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Carbon Nanomaterial-Incorporated Supramolecular Drug Delivery
Noshin Tasnim Tuli, Nuzhat Aqila Tushe, Adib Bin Rashid,
and Md Enamul Hoque
Abstract The integration of carbon nanomaterials in supramolecular architectures
has demonstrated potential as a viable approach for drug delivery, and this chapter
presents a concise overview of this prospect. Because of their one-of-a-kind physicochemical features, carbon nanostructures are being eyed as potential medication
delivery devices. To enhance pharmaceuticals’ solubility, stability, and bioavailability, supramolecular chemistry enables synthesizing complex structures with
distinctive characteristics and activities. The chapter examines the fundamental principles underlying supramolecular chemistry, an exploration of the characteristics
and implementation of carbon nanomaterials, and a comprehensive analysis of the
benefits and constraints associated with their use in drug administration. Examples of carbon nanomaterial-incorporated supramolecular drug delivery systems are
presented, and the future directions and potential applications of this approach are
discussed. In conclusion, this chapter emphasizes the promise of carbon nanomaterial
as an efficient and effective supramolecular drug delivery technology with various
therapeutic applications.
Supramolecular chemistry·Drug delivery
Keywords Carbon nanomaterials
Cyclodextrins · Cucurbiturils
N. T. Tuli · A. B. Rashid
Department of Industrial and Production Engineering, Military Institute of Science and
Technology (MIST), Dhaka 1216, Bangladesh
N. A. Tushe
Department of Mechanical Engineering, Military Institute of Science and Technology (MIST),
Dhaka 1216, Bangladesh
M. E. Hoque (
Department of Biomedical Engineering, Military Institute of Science & Technology (MIST),
Dhaka 1216, Bangladesh
e-mail: enamul1973@gmail.com
B
)
·
·
129
130 N. T. Tuli et al.
Abbreviations
1G First Generation
2G Second Generation
3G Third Generation
CNT Carbon Nanotube
DDS Drug Delivery System
CB Cucurbituril
MWNT Multi-Walled Nanotube
EPR Enhanced Permeability and Retention
CVD Chemical Vapor Deposition
CQD Carbon Quantum Dot
CNH Carbon Nanohorn
CNOs Carbon Nano-onions
HA Hyaluronic Acid
SEM Scanning Electron Microscope
HPG Hyperbranched Polyglycerol
SOF Supramolecular Organic Framework
LMWH Low-Molecular-Weight Hydrogelators
DNA Deoxyribonucleic Acid
RNA Ribonucleic Acid
CNM Carbon Nanomaterials
SWNT Single-Walled Nanotube
NP Nanoparticle
CNF Carbon Nanofiber
CB Cucurbituril
PDT Photodynamic Therapy
CNHs Carbon-Nitrogen Hybrid Materials
HPHT High Pressure High Temperature
PA Peptide Amphiphile
ZOL-GO Graphene Oxide-Zoledronic Acid
1 Introduction
Drug delivery systems refer to the mechanisms by which therapeutic substances,
including pharmaceuticals, are conveyedto designated sites inside the human body.In
the past, drugs were typically administered by mouth (in the form of pills or capsules)
or by injection (intravenously, intramuscularly, or subcutaneously). However, technological and methodological developments in the pharmaceutical and biomedical sciences have created more refined drug delivery systems, allowing for more
precise drug release regulation, localization, and targeting. The development of firstgeneration (1G) drug-delivery approaches occurred throughout the period spanning
Carbon Nanomaterial-Incorporated Supramolecular Drug Delivery 131
from the 1950s to the 1970s. These systems played a significant role in establishing
the fundamental understanding of drug release mechanisms, particularly on transdermal and oral dosage forms. Transdermal preparations exhibiting a release duration
of 1 week and oral formulations with a release duration of 12 h (administered twice
daily) were observed [1].
From 1980 to 2010, second-generation (2G) drug delivery formulations failed
to introduce clinical systems like 1G formulations. This is because 2G technologies handle more complex formulations. Insulin pulmonary delivery methods were
invented in 2G. Nanoparticle-targeted tumor medication delivery has dominated the
2G period (2000–2010) [2]. The modest accomplishments of 2G technologies need
rigorous analysis to prepare third-generation (3G) technology for clinical applications [3]. Dendrimers and analogs, hydrogels, molecular and polymeric micelles
and liposomes, discrete nanoparticles, carbon nanotubes (CNTs) and dots, and polymeric prodrugs constitute the most researched drug delivery systems (DDSs) [4].
Dendrons and dendrimers may self-assemble into systematically ordered structures, glue supramolecular structures, mediate chirality, and help viruses build crystalline compounds [5]. In recent years, there has been a growing prevalenceof stimuliresponsive drug delivery systems (DDSs) that offer the potential for tumor-specific
radiation therapy. These DDSs havegained popularity due to their capacity to enhance
treatment efficacy while minimizing adverse reactions in the body [6]. Others have
used hydrophobically induced encapsulation of automatic dimers by the cucurbituril (CB) ring to create homogenous periodic supramolecular organic frameworks
(SOFs) in water [7].
Significant advancements in supramolecular chemistry have been observed during
the past two decades, resulting in a diverse range of practical applications [8].
The application of supramolecular chemistry in comprehending the nanoscale has
yielded significant advantages across various academic disciplines, with medicine
and cutting-edge research being particularly prominent beneficiaries. There has been
significant progress in materials research in the past few decades, particularly in
biomedical materials. This progress has been driven by the development of artificial molecular machinery and smart supramolecular devices based on macrocyclic
and host–guest chemistry. These advancements have resulted in the emergence
of materials with exceptional mechanical and reversible properties and desirable
responsiveness to various stimuli [9]. Synthesized expertise suggests supramolecular
remedies for progression and potential. Biomedical applications require advanced
drug delivery systems [10]. Supramolecular nanovalves control drug molecule
transit by reversibly joining several components, creating a new frontier in limited
materials for precision dosage [11]. Biomaterials that rely primarily on noncovalent cross-molecular interactions between tiny molecules are called supramolecular
biofunctional materials [12].
In addition, stimuli-responsive supramolecular vesicles can effectively encapsulate pharmaceuticals, preserve them from deterioration, minimize their impact
on cells, and unleash them with precise external stimuli [13]. Various techniques have been employed to fabricate singular stimulus-responsive supramolecular vesicles that exhibit responsiveness to pH, enzymatic stimuli, electrochemical,
132 N. T. Tuli et al.
thermal, chemical, or photochemical. However, the construction of multi-stimuliresponsive supramolecular vesicles has been minimal in comparison [14]. Hence,
the generation of supramolecular vesicles that are responsive to many stimuli by
supramolecular amphibians via noncovalent interactions holds great importance
and relevance in biomedicine and biotechnology, particularly in drug administration [15]. Supramolecular hydrogels have been extensively investigated to address
social issues. Low bioaccumulation, chemical functionalization, structural plasticity, and low cost make low-molecular-weight hydrogelators (LMWH) superior to
polymer-based hydrogels [16]. Due to their easy metabolism, non-immunogenicity,
biocompatibility, and targeted therapy, amino acid-based LMWHs are ideal for
nanomedicine [17]. Furthermore, there has been significant interest and progress
in the field of supramolecular hydrogels that are based on host–guest interactions,
particularly in their application within the realm of biology. These hydrogels have
shown promise in several areas, such as bio-/chemo-sensing, controlled drug delivery,
pollution mitigation, and cell culture [18].
Supramolecular drug delivery systems utilizing carbon nanomaterials can be
designed to enable the controlled and prolonged release of therapeutic substances
[19]. The capability of these systems to respond to external stimuli, such as changes in
pH, temperature, or biomarkers, enables medication administration in a targeted and
on-demand manner. The implementation of this approach to controlled drug delivery
enhances the effectivenessof therapy while concurrently mitigating the occurrence of
adverse effects [20]. Carbon nanostructures possess a significantly elevated ratio of
surface area to volume, rendering them highly suitable for transporting pharmaceutical agents. Its versatility in drug delivery applications stems from its easy functionalization with various chemical groups [21]. Carbon nanotubes (CNTs) have recently
captured interest for their excellent electrical characteristics [22]. They are ideal
nanomaterials for biosensors, especially electrochemical sensors that can measure
nanoscale quantities. Based on the observation, many biosensors and chemosensors
for pesticide, amino acid, and microbe detection have been proposed [23].
Moreover, CNT supramolecular assemblages (aggregates) are also gaining attention [24]. The substance has a significant surface area and offers numerous drugtargeting locations, enhancing its efficacy as a delivery vector [25]. This chapter
mainly focuses on types and properties, pros and cons, functionalization, and characterization of carbon nanomaterials in drug delivery. Discussions have been done about
supramolecular chemistry in drug delivery systems and incorporating supramolecular chemistry with carbon nanomaterials. Lastly, conclude by deliberating what the
future and obstacles hold for carbon nanomaterial incorporated into supramolecular
drug delivery system.
Carbon Nanomaterial-Incorporated Supramolecular Drug Delivery 133
2 Different Carbon Nanomaterials in Drug Delivery
Nanotechnology has created many nano-enabled devices and nanosystems used in
various medical disciplines. Strategic nanotechnology use in upcoming drug delivery
technologies could expand drug markets. This method would be employed for drugs
chosen for substantial research based on data on safety and effectiveness but cannot
undergo clinical testing due to bio-pharmacological characteristics. Nano-structural
implications involve integrating viruses, cellular lipid bilayers, medicines, DNA/
RNA, antibodies (important in immunology), cellular receptor sites, and proteins into
nano-constructs and assemblages. Chemical molecules such as polymers, liposomes,
and substantial metal-containing nanoparticles are being studied as drug-delivery
automobiles, as well as biological entities such as albumin, phospholipids, and
gelatin have also been explored [26]. Nanomaterials made from carbon have attracted
considerable interest in the scientific community, mostly because of their ability to
undergo surface functionalization. This characteristic allows for integrating nucleic
acids, peptides, and proteins onto these nanomaterials. Among the many nanosystems studied for their potential in fields including the delivery of drugs, biosensing,
and medical imaging are carbon nanomaterials (CNMs). Carbon nanostructures have
unique properties, such as high surface area and remarkable mechanical and electrical
attributes, making them suitable for medical and diagnostics applications [27].
2.1 Carbon Nanotubes (CNTs)
Carbon atoms are arranged in hexagonal lattices to form cylinder-shaped carbon
nanotubes (CNTs). The nanoscale tubes can be conceptualized as cylindrical structures formed by the rolling up of individual graphene layers, resulting in a hollow
configuration. Over the last decade, there have been notable advancements in
nanotechnology that have contributed significantly to the detection and treatment
of several diseases, including cancer. Extensive research has been conducted on the
potential utilization of sp
and graphene, as agents for inhibiting cancer progression. While carbon atoms stack
in a single layer on the inside of single-walled nanotubes (SWNTs), they stack in
several layers on the inside of multi-walled nanotubes (MWNTs). In addition to their
use as a drug-delivery vehicle, CNTs and their derivatives have prospective services
in biomedicine, nanoelectronics, energy storage, and nanocomposite materials [28].
Nevertheless, the fundamental limitation of nanomaterials made from carbon
seems to be their potential toxicity. Empirical investigations have provided evidence
indicating that carbon nanotubes (CNTs) can impede cell proliferation and induce
apoptosis. Despite carbon nanotubes (CNTs) being less dangerous than carbon fibers
and NPs, it is known that the presence of carboxyl, carbonyl, and hydroxyl functional groups on their exterior greatly increases their toxicity [29]. Due to the welldocumented toxicity of carbon nanotubes (CNTs), as reported in previous studies
2
carbon nanomaterials, including carbon nanotubes (CNTs)
134 N. T. Tuli et al.
[30–32], continuing research is being conducted to explore their potential application in medication delivery systems. The carriers used for drug delivery include many
compelling properties that make them highly attractive [33].
To begin with, nanocarriers, including nanoparticles (NP), liposomes, and carbon
nanotubes (CNTs), exhibit the phenomenon known as the increased permeability and
retention (EPR) effect. This effect leads to a higher accumulation of nanocarriers in
tumor tissues than in healthy tissues due to the inadequate development of blood and
lymphatic arteries in tumors [34]. CNTs can selectively transport chemotherapeutic
medicines to tumor sites due to their increased permeability and retention (EPR)
impact [35]. Furthermore, the morphology of CNTs in the form of needles enables the
penetration of cell membranes and the accumulation of drugs within cells through the
mechanism of “nanoneedles.“ This process is not reliant on further functionalization
of CNTs or specific cell types, as evidenced by previous studies [36].
In addition to their direct transfer through cellular membranes, it has been demonstrated that CNTs can also penetrate cells through endocytic pathways that rely on
energy, as reported in reference [37]. According to recent research, functionalized
carbon nanotubes (CNTs) can penetrate cells via endocytosis and exocytosis mechanisms, resulting in the aggregation and accumulation of CNTs within the lysosomes
and endosomes of the targeted cells [38]. At lower concentrations, fully functionalized carbon nanotubes (CNTs) exhibit no cytotoxicity. The primary mechanism
by which nanoparticles are internalized into cells is endocytosis, a process that
is controlled by the size and surface properties of the nanoparticles. Furthermore,
carbon nanotubes (CNTs) exhibit considerable potential as a viable platform for
drug conjugation owing to their exceptional drug-loading capability, attributed to
their elevated aspect ratios and expansive surface areas [39]. The loading of phar-
macological molecules onto t he outer layer or within the interior core of carbon
nanotubes (CNTs) is possible via covalent and non-covalent interactions [40].
2.2 Carbon Nanofibers (CNFs)
One-dimensional nanostructures called carbon nanofibers (CNFs) are carbon atoms
organized in a fibrous pattern. The structures in question share a carbon-based
composition with CNTs but exhibit distinct morphological characteristics. CNTs
possess a tubular structure, whereas CNFs exhibit a solid morphology and a fibrous
configuration. Various techniques can generate CNFs, such as chemical vapor deposition (CVD), template synthesis, or electrospinning. Carbon nanofibers (CNFs)
exhibit distinctive configurations that confer unique characteristics. Specifically, they
possess a high electrical conductivity and a significant proportion of active sites,
indicating the graphite platelets’ exposed edge areas. These active sites are available for physical and chemical interactions with various species. One of the most
noteworthy discoveries is the ability of organized crystalline solids to demonstrate
elevated surface areas ranging from 300 to 700 m
area is chemically reactive. Carbon nanofibers (CNFs) exhibit a range of physical
2
g−1, wherein the entire surface