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31 October 2024

A Review on Recently Developed Antibacterial Composites of Inorganic Nanoparticles and Non-Hydrogel Polymers for Biomedical Applications

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and
1
Prokhorov General Physics Institute, Russian Academy of Sciences, 119333 Moscow, Russia
2
Institute of Biology and Biomedicine, Lobachevsky State University of Nizhny Novgorod, 603950 Nizhny Novgorod, Russia
*
Author to whom correspondence should be addressed.
Nanomaterials2024, 14(21), 1753;https://doi.org/10.3390/nano14211753
This article belongs to the Special Issue Nanomaterials for Green and Sustainable World
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Abstract

Development of new antibacterial materials for solving biomedical problems is an extremely important and very urgent task. This review aims to summarize recent articles (from the last five and mostly the last three years) on the nanoparticle/polymer composites for biomedical applications. Articles on polymeric nanoparticles (NPs) and hydrogel-based systems were not reviewed, since we focused our attention mostly on the composites of polymeric matrix with at least one inorganic filler in the form of NPs. The fields of application of newly developed antibacterial NPs/polymer composites are described, along with their composition and synthetic approaches that allow researchers to succeed in preparing effective composite materials for medical and healthcare purposes.

1. Introduction

Over the last few centuries, the development of civilization has led to global environmental problems that human society has only recently begun to recognize. Currently, new safe and cost-efficient methods and industrial approaches, resource-extracting processes, and human everyday life are gradually being developed and implemented. However, environmental deterioration already affects the quality of life and humans’ health. In the biomedical sector, bacterial infections are still an important opened issue. Acquired antibiotic resistance of the bacteria makes medical devices (either disposable or long-term used, such as implants), hygiene items, and even presence in a medical institution unsafe and potentially dangerous. That is why the development of new antibacterial materials for solving biomedical problems has become an extremely important and very urgent task.
The development of composites containing polymer and nanoparticles (NPs) for biomedical purposes is a fast-growing field with a number of diverse applications. According to the PubMed source, overall, about 1800 articles with the key words “composite AND polymer AND nanoparticles AND antibacterial” have been published to-date (see Figure 1a). The first publication was found to be made in 2000, the next one was published in 2001, after which a slow rise can be noticed, with the first doubling of the number of articles published per year observed in 2008. Afterward, a gradual and steady increase in the number of published articles can be seen until now (see Figure 1a). Thus, new and improved composites of NPs and polymers are constantly being developed, and this field deserves close attention from researchers worldwide [1,2].
Figure 1. (a) Histogram indicating the publication activity in the field (according to the PubMed). (b) Pie diagram showing the application of the polymer/NPs composites in medical fields.
The present review aims to summarize recent articles (from the last five, but mainly from the last three years) on the NPs/polymer composites prepared for biomedical applications. We excluded from the overview the articles dedicated to polymeric NPs and hydrogel-based systems, focusing our attention mostly on the composites of polymeric matrix with at least one inorganic filler in the form of NPs (metal, oxide, etc.). The fields of application of newly developed antibacterial NPs/polymer composites are described, along with their composition and synthetic approaches that allow researchers to succeed in preparing effective composite materials for medical and healthcare purposes.

2. Fields of Application for NPs/Polymer Composites

Among the biomedical applications of NPs/polymer composites developed during the last five years, many different directions can be seen (Table 1). Figure 1b shows that the most popular direction (31%) is the development of materials for wound treatment. Here, new antibacterial composites for wound dressings are under active development [3,4,5,6,7,8,9,10,11,12,13,14,15,16], along with materials for wound healing [17,18,19,20,21,22,23,24,25,26,27]. Materials for wound infection therapy [28], especially those for fighting drug-resistant bacterial infections [29], are also described. The treatment of chronic wounds that have prolonged healing time is one of the most important tasks in this direction, which challenges researchers [30,31]. Active wound dressing systems [32] and multifunctional materials for skin wound repair [33] are developed as well. Chen and co-authors [34], for example, prepared composite nanofiber membranes for medical wound dressing that combine antibacterial, anti-inflammatory, and antioxidant actions. Miralaei etc. [35] developed composite biofilms for rapid wound dressing, which among others are able to control bleeding. Composites for wound healing and blood clotting were also reported by Alizadeh and co-authors [36].
Table 1. Composition and preparation methods of the antibacterial NPs/polymer composites under review.
After wound treatment, the next most popular application for NPs/polymer composites is medical devices (12.9%). Antibacterial materials described here can be used in either a wide range of different devices and disposable medical equipment [50,54,71,74,98], or have specific applications, for example, for orthotic [43,79] and orthopedic devices [68], for prosthetics [43,53,110] and implants [108], for medical gloves and multipurpose rubber sheets [86], and for catheters [31,51,61].
The third place in the analyzed fields belongs to the antibacterial NPs/polymer composites for bone and tissue engineering (9.5%). Among the materials developed in this direction, there are agents for tissue engineering [80,95], and more specifically, for bone tissue engineering [64,69,102], bone regeneration [42,59,99], and bone reconstruction [109]. For example, Benedini et al. reported on alginate/nanohydroxyapatite composites that can be potentially used as antibacterial bone filler [107], Table 1. Composition and preparation methods for the antibacterial NPs/polymer composites are under review.
The materials for skin tissue engineering are also described in the literature [13], with one of the best examples being a conducting polymer/silver NPs composite as a potential xenograft for burn treatment [32].
Antibacterial coatings made of NPs/polymer composites occupy the fourth popular place (9.9%) in the field under view (Figure 1b). In this direction, mostly antibacterial coatings for non-specified biomedical purposes are developed [45,46,48,87]. Multifunctional antibacterial coatings with self-healing properties can be found [37,66], with additional specific coatings mentioned. For instance, Chacko with co-authors [112] prepared a composite system with bacterial-resistant and magnetoelectric properties that can be used in electric and magnetic field-tuned coatings, which are ideal for implantable medical devices and smart textiles for healthcare uses.
Composites of NPs and polymers developed in the last five years also include materials for dental applications (6%). Dental composite resins [55,85], including compositions with self-healing capabilities [103,105], and systems with therapeutic [56], defect repairing [81] and restorative filling [104] capabilities were reported to be developed in this direction.
NPs/polymer composites with antibacterial properties are also used for different wearables (3.4%). Here, materials for wearable electronics [52,58], flexible wearable strain sensors [39], and textile sensors for wearables and smart clothes [65] can be mentioned.
Antibacterial composites for drug delivery are another direction for the development of NPs/polymer systems, which occupy some 2.6% of publications in the field; these include research on materials for drug delivery [40,101] and scaffolds for drug sustained-release through direct coating or blending [60].
About 22.4% of the authors did not specify the applications for their developed materials, only indicating that they were aiming at preparing materials for biomedical [5,44,47,76,77,83,88,89,91,92,93,94,97,113,114,115] and healthcare [70,73,84] uses. Some studies were aimed at the preparation of materials that can act as advanced antibacterial agents [62,63], to reduce the future risks of conventional antibiotic misuse [90] and to manage drug-resistant bacteria [31] and biomaterial-centered infection [72].
The other articles reviewed (5.2%) were found to be dedicated to very specific applications. Among them, there is an antibacterial material for use as a hemoperfusion adsorbent for efficient bilirubin removal [96]. A material for the treatment of visceral leishmaniasis is also described [116]. Datta et al. [57] developed a material that has a strong effect against Shigella. Bashal with co-authors [95] prepared a composite that has potential for pharmaceutical applications. MRI imaging with a cytocompatible and antibacterial agent was proposed by Kafali et al. [100]. Banerjee with co-authors reported on films that can be used as top-sheets in feminine sanitary hygiene napkins [82].
Thus, it can be concluded that the NPs/polymer composites developed over the last 5 years have a wide variety of different biomedical applications, starting with wound dressing and ending with xenografts and MRI.

3. Nanoparticles for Composites

The NPs incorporated into the polymer matrix provide not only antibacterial properties but can also enhance the mechanical performance of the polymer matrix [86], improve the pore size distribution of the matrix [96], and affect the electric conductivity [33,84]. Moreover, they can provide additional cross-linking of the polymer components [86], adjust semiconductors properties [84], bring a self-healing effect [41], enhance the composite functional properties [81], and so on. Thus, the role of NP filler in the composites under consideration is quite multifunctional.
The dispersion of particles at the nanoscale level is known to result in a very high interfacial area for interaction of polymer chains with NPs. This can lead to enhancement of certain properties even at a low loading of the filler [87]. The amount of filler added to composites differs among studies. Typically, researchers prepared composites with different loadings of NPs and compared the properties of the resulting materials. The loading ranges (minimal and maximal content of NPs) are graphically presented in Figure 2. It is seen that the average minimal loading was 1.4 wt.%, and maximal was 7.0 wt.%. The overall minimal concentration found was 0.001 wt.% of NPs [110], and the overall maximal loading was 26.01 wt.%, reported in the work by Luo [24].
Figure 2. Minimum and maximum concentrations of NPs loaded into NPs/polymer composites, as reported in 72 reviewed articles.
In the following sections, we discuss and summarize the types of fillers and their origination and composition mentioned in the literature.

3.1. Type and Composition of Filler

This review focuses on composites containing at least one kind of inorganic NP as the filler. In this respect, the composites covered here can be classified as containing one-component filler or complex filler (more than one component). Complex fillers, in turn, can be divided into two groups. The first group contains fillers represented by two or more different materials (at least one of them being in a form of NPs). The second group is fillers that contain NPs modified with different modifiers. The resulting percentage of each type can be seen in Figure 3a. It is seen that, at present, the one-component fillers are preferable in such antibacterial NPs/polymer composites (51.8%). Multicomponent and modified fillers were reported by almost the same number of surveyed reports (23.7 and 24.5%, respectively).
Figure 3. Pie diagrams on the type of filler (a) and origination of NPs (b).
As for the composition of fillers, silver-containing particles are seen in Figure 4 to occupy the leading position (43%) in the field. Concerning this, in 61 out of 64 articles, composites with Ag NPs are prepared (see, for example, [37,39]). The other articles on Ag-containing fillers are devoted to Ag2O [53], AgBr [31], and Ag2[Fe(CN)5NO] [26] NPs. The second place in Figure 4 is occupied by Zn-containing fillers (10.7%). Here, 14 out of 16 published articles deal with ZnO NPs fillers (for example, [79,81]). About 10.1.% of works published reports on Cu-containing NPs, with CuO NPs occupying 8 out of 15 positions (for example, [87]). The other articles devoted to Cu-containing NPs mentioned Cu [87,88,92], CuS [90], Cu2O [89], and CuFe2O4 [89] NPs. The same percentage (7.4%) belongs to the works that consider TiO2 (for example, [9,16]) and carbon-based fillers. The latter type of fillers is mostly represented with graphene oxide (GO, see, for example, [65,67]), and then there are graphene [71], C3N4 [66], carbon nanotubes [63], and carbon quantum dots [98]. In the case of Fe-containing fillers (4%), about half of the papers found consider Fe3O4 magnetic NPs (for example, [28,100]), with the other half devoted to LiFe5O8 [112], CuFe2O4 [89], and Ag2[Fe(CN)5NO] [26]. Silica [35,105], MgO [106], and hydroxyapatite (HAP) [59,97] were reported as fillers with roughly the same frequency (3.4%, 2.7%, and 2.7% of the pie, respectively). Finally, the other fillers, including noble metals (Au NPs [33], Pt NPs [3], Pd NPs [3]); CoO [111]; Al2O3 [110]; NiO [116]; CaO [113]; Te [115]; CeO2 [99]; glass [108,109] NPs; etc., are seen in Figure 4 to occupy the remaining 8.7%.
Figure 4. Pie diagram indicating the type composition of the filler.
So, it is seen that over the last five years, the research on antibacterial NPs/polymer composites tended to focus on one-component fillers, predominantly containing silver. However, more complex and complicated fillers based on other metals, metal oxides, etc., were also tested and applied for different biomedical purposes.

3.2. Origination of Nanoparticles

To obtain NPs/polymer composites for medical applications, either commercial or home-made NPs can be used. The latter NPs could be both synthesized in situ (during composite formation or in the presence of the pre-prepared polymer matrix) or preliminarily prepared before fabricating composite. Some examples for all these cases can be found below.
Commercial NPs were reported in 20.2% of reviewed articles (Figure 3b). Such NPs could be used either as-supplied (for example, [36,42,111]) or modified (for example, [96,102,103,105]), or after additional treatment (for example, [97]). Modification is made with different purposes. For example, Ahangaran and co-authors [103] modified SiO2 NPs with 3-methacryloxypropyl-trimethoxysilane in order to enhance their dispersion inside the acrylic matrix and to improve their adhesion in it. This permitted the derivation of a new self-healing dental composite. In the work by Du et al. [96], TiO2 NPs were modified with vinyl-triethoxysilane for the sake of improving its hydrophobicity, along with formation of double-bond composite with styrene, which was used as a novel antibacterial bilirubin adsorbent with high bilirubin clearance capacity. Modification of MgO NPs with FeCl3 and tannic acid was reported to lead to the formation of a composite with both good antibacterial activity and excellent photothermal effect [102]. Additional treatment can be made to further decrease particle size, as was reported, for example, by Babers et al. [97], who converted commercial micro-sized particles of TiO2 into nanosized ones by means of grinding.
However, the majority (79.8%) of researchers working on developing new NPs/polymer composites preferred to prepare NPs instead of using commercial products. The methods used to prepare NPs for NPs/polymer composites are schematically presented in Figure 5. It is clearly seen that a wide spectrum of chemical, physical, and physico-chemical approaches known for inorganic NPs were applied by the authors of the articles.
Figure 5. Methods used by the authors of reviewed publications to prepare their inorganic NPs (as composite fillers).
Synthesis of NPs prior to preparing the composite was a choice of 50.0% of the authors. Both chemical and physical preparation methods were described in the articles under review. The most popular preparation techniques were wet-chemistry approaches [6,15,22,35,44,59,63,70,76,79,100,105,114], including precipitation [72] and co-precipitation [101] techniques, chemical reduction [5,10,13,29,41,43,50,55,57,67,68], and chemical synthesis, where a polymer acted as NPs’ stabilizer [38,54,61,62,112]. Moreover, sol–gel synthesis [77,84,85,108,109], solvothermal [90], and hydrothermal [92,99] approaches were described. Green synthesis [9,12,17,59], biosynthesis [4,32], and template-synthesis [104] can also be found in the reviewed articles. Among physical and combined physical–chemical methods used to prepare NPs for composites, thermal decomposition [60], electrical explosion [89], and laser ablation in liquids [7,74,87,110] can be mentioned.
In situ preparation of NPs during composite synthesis or directly in the presence of polymer matrix was also a popular approach; about 29.8% of articles considered NPs prepared in situ. One-pot preparation of composites seems to be quite simple and controllable in terms of NPs size and distribution inside the polymer matrix, along with their better fixation. For example, in the work of Jia and co-authors [28], Ag NPs were obtained on the surface of FCE hybrid (Fe3O4NPs/carboxymethyl cellulose-ε-polylysine) via chemical reduction. The abundant functional groups available in the polymer matrix resulted in good anchoring of Ag NPs inside the prepared FCE hybrids.
The one-step method reported by Chen with co-authors for in situ reduction of Ag+ directly in the spinning solution was found to significantly simplify the preparation process of Ag NPs/PVA/PAA composites [34]. Importantly, it also decreased the amounts of raw material waste, thus making the process “greener”. As for the product, such an approach helps avoid the aggregation of Ag NPs. Luo et al. co-polymerized cheap and industrially produced imidazole-2-carbaldehyde and melamine, obtaining porous organic polymer that had a very high content of N (almost 40 at.%) [24]. This allowed them to effectively anchor Ag on the porous skeleton with quite high loading (26 wt.%) without aggregation. Also, such an approach helped greatly to reduce the toxicity of the Ag NPs.
Laser ablation in situ was also used to prepare NPs/polymer composites. For example, laser ablation of a copper target in a polyvinyl alcohol (PVA)/polyvinyl pyrrolidone (PVP) blend was carried out to form a composite with enhanced antibacterial activity for wound healing [20]. Haladu et al. [40] applied laser ablation in situ to form silver quantum dots (Ag QDs) in polyaspartate, with the composite resulting in well-dispersed Ag QDs in the polymer matrix, which was shown to have potential as an antibacterial agent for drug delivery.
Thus, the majority of authors working on new antibacterial composites of NPs in polymer preferred to use preliminarily prepared NPs. In situ preparation of NPs was also reported, while commercial NPs were considered within about a quarter of reviewed works.

4. Polymers for Composites

Polymers are unique materials with specific properties which are particularly attractive for biomedical applications. They are non-toxic, sustainable, renewable, very adaptable, tunable, and well compatible with biosystems, having low risk of rejection and adverse reactions [84,88,99]. They can be produced with tuning of desired specific properties, such as flexibility, conductivity, mechanical strength, thermal behavior, degradation rates, permeability, and processability [84,87]. They can also be filled with different fillers and, which is of most importance, they can be prepared in different forms, starting with protective coatings and films (for example, [49,86]), and ending with nanofibers [34], and patient-specific implants [108].
In the following sections, the types of polymer matrices together with their composition and preparation methods described by the researchers working on novel NPs/polymer composites are considered.

4.1. Polymer Matrix Composition

The list of polymers used for obtaining NPs/polymer composites for medical purposes is quite long. All of the diversity in the matrix compositions can be divided into two groups, namely, one-component polymer matrices, and complex ones. The group of complex matrices combines two-component matrices and matrices of three or more components (Figure 6a). It can be noticed that one-component matrices (for example, [17,82]) are more common (57.0%). Two-component matrix compositions (for example, [7,96]) were used in 28.1% of works, while only 14.9% of the authors working on new NPs/polymer compositions used polymer matrices consisting of three or more components (for example, [16,51]).
Figure 6. Pie diagrams showing the type of polymer matrix (a) and its origin (b).
The majority of polymers used in antibacterial composites for biomedical applications are listed in Figure 6 and Table 2 and Table 3, whereas the basic properties of the polymers are presented in Table 2. Table 3 provides information on the polymers’ features that are of particular importance for biomedical applications.
Table 2. General properties of polymers.
Table 3. Properties of polymers specific to their use for biomedical applications.
There are leaders among polymers that were most commonly mentioned in the literature (Figure 7). Polyvinyl alcohol (PVA) was used for the formation of polymer matrix in 13.9% of reviewed articles (for example, [9,20]). PVA is a semi-crystalline, non-toxic, and low-cost polymer with excellent flexibility, transparency, and hydrophilicity. It is also soluble in hot water, which makes it even more attractive for use. Chitosan was used by 12.5% of the authors (for example, [49,88]). Chitosan is a vital polysaccharide with unique biological activity. It contains different reactive groups (primary amine groups, primary hydroxyl groups, secondary hydroxyl groups), which are the source of the chitosan specific bioactivity. It is also non-toxic, biocompatible, and possesses antibacterial properties. The third place (with the score of 10.4%, see Figure 7) belongs to cellulose (for example, [52,84]). It is a biodegradable, sustainable, renewable, and biocompatible polymer. An abundance of surface hydroxyl groups results in extensive hydrophilic properties of cellulose. Its applicability for biomedical purposes cannot be overestimated. Polycaprolactone (PCL) was used by 5.6% of the authors (for example, [82,99]). PCL is a synthetic polymer which possesses such beneficial properties as excellent biocompatibility, good mechanical properties, flexibility, thermal stability, and low melting point (60 °C). Also, it has good blend ability with other polymers, and it can be easy functionalized. Polylactic acid (PLA) occupies 5.6% of the pie in Figure 7 as well. It shows favorable biocompatibility and biodegradability, along with shape-memory properties [70,102].
Figure 7. Pie diagram showing the polymer matrix composition.
Polyvinylpyrrolidone (PVP, with its 4.2% fraction in Figure 7) is a low-toxic, biodegradable amorphous polymer. Its films are easy-forming and can act as a protective agent for different surfaces [20]. Sodium alginate (SA, mentioned in 4.2% of works) is a cheap, hydrophilic, biocompatible, and biodegradable polymer. Also, it is well tolerated by the immune system of humans [9]. Polymethyl methacrylate (PMMA, mentioned in 3.5% of publications) exhibits good biocompatibility, physical and chemical stability, affordability, and malleability, which is extremely desired for, for instance, modeling of innovative orthopedic prostheses [79,89]. Polydopamine (PDA, also used in 3.5% of studies) is a durable and biocompatible coating material that can be used for functionalization and modification [49,52]. Polyethylene oxide (PEO, used in 3.5% of articles) is quite often used as a matrix-forming agent (for example, [22,29]). Polypropylene (PP) is a thermoplastic with high distortion temperature and low density. It is transparent, flame resistant, corrosion resistant, stable and easily reprocessed. It was used by the 2.8% of the authors (for example, [47,92]).
There are also other polymers (30.6%) used for the matrix formation, such as polyaniline [90], polyurethane [51], gelatin [13], polyethylene [76], polyvinylidene fluoride [69], polystyrene [96], fibroin [3], and so on.
Thus, it is seen that in recent years the studies devoted to novel NPs/polymer composites dealt preferably with one-component matrices, with the most popular polymers being PVA, chitosan, and cellulose. However, much more complex systems and rarer polymers were also applied.

4.2. Origination of the Polymer Matrix

The polymer matrices used for composites were prepared either from commercial polymers or from homemade materials. In the latter case, polymerization (or other ways of preparing polymer matrix) was carried out either in situ or prior to the composite formation. Figure 6b shows that commercial polymers were used the most frequently (64.0%), while preliminary preparation and in situ polymer synthesis were applied by 27.2% and 8.8% of the authors, respectively. The methods used for polymer preparation are exhibited in Figure 8, where essentially all methods known for polymer preparation can be seen.
Figure 8. Methods used by the authors of the reviewed publications to prepare their polymers (as composite matrix).
To obtain a polymer matrix for the composite from commercial polymers, the solution mixing method [10,60,62,94], reactive melt mixing [47], latex processing technique [86], and others were employed. Among the methods used to obtain polymers “in-house” were polymerization and co-polymerization [24,26], solution [31] and emulsion polymerization [41,48], poly-condensation [40,71,109], and reversible addition-fragmentation chain transfer (RAFT) polymerization [27,56,73]. As for preparation of the polymer matrix during composite formation, in situ polymerization was typically applied [43,90,96,105,107]. Also, NPs could be obtained in situ on the surface of a pre-prepared polymer matrix [28,33,46,50,58].
Figure 9 presents the methods that were used for composite preparation. The first stage of the process was typically combining the components, i.e., polymer(s) and filler(s), after which the product’s formation was performed.
Figure 9. Methods used by authors of reviewed publications to prepare their composites (filler in polymer matrix).
To prepare a resulting product in a form of composite film, the solution or solvent casting approach was used [4,6,9,72,83,89,99,111]. Wang et al. [49] used simple immersion of the substrate (catheter) in a solution with reagents to prepare very uniform composite antibacterial coatings. To obtain composite scaffolds or mats, electrospinning was often applied [3,8,17,22,30,34,80,82]. For composite scaffold formation, the selective laser sintering process could also be used [68]. Babers et al. [97] produced composite sheets via the compaction technique. Su and co-authors prepared composite fibers by the solution blow-spinning process [70]. Also, 3D printing [98,108] and 4D processing [102] were reported for production NPs/polymer composites for biomedical applications.
Thus, commercial polymers were most frequently used to obtain antibacterial NPs/polymer composites. At the same time, preliminarily prepared and in situ synthesized polymers were also applied.

5. Antibacterial Activity of NPs/Polymer Composites

5.1. Comparative Antibacterial Activity of the Composites

An attempt to compare the antibacterial activity and cytotoxicity (in terms of cell viability) of the materials described in the reviewed articles was also made. For this, relative values of the mentioned parameters were calculated as follows:
R e l a t i v e   P , % = P n / P 0 · 100 − 100 ,
where P is the parameter (antibacterial activity or cell viability), Pn is a value for the composite material, and P0 is a value for the polymeric material without filler.
Values of Pn and P0 parameters were obtained from the articles (note that not all the authors provided such data). The results of calculating relative P parameters related to different filler NPs are presented in Figure 10.
Figure 10. Relative antibacterial activity (a) and cell viability (b) of composites as a function of load for different fillers (NPs).
In general, it can be noted that the highest relative antibacterial activity was shown by composites loaded with TiO2-, Ag-, and Cu-based nanosized fillers (see Figure 10a). Furthermore, Figure 10b shows that these three types of fillers could also exhibit negative relative cell viability. This implies that loading fillers such as Cu, Ag, and TiO2 can lead to lower cell viability (and higher cytotoxicity). Thus, researchers working on developing systems that incorporate highly antibacterial active fillers must find an optimum between antibacterial activity and cytotoxicity.

5.2. Antibacterial Mechanisms of the Composites

The existing mechanisms known for NPs that demonstrate antibacterial activity are schematically presented in Figure 11. Such antibacterial activity was found to be based on the action of NPs themselves, and/or on metal ions they release, and/or on the action of reactive oxygen species (ROS) generated in their presence. All of these agents can potentially influence the microorganism’s cells, both extracellularly and intracellularly. The concrete effects of NPs, as well as of ions and ROS released or produced by them are listed in the scheme below (Figure 11).
Figure 11. Mechanisms of antibacterial action/activity known for inorganic NPs.
Since Ag-based filler is the most popular for reviewed NPs/polymer composites (see Section 3.1.), antibacterial action via Ag NPs penetration of the cell membranes and Ag ions release are met very often in the literature (for example, [25,50]). But intensive release of Ag ions can be harmful for human cells. Immobilization of Ag NPs onto different substrates can help avoid the side effects of silver. For this, Jatoi with co-authors [62] immobilized Ag NPs onto TiO2 NPs and then prepared their composite with cellulose acetate nanofiber. Thus, silver ions and NPs themselves acts as antibacterial agents.
Then, the oxidative stress of bacteria is described by Sun et al. [45] as a possible main mechanism of the bactericidal activity of chitosan composite with Ag NPs. In the work by Du et al. [96], bacteria were found to adsorb onto the composite, and TiO2 under UV-light excitation produced reactive oxygen species (ROS) that killed the bacteria. Sebak et al. [94] suggested that TiO2 NPs interact with the cell membranes and penetrate inside the bacteria, releasing ROS.
Along with TiO2 particles and Ag NPs and ions, other NPs and ions were also reported to provide antibacterial properties to composites. Glazkova with co-authors [89] demonstrated three possible antibacterial mechanisms of CuFe2O4/Cu2O/CuO/PMMA composite, namely, NPs interaction with bacteria, copper ion release, and ROS generation. Jardon-Maximino et al. [91] pointed out that the ability of composite to release Cu ions was in agreement with its antibacterial properties, so functionalized Cu NPs were the source of the ions.
Liu et al. [83] showed that ZnO modified with citric acid monohydrate (ZnO-CA) could only exhibit antibacterial effect when it was in direct contact with bacteria. Incorporation of such NPs into PCL matrix, which gradually degraded exposing more ZnO-CA, was shown to result in a long-term antibacterial effect. Abdelaziz et al. [59] revealed that the inhibiting activity of Ag NPs-loaded nanofiber increased with time and maximal effect was observed after 32 days. Nanofiber of polylactic acid/cellulose acetate and poly(caprolactone) polymers degraded and higher concentrations of Ag NPs became available. Similar long-term antibacterial activity was described by Guo with co-authors [60] for scaffolds with sustained release of Ag+. Haladu et al. [40] described synergistic interaction between polyaspartate (PASP) and Ag QDs. PASP biocompatibility was due to electrostatic adsorption of amino groups on the membranes of bacteria. Then, the polymer provides a long-term release of Ag ions for prolonged antibacterial action.
Many examples of synergistic effects were found in the reviewed articles. Bagheri et al. [18] revealed that the presence of both ZnO and Ag NPs in the composite scaffold showed a stronger synergistic antibacterial effect compared to the control antibiotic and bare polymeric disks. Hezma and co-authors [77] pointed at the fact that the antibacterial activity increase was a result of synergy between co-polymer CS-PVA and ZnO NPs via reactive oxygen species (ROS) formation and Zn2+ release, respectively. Astashev et al. [110] described a synergistic effect, in which borosiloxane matrix protects NPs of different influences (physical and chemical), while aluminum oxide NPs accelerated the formation of ROS. Such a synergistic effect allowed a reduction in the amount of incorporated NPs without a decrease in the antibacterial activity. In the work of Jia and co-authors [28], cellulose-based composite with Fe3O4 and Ag NPs showed the best antibacterial results with the assistance of H2O2, indicating the synergistic strategy. Guo et al. [21] hypothesized the following factors for outstanding synergistic antibacterial capability of polyCu-MOF@AgNPs composite: intracellular ROS production, Ag ion release under acidic conditions, entrance of Ag NPs and metal ions into the cell, morphological change in bacterial membrane, and damage of DNA or proteases.
Along with synergistic effect, a combined action of the composite’s components can be the basis for its antibacterial activity. Joy et al. [99] suggested that the antibacterial effectiveness of the PCL-GO-CeO2 composite is based on the combined action of the filler’s components. Thus, CeO2 generates ROS, and GO physically destroys the bacterial cell membranes by its sharp edges. In the work by Shah et al. [90], the combined effect of CuS and PANI was described as the factor improving the antibacterial activity via ROS generation.
The structure of the composite can also be an important factor for antibacterial activity. Su and co-authors [70] pointed out that the pore structure of the composite fibers plays quite a significant role in antibacterial activity. The release of Zn2+ and Ag+ is facilitated by high porosity and specific surface area, and causes generation of a large number of ROS, which induce oxidative stress in bacteria. Also, in the work by Wang et al. [71], the structural effect on antibacterial activity appeared in a form of maximizing the loading of Ag NPs via increasing the accessible surface area of the substrate material, and its highly porous structures. They used in situ reduction of Ag+ by tannic acid (TA) and revealed the TA concentration-dependent antibacterial activity (as more TA could reduce more silver ions). Another structure-based antibacterial effect was described by Balan et al. [95]. The poly-ortho-toluidine-TiO2/PCL scaffolds’ porosity and hydrophobicity improved the bacteria interactions with substrate, leading to antibacterial activity enhancement.
Other properties can also affect the antibacterial behavior of the composite. For example, in the work of Chacko and co-authors [112], the PVDF and micro-crystalline cellulose-based composite with LiFe5O8 NPs showed a correlation between antibacterial properties and electro-active nature. So, the electrical activity of the material can also play some role in hindering bacterial growth.
Thus, different mechanisms of antibacterial activity can be found in the reviewed works. The described mechanisms are mostly complex and may include both effects of NPs and polymer matrix. New synthetic approaches for preparation composites with structure-dependent effects, combined antibacterial action of components, and synergistic effect result in excellent bactericidal and inhibition effects of NPs/polymer composites for biomedical applications.

6. Conclusions

Thus, it can be concluded that antibacterial NPs/polymer composites developed over the last 5 years have a wide variety of different biomedical applications, starting with wound dressing and ending with xenografts and MRI.
Within this period of time, the main trend in developing NPs/polymer composites was combining one-component filler and one-component polymer matrix. The most commonly used filler was Ag-containing NPs; the most popular matrices were based on PVA, chitosan, and cellulose. Concerning this, NPs produced “in-house” and commercial polymers were used more frequently. The average range of filler loading was found to be 1.4–7.0 wt.%, while the overall minimal and maximal concentrations used were 0.001 wt.% and 26.01 wt.%.
Based on analysis of the reviewed articles, the growing trend was found on trying new, cheaper, and more-readily available fillers, which in the future would substitute for Ag-containing NPs. Also, different methods of filler modification or combination/conjunction of different filler components has become popular. As for polymer matrices for such composites, the latest trend has been in creating new blends or complex polymeric compositions aiming to obtain composites with enhanced and multifunctional properties.
As for antibacterial properties, different mechanisms are described; they are mostly complex and may include effects from both the NPs and polymer matrix. New synthetic approaches for composites prepared with structure-dependent effects, combined antibacterial action of components, and synergistic effects result in excellent bactericidal and inhibition effects of NPs/polymer composites for biomedical applications.
For every application, there are specific challenges faced by the new antibacterial composites being developed. For wound treatment, for instance, such materials should exhibit not only antibacterial, but also antioxidant, blood clotting, and healing properties. For medical devices and tissue engineering, a balance should be achieved between required mechanical properties and bioactivity provided by the fillers, since the latter fillers affect the material’s strength and flexibility. Overall, researchers have been developing new antibacterial composites and need to find an optimum between antibacterial activity and cytotoxicity, as fillers with the highest antibacterial action are quite often highly cytotoxic. Here, different approaches for lowering toxicity should be used, starting with capsulation or partial blockage of the toxic component and ending with substitution of widely used antibacterial fillers with new non-trivial agents.

Author Contributions

A.V.S.: investigation, validation, visualization, writing—original draft, and writing—review and editing. V.A.K.: conceptualization, funding acquisition, project administration, visualization, writing—original draft, and writing–review and editing. I.A.P.: investigation, validation, visualization, writing—original draft, and writing–review and editing. S.V.G.: conceptualization, supervision, writing—original draft, and writing—review and editing. All authors have read and agreed to the published version of the manuscript.

Funding

This research received no external funding.

Data Availability Statement

No new data were created or analyzed in this study.

Conflicts of Interest

The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as potential conflicts of interest.

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