymatic glucose sensing in various fields [138]. electrical properties of PAni/Graphite composites.
Haritha et al. investigated the dielectric properties of Results showed that PAni acts as a charge transfer
PAni-coated MWCNTs synthesized by in situ polym- agent between the basal planes of graphite and exhib-
erization of aniline in the presence of MWCNTs. The ited the highest electrical conductivity with a PAni/
results showed an improved dielectric behavior, with Graphite mass ratio of 4:96 with high thermal stabil-
a uniform coating of PAni and a rise in the complex ity. Composites have shown potential applications in
permittivity and permeability as the filler concentra- nanoelectronics, electromagnetic interference shield-
tion increased. The study proposes the use of these ing, and rechargeable batteries [160]. For example,
materials for lightweight structures in microwave Xiang et al. studied PAni/expanded graphite com-
absorption applications [139]. Awata et al. studied the posites prepared through emulsion polymerization.
effect of CSA doping in PAni/MWCNTs as a superca- The composites displayed significantly improved
pacitor electrode prepared via in situ chemical oxi- electrical conductivity (~ 298.51 ­Scm−1) compared to
dation polymerization. The results showed that the pure PAni. The composites also showed outstanding
PAni/MWCNTs supercapacitor electrode with 2 wt% dielectric loss characteristics with in the frequency
exhibited improved reversibility compared to pure range (~ 1 MHz to 3 GHz), with a peak dielectric loss
PAni [140]. factor (~ 15,000) [161]. Ghanbari et al. investigated Zn-
PAni/Graphite composites as the active material of
the electrode. The results showed that the battery had
142.4 Ah ­kg−1 of output capacity with 97–100% effi-
PAni‑CNT nanofiber composites
ciency (columbic) between ~ 0.70 and 1.70 V over 200
cycles, resulting in a 162.3 Wh ­kg−1 of specific energy
Wang et al. investigated the functionality of the PAni/
[162]. On the other hand, Liu et al. studied that by add-
PAni-CNT composite fibers using an ionic liquid ethyl
ing 15% graphene to polyaniline in a composite-coated
methyl imidazolium bis(trifluoromethane sulfonyl)
fabric, they could improve the thermal conductivity
amide (EMI.bis-TFSA) as an electrolyte through a
up to ~ 82%. Because the graphene worked as a filler
wet-spinning method. The results showed that the
to fill gaps between the polyaniline molecules and cre-
incorporation of CNTs improved the electrochemi-
ated an effective heat-conduction pathway to improve
cal properties of fibers, making PAni/CNT compos-
composite thermal dissipation performance [163]. The
ite fiber, a promising candidate for use in wearable
overall view of the graphite/graphene oxide–PAni
diagnostic systems [141]. However, Liao et al. [142]
composites is summarized in Table 4.
suggested CNT/PAni composite nanofibers prepared
by facile synthesis and results showed that nanofibril-
lar composite was found the best potential material Metal and metal oxide composites
as an electrode and also as a low-cost, disposable sen-
Metal and metal oxide composites represent promis-
sor due to high sensitivity, processability, and tun-
ing areas of research for developing new materials
able conductivity. Further, Liao et al. investigated
with improved properties and novel applications.
electrically conducting ultrafiltration membranes by
Table 5 comprises the method of fabrication, prop-
incorporating SWCNT/PAni nanofibers into a poly-
erties, and prospective applications of synthesized
sulfone matrix. Results showed that these thermally
metal and metal oxide composites with polyaniline,
stable composite membranes have the potential due to
respectively.
J Mater Sci (2024) 59:6206–6244 6223

Table 3  Various carbon material-based PAni composites, their properties, and applications
Composite type Method of fabrication Properties Application References

PAni-carbon Oxidative polymerization Specific surface area and Symmetric supercapacitor [144]
electrochemical perfor-
mance
PAni-activated carbon In situ polymerization Higher mesopores/surface Capacitive deionization [145]
area
PAni-DBSA/carbon In situ polymerization Enhance electrical conduc- Electronic device:–sensor, [146]
tivity charge storage device
PAni-CNT In situ chemical oxidative Thermal stability Electronic devices [147]
polymerization
Pt-Ru/PAni/CNT In situ electrochemical Longer-term stability and Bimetallic electro-catalysts [148]
higher current density
PAni/SWCNT thin film Electrochemical polymeriza- Optical transparency and Flexible energy storage [149]
tion mechanical flexibility
PAni-DMSO/SWCNT Electrochemical polymeriza- High charge mobility and Thermoelectric devices [150]
tion and physical mixing thermoelectric performance
MnCl2/PAni/SWCNT In situ chemical oxidative Higher electrical conductiv- Electrochemical super- [151]
polymerization ity and specific capacitance capacitors
PAni/PS/-MWCNT Solution casting method Enhance conductivity and Hall effect sensor, Electro- [152]
n-type semiconductor magnetic shielding
behavior
HCl/PAni/-MWCNT In situ chemical polymeriza- Improved thermal stability, Electrical, thermal, sensing, [153]
tion high room temperature DC and actuator application
electrical conductivity, and
charge transport properties
Bacteria/PAni-MWCNT In situ polymerization Specific capacitance Supercapacitor electrode [154]
enhanced electrochemical
performance
PAni/MWCNTs Catalytic chemical vapor Enhance sensing property Relative humidity sensing [155]
deposition technique property
Au/PAni-MWCNTs Electro-polymerization Sensing, stability, selectivity, Electrochemical sensing for [156]
reproducibility, and repeat- Zn, Pb, Cu
ability
PAni/PAni-CNT nanofiber Single-step electrospinning Specific capacitance reten- Super-capacitor Electrodes [157]
process tions
PVDF/PAni-nanofiber Emulsion polymerization Tensile strength and thermal Thermal conductive poly- [158]
conductivity meric materials
P olyimide/CFC-PAni- Thermocuring High thermal stability, tensile Tribology [159]
nanofiber strength and modulus

Microscopic exploration of PAni composites intrinsic properties of pure PAni prevent agglomera-
tion, due to a lower inverse barrier. This is attributed
To comprehend the morphological transformation to the potency of aniline molecules to establish a bar-
during the composite formation, Oyetade et al. [177] rier effect, thereby reducing polyaniline aggregation
exposed in their review by explaining SEM micro- [178]. Further, Chatterjee et al. in their FE-SEM study
graph, because the microscopic techniques unveil revealed that PAni undergoes agglomeration at high
agglomeration points in the composite fabrication; as aniline concentrations, with results found similar to
illustrated in Fig. 14, Gilja et al. demonstrated that the Fig. 14. However, after composite fabrication, the
6224 J Mater Sci (2024) 59:6206–6244

Table 4  Overall view of graphite/graphene oxide–PAni composites

Composite type Method of fabrication Properties Applications References

PAni/graphite In situ polymerization Enhanced electrical conduc- Electromagnetic interface [164]

tivity Shielding
PAni/graphite/CoFe2O4 Emulsion polymerization Increased electric and mag- Microwave shielding [165]
netic properties
PAni/graphite/MoO2 Chemical polymerization Enhanced electrical and Eco-friendly application: [166]
thermal stability power density system
PAni/graphite Solution method Increased thermal stability Sensor application [167]
Cellulose/graphite/PAni Novel approach/electro- Increase specific energy& Power flexible electronic [168]
deposition power, coulombic efficiency devices, flexible superca-
pacitor
PAni/CNT/graphite Facile sol–gel chemical route Superior sensitivity and Detection of Bisphenol A [169]
stability
PAni/tannic acid/rGO Green and facile synthesis High energy density, power Supercapacitor electrode [170]
density/current density
PAni/graphene fiber Self-assembly method and Structural stability of Wearable/flexible electronic [171]
chemical reduction process PAni and high capacitive devices
response
PANi/graphene In situ facile synthesis Increased surface rough- Nanodevice sensor [172]
ness, electrical property, &
stability
PAni/graphene Chemical method Charge storage capacity Electrochemical energy stor- [173]
age devices
Strontium/PAni/graphene Facile synthesis Improve specific capacity, Hybrid energy storage [174]
electrochemical perfor- devices
mance
PAni/graphene Novel self-assembly method Synergistic effect between Flexible high-performance [175]
polyaniline and graphene supercapacitor, wearable
sheets electronics
PAni/reduced graphene oxide In situ chemical oxidation Enhanced diffusion pathway/ Detection of trace level of [176]
charge transfer mechanism ammonia

interaction of PAni with single-walled carbon nano- pore size, enhanced surface area, and chemical stabil-
tubes hinders agglomeration, ultimately enhancing ity [212, 213]. These properties make MOFs a promis-
the blend’s surface area [179]. Hence, Fig. 14 reveals ing material for various applications, and they have
that agglomeration hinders synergistic effects with been the subject of much research and development.
available binding sites, limiting dye degradation in The combination of MOFs and PAni provides a sig-
the composite photocatalyst. Microscopic elucidation nificant approach and promising results in develop-
exposes agglomeration points and morphological ing new materials with improved properties which are
transformations during pre-dye photocatalysis fabri- summarized in Table 6.
cation [177, 180].
PAni and biomolecules
PAni and metal–organic frameworks
In the recent development of biomolecule composite
Metal–organic frameworks (MOFs) are a class of materials, PAni is typically combined with biopoly-
porous materials composed of metal ions linked by mers such as proteins, polysaccharides, nucleic acids,
organic ligands. MOFs have gained significant atten- and/or biocompatible materials. By combining PAni
tion because of their unique characteristics like tunable with different biomolecules, novel materials with
J Mater Sci (2024) 59:6206–6244 6225

Table 5  Overall view of metal and metal oxide—PAni composites

Composite type Method of fabrication Properties Applications References

Au/PAni Ultrasound mixing High surface energy CO sensing properties [181]

Au/PAni Two-step methods High-rate catalytic activity Reduction of organic dye, [182]
biosensor
PAni/Pr In situ polymerization Increased self-healing Anti-corrosion [183]
behavior
PAni/Pt Wet chemical synthesis High specific capacitance, High performance superca- [184]
high elasticity, and flex- pacitor
ibility
PAni/Cu In situ chemical polymeriza- Higher electrical conductiv- Memory devices, sensor [185]
tion ity, thermal stability
PAni/Zn Solution mixing Increase electrical conductiv- Anti-corrosion [186]
ity, the synergetic effect of
Zn NPs
PAni/Ag Chemical method/matrix- Saturable and reverse satura- Nonlinear optical properties [187]
assisted pulsed laser ble absorption for laser
deposition
PAni/Ag Chemical synthesis Enhanced thermoelectric Thermoelectric application [188]
performance
PAni-Ag core–shell Chemical oxidative polym- Enhanced sensitivity and X-band electromagnetic [189]
erization conductivity interface (EMI) shielding
Iron/PAni In situ polymerization Improved methanogenesis Anaerobic waste water treat- [190]
and microbial extracellular ment
electron transfer rate
Ta/PAni In situ chemical oxidative Better response value and Gas sensing application [191]
polymerization sensitivity
PAni/Se Chemical polymerization A significant increment in Transistor and diode [192]
method conductivity
Pt/PAni Electrochemical Excellent catalytic tolerance, Fuel cell technology [193]
electro-catalytic oxidation
PAni/Fe–Ni–Co3O4 In situ polymerization Good mesoporosity, Supercapacitor [194]
improved cyclic stability,
thermal stability, specific
capacitance, and charge
stability
PAni/SnO2/Pd Hydrothermal synthesis Improved gas sensitivity at Gas sensing application [195]
technique room temperature
Pd/PAni/foam nickel Two-step electro-deposition Enhance electrochemical Electrocatalytic degradation [196]
method catalytic performance. good
stability
PAni/CuO, ­TiO2, ­SiO2 Sonochemical Good electrostatic and hydro- Anti-microbial properties [197]
phobic interactions
Atomic Au-PAni/Pt Cyclic process Fast reaction rate, electro- Amperometric gas sensor [198]
catalyst
Cu–Co–Nickel ferrite/GO/ Two-step method Excellent absorbing property Microwave absorption coat- [199]
PAni ing
PAni/CuO Electro-chemical deposition Improved specific capaci- Energy storage device appli- [200]
method tance, thermal stability cation
PAni/Zn-ferrite Pickering emulsion polym- Increase shear stress and Mechanical and industrial [201]
erization shear viscosity application
6226 J Mater Sci (2024) 59:6206–6244

Table 5  continued
Composite type Method of fabrication Properties Applications References

PAni/ZnS Mechanical method High conductivity and Dielectric application [202]

dielectric constant
TiO2/PAni In situ chemical oxidative Good photo catalyst, sedi- Environmental pollution [203]
polymerization mentation ability
PAni/TiO2 Surface polymerization Improved stability and Water treatment [204]
photocatalytic reduction
performance
PAni/SnO2 Chemical method High specific capacitance, Supercapacitor [205]
specific energy density, and
coulombic efficiency
PAni/SnO2 Hydrothermal route High retention, High specific Energy source system [206]
capacitance devices
PAni/V2O5 Micelle solution method Improved power Cathode catalyst in microbial [207]
fuel cell
PAni/ZnO Wet chemical method Better hydrophilicity, sensi- Humidity sensor [208]
tivity, linearity, and quick
response
PAni/ZnO Combustion method Spherical crystalline Biosensor, solar cell, waste [209]
nanoparticles, High thermal water treatment
stability, Enhanced antibac-
terial activity
CdS/PAni Electrochemical route Enhance local field effect Nonlinear optical and trans- [210]
port-related application
PAni/CdS Hydrothermal method Enhancement in photogen- Photocatalytic applications [211]
erated electron–hole pairs
separation, Improvement in
the photodegradation

Figure 14  SEM micrographs of a 10 PAni/TiO2, b 15 PAni/TiO2, and c 20 PAni/TiO2 composites (magnification×15,000). Source:
Adapted with permission from reference [177], copyright [2023], [The Royal Society of Chemistry].
J Mater Sci (2024) 59:6206–6244 6227

Table 6  Overall view of metal–organic frameworks–PAni composites

Composite type Method of fabrication Properties Application References

MOFs-derived porous car- In situ–chemical oxidative Excellent specific-capaci- Pseudocapacitive devices [214]
bon/PAni polymerization tance and retention
MOFs/PAni Electrochemical method Stable mechanical flexibility, Flexible solid-state micro- [215]
high power density supercapacitors, power
supply for small, wearable
devices
MOFs/PAni In situ–synthesis A high specific area, power Supercapacitor devices [216]
density, energy density
Co-MOF/PAni Wet chemical route Fast ion transport mechanism Energy storage devices [217]
Mo-MOF/PAni In situ chemical polymeriza- Fast electrolyte ion diffusion Supercapacitor [218]
tion coefficient, Low charge-
transfer resistance
rGO/MIL-101(Fe)/PAni In situ polymerization Improved capacitive energy Supercapacitor [219]
storage
PAni/Cu-MOF Two-step process With good electrochemi- Supercapacitor [220]
cal cycling stability, PAni
increases the active site for
the redox process
CNT/MOF/PAni Three-step process High mechanical properties Flexible electronics applica- [221]
and specific capacitance tions; sponges supercapaci-
tor
MOF/PAni Interfacial polymerization Highest capacitance value Highly flexible and light- [222]
weight energy storage
applications
Cu3(BTC)2/PAni Facile synthesis Highly sensitive detection E. coli bacteria sensing [223]
(MOF)MIL-100(Fe)/PAni Ball-milling Good reusability and stability Wastewater treatment [224]
in water
Cu-MOF/graphene/PAni In situ oxidation Highly porous, Improved Ammonia sensing [225]
semiconducting nature
Sn-MOF/PAni Ultra-sonication Improved mechanical proper- Flame retardant [226]
ties
MOF/PAni Photo thermal membrane High VOCs rejection by Water treatment containing [227]
molecular sieving VOCs
VOCs; Volatile organic compounds

unique functions, such as improved conductivity, bio- reviewed some of the latest non-specific PAni com-
compatibility, and sensing capabilities can be devel- posites and summarized them in Table 8.
oped. The properties of the resulting PAni-biomole-
cule composites depend on the specific combination
of biomolecules and the conditions under which they
are synthesized. Recent developed biomolecules/PAni
Current potential application
composites are listed in Table 7.
Polyaniline composites have shown a broad spec-
trum of applications in various fields, including
electronics, medical science, energy storage, sens-
Non‑specific composites with PAni
ing, surface protection, and more. The exclusive
PAni has also been combined with other materials combination of properties, such as electrical con-
to tailor its properties for specific applications. We ductivity, mechanical stability, thermal stability,
6228 J Mater Sci (2024) 59:6206–6244

Table 7  Overall view of PAni and biomolecules composites

Composite type Preparation method Properties Applications References

PCL/Ge/PAni Electrospinning Good biocompatibility, scaffold Cardiac tissue engineering [228]

conductivity
Ge/PAni Electrospinning Improved synergy effect Tissue engineering [229]
Ge-MA/PANI Interfacial in situ polymeriza- Improved electrical properties Bioelectrical interfaces [230]
tion
Ge/PAni Suspension method Moderate temperature produc- Electromagnetic compatibility [231]
tion and dielectric permittivity
BC/PAni Interfacial polymerization Higher electrical conductivity, Biocompatible actuator, cloth- [232]
improved tensile stress ing sensor
PAni/CTS Chemical synthesis Improved synergetic adsorption Anti-corrosion [233]
CTS/PANi/CuO Batch adsorption method Better adsorbent behavior Dye decontamination [234]
CTS-Ge/n-HA-PAni Lyophilization technique High porous and mechanical Tissue engineering [235]
strength
Substituted PAni/CTS In situ chemical oxidation Higher conductivity and ther- Glucose biosensor [236]
polymerization mal stability
A-G/PAni In situ polymerization Better adherence property, Electrochemical sensor and [237]
mechanical and conductivity biosensor
Starch/PAni Oxidative polymerization Enhanced biocompatibility Biomedical application [238]
PCL; polycaprolactone, Ge; gelatin, BC; bacterial cellulose, CTS; chitosan, nHA; nanohydroxyapatite, MA; Methacrylate, A-G; Aga-
rose-guar gum

Table 8  Overall view of non-specific PAni composites

Composite type Method of fabrication Properties Applications References

Nanosilicon/PAni Chemical polymerization Improved electrochemical lithium storage [239]

properties
PAni/silica gel Chemical oxidative polym- synergetic effect Anti-corrosion [240]
erization
Macro-porous silicon/PAni Anodizing and deposition Homogeneous electrical Sensor [241]
hetero-junctions method properties
n-Si/PAni/horseradish per- Electrodeposition method High detection capacity Biosensor technology [242]
oxidase
Bacterial cellulose/PAni/clay In situ polymerization Synergetic effect on biocom- Tissue engineering applica- [243]
patibility tion
Binder-free FTO/PAni Chemical oxidative synthesis Excellent capacitance reten- Energy storage devices [244]
tion
MMT/PAni Chemical oxidation synthesis Enhanced electrochemical Commercial separator for [245]
performance LIBs
FTO; fluorine-doped tin oxide, MMT; montmorillonite, LIBs; lithium-ion batteries

and biocompatibility, makes them a highly desirable Energy storage applications

material for various industrial applications. Here,
we have highlighted some potential applications of Polyaniline composites have shown potential for their
polyaniline composites that are expected to bring use in a variety of energy storage devices, including
significant benefits to society shortly. supercapacitors [216, 219–221], lithium-ion batteries
J Mater Sci (2024) 59:6206–6244 6229

[239, 246], sodium-ion batteries [247], and fuel cells small molecules in fuel cell technological applications
[193, 207]. [193].
The supercapacitor is a type of high-energy stor-
age device in an electric field. Liu et al. [216] prepared Sensing applications
MOF(ZIF-67)/PAni supercapacitor materials in a three-
electrode system that exhibited ultrahigh specific Polyaniline composites can improve the properties of
capacitance 1123.62 ­Cg−1 at a current density ~ 1A ­g−1. sensors for specific applications, for example, envi-
The rGo/MIL-101(Fe)/PAni composite showed energy ronmental monitoring, medical diagnosis, and indus-
storage properties due to higher capacitance and trial process control, by detecting analytes in difficult
superior cyclic performance without capacity reten- conditions with additional materials. Mohajeri et al.
tion after 300 cycles [219]. According to Sharma et al. demonstrated the sensing mechanism of the PAni/
the C/graphene/PAni composite demonstrates excep- ZnO/MWCNT electrode that showed potential value
tional potential for energy storage applications. In a for effective glucose detection with fast response
three-electrode system, the supercapacitor exhibits time (< 5 s), high stability (93.7%), and reproduc-
an outstanding areal capacitance of 7142 mF ­cm−2 at a ibility (3.2%) [138]. Yavuz et al. [236] found that the
current density of 80 mA ­cm−2 [168]. Neisi et al. [220] PAni/chitosan composite has high conductivity
reported PAni/Cu(II) MOFs composites which exhib- (1.68 × ­104 ­Scm−1), good thermal stability, and a homo-
ited enhanced capacitance 734 ­Fg−1 at 5 ­mVS−1. Gong geneous structure and suggested that the developed
et al. [221] prepared CNT/MOF/PAni composite, a new composite is the best for glucose biosensor applica-
type of flexible supercapacitor device that exhibited tions. Pippara et al. [195] reported the PAni/SnO2/Pd
enhanced capacitance of 746 ­Fg−1. Awata et al. [140] nanocomposites exhibited the highest sensitivity and
reported PAni/MWCNT composite at ~ 2 wt% which high-performance factor for hydrogen gas detection at
exhibited excellent specific capacitance of 2053 F/g room temperature. Chakraborty et al. [198] reported
and was employed as a high-performance superca- a PAni/Au2/Pt composite with tunable properties, fast
pacitor in electronic devices. A lithium-ion battery is response time, and potential for use in amperomet-
a rechargeable battery that stores energy using lithium ric gas sensors. Yang et al. [44] prepared conductive
ions. Si/PAni composite with excellent electrochemi- organic sulfonic acid co-doped bacterial cellulose/
cal performance, including 766.6 mAh ­g−1 reversible PAni nanocomposite films with an excellent response
capacity and ~ 72% retention after 50 cycles, is a top (~ 6.1) and fast recovery/response time (~ 10.2 s/8.6 s)
choice for lithium-ion batteries [246]. Nano-Si/PAni for ammonia sensing at room temperature. Bhardwaj
composite was also for lithium storage and showed a et al. [225] studied a copper MOF-graphene-polyani-
capacity of 1870 ­mAhg−1 up to 25 cycles reported by line composite with high porosity and superior con-
Cai et al. [239]. Yi et al. [248] reported graphite/SnO2/ duction in ammonia detection. The composite showed
PAni composite as an anode material for lithium bat- a linear detection range of 1–100 ppm with 0.6 ppm of
teries and demonstrated a prompt reversible capac- low-limit detection. Further, Jia et al. [249] reported
ity of 1021 mAh ­g−1 at a current density of 0.1 A ­g−1. Ni-MOF/PAni nanocomposite to construct a non-
Sun et al. [247] reported a PAni/PEDOT composite as enzymic sensor (electrochemical) by applying a layer
a cathode for sodium-ion batteries with an improved on an electrode (glassy carbon) and the result showed
reversible capacity of 81.9 mAh ­g−1 and high cycling a 5 × 1­ 0–7 to 3 × 1­ 0–3 mol/L range detection with high
stability at 100 mA ­g−1 current density. A fuel cell con- sensitivity of ~ 1144 μA/mM/cm2.
verts fuel’s chemical energy into electricity through an Kundu et al. [155] fabricated a flexible relative
electrochemical process. According to Ghoreishi et al. humidity sensor with a PAni-encased multiwall car-
[207] PAni/V2O5 nanocomposite showed enhanced bon nanotube (MWCNT) matrix. Sensors showed
power density as a microbial fuel cell cathode catalyst, excellent linearity, reproducibility, and low hyster-
producing ~ 79.26 mW/m2 compared to 65.31 mW/m2 esis error, achieving a maximum response (~ 42.6%),
for ­V2O5 and 42.4 mW/m2 for PAni. Yan et al. presented and were successfully applied for human respiration
a low Pt concentration catalyst synthesis approach. Pt monitoring. Shukla et al. developed an electrochemi-
nanoparticles/PAni composite showed improved sta- cal humidity sensor using zinc oxide encapsulated
bility and catalytic activity, offering promising poten- polyaniline. The composite showed good sensitiv-
tial as electro-analytical oxidation catalysts for organic ity, linearity, and faster response time compared to
6230 J Mater Sci (2024) 59:6206–6244

other humidity sensors. The sensor was responsive Alam et al. demonstrated that PAni/alkyd coatings
to humidity in the range of 5–80% relative humidity provide efficient and environment-friendly corrosion
(RH) with a response time of 32 s and recovery time protection against acid, alkaline, and saline environ-
of 45 s. [208]. Parangusan et al. fabricated humidity ments, without requiring a top barrier coat. These
sensors using poly(lactic acid)/PAni–ZnO composite coatings function as electronic barriers, hindering
micro-fibers. The sensors showed good response time anodic reactions and exhibiting high resistance to
(~ 85 s) and recovered quickly (~ 120 s) in the RH range corrosive ions [122]. Further, Kong et al. [233] found
of 20–90%. [250]. that increasing concentrations of PAni/chitosan com-
posite resulted in improved inhibition efficiency and
Surface‑protective applications decreased corrosion rates for the metal in an acidic
medium.
Polyaniline composites offer excellent surface pro-
tection against water, oxygen, and corrosion and
improve the corrosion resistance of metals. They Biomedical applications
also have good electrical conductivity and can pro-
vide anti-static properties, making them useful in Polyaniline composites have several potential bio-
many applications. Wong et al. found that adding medical applications due to their unique properties
15% PAni to poly(lactic acid) resulted in an excellent obtained after synthesis and their examination such
anti-static performance, with a surface resistivity of as drug delivery, tissue engineering, wound healing,
2.45 × 1010 ohm/sq. These findings suggest that PAni biosensors. We have summarized the latest work in
could be used in poly(lactic acid)/PAni systems to tissue engineering applications. Castell et al. stud-
achieve suitable surface resistivity and potential use ied polycaprolactone/gelatin/PAni nanofibers for
in anti-static packaging applications [251]. Mauro cardiac tissue regeneration. Results showed that the
et al. prepared a polyaniline/organoclay nanocom- inclusion of PAni in the scaffold was non-toxic and
posite with superior electromagnetic shielding and increased electrical conductivity, leading to cardio-
antistatic properties. The composite demonstrated myocyte proliferation in vitro. The researchers also
effective broadband absorption and satisfactory ther- observed cellular centers near PAni microparticles in
mal/mechanical stability, highlighting its suitability the scaffold, indicating its potential usage in cardiac
for microwave absorption and antistatic packaging tissue engineering [228]. Composite gelatin-PAni
applications [252]. Chang et al. reported polyaniline/ nanofibers enhanced myotube formation, matura-
graphene composites to protect steel from corrosion. tion, and contractibility compared to gelatin nanofib-
These coatings are effective due to their resistance ers alone, likely due to their combined topographi-
properties against ­O2 and ­H2O gases. Well-dispersed cal and electrically conductive cues were studied by
graphene, with a high aspect ratio, enhances the gas Ostrovidov et al. These have potential applications in
barrier and produces highly desirable anticorrosion improving skeletal muscle cell organization, cellular
features [253]. Silane coatings with praseodymium/ maturation and functionality, and promoting tissue
polyaniline composite as corrosion inhibitors were formation [229]. A highly porous composite scaffold
found by Najibzadeh et al. to display improved (CS-Gel/nHA-PAni) was studied by Azhar et al., and
performance, particularly at a concentration of the result showed that the scaffold had a mean pore
2000 ppm. The coated samples showed less dam- size of 200 μm, lower degradation rate, increased
age after 24 h and generated a protective layer at the biomineralization and mechanical strength, and sup-
scratch site, making them promising candidates for ported cell attachment and proliferation without tox-
corrosion protection applications [183]. George et al. icity. The scaffold has potential applications in hard
investigated the anti-corrosive properties of polyani- tissue regeneration [235]. Further, Salehi et al. [243]
line coatings containing silica gel, zinc chromate, and demonstrated an electrically conductive bio-com-
alkyd primer. The 5 wt% of PAni-Silica gel/primer posite aerogel based on BC/PAni/nanoclay, which
composite, which contains 2.5 wt% PAni, exhibited exhibited improved electrical conductivity, thermal
improved corrosion protection efficiency up to 7% stability, and biocompatibility due to the synergistic
with a penetration rate of 0.599 × ­10–4 mm/yr [240]. effect of the properties of clay and PAni.
J Mater Sci (2024) 59:6206–6244 6231

Thermoelectric application of PAni composites network of SWCNTs, providing additional pathways

for carrier transport. Additionally, the synergistic
Thermoelectric (TE) materials, converting waste heat impact of strong π–π interactions and the doping
directly into electricity, are gaining attention as a effect of SWCNTs further contributed to this improve-
promising solution for green power generation, with ment. Collectively, these factors promote the ordered
the increasing release of wasted heat into the environ- arrangement of PAni chains [131, 256]. Wang et al. fur-
ment. The urgent demand for efficient energy harvest- ther reported the synthesis of PAni/MWCNT compos-
ing technologies supports sustainable and renewable ites through a combination of in situ polymerization
energy development. Hence, PAni-based thermoelec- and electrostatic spinning. The results show a highly
tric (TE) materials are preferred for flexible energy ordered arrangement of PAni chains, coupled with a
harvesting, by providing solution processability, envi- substantial degree of molecular-level orientation, as
ronmental stability, and cost-effectiveness. Attaining illustrated in Fig. 15c, d. Also, Fig. 15e, f shows clearly
equilibrium between electrical conductivity and the that in situ polymerization improved PAni chain order
Seebeck coefficient poses a challenge, motivating con- due to π–π interactions, and the electrostatic spinning
tinuous efforts to enhance TE efficiency [254, 255]. The aligned the PAni/CNT structure along fibers, reducing
recent review highlights vital advances in PAni/CNTs defects and enhancing carrier properties. At 40 wt%
thermoelectric composites, emphasizing the need CNT, exhibited maximum TE performance: conductiv-
for uniform CNT dispersion exposed by Zhang et al. ity (σ) and Seebeck coefficient (S) reached 17.1 ­Scm−1
They explore key fabrication techniques: (i) physical and 10 µV ­K−1, respectively, at room temperature [256,
blending and (ii) in situ polymerization, enhancing 257].
integration. Post-fabrication solvent treatments led Additionally, Yin et al. demonstrated the dynamic
to fine-tuning doping and microstructure, optimizing 3-phase interfacial electro-polymerization of aniline,
electrical and thermal properties. Additional compo- combined with the physical mixing of single-walled
nent integration aims to improve the energy filtering carbon nanotubes (SWCNTs), to create polyaniline/
effect and boost the Seebeck coefficient (S), enhanc- SWCNT (PAni/SWCNT) thermoelectric (TE) compos-
ing overall thermoelectric performance. The review ites. Results revealed that the addition of dimethyl sul-
emphasizes microstructure modulations and signifies foxide (DMSO) significantly improved the TE perfor-
an essential role in shaping conduction mechanisms, mance of the composite films while varying SWCNT
offering essential insights for researchers in thermo- loadings conveniently fine-tuned their TE properties.
electric composite development. Further, Li et al. dem- Consequently, these composites achieved the highest
onstrated the impact of varied doping levels on PAni/ power factor (PF) of 236.4 ± 5.9 μW ­m−1 ­K−2 at room
SWCNTs film microstructure and thermoelectric (TE) temperature. This study highlights the efficacy of
properties by adjusting PAni/CSA molar ratios. The introducing DMSO into the electrolyte and employing
results revealed that lower levels shifted PAni chains electrochemical polymerization for fabricating high-
from quinone to benzene, reducing electron trans- performance PAni/SWCNT thermoelectric composites
port and conductivity (σ). Despite this, strong π–π [150].
interactions between PAni and SWCNTs improved
ordered PAni orientation, enhancing carrier trans- Electromagnetic interference shielding
port. The study emphasizes the sophisticated balance application of PAni composites
among doping levels, PAni chain structure, and the
reinforcing impact of SWCNTs, offering key insights The rapid progress in communication systems and
for optimizing PAni/SWCNTs films in thermoelectric electronic devices has elevated electromagnetic inter-
applications, as illustrated in Fig. 15a. However, as ference (EMI) to a critical concern, disrupting elec-
shown in Fig. 15b, at a PAni/CSA molar ratio of 3:1 tronic operations and posing potential health risks.
with 69 wt% SWCNTs loading, there was a notable Conventional metal-based EMI shielding materials
increase in the PF value to 321 ± 21 µW ­m−1 ­K−2. This face drawbacks such as high density, limited flex-
is a remarkable contrast to pure PAni and is explic- ibility, and susceptibility to corrosion [258–260]. In
itly higher than the power factor (PF) value at a PAni/ recent years, conducting polymers, especially poly-
CSA molar ratio of 2:1, which was 234 µW ­m−1 ­K−2. aniline, have been widely used for EMI shielding due
The enhancement can be attributed to the conductive to their corrosion resistance and lightweight nature.
6232 J Mater Sci (2024) 59:6206–6244

Figure 15  a Schematic representation of the pristine PAni and chains on the surface of CNTs noted by the enlarged part; e and
PAni/CNTs composites by modulating the doping level; b power f exposed the electrical conductivity and Seebeck coefficient of
factor versus PAni/CSA molar ratio variation for PAni/CNTs; DM-CNT/PAni and CNT/PAni nanofiber pellets as a function
and enlarge view of power factor of pristine PAni (inset) [133 of CNT contents in parallel and perpendicular to the fiber axis,
Li108797]. Schematic diagrams shown by: c DM-CNT/PAni and respectively [260 Wang]. Source: Adapted with permission from
d CNT/PAni nanofibers, respectively; the highly ordered PAni reference [256], copyright [2022], [MDPI].

PAni, among intrinsically conducting polymers, is using PAni mixed with conducting fillers like graphite,
the ideal choice for effective shielding [261, 262]. Saini carbon black, and silver across a frequency range of
et al. reported an in-depth investigation of PAni-based 10 MHz to 1 GHz. Results showed that PAni/graphite
hybrids, like blends or nanocomposites. Studies sug- and PAni/silver exhibit SE of 27 dB and 46 dB, respec-
gested an effective solution for EMI shielding due to tively, while unfilled PAni was only 17 dB because
their unique combination of electrical, thermal, and the SE rises with higher electrical conductivity, par-
mechanical properties [263]. Kumar et al. demon- ticularly with chemical doping and the addition of
strated that incorporating CNT into PAni nanostruc- conducting fillers [265]. To comprehend the general
tures creates a versatile PAni/CNT nanocomposite. process, electromagnetic waves exhibit three aspects:
These functional materials exhibit diverse applica- (i) reflection ­(SER), (ii) absorption ­(SEA), and (iii) mul-
tions. The incorporation of CNT in PAni brings about tiple reflections ­(SEM). The EMI performance results
changes in electronic and physical structures, leading from the interaction between electromagnetic waves
to the generation of novel properties [264]. Lee et al. and free electrons on material surfaces. High electri-
reported that the EMI shielding effectiveness (SE) cal conductivity in a material allows for the formation
J Mater Sci (2024) 59:6206–6244 6233

of electric dipoles. When incident electromagnetic ratio of Gr to PAni is 10:1) exhibited superior electrical
waves encounter free electrons on the surface, some conductivity (σ) at 2.1 ± 0.1 S ­cm−1, and is 1.45 times
waves are reflected. If electric dipoles intermingle with higher than Gr/PI film at the same loading. Moreover,
the electromagnetic fields, the remaining waves are Gr-PAni (10:1)/PI achieved total shielding effectiveness
absorbed [266, 267]. Further studies suggested that ­(SET) of 21.3 dB and accompanied by an extremely
thickness influences both ­SEM and ­SEA values; when high specific shielding effectiveness value (SSE) of
the ­SET value exceeds 10 dB, then ­SEM becomes neg- 4096.2 dB ­cm2 ­g−1. Experimental analysis of the EMI
ligible [268]. Hence, the total EMI shielding effective- phenomenon is detailed in Fig. 16a, b. The EMI shield-
ness ­(SET) can be simplified by the given equation ing effectiveness ­(SET) of Gr/PI and Gr-PAni(10:1)/PI
[269]: is measured using a vector network analyzer. The Gr-
PAni (10:1)/PI composite demonstrates superior elec-
SET (dB) = SER + SEA (1) tromagnetic shielding effectiveness ­(SET) in Fig. 16a,
The total EMI shielding effectiveness ­( SE T) is achieving 21.3 dB at 40%; a remarkable 125% improve-
defined as the logarithm of the ratio of the incident ment over Gr/PI (17.1 dB). This enhancement is mainly
wave (PI) to the transmitted wave (PT), calculated by due to the efficient attenuation of electromagnetic
the following equation [270]: radiation by the uniformly dispersed graphene (Gr)
sheets in the Gr-PAni (10:1)/PI film through reflection
and microwave scattering. The absorbed incident elec-
( )
PI
SET (dB) = 10lg (2)
PT tromagnetic microwaves result in the conversion of
energy into heat. The EMI shielding performance of
Cheng et al. demonstrated the in situ polymeriza- the thin film is attributed to the high electrical con-
tion of graphene-polyaniline/polyimide (Gr-PAni/ ductivity and formation of the conductive networks
PI) composite films using a non-covalent welding in the PI matrix.
approach. The 40% content of Gr-PAni (10:1) (mass

Figure 16  a Representation of the comparative analysis of PAni(10:1)/PI; the inset shows the magnification of the selected
the average of ­SET of Gr/PI and Gr-PAni(10:1)/PI and b EMI area and the scale bar is 0.5 µm. Source: Adapted with permis-
shielding mechanism of Gr-PAni(10:1)/PI ­(PI: incident wave, ­PR: sion from reference [271], copyright [2020], [The Royal Society
reflected wave, P
­ T: transmitted: wave; the sheet represents the of Chemistry].
Gr and curled shown the PAni), c shown SEM image of 40% Gr-
6234 J Mater Sci (2024) 59:6206–6244

As depicted in Fig. 16b, the EMI shielding mecha- generate macrostructural complexity throughout the
nism of the Gr-PAni (10:1)/PI film effectively attenu- last several years. To meet the demands of portable,
ates incident electromagnetic waves. The film’s con- electrical, transport, flexible, wearable electronic,
ductive networks, rich in charge carriers, enhance tunable, and hybrid vehicles, research is still being
EMI shielding through reflection at the film interface, done to fabricate a methodology for the synthesis of
while absorbed or multiple-reflected waves within the various scales and dimensions of materials, as well
graphene (Gr) layers minimize electromagnetic trans- as effective and cost-efficient methods, designs, and
mission. The outstanding EMI shielding performance techniques for large-scale processes [275]. There are
is attributed to the excellent conductive network drawbacks to both lithium-ion batteries and electro-
between Gr and PAni in the PI matrix, coupled with chemical capacitors [276]. An in situ polymerization
the more effective continuously cross-linked network process was employed to generate a nanocomposite
structure of Gr-PAni layers. Together, these features of graphene oxide, polypyrrole, and polyaniline. An
significantly improve the overall EMI performance of in situ polymerization process was employed to gener-
the Gr-PAni (10:1)/PI film [271]. Additionally, Fig. 16 ate a nanocomposite of graphene oxide, polypyrrole,
(c) illustrates the cross section of the SEM image of the the polypyrrole-coated graphene oxide composite had
40% Gr-PAni (10:1)/PI composite. The image reveals a greater capacitance (about 122.73%), storage capacity
a distinctive stacked-up morphology, indicating a (due to the coating’s synergistic impact on graphene
well-distributed presence of Gr sheets within the PI oxide), and binding energy (because to the lack of
matrix, resulting in the coarser fractured surfaces. The oxygen-containing functional groups) was higher
uniform distribution and interaction between Gr-PAni in the composite. In light of this, the PAni-graphene
(10:1) and PI matrix, facilitated by polyaniline, create composite proved less effective than polypyrrole-gra-
an integrated conductive structure with minimal gaps, phene oxide [277]. Supercapacitors, electrocatalysts,
ultimately enhancing the EMI performance of the com- methane gas storage, lithium-sulfur batteries, fuel
posite [271]. Further, in recent research, Li et al. devel- cells, and lithium-oxygen batteries have all employed
oped lightweight flexible films using amine-function- nanoporous carbon electrodes, media, and nanocom-
alized carbon nanotube (CNT)/polyaniline by in situ posites [278]. Controlling the nanoscale and high-level
polymerization. The results show the outstanding EMI structures and functionalities, as well as the develop-
shielding property and the highest reported specific ment of straightforward, scalable, environmentally
shielding effectiveness (SSE) of 7.5 × 1­ 04 dB ­cm2 ­g−1, friendly production procedures, continue to be prob-
attributed to the high conductivity (σ): 3009 S ­cm−1 lems. By electrochemically reduced graphene oxide
and low density of the amine-functionalized CNT/ and polyaniline (PAni) nanofilm, Chauhan et al. [279]
PAni composites [272]. discussed the production of reduced graphene oxide
and the electroactivity of polyaniline. This, however,
has drawbacks including cyclic stability and weaker
Challenges of polyaniline electrochemical characteristics. The volumetric energy
density of a composite hybrid with macropores in
PAni is often employed in the manufacturing process micropore size is not favorably influenced by the
of supercapacitors owing to its outstanding pseudo- three-dimensional structure [280]. As a result, it is very
capacitive characteristic. These chemically active sub- difficult to create porous, ultrathin, and homogenous
stances operate as a barrier to satiate the rapid elec- nanocomposite layers. Due to PAni’s poor solubility in
tron movement, which inhibits the rapid Faradic redox common solvents, it might be challenging to process
processes that are necessary for this substance’s rate it into other forms such as thin films, fibers, or coat-
capability. As a result, the process rate is restricted ings. PAni is susceptible to environmental elements
[273]. As a consequence, these are the main difficulties including oxygen and moisture, which may eventually
encountered by supercapacitors in manufacturing an reduce its stability and electrical conductivity. PAni
electrode material with good performance. In addi- is susceptible to environmental elements including
tion, supercapacitor assembly control is necessary. oxygen and moisture, which may eventually reduce
If these problems are resolved, energy density may its stability and electrical conductivity. PAni-based
increase without compromising high power capabili- devices may have long-term stability problems and
ties [274]. Numerous studies have been conducted to slow electrical property deterioration, which may be
J Mater Sci (2024) 59:6206–6244 6235

a serious negative for applications requiring lengthy to better compatibility between the matrix and nano-
operating lifetimes. It might be difficult to precisely filler. The shape and fine dispersion of the nanocom-
regulate PAni’s doping level to get the correct electri- posite seemed to be key factors in all of the enhanced
cal conductivity. For consistent performance across a attributes. The development of a homogeneous gra-
range of applications, maintaining a steady doping phene nanoplatelet network in the matrix has enhanced
level is essential. The use of potentially dangerous the stability of the structure, physical characteristics,
chemicals in certain types of PAni synthesis may lead and performance of graphene/polyaniline nanocom-
to issues with safety and the environment during both posites in addition to their microscopic qualities. The
manufacture and disposal. The search for better envi- inclusion of graphene nanoplatelets in the polyaniline
ronmentally friendly synthesis techniques is continu- matrix and improved properties were noted in this lit-
ing. PAni, particularly when it is in its highly conduc- erature study. In this respect, the choice of an appropri-
tive state, may be fragile. This prevents it from being ate PAni synthesis method, the design of the nanofiller,
used in applications that need strong mechanical qual- and the dispersion of the nanofiller are crucial elements
ities, including structural components. High-quality for improving the properties of these materials. The
PAni materials continue to be difficult to produce on inclusion of graphene nanoplatelets had a significant
a large scale. There is ongoing study on the subject of impact on the nanocomposite capacitance, sensing,
scaling up production methods while keeping the nec- mechanical, thermal, electrical, and shielding charac-
essary features. For its usage in medical applications, teristics. The interactions between the physical, cova-
PAni’s biocompatibility is a crucial factor. Ensuring lent polymer, and nanofiller may also be responsible for
that PAni-based materials do not elicit adverse biologi- the property enhancement process [281, 282]. Through
cal responses is a significant challenge. the study of the interfacial interactions between the gra-
phene nanofillers and polymer, a reinforcing behavior
has been created [283]. Microstructure characterizations
Future scope of polyaniline have been done to investigate the special structure and
characteristics taking into account the interfacial interac-
The graphene/polyaniline nanocomposites have thus tions. Consequently, new high-performance engineer-
been used in a variety of technological applications, ing applications for polyaniline/graphene nanoplate-
including electronics, energy storage, sensors, solar let nanocomposites are possible. Due to continuous
cells, and other devices. Graphene nanoplatelet/poly- research and development efforts aimed at overcoming
aniline composite supercapacitors have high capaci- its difficulties and using its special features, polyani-
tance, excellent performance (electrochemical), high line (PAni) has great potential for the future in several
charge densities, and cycle stability. Polyaniline and fields. Because of its electrical conductivity, PAni is a
graphene nanoplatelets were used in the fabrication of potential material for cutting-edge electronic applica-
the adaptable, simple, and selective gas sensors. Due tions. Researchers are investigating its usage in organic
to their excellent efficiency, graphene and polyaniline transistors, flexible and wearable electronics, and even
nanoplatelet-based nanocomposites were employed in as a possible substitute for conventional semiconductors
solar cells. The graphene/polyaniline nanoplatelet nano- in certain circumstances. PAni is a potential contender
composites have vital applications in radiation shielding for environmental remediation applications due to its
as well. Future studies may uncover uses for these nano- capacity to absorb and catalyze certain contaminants.
composites in the realms of electronics, coatings, and Materials based on ani offer promise for use in bat-
biomedicine. Future aerospace and automotive applica- teries and supercapacitors, two types of energy stor-
tions need the development of extreme temperature and age. Improved energy density, quicker charging, and
flame-resistant polyaniline/graphene nanoplatelet nano- longer cycle life might all result from future improve-
composites. Applications that may benefit from study- ments, which would increase energy storage systems.
ing thermal conductivity qualities are possible. Focus To improve the electrical, thermal, and mechanical
should be placed on simple large-scale processing of the characteristics of composite materials, PAni may be
graphene/polyaniline nanocomposite in the engineering used. PAni is useful for sensor applications because
industries. The enhanced graphene nanoplatelet may of its sensitivity to a variety of analytes and gases. The
be a more effective reinforcing agent in this instance to future of PAni may entail the creation of very sensitive
synthesize the high-performance nanocomposites due and selective sensors for use in industrial, medical, and
6236 J Mater Sci (2024) 59:6206–6244

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