Biomedical Applications of Nanofiber-Nanoparticle Hybrids

Version	Summary	Created by	Modification	Content Size	Created at	Operation
1		Deng-Guang Yu	+ 2803 word(s)	2803	2022-01-27 03:56:58	\|
2	Done	Jason Zhu	Meta information modification	2803	2022-01-28 02:34:35	\|

When nanoparticles and nanofibers are combined, the composite material can perform more functions, such as photothermal, magnetic response, biosensing, antibacterial, drug delivery and biosensing.

Drug Delivery Antibacterial Tissue Engineering polymer composites nanoparticle

1. Drug Delivery

Drug delivery systems (DDSs) release drugs through specific control devices and certain doses to achieve the purpose of enhancing the immunity of the body or treating diseases ^[1]^[2]. It is difficult to advance medicine without the use of medications. While drug activity is crucial, the method of administration is more so. Pharmacokinetics (PK), duration of action, metabolism and toxicity are the key elements that influence drug delivery ^[3]. NNHs inherit the excellent biocompatibility and high specific surface area of electrospun fibers but also the function of NPs, which can load different drugs into NNHs for a precise controlled release ^[4]^[5]. The advantages of NPs are their high specific surface area, superior bioavailability and functionalization. Similarly, in practical drug delivery applications, nanofibers can be electrospun with biocompatible polymers, resulting in minimal harmful effects on humans ^[6]. Tuğcu-Demiröz and co-workers employ ionic gelation to load benzydamine onto chitosan NPs. Composite NPs were embedded in NFs and hydrogels, respectively. On the one hand, NFs have a large specific surface area. The medicine, on the other hand, diffuses across a short distance in the fiber. Benzydamine released 53.03% in the composite fiber system after 24 h. Because of the strong polymer matrix, the hydrogel system only released 15.09% of benzydamine. This is insufficient for the required drug concentration for vaginal infections ^[7]. In the process of release, benzydamine enters the nanofiber after the initial release of chitosan nanoparticles, and the secondary release can achieve a slow release and prolong the action time.

For the mechanism of release of NNHs-loaded drugs: (1) one drug in two phases: the drug is loaded on nanoparticles that need to cross the barrier between nanoparticles and nanofibers during the release to achieve the effect of slow release. (2) Dual drug biphasic: two drugs are loaded in separate materials with different properties to achieve the required effect by different types of release mechanisms.

1.1. One-Drug Biphasic

One-drug biphasic is an advanced therapeutic approach to chronic diseases by precisely designing the carrier to act rapidly in the first burst and then to work longer with chronic illness. For example, He and co-workers used ethylcellulose (EC) and polyethylene glycol (PEG) small-molecule solutions in the core sheath to simultaneously load ibuprofen (IBU) through an improved coaxial ESP. The prepared engineered spindles-on-a-string (SOS) nanofiber hybrid possesses typical controlled drug release properties. When the SOS structural mixture contacts water, the hydrophilic small molecule PEG rapidly dissolves to release IBU, while the hydrophobic EC drug on the other side is continuously released in a slow-release form ^[8]. This precise controlled release means providing the patient with the desired drug environment in the first instance, followed by a prolonged slow release to provide effective blood levels ^[9]^[10]^[11]^[12].

Facing the complex living system of organisms, hydrophobic drugs confront barriers in the delivery pathway. The use of NPs as carriers can improve the solubility of hydrophobic drugs. Simultaneously, the Enhanced Permeability and Retention (EPR) effect of NPs can stabilize tumor aggregation ^[10]. These benefits steadily improve the use and efficacy of hydrophobic drugs ^[12]. Recently, Xu et al. prepared CUR/CUR@MSNs-NFs by ESP by loading curcumin (CUR) in SiO₂NPs. The scaffolds exhibited excellent biphasic release, which released 54% in the first 3 days and all in 35 days ^[13]. In addition, by modifying the SiO₂NPs, the amine-functionalized MSNs are hydrophilic and positively charged, resulting in a more prominent anti-cancer effect ^[14]. Li and co-workers used amphiphilic lignin nanoparticles (LNPs) loaded with the anticancer drug paclitaxel (PLNPs) encapsulated in PVA/PVP nanofibers, which exhibited a 59% initial abrupt release compared to the rapid abrupt release of PLNPs ^[10]. In the same manner, adriamycin DOX was inserted into layered nanohydroxyapatite LHAp (DOX@LHAp) to blend it with PLGA. For obtaining nanofibers, DOX was loaded with 2D layered material. The release showed significant attenuation at the initial stage of release and subsequent strong prolonged release. The in vitro release showed excellent controlled release ability ^[11]. However, the relevant tests are still in the laboratory stage, and the in vivo situation is more complex because there are many influencing factors. Therefore, the in vivo drug release situation needs further research.

1.2. Dual-Drug Biphasic Approach

Inside the face of this more complicated therapeutic environment, the role of a single drug is considerably limited. To treat this shortcoming, the dual-drug biphasic approach is adopted. The ES process is used to load various drugs onto different materials. In a dual-drug biphasic release, core-shell and Janus composite fibers are frequently employed ^[15]. The existence of beads on a string in the ESP is frequently unloved, with most people believing that smooth fibers and uniform particles are the desired result. Nevertheless, according to the Janus beaded fibers prepared by Li and co-workers through a homemade eccentric spinning head with a hydrophilic polymer PVP containing the MB model drug and a hydrophobic polymer EC containing ketoprofen (KET) on other side, the beads on a string have more advantages in the drug release phase compared to the prepared Janus nanofibers. The drug is evenly enclosed in the fibers throughout the stretching process, forming a good compartment. Because of the low viscosity of the solution during the stretching phase, the beaded structure generates an unstable jet during electrospinning. This phenomenon causes polymer aggregation to generate discrete bumps. The hydrophilic side of Janus beads releases MB quickly, whereas the hydrophobic side takes longer to release ketoprofen (IPU). This facilitates a dual-drug controlled release ^[16]. Then, encapsulating a nanoparticle-loaded drug in a nanofiber loaded with another drug may yield pleasantly exciting results in a controlled drug release through the difference of their properties ^[11]. Gupta et al. formed core-shell fibers by loading kaempferol in biodegradable albumin nanoparticles that were monolithically encapsulated in PCL loaded with dexamethasone ^[17]. After a weak burst release at 24 h, a sustained slow release of 15 days is possible, allowing the prolonged simultaneous action of both drugs to synergistically promote osteogenesis. Furthermore, single encapsulation of kaempferol-loaded albumin nanoparticles in PCL nanofibers with in vitro dissolution of the drug revealed a decrease in drug release rate from both composite fibers, but this is a gratifying result, where the presence of nanoparticles reduces the continuity of the fibers, resulting in a decrease in the drug release rate.

1.3. Smart Response Drug Delivery

Characteristics, such as site-specific rather than systemic action, controlled drug release and intelligent responsive release, need to be satisfied for effective drug delivery systems ^[18]^[19]^[20]. The advantages of NNHs are evident in blending functionalized nanoparticles within electrospun fibers, which can facilitate the combination of material benefits to achieve the desired properties ^[21]. Liu et al. developed a fiber surface growth particle morphology fiber through secondary growth of an MOF material by adjusting different concentrations of ligands (2-MIM) and the reaction time. The number of fiber surface particles (ZIF-8) grown produced differences in drug release analysis. When the concentration of ligands (2-MIM) is increased, the more ZIF-8 particles grow on the fiber, leading to a decrease in the amount of drugs released. The presence of nanoparticles significantly reduced the drug release capacity. After 72 h of dissolution experiments, 89% of APS was released at pH = 5.5, and only 40% of APS was released at pH = 7.2. The relative extremely slow rate obviously depends on the pH value^[22]. Croitor et al. prepared NNHs by a single-step blending process of 10% PLA with different masses of GO stirred well and by ESP ^[15]. The surface of the fiber is flat and smooth, and the diameter of fiber decreases significantly after loading GO nanoparticles. GO has superior electrochemical properties and can respond rapidly under external electric field stimulation. Through an in vitro drug dissolution test, the drug release capacity at 10HZ PLA/GO/Q is about 8000 times more than that without external stimulation. In the treatment process, the ability to achieve an intelligent response to the characteristics of drug release through the modulation of electrical signals alone is undoubtedly a groundbreaking innovation. However, in the drug delivery process, it is necessary to provide the appropriate release rate. Too fast a release of drugs can easily reach the peak, biological activity can become to high or a certain degree of toxicity can even be produced. How to precisely regulate the ability to release drugs through changes in electrical signals is still a challenge ^[23].

For the same purpose, Banerjee et al. generated a PCL composite fiber containing superparamagnetic iron oxide nanoparticles (SPIONs). The NPs can carry rhodamine B model drugs. Under external stimulation, the NPs generate magnetically. Furthermore, the NPs create thermal energy as a result of Néel–Brownian relaxation ^[24]. The morphology of the composite under human-acceptable laser irradiation showed a molten state compared to pure PCL electrospun fibers with no significant change, which was attributed to the second effect of SPIONs. In vitro assays showed that the release of rhodamine B from RF-EMF exposure showed a linear increase at a certain time, reaching 40% release after the fifth activations. Controllability is perfectly illustrated. Nevertheless, one should be aware that the magnetocaloric effect of SPIONs is complementary to thermosensitive polymers, but the generated high heat may affect the performance of the polymers as well as the biological activity of the heat-insensitive drugs ^[25]^[26].

2. Antibacterial

Recently, with the abuse of antibiotics, different types of drug-resistant bacteria emerged ^[27]^[28]^[29]^[30], and the combination of different types of materials based on NNHs can also generate excellent antibacterial ability against drug-resistant bacteria. The preparation of NNHs by loading the bactericidal nanoparticles in the precursor solution begins with the mixed uniform solution, which is prepared into fibers by ESP. Mainstream bactericidal nanoparticles mainly include metal (AuNPs ^[31]^[32], AgNPs ^[33]^[34]) and metal oxides (ZnO ^[35], CuO ^[36] and TiO₂ ^[37]), etc. The accumulation of AgNPs in mitochondria leads to mitochondrial dysfunction. Additionally, AgNPs disrupt the DNA structure, resulting in non-replication and effectively suppressing bacterial multiplication. These two fundamental factors lead AgNPs to possess potent bactericidal potential ^[38]. Li et al. manufactured PCL nanofibers loaded with AgNPs and cisplatin (DDP), which can be used to prevent airway inflammation and resist granulation tissue proliferation. In comparison with the control group, the PCL-DDP-AgNPs scaffold showed no adhesion to rabbit peritracheal tissues, while the coated plate had a superior antibacterial effect ^[33]. Yang and co-workers prepared Janus nanofibers PVP-CIP/EC-AgNPs by loading AgNPs on the EC side through bide-by-side electrospinning. The Janus fibers from the disc-diffusion experiment showed a larger circle of inhibition against S. aureus and E. coli than fibers loaded with a single antimicrobial agent, which may be due to the simultaneous action of AgNPs and CIP, steadily increasing the antimicrobial capacity ^[28]. AgNPs are easily aggregated in polymer fibers, which affects the mechanical properties of the fibers and significantly compromises the antibacterial effect. Bakhsheshi-Rad et al. doped GO/AgNPs into PLLA fibers. They deposited composite fibers onto a bio-implant Mg alloy. SEM images of composite fibers co-cultured with bacteria revealed considerable bacterial cell membrane disruption. When compared to PLLA nanofibers, GO/AgNPs/PLLA efficiently inhibits bacterial proliferation ^[29]. This strategy provides new ideas for surface modification of metallic biomaterials, but high concentrations of AgNPs possess a degree of toxicity to normal cells. There is no presence of Ag elements in the organism. For example, if they are mostly deposited inside the liver, they will cause irreversible damage to the organism. Therefore, how to effectively and precisely control the amount of AgNPs released deserves researchers’ deep thinking ^[39]. There is a similar situation for AuNPs. Ibrahim et al. employed carboxymethyl chitosan (CMCS) as a green reducing agent for AuNPs. AuNPs were encased in PVA nanofibers. This technique reduces the cytotoxicity of AuNPs generated by the chemical reductant method while efficiently preventing bacterial growth. It signifies that safety has been improved further ^[31].

3. Tissue Engineering

Simulating the structure and composition of the extracellular matrix (ECM) is a method to provide suitable conditions for cell adhesion, differentiation and proliferation. Researchers have found that electrospun fibers are identical in properties to natural tissues through the intersection of biological, medical and nano-engineering technologies ^[40]^[41] while offering high porosity. Electrospinning (ES) is considered one of the most eligible technologies for tissue engineering, providing scaffolds for tissues to mimic ECM composition and deliver Biofactors, thus promoting the growth of new tissues ^[42].

Lu and colleagues used SiNPs deposited on the surface of PLLA electrospun fibers, which effectively enhanced the mechanical properties and hydrophilic ability of the composite membrane, leading to better biocompatibility and promoting cell adhesion and proliferation ^[43]. Orthopedic clinical challenges are surgical risks of bone loss aptamers and pathogenic infections. Placing autografts or an Allograft is the best clinical option to combat bone loss but with immune rejection problems and infection risks ^[44]. Following the development of NNHs, electrospun fiber tissue engineering scaffolds can be fabricated from nanofibers and several nanoparticle hybrids, which mainly include: inorganic nanoparticles (nanohydroxyapatite (nHA) ^[45], calcium phosphate (CaPs) ^[46], Molybdenum Disulfid (MoS₂) ^[47], Cerium dioxide (CeO₂) ^[48] and Magnesium oxide (MgO) ^[49]) and metal nanoparticles (gold nanoparticles (GNPs) ^[50]), etc.

Nanohydroxyapatite (nHA) enhances the osseointegration and osteoconductive properties of hard tissues by embedding itself in the collagen matrix of hard tissues. Song and co-workers spun NELL-1 functionalized chitosan nanoparticles (NNPs) and nHA in PCL fibers. By incorporating the NPs into PCL electrospun fibers, the authors clearly increased the fiber diameter and demonstrated that nHA and NNPs enhanced cell adhesion sites. nHA presence compared to unmodified nanofibers MC3T3-E1 cell proliferation and differentiation were enhanced ^[51]. Liu and colleagues prepared hydrogel fibrous scaffolds containing gelatin-methacryloyl (GelMA) and calcium phosphate nano-particles (CaPs). After 14 days of incubation in SBF, significant mineralized nodules developed on the surface of CaPs@GelMA-F. Faster Ca²⁺ deposition in the early stage can significantly boost the development of calcified nodules later on. Moreover, bone defects are accompanied by rupture of blood vessels. CaPs@GelMA-F cells were co-cultured with HUVECs cells, resulting in pictures of dense vascular network topology. CaPs@GelMA-F is also very effective in promoting angiogenesis ^[52].

Because of its unique physicochemical properties, where S is an important component of many amino acids in living organisms, MoS₂ is also an essential trace element in the human body ^[37]. Researchers found that doping MoS₂, a two-dimensional material, with nanofibers can effectively promote cell proliferation and maintain cell viability of BMSCs, and at the same time, the higher the MoS₂ content, the stronger the osteogenic ability ^[53]^[54]. Furthermore, Ma et al. found that the NIR photothermal properties possessed by MoS₂ can respond quickly, reaching the optimal temperature required for osteogenesis (40.5 ± 0.5 °C) in 30 s with 808 nm NIR irradiation. The BV/TV capability under NIR irradiation reached 41.41 ± 0.52% ^[47].

In addition to the various applications in osteogenic tissues, NNHs also have a positive role for other tissue engineering formation. Neural tissue engineering (NTE) is an emerging field. Material preparation requires excellent biocompatibility, certain mechanical properties and good permeability to oxygen and nutrients, etc. ^[55]. Chen and co-workers demonstrated the combination of melatonin MLT and Fe₃O₄-MNP with PCL to prepare an outer-middle-internal triple-layer structural scaffold of PCL, Fe₃O₄-MNPs/PC and MLT/PCL, with MLT effectively reducing oxidative loss. The results revealed that the scaffold had a medullary axon diameter (3.30 μm) similar to the autograft group, which significantly promoted neuronal axon growth^[56]. Myocardial infarction is one of the more common diseases in humans. Myocardial cells are gradually replaced by scar tissue after necrosis, leading to heart failure and arrhythmias caused by changes in electrophysiological properties, so it is most important for cardiac tissue engineering to have excellent elasticity, high electrical conductivity and promote the growth of myocardial cells ^[57]. Zhao et al. employed the ES process to create carbon nanotube/silk protein (CNT/silk) scaffolds. The majority of carbon nanotubes are contained within the fibers and dispersed along the fiber development direction. Compared to monospun silk protein, the elongation at the break of the composite fiber is up to 200% or more, and the tensile strength reaches 5.0 Mpa. The CNT/silk stent’s excellent electrical conductivity implies that it is efficient in avoiding arrhythmia^[58].

The human immune system’s first line of defense is the skin. Skin injury is common in everyday life. Wound dressings to meet the demands of skin tissue engineering are scarce. A great wound dressing must not only support ECM regeneration but also protect the skin from exogenous microorganisms ^[59]. NNHs fulfill the need for skin tissue engineering owing to their versatility. Janus nanofibers were loaded with AgNPS and RCSPs to impart antibacterial ability and bioactivity to electrospun fibers. In the present work, interestingly, Janus nanofibers can be obtained based on the uniaxial electrostatic spinning process through the presence of phase separation of PCL and PVP in a solution. AgNPS in the free state is very susceptible to phagocytosis by normal cells due to its fine particles and exists a certain degree of cytotoxicity, and RCSPs-Ag nanofibers in this study had only 78.86% viability on NIH 3T3 cells ^[60]. The team designed a sandwich wound dressing with AgNPs loaded with an intermediate layer of nanofibers to both impede the invasion of exogenous microorganisms and avoid cytotoxicity ^[61].

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Deng-Guang Yu

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Update Date: 28 Jan 2022

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