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196 Carbon-Based Nanocarriers for Drug Delivery
of UV radiation. However, it lacks active areas on the cages for direct catalytic uses
and is inaccessible in polar solvents such as water.
This chapter discussed the various structural attributes and physicochemical characteristics of fullerene and its signicance and prospects as a nanocarrier for drug
delivery. It illustrated the methods with advancements for synthesizing fullerene and
highlighted functionalization strategies to enhance the surface characteristics. The
chapter also discussed recent advancements in fullerene for nucleic acid delivery,
chemotherapeutics, and neurodegenerative diseases.
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Carbon-Based
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8
Nanocomposites
for Drug Delivery
8.1 INTRODUCTION TO CARBON NANOHYBRIDS
Researchers have grown interested in developing innovative drug delivery methods
for various medical substances in recent years. In fact, many studies examine the
design, synthesis, and characterization of new materials to be employed as delivery systems to improve the efcacy of a particular medication [1]. To maximize the
therapeutic agent’s efcacy and safety, the optimal drug delivery system (DDS) must
carry the therapeutic agent in the appropriate quantity, at the correct rate, and to
the right place in the body. This strategy can prolong the pharmacological impact,
reduce unpleasant effects, and reduce administration frequency, enhancing patient
compliance [2].
The demand for carriers for novel biological therapeutic agents, such as nucleic
acids and proteins, and the pharmaceutical industry’s interest in generating novel
formulations due to looming patent expirations necessitate the adoption of innovative
drug delivery systems. Biologics, polymers, silicon-based, carbon-based, metals, or
mixes thereof are employed in alternative drug delivery techniques, and these substances can be organized in microscale or, more recently, nanoscale forms [3].
Nanomedicine is described as “the monitoring, repair, production, and control
of human biological systems at the molecular level” using nanodevices and nanostructures [4]. It entails applying nanotechnology for disease detection, prevention,
and treatment, and it acts as a valuable tool for understanding particular molecular
mechanisms causing disease [2].
Nanomaterials have signicant potential for the early detection and diagnosis of
infectious and malignant diseases, as well as for the creation of drugs, the administration of medications, and the delivery of genes and proteins. Due to the extraordinary selectivity of their interactions with subcellular structures in the human body,
these cutting-edge materials have the potential to be utilized in clinical settings as
drug-targeting systems to reduce side effects [5]. Nanocarriers can carry the active
chemical directly into cells by eliminating biological barriers and separating the
problematic target tissue from the healthy tissue [6].
Using nanocomposites may be advantageous in various industries, including technology, medicine, biotechnology, pharmacy, polymeric materials, ceramics, textiles,
paint, automobiles, food, and a great deal more. Nanocomposites fall into natural or
articial categories, depending on where the component phases originated. The discontinuous phase often comprises a smaller portion of the total than the continuous
DOI: 10.1201/9781003358114-8 201
202 Carbon-Based Nanocarriers for Drug Delivery
phase. The continuous phase, which might be made of polymeric, metallic, ceramic,
or a combination of these and other materials, is often chemically different from the
nanoscale discontinuous phase. Here, we will look closely at natural nanocomposites. “In-situ,” “mixed in solution,” and “melt compounding” stand out as particularly
benecial among the several known production techniques. For both organic and
inorganic discontinuous phases, dispersion is essential. Most of the time, supercially altering the discontinuous phase with a chemical similar to the continuous
phases will result in better integration. Nanocomposites are materials that can have
a variety of benecial properties depending on their composition and compatibility
with different organic and inorganic llers and reinforcements. For instance, natural
nanocomposites are a class of materials with a wide variety of potential applications
in industries, including farming, food science, medicine, and pharmacology. Natural nanocomposites are desirable from an environmental perspective since they are
derived from natural sources, may be regenerated, and disintegrate more quickly
[7]. Nonetheless, they often have poor mechanical, chemical, and physical characteristics. From the original design through the use of renewable raw materials, clean
energy, zero waste manufacturing, shorter processing times, etc., the notion of green
chemistry, preventive is better than clean, is used throughout the whole process of
developing natural nanocomposites [8].
Obtaining copper chitosan nanocomposites for use in tissue engineering has been
the subject of numerous studies; these materials are produced using a solution-based
mixing method assisted by ultrasonic energy and exhibit promising antimicrobial
activity against common pathogens like Staphylococcus aureus [9]. In addition to
chitosan, there are currently natural nanocomposites made from cellulose, nanocellulose, starch, polylactic acid (PLA), various polysaccharides derived from glucose,
and cellulose with the addition of various nanoparticles, including single, double, or
multiple walled carbon nanotubes, graphene, carbon nanobers, and fullerenes.
8.2 TYPES OF CARBON NANOHYBRIDS
Natural nanocomposites are multi-phase compounds, i.e., having two or more phases,
generated from natural sources such as plants, vegetables, trees, seeds, microorganisms, and animals [10]. At least one phase has a nanometric dimension (usually 100
nm). Research interest in this nanomaterial is growing due to its durability, affordability, low weight, high specic resistance, strong mechanical properties, and biodegradability [11]. Natural nanocomposites can be classed by source—plant, mineral,
or animal. Animal nanocomposites are usually generated from animal waste or
skins, mineral nanocomposites can be made naturally or chemically, and vegetable
nanocomposites are made from leaves, stems, and roots, with cellulose as the main
component [11,12].
A natural nanocomposite requires at least one natural component. Compared to
synthetics and composite materials with typical padding, nanocomposites consisting
of chitosan, chitin, starch, glucose, cotton, different polysaccharide derivatives, cellulose and derivatives, natural bers, and natural rubber have remarkable mechanical
and thermal qualities [13]. Natural nanocomposites are those materials made up of
two or more phases, at least one of which has a nanometric scale (generally <100 nm)
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and which are also obtained from natural sources, such as plants, vegetables, trees,
seeds, bacteria, etc. animals, among others [12]. At present, this type of nanomaterial
has increased the interest of its research since it has multiple favorable properties
such as durability, low cost, low weight, high specic resistance, good mechanical
properties, and biodegradability.
There are different classications of natural nanocomposites; one regarding their
source, which can be animal, mineral, or vegetable. The nanocomposites extracted
from animal sources are generally taken from the skins or waste produced by animals, those obtained from minerals can be obtained in a natural or modied way,
and nally, the vegetables that are taken from their leaves, stems, and roots, cellulose
being the main one [10]. According to Franco-Aguirre etal. in 2023 [7], nanocomposites can also be classied by their size and dimension, where we will nd four
different nanometric scales that are described in Table8.1 [7].
In recent years, natural polymer nanocomposites have been widely studied
because the addition of nanometric llers signicantly increases the physicochemical properties, which is attractive for their application in different areas [14]. The
union of two or more materials on a nanometric scale can occur in multiple combinations using various materials. However, to obtain a natural nanocomposite, the
addition of at least one component of natural origin will be necessary. An example
is nanocomposites based on chitosan, chitin, starch, glucose, cotton, different polysaccharide derivatives, cellulose and derivatives, natural bers, and natural rubber,
among others of great interest, thanks to their extraordinary mechanical and thermal
properties concerning polymers—synthetics and composite materials with conventional padding [13].
8.2.1 graphene-BaseD nanohyBriDs
Graphene (GN) is the term given to the atomically thin layer of graphite composed
of carbon atoms organized in a honeycomb conguration in two dimensions. When
nearby carbon atoms’ sp2 orbitals meet, three bonds are formed in the GN layer [15].
The remaining pz orbitals then form the conduction and valance bands related to the
full π and empty π* orbitals. The unique honeycomb structure of carbon atoms and
their sp2-hybridized bonds give GN not only a high specic surface area but also
TABLE 8.1
Classication of Nanocomposites according to Their Size and Dimension.
Reprinted with permission from Franco-Aguirre et al. (2023) [7]
Classication Dimension Examples
0D Nanometer-scale from 1 to 50 nm Fullerenes, nano clays, nanodiamonds, etc.
1D Nanometer-scale from 1 to 100 nm Nanotubes and nanobers
2D It is found on the nanometric scale and with
another dimension on the micron scale
3D All dimensions are microscale Nanostructure
Graphene, nanolms, and nanocoatings
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exceptional mechanical (stiffness 1 TPa), thermal (conductivity 5000 W m1 K1),
optical (transparency 97.7% transmittance), and electronic (charge-carrier mobility
250,000cm2 V-1 s-1 at room temperature) properties [16–19]. Since GN lacks a band
gap and is inert to chemical processes, it must be functionalized to enhance its dispersion and overcome restrictions in technical applications such as semiconductors
and sensors [20,21].
Mechanical exfoliation, epitaxial growth, and thermal reduction of graphene
oxide (GO) are the most common ways of producing graphene nanoribbons (GN);
nevertheless, the latter two are preferred because they provide a large-scale synthesis of GN [19,20,22]. GO is produced by grafting epoxide, carbonyl, carboxyl,
and hydroxyl groups onto the GN structure. GO’s 2D layer structure is made of sp2hybridized carbon atoms organized in a hexagonal lattice and amorphous domains
of sp3 C-O bonds due to the inclusion of these oxygenated functional groups. The
polar oxygen functional groups make GO hydrophilic, allowing for its dispersion
in a range of solvents, and the included functional groups serve as anchor sites for
further chemical functionalization of GO to tune its physicochemical properties [15].
Because of the simplicity with which GO may be disseminated and functionalized,
a variety of graphene-based structures with tunable electrical, optical, mechanical,
and transport characteristics can be fabricated. This permits its manufacture on a
wide scale. Some applications, however, necessitate the reconstruction of certain GN
features. The oxygenated functional groups of graphene oxide (GO) are removed
chemically or thermally to produce reduced graphene oxide (RGO). Polymer-based
nanocomposites supplemented with RGO by in-situ GO reduction via polymerization or melt process in a polymeric matrix are one of the potential strategies [23–25].
8.2.2 carBon nanoTUBe-BaseD nanohyBriDs
The hexagonal arrangement of sp2-hybridized carbon atoms that make up carbon
nanotubes (CNTs) has a C-C spacing of around 1.4 [26]. These may be seen as
nanometer-sized cylindrical structures made of rolled-up graphite planes [27].
Ahemisphere with a fullerene structure is often present on at least one end of the
cylindrical nanotube [15]. Two different forms of CNTs depend on the production
process: single-wall CNT (SWCNT) and multiwall CNT [18]. (MWCNT). Whereas
MWCNTs comprise two or more concentric cylindrical shells of graphene sheets
coaxially organized around a central hollow core with van der Waals forces operating between neighboring layers, SWCNTs comprise a single rolled layer of graphene.
MWCNT has an average interlayer spacing of 0.34 nm for the graphene layers, with
each layer creating a separate tube with an outside diameter of 2.5 to 100 nm, compared to a range of 0.6 to 2.4 nm for SWCNT [18].
CNTs have been used for numerous applications in the eld of biotechnology,
such as platforms for ultrasensitive antibody recognition, nucleic acid sequencers,
bioseparators, biocatalysts, and ion channel blockers for accelerating biochemical
reactions and biological processes [19,21–24,28,29]. They have been used in nanomedicine as carriers of contrast agent magnetic resonance imaging, scaffolds for
neuronal and ligamentous tissue growth for regenerative interventions of the central
nervous system and orthopedic sites, substrates for detecting antibodies associated
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with human autoimmune diseases with high specicity, and substrates for detecting
antibodies associated with autoimmune diseases [15]. They have been demonstrated
to be efcient substrates for gene sequencing and as gene and medication delivery
vectors to challenge traditional viral and particle delivery methods when coated with
nucleic acids (DNA or RNA), vaccines, and proteins [30,31].
It should be noted that the exceptional reactivity of CNTs—due to their enormous
surface area and achieved by their innitesimal size—serves as both their best and
worst qualities, particularly when they enter the bodies of humans and other living things, even though the precise mechanisms governing their toxicity are still
unknown [32,33].
The World Health Organization (WHO) denes CNT as having a ber-like structure, and the physical resemblance to asbestos bers is the primary cause for worry in
terms of public health [34]. It has been established that when long MWNT, a nanotube
that resembles asbestos, is exposed to the mesothelial lining of a mouse body cavity
(used as a model for the mesothelial lining of the chest cavity), length-dependent
pathogenic processes are seen. Inammation and the development of granulomas are
examples of these processes [35]. Moreover, it has been observed that CNTs have
carcinogenic qualities and frequently result in mesothelioma in intact male rats [36].
As the CNT’s water insolubility or near insolubility is the primary source of toxicological concerns, several investigations have been carried out to create highly
functional CNT derivatives with less toxic effects [37]. The hydrophobic interactions
between the sp2 carbon tube shells of a CNT always result in aggregation or bundles
that are securely linked in their purest form [38].
Covalent and non-covalent functionalization must be distinguished when discussing the functionalization of a CNT. Covalent functionalization is based on the covalent attachment of functional components to the carbon scaffold of the nanotube.
It may be carried out at the tubes’ termini or sidewalls. Direct covalent sidewall
functionalization is connected to a shift from sp2 to sp3 hybridization and a concomitant loss of conjugation. Using previously existing defect sites to undergo chemical
reactions is known as defect functionalization. Defect sites can include the irregular
pentagon and heptagon shapes seen in the hexagonal graphene structure, as well as
open ends and sidewall holes that are terminated, for instance, by carboxylic groups.
Moreover, oxygenated sites created during oxidative purication must be seen as
aws [39,40].
Using different adsorption forces, such as van der Waals’s and π-π stacking interactions, a non-covalent functionalization is primarily based on supramolecular complexation. These functionalizations are all derivatizations of exohedral structures.
Endohedral functionalization of CNTs, or the lling of the tubes with atoms or tiny
molecules, is a specic instance [41]. Covalent or non-covalent bonding (wrapping) of
polymer molecules on the surface of the CNT is one surface modication method [42].
8.2.3 graphene oXiDe-BaseD nanohyBriDs
The graphene analogs that are both oxidative and hydrophilic functional groups such
as hydroxyl, carboxyl, and epoxy are highly concentrated in graphene oxide (GO)
and reduced graphene oxide (rGO), enhancing their stability, water dispersibility,
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