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Cellulosic Textiles—An Appealing Trend for Different Pharmaceutical Applications

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2023-12-11 17:45
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1. Introduction

A healthy body is an intrinsic requirement for all human beings. Pharmaceutical textiles, like cellulosic textiles, are widely used in our daily lives for several purposes like wound healing, drug delivery, and tissue regeneration [1,2,3,4].

The production of textiles is a very long and complex process that involves preparation of fibers, as well as numerous raw materials, which is the starting point. This multistage process starts from the producing of fibers and continues till the final fabric is created [5]. Production steps comprise spinning, fabric formation through knitting/weaving, followed by the so-called wet–processing. which includes pretreatment procedures through desizing, scouring, bleaching, and then dyeing and finishing—hence producing the final fabric. These stages differ depending on the nature of the used fibers as well as the properties of the desired products allowing for the production of the required textiles [6].

Fibers are either natural or man-made. Natural fibers represent those of vegetable origin (cotton, hemp, and flax) or from animals (wool and silk). For many years, natural fibers were the prevailing type in the textile market. However, the elevated expenses of using arable areas together with the increasing demand for more fibers resulted in enormous progress in man-made fibers production [7]. Cellulose is one of the main materials used for the fabrication of fibers.

Cellulose, as a natural polymer, has many advantages over synthetic polymers. It is a cheap and eco-friendly polymer in addition to its excellent mechanical properties, such as flexural and tensile strengths, as well as its thermal stability that enhances the usage of cellulose instead of synthetic polymers [8]. It is composed of small units called D-glucose, which can be obtained from different natural sources—mainly plants. A huge amount of cellulose is obtained from agricultural wastes. Based on the physical and chemical characters of cellulose, many structural modifications can be applied to improve its physical properties and reactivity. The modifications can be divided into physical and chemical. Physical modification controls shape and size and leads to the formation of micro- and nano-cellulose, while chemical modification includes oxidation, esterification, etherification, grafting, and hybridization.

The multiple benign properties of cellulose have encouraged its exploitation in the pharmaceutical field [9,10,11,12]. Recently, our team used nanocellulose isolated from agro-wastes (e.g., sugarcane bagasse) as a pharmaceutical ingredient for formulations designed for tissue regeneration [13,14,15,16,17,18,19].

Over the past few years, tissue engineering has become an alternative to tissue or organ transplantation. Tissue engineering is a vital process that involves the use of live tissues, growth factors, and biomaterials for improving or replacing injured tissues. The regeneration procedure totally replaces the damaged tissues through proliferating the adjacent intact cells [20,21]. Nanofibers have been widely investigated for tissue engineering applications due to their ability to produce more complex macro structures than scaffolds and sutures. They also represent a suitable structural replica of the extra cellular matrix (ECM) that is mainly composed of nanofibrous protein, allowing cell attachment, growth, differentiation, and organization [22]. The nanofibrous scaffolds are characterized by their biocompatibility, thus providing the needed substrate for tissue regeneration with complete and safe disintegration.

Also, cellulosic and nanocellulosic pharmaceutical textiles have emerged as a remarkable avenue in the pursuit of innovative solutions for infection control within the healthcare sector. Cellulosic textiles, such as cotton, have paved the way for the integration of antimicrobial formulations, opening up a realm of possibilities for enhanced medical textiles with profound implications. However, since cellulose lacks inherent antimicrobial activity, fibers can be readily loaded with antimicrobial agents. The hydroxyl groups present in cellulose and nanocellulose make this possible. Techniques like oxidation, esterification, and etherification are commonly employed to attach compounds that confer biocidal capabilities. These modifications allow for the incorporation of various antimicrobial agents into cellulose [23,24]. Bacterial infection of the skin can result in serious complications such as microbial resistance and dose-dependent toxicities besides the significant delay of the healing process, especially in complicated conditions as in surgical procedures, traumatic injuries, and burn wounds [25]. Thus, more attention has been directed towards the development of effective antimicrobial dressing. Recently, novel antimicrobial nanofibers have been introduced as antimicrobial dressings with high interconnected porosity (60–90%), gas permeability, balanced moisture, and great absorbance with structures similar to that of the extracellular matrix, thus providing suitable environments capable of protecting injured areas from exogenous infections [26]. However, even nanocellulose is not capable of controlling bacterial infection itself, as it has no antimicrobial activity, but nanofibers can be readily loaded with antimicrobial agents, metal nanoparticles, and natural and synthetic products [23,27,28].

This review article is focused on clarifying cellulose sources and physicochemical properties, and polymorphs are also covered together with the methods of preparation of specific cellulosic fibers for pharmaceutical use. The different methods of chemical modifications are also highlighted. Moreover, different aspects are examined related to cellulose- and nanocellulose-based textiles and their pharmaceutical applications, mainly for tissue engineering and anti-microbial, anti-viral, and wound dressing applications. Merging between cellulose and other materials like drugs, metal nanoparticles, and plant-derived materials as well as synthetic materials are also illustrated. This review also highlights some of the challenges and limitations faced due to the use of cellulose textiles in pharmaceutical fields. Researchers are addressing these challenges with great commitment, as most of the referenced works discussed in this review cover the period from 2020 to 2023. The substantial number of publications in these years emphasizes the tremendous scientific dedication to this topic.

2. Origin of Cellulose and Its Physicochemical Properties

Cellulose is one of the most abundant natural compounds. Similarly to other natural products, such as chitosan and gelatin, it is used in different medical applications related to human healthcare [29]. Cellulose is a polymer composed of small units called D-glucose and can be found in different organisms from bacteria and plants to algae and marine animals [30]. The major cellulose production (about 140 billion tons) is of plant origin [31]. It can be used directly as extracted from natural sources or can be chemically modified to enhance its physicochemical properties.

Based on the origin and method of preparation, there are four main subtypes of cellulose based on the arrangement of the monomer in the crystal structure. These types are I, II, III, and IV (Figure 1). Cellulose type I can be divided into two main subtypes, Iα and Iβ, and both types can be found in algal cell walls. Subtype Iβ exists in high percentages in higher plant and marine creatures such as Halocynthiaroretzi [32]. Cellulose I is considered a native type of cellulose, and it consists of 15,000 sugar units and decomposes at 400 °C [33]. It is composed of parallel polymer chains with highly random arrangements [34].

Figure 1. Crystal structures of different cellulose subtypes (A) Type Iα, (B) Type Iβ, (C) type II, (D) Type III, and (E) Type IV.

On the other hand, cellulose type II is produced mainly by mutant bacteria, such as Acetobacter xylinum, in a cold atmosphere [35] and is characterized by anti-parallel polymer chains compared to type I [36]. It is worth mentioning that cellulose type II can be converted to type I via mercerization (using an alkali) or solubilization and recrystallization (regeneration) [37]. The regeneration method results in higher crystallinity, purity, and yield compared to mercerization [38]. Mercerization is a technique where textiles (typically cotton) are treated with a caustic solution (mainly NaOH) or sometimes with a liquid ammonia solution to enhance features such as fiber strength, shrinkage resistance, luster, and dye affinity. The process involves treatment of cellulose with different concentrations of NaOH starting from 10 to 50% at room temperature for a specific period of time (4 h) [39].

On the other hand, cellulose type II is more reactive compared to type I, is considered as one of the most useful types of cellulose, and is used to make cellophane [36].

Cellulose III represents the amorphous form of cellulose. It is produced via the thermal treatment of both cellulose I and cellulose II. It has a high surface area as well as the property of high adsorption due to the fact that its crystalline form is destroyed irreversibly during the manufacturing process, especially in the swelling and washing steps [40]. Finally, cellulose IV is produced from type I and type II via thermal treatment and is known as high-temperature cellulose [41].

Cellulose IV1 and IV2 are prepared from cellulose III1 and III2, correspondingly, via thermal treatment in hot glycerol. It has also been stated that cellulose IV1 and IV2 have unit cells of nearly the same size but with different arrangements of cellulose chains—parallel for cellulose IV1 and antiparallel for cellulose IV2 [42].

3. Preparation of Different Cellulose Polymorphs

During earlier decades, there were many attempts to separate cellulose (native cellulose type I). Nowadays, the main sourcing of cellulose type I is through the extraction from different plant sources such as wheat husk, rice husk, maize husk, cotton, etc. In addition, bacteria and algae can participate in total cellulose production [43]. On the other hand, the early work of Badenhuizen and Meyer paved the way for the polymorphic transformation of different types of cellulose [44]. The source of cellulose is mainly agricultural waste, and the extraction process can be divided into three major steps. The first step is pre-hydrolysis, in which the main matrix of the plant is destroyed to reach the cellulose-containing parts. The second step is pulping in which an alkali is used to obtain the cellulose fibers. The last step is bleaching with hydrogen peroxide to obtain pure fibers [45]. These three processes ensure that cellulose is produced free of other plant contents such as lignin and hemicelluloses. It is worth mentioning that the product of these steps is cellulose type Iα.

The production of cellulose polymorphs is summarized in Figure 2. Starting from cellulose type Iα, heating it at a high temperature (260 °C) in the presence of sodium hydroxide will lead to the formation of cellulose type Iβ, which when boiled in water will form cellulose type III. Cellulose type III can be reconverted to cellulose type Iβ using an ammonia solution or another amine at a very low temperature (−80 °C). Also, cellulose type Iβ can be converted to cellulose type II via the mercerization process or regeneration process. Cellulose type II can be converted to cellulose type III using hot water, after which the use of liquid ammonia or an amine at low temperature can regenerate cellulose type II. Cellulose type IV is prepared by heating cellulose type III in glycerol at 260 °C [46].

Figure 2. Diagram of the preparation of different cellulose polymorphs.

Although cellulose polymorphs have been extensively researched as multidisciplinary materials, cellulose suffers from a major drawback with the hydrophobic polymeric matrix. The poor fabrication ability and the tendency to clump and aggregate during processing are mainly due to low solubility in organic solvents, as a result of the strong inter- as well as intramolecular bonding [47,48]. At the same time, increasing the temperature does not result in a subsequent increase in solubility, as cellulose is totally insoluble at <300 °C, while it degrades instantly above this temperature [49]. Additionally, the insolubility of cellulose is significantly affected by the length of the polymeric chains as at a polymerization degree higher than that of celloheptaose, the solubility of the cellooligomers reaches zero [50].

This risk of aggregation or clustering, which may occur within fiber walls, due to the collapse of the internal structure during drying is known as hornification. As a result of fiber aggregation, another problem emerges: the consumption of more energy under the high temperatures required to liberate aggregated fibers. However, in serious cases of hornification, highly refined fibers become harder, or sometimes even impossible, to extract during drying. Meanwhile, incomplete drying might result in microbial growth during long periods of storage. Cellulose fibers can aggregate/hornify regardless of the drying method, resulting in aggregates of variable structures and sizes [51,52,53,54].

4. Preparation of Specific Cellulose Types for Pharmaceutical Applications

4.1. Regenerated Cellulose Fibers (RCFs)

In the beginning of the twentieth century, regenerated cellulose was developed as the first man-made fibers to improve the softness and comfort of woven materials, representing an alternative to natural fibers like silk and cotton. These fibers combine the lustrous and smooth nature of the former together with the remarkable water absorption ability of the latter [55]. In the early twenties, rayon was the first accepted generic name used to label RCF comprising viscose, lyocell, cellulose acetate, modal, and cupro [56]. RCF is considered as the conventional textile raw material utilized in different fields from sportswear to medical and pharmaceutical, either alone or in combination with other fibers [57]. This versatile use of RCF is related to its unique characteristics such as biodegradability, smoothness, moisture absorption, and ease of dyeing in addition to it being soft and comfortable, which identifies it as a skin-friendly material [58,59].

4.2. Cellulose Nanofibers (CNFs)

In the few past decades, academics have shown growing interest towards exploring nanotechnology in the production of nanofibers and investigating their newly unique distinguished size-dependent properties [77]. The characteristics of developed nanofibers depend mainly on their diameter, length, fiber shape, either hollow or core-shell, surface area, and texture. Nanofibers have a number of exceptional novel features including their high surface area and promoted mechanical, physical, and organic properties as well as their good permeability and compatibility. Therefore, they are considered as promising candidates for many healthcare and medical applications comprising drug delivery, wound dressing, and tissue engineering [78].

Cellulose nanofibers (CNFs)—which are also known as nanofibrillated cellulose (NFCs), microfibrils, macrofibrillated cellulose, nanocrystalline cellulose, or crystallites [79]—are thin nanosized fibrils with a diameter less than 100 nm and several micrometers in length. Such fibrils are characterized by their dense fibrillary network structure with crystalline and amorphous areas. The amorphous region is responsible for the plasticity and flexibility of the CNF, while their stiffness and elasticity are attributed to the crystalline region [25]. As of recently, the production of CNFs can be performed using different cellulosic resources. Several processing techniques have been developed for CNF fabrication [80,81]. These techniques can be typically categorized into (i) mechanical, (ii) biological, (iii) physical, and (iv) chemical.

5. Pharmaceutical Applications of Cellulose-Based Textiles

Cellulose is a biocompatible material used for different biomedical applications. As previously mentioned, cellulose is considered as a material of growing interest, stimulating researchers to investigate its potential for biomedical applications as part of promising textiles. Cellulose is characterized by biocompatibility with reduced cytotoxicity, sustainability, and biodegradability [115,123,124] and having tunable physical, chemical, and mechanical properties. Biocompatibility can be defined as the ability to be in contact with a living system without producing an adverse effect [125]. Therefore, by definition, cellulose as a polymer of glucose subunits is considered a biocompatible material, minimizing the risk of adverse reactions while promptly integrating with the human body. As proven by some early reports, cellulose can be considered to be broadly biocompatible and causing no foreign body responses in vivo [25].

Cellulose has a peculiar composition containing both amorphous regions that confer flexibility and plasticity as well as crystalline ones responsible for stiffness and elasticity. This observed balance between amorphicity and crystallinity introduces cellulose as a very interesting biocompatible material [124,126] for different biomedical applications like drug delivery [126], tissue engineering [127], wound healing [128], and antimicrobial [129] and antiviral [130] applications.

As stated above, cellulose is the main component of plant cell walls. It plays an important role in the mechanical strength and shape of the plant [131]. The mechanical strength of a material is determined according to two factors: (a) Young’s modulus, also known as elastic modulus, which measures the stiffness of the material or the resistance to elastic deformation under stress; and (b) tensile strength, which refers to the maximum stress applied to a material that it can withstand while being stretched before breaking. Since plant cell walls bend but do not break, this means that cellulose fibers have high tensile strength and Young’s modulus [125]. Cellulose has a wide range of porosities and mechanical properties depending mainly on the source of production [132]. For instance, cellulose I crystals exhibit extraordinary mechanical properties characterized by their high strength and intrinsic stiffness, thus making them promising candidates for biomedical applications. Interestingly, as they are highly crystalline, CNFs show high specific modulus and strength together with the intermolecular hydrogen bonding between cellulose chains that results in their remarkable intrinsic mechanical properties [133]. Moreover, different types of cellulosic reinforcements have proved very impressive with favorable mechanical properties as seen by their optimum elastic modulus and tensile strength, which make them very convenient for various biomedical applications where stable and strong structures are desired and high mechanical performance is required [133]. Some of the pharmaceutical applications of cellulosic textiles are discussed below.

5.1. Tissue Engineering and Regenerative Medicine

Regenerative medicine stands at the forefront of health sciences, offering potential solutions for complex conditions. It harnesses stem cells, tissue engineering (TE), and gene therapy, either individually or combined, to repair, regenerate, or replace damaged cells, tissues, or organs [134,135,136].

Cellulose fibers and nanofibers (CNFs) have garnered significant attention in the field of regenerative medicine due to their distinctive properties and wide-ranging applications. The scientific literature prominently highlights CNFs’ versatility, notably in TE [137] and drug delivery [138].

TE plays a pivotal role in comprehending techniques to regenerate the human body [139]. It combines scaffolds, cells, and biologically active molecules to craft functional tissues, aiming to restore, maintain, or enhance damaged tissues or organs [140]. TE often utilizes both scaffolds [137] and hydrogels [141] as essential components of its approaches.

Scaffolds provide structural support, often mimicking the extracellular matrix and thus aiding in tissue regeneration and repair [142]. Hydrogels, on the other hand, offer a biocompatible and porous environment suitable for cell growth and diffusion [143,144].

In the field of bone TE, scaffolds and hydrogels play a pivotal role [111,145]. A natural bone is characterized by its high porosity with a matrix composed mainly of collagen and hydroxyapatite arranged in a hierarchical structure, and it also contains non-collagenous protein and proteoglycans [22]. The various bone cells, known as osteoblasts, osteoclasts, and osteocytes, are the main factors controlling bone formation and remodeling. Therefore, imitating this complex composition using highly porous biomimetic materials is an essential prerequisite for appropriate bone TE. CNF/hydroxyapatite composites can be used to mimic the natural bone environment regarding biocompatibility and porosity together with the required compressive modulus and compressive strength [146,147].

Cellulose structure can be readily modified to produce a bioactive material with a highly porous nature. This modification can be performed through oxidation with compounds such as TEMPO that yields nanofibers of negative charge and allows the desired dispersion of hydroxyapatite, creating a hydrogel that can be crosslinked [147]. Moreover, CNF can be considered as an excellent carrier of bone morphogenic proteins (BMP) and the vascular endothelial growth factor (VEGF) and thus can be very beneficial in bone tissue engineering. Sukul et al. [148] revealed that the incorporation of BMP and VEGF with CNF resulted in good cell adhesion and proliferation, where BMP enhances osteogenesis and VEGF helps angiogenesis, thus playing an important role in the bone healing process. Additionally, CNF/BMP/VEGF loaded with biphasic calcium showed enhanced proliferation and better cell attachment [149]. In another study, Salama et al. [150] showed calcium phosphate deposition on bones upon using soy protein hydrolysate grafted TOCNFs (TEMPO-oxidized cellulose nanofibril), while treating TOCNFs with SPH also resulted in the precipitation of calcium phosphate and consequently in bone tissue repair.

RCFs offer a multifaceted solution to the challenges of bone TE. They enhance mechanical strength, promote biocompatibility, and create an environment conducive to cell adhesion and growth [151]. In the study conducted by Chakraborty et al., the potential of regenerated cellulose scaffolds as biomaterials for bone TE is highlighted [152]. The researchers used electrospinning to create non-woven nanofibrous scaffolds using cellulose acetate solutions with varying concentrations in an acetone–water system. These scaffolds known as CAS (cellulose acetate scaffolds) have average fiber diameters ranging from 300 to 600 nm. To optimize these platforms, researchers created regenerated cellulose scaffolds (RCS) through deacetylation in alkaline solutions for varying time periods. The RCS underwent heat treatment at different temperatures to explore the benefits of the heating process on mechanical strength enhancement. Surface chemistry, morphology, and physiochemical characterizations were studied using attenuated total reflection Fourier-transform infrared spectroscopy, scanning electron microscopy, and other characterizations. The ideal fabrication conditions were found to be related to solvent system composition, deacetylation time, and heat treatment temperatures. In vitro investigations were conducted on selected RCS samples using MC3T3-E1 osteoblast cells, which showed improved cell adhesion and proliferation. These findings highlight the potential of cellulose-based materials—especially CNFs and RCFs—to improve bone tissue engineering through bettering cell behavior and encouraging bone tissue regeneration.

Skin TE is another field where RCFs are engaged. The skin is the body’s main defense barrier and is composed of dermal and epidermal layers. The epidermis, which makes up the skin’s outer layer, serves as a protective barrier between the outside world and the inner body. The keratinocytes, which make up the epidermal layer, continuously proliferate and differentiate [153]. Quick coverage is needed to help restore the repair and functionality as these are lost due to skin injuries like superficial burns, fissures, or lesions [154]. For complete tissue regeneration, implantable scaffolds have been developed [155,156] in order to create a favorable environment for cells to interact and proliferate. Since commercial solutions are quite expensive, in recent years, a great deal of research has been conducted on nanocellulose-based materials [157,158].

The use of cellulose nanofibers for skin TE applications has several benefits [159]: one, their high surface area that can accommodate various molecules or microbial cells; two, their high-water absorption capacity, which maintains the moisture in the injured skin while absorbing the exudate from the wounds; three, cellulose nanofibers are construction blocks that look like the nanoscale architecture. Several materials were combined with CNF for skin TE purposes. Among those materials, the poly (globalide) (PGl) is created via the enzymatic ring-opening polymerization of unsaturated 16-membered macrolactone globalide. Like most macrolactone polymers, it is non-toxic, highly hydrophobic, semi-crystalline, has a low melting point, and is exposed to hydrolytic or enzymatic breakdowns [160].

Previous studies have demonstrated that PGl can be altered to create useful crosslinked films and fibers. A possible route to successful skin epidermal treatments is the combination of both cellulose and PGl into a bilayer scaffold, where one layer is hydrophobic to prevent water loss from the skin, while the other layer is hydrophilic in direct contact with the skin injury. Layer-by-layer casting at ambient temperatures was used by Amaral and coworkers [161] to create a regenerated cellulose nanofibers (CNF)/PGl bilayer film. The PGl film was first created by pouring 10 mL of a 10% wt/v PGl in chloroform solution onto a Petri plate, which was then allowed to dry at room temperature during the next day. Then, 10 mL of a 0.1% wt/v CNF in water suspension was added to an ultrasonic bath. The suspension was applied to the PGl layer after two hours, and the resulting CNF/PGl film was then allowed to dry at room temperature overnight. For the purpose of removing any remaining solvent and preventing moisture absorption, the produced films were held under vacuum. The top and bottom surfaces of the CNF/PGl film were seeded separately with in vitro spontaneously transformed keratinocytes from histologically normal human skin (HaCaT, AddexBio T0020001) at a density of approximately 50,000 cells/cm2. Living/DEAD staining revealed a significant number of living cells on both surfaces of the film, supporting the metabolic activity of the cells. More studies are required to investigate the ability of the CNF/PGl bilayer film to quicken the wound healing process. Based on these results, we may conclude that the CNF/PGl bilayer scaffold has the potential to promote tissue regeneration in skin epidermal treatments by maintaining the viability of live cells. To validate its efficacy in wound healing, in vivo studies and clinical trials ought to be conducted in the future. The scaffold’s ability to repair wounds will be enhanced by improving its design and carrying out further biological tests. Prior to clinical use, safety evaluations and regulatory permissions are also essential processes to guarantee standards compliance and safety.

In addition to scaffolds, hydrogels have also been assuming an increasingly significant role in regenerative medicine applications. In this context, CNFs possess high strength and stiffness [162], low coefficient of thermal expansion [163], high crystallinity [164], hydrophilicity, and an easily modifiable surface [165]. Such excellent properties hold significant potential as foundational components for crafting high-performance and functional hydrogels.

CNFs hydrogels have already demonstrated their utility in different applications: they have been employed in the development of burn dressing, leveraging their properties to aid in wound healing [165]. Additionally, CNFs hydrogels exhibit noteworthy attributes like self-healing capabilities and facilitation of neural regeneration [166]. Impressively, they also exhibit considerable potential for use in bone tissue repair [167] and as a platform for controlled drug delivery, offering both redox and thermo-responsive characteristics [168,169,170]. Together, these results demonstrate how the field of regenerative medicine is developing and how innovative substances like CNFs are essential for increasing therapeutic options.

5.2. Antimicrobial Uses

The strategic integration of antimicrobial agents into cellulosic and nanocellulosic pharmaceutical textiles marks a pivotal advancement in the ongoing battle against microbial threats within healthcare and beyond. This innovative approach capitalizes on a wide spectrum of antimicrobial agents, each harnessing distinct mechanisms to counteract the proliferation of microorganisms. These agents span a rich diversity, encompassing metal nanoparticles [184], natural extracts originating from plants [185], and engineered synthetic compounds [28]. The judicious selection and incorporation of these agents empower the creation of textiles with multifaceted defenses that effectively mitigate the presence of pathogens on their surfaces [24].

Metal nanoparticles, particularly silver (Ag) and copper (Cu), have garnered substantial attention for their antimicrobial properties. Metal nanoparticles can be composed of different metals, with silver nanoparticles (AgNPs) being of particular interest [186]. Ag and its salts have a long history of medical use, with metallic silver being utilized since ancient times to heal wounds and aid in food preservation. Silver salts, especially in the form of creams or ointments, were extensively employed as antiseptics for treating burns and wounds during World War I [186]. AgNPs possess strong antimicrobial properties due to their large surface area that enhances their contact with microorganisms. They attach to cell membranes, permeate bacteria, and interact with sulfur-rich proteins and phosphorus-containing DNA within the cells. By targeting the respiratory chain and cell division, these nanoparticles lead to bacterial death. The release of silver ions further boosts their bactericidal potency [186]. Integrating these nanoparticles into textiles capitalizes on their ability to interact with bacterial cell membranes.

In parallel, the integration of natural extracts derived from plants, or insects, into cellulosic textiles offers an eco-friendly approach to combat microbial growth. Plants synthesize a plethora of secondary metabolites, such as tannins, terpenoids, alkaloids, and flavonoids, and these compounds possess inherent antimicrobial attributes developed as part of their evolutionary defense mechanisms. These compounds can target various microbial components interfering with vital cellular processes. For instance, they might hinder microbial enzyme activity, disrupt DNA replication, or interfere with nutrient uptake, collectively impeding the ability of microorganisms to thrive. Recently, some authors combined the antimicrobial properties of metallic NPs with those of natural substances, obtaining composite materials with enhanced antimicrobial effects and therefore, potentially usable in the biomedical field [187].

Synthetic antimicrobial compounds (like sulfadiazine, tetracycline, etc.), introduce a chemically engineered dimension to antimicrobial formulation. These compounds are designed to interact with microbial cell surfaces, leading to the disruption of the integrity of the cell membrane. Moreover, they can affect intracellular processes, interfering with crucial metabolic pathways and rendering microorganisms incapable of sustaining growth. The incorporation of synthetic compounds complements natural antimicrobial agents, presenting a synergistic approach that amplifies the overall antimicrobial efficacy [188].

Studies showing the merging between cellulose or nanocellulose and the active compounds mentioned above are discussed in detail, aiming to highlight the most recent innovations in the field.

5.3. Antiviral Studies

The applications of cellulose in defense against microorganisms are not limited to bacteria and fungi. There are also studies regarding viruses, although these are not as numerous. This section will provide some examples of the various applications of cellulose in antiviral preparations. In fact, in this field, cellulose fibers can be used both as a vehicle for therapeutic agents and as a material to control the spread of viruses (innovative antiviral textiles).

In a recent study conducted by Qian et al. [130], an innovative method has been proposed to prepare cotton fabric with persistent antibacterial and antiviral properties over time. To summarize, the authors introduced a technique capable of creating antimicrobial cotton textiles by integrating Cu ions into the cotton structure at the molecular level. This process hinges on disrupting the hydrogen bonds between cellulose chains, allowing Cu(II) ions to permeate swollen cellulose materials and establish a stable Cu(II) ion-cellulose complex. This method is realized through a one-pot reaction where cotton fabric is immersed in a Cu(II)-saturated NaOH solution, ensuring that the resulting Cu(II) ion-textile (Cu-IT) remains highly resistant to exposure to air, water, and physical wear and tear. Cu-IT exhibits effective interactions with viral genomes, thereby impeding virus replication, and it efficiently eliminated bacteria and fungi by damaging cell membranes and inducing the production of reactive oxygen species.

Similar findings were achieved in another study, where nanoflower-shaped Cu(I) oxide (Cu2O) NPs were fabricated in-situ within cotton fabric under gentle conditions, devoid of supplementary chemical reducing agents, and derived from a Cu(II) precursor. The Cu2O securely embedded within the cotton textile and demonstrated persistent antibacterial effectiveness (≥99.995%) against K. pneumoniae, E. coli, and S. aureus, total antifungal efficacy (100%) against A. niger, and noteworthy antiviral performance (≥90%) against human coronavirus, strain 229E, even following 50 washing cycles (Figure 5) [215].

Figure 5. Cu2O nanoparticles in cotton fabrics demonstrated excellent antibacterial, antifungal, and antiviral activities. Antibacterial inhibition activity for (A) control fabric and (B) Cu2O NF cotton fabrics. Antifungal inhibition for (C) control fabric and (D) Cu2O NF cotton fabrics [215]. Abbreviations: NF; Nanoflower.

It is noteworthy that at present, no single formulation or preparation method has been conclusively identified as superior to another. Extensive literature data suggests that ongoing research is dedicated to the exploration and identification of formulations that effectively enhance the antimicrobial properties of various active ingredients. The focus remains on optimizing formulations not only to maximize antimicrobial efficacy but also to improve patient compliance. Despite the absence of a definitive conclusion regarding the superiority of one formulation over another, the collective efforts in research aim to uncover formulations that not only excel in antimicrobial activity but also contribute to enhanced patient adherence and overall treatment outcomes.

5.4. Wound Dressing

The skin is the largest organ of the body and is the most vulnerable and susceptible to injuries, thus affecting its function as the main barrier against the external environment [216]. Skin wounds can be classified as acute or chronic: the former happens incidentally and healing takes place in 8 to 12 weeks, while the latter happens over time, such as in diabetic foot ulcers where the healing of such wounds is more challenging and the time required for complete healing cannot be determined precisely [217]. After skin damage, the process of wound healing is a complicated yet very coordinated biological process including hemostasis, inflammation, cell proliferation, and maturation, involving different types of cells, growth factors, and extracellular matrix components (ECM) [218,219]. Thus, the main purpose of a wound dressing is to maintain the hydration of the injured site, protect it from being exposed, absorb/remove excess exudates, enhance the healing process, and keep the wound safe and away from external contaminants [220].

The most commonly used wound dressings include antibacterial or antibiotic-loaded creams, hydrogels, or ointments. However, these topical preparations require frequent cleaning and reapplication [221]. Therefore, the use of nanofibers-based wound dressings has been extensively growing owing to their biodegradability, high air permeability, hypoallergenic properties, high surface-to-volume ratio, and their ability to absorb secretions from the injured site in addition to their effective enhancement of cell proliferation, allowing for the gradual release of nanofibers-loaded active agents into wounded areas [18,222,223].

Wound dressings are produced using numerous fabrication techniques—most commonly solvent casting, electrospinning, electrospraying, and 3D printing. The selected fabrication technique should fulfill the main criteria for the fabrication of an effective dressing of high porosity in order to guarantee wound respiration and to help the permeability of oxygen gas [224]. Solvent casting is considered the most commonly utilized technique producing flexible, easy-to-apply wound dressing films with enhanced gas permeability while preventing bacteria/liquid permeation [225]. However, some difficulties are encountered with the production of porous films, as the method lacks adequate control over the porosity as well as the permeability of the produced dressings in addition to the need for salt or particulate leaching [226]. On the contrary, the electrospinning technique has been extensively used for the production of wound dressings. This method provides dressings with enhanced properties suitable for various functions with controlled porosity and a high surface-to-volume ratio [227]. Similarly, the electrospraying technique has been widely explored for the preparation of various wound dressings [228]. Interestingly, of all the methods used for fabricating wound dressing nanofibers, 3D printing attracts the most attention. This technique guarantees excellent control over porosity and can be loaded with various biomaterials and/or active therapeutic agents necessary for different stages of wound healing. This unique property is offered only by the 3D printing technique: producing several layers of biomaterials having different compositions arranged over each other to obtain finally arbitrary geometries [229,230].

Accordingly, CNFs are considered as ideal substrates for wound dressings owing to their highly porous structure, excellent biocompatibility, and good mechanical properties in addition to their ability to act as a barrier against any external factor, thereby preventing secondary infections. CNFs provide various chemical reaction sites for hydroxyl groups with the potential to accommodate glycosides, proteins, polysaccharides, nanoparticles, antibiotics, local anesthetics, or other active agents at the injured area [231]. Several studies have demonstrated the superior wound healing potential of CNF dressings. Aminated silver nanoparticles and gelatin loaded CNF was prepared by Liu et al. [232] and showed adequate mechanical characteristics with pronounced antibacterial properties maintaining the homeostatic conditions and proper fluid balance at the wound site (Figure 6I). Both the in vitro and in vivo evaluations highlighted the good biocompatibility, distinguished efficacy, and wound healing capabilities of the dressing. In another study, Md Abu et al. [233] prepared CNFs loaded with honey using polyvinylpyrrolidone as a binder, and they showed pronounced wound healing properties owing to their anti-microbial efficiency against both Gram-negative and Gram-positive bacteria. Similarly, calcium ion cross-linked CNFs dressings have been proven to have good biocompatibility and convenient maintenance of moisture with good mechanical stability, where calcium plays an additional role in homeostasis and epidermal cell migration and regeneration [234].

Figure 6. (I) Zones of inhibition of silver nanoparticles and gelatin loaded CNF wound dressing compared to plain CNF dressing against S. aureus and P. aeruginosa. Reprinted from reference [232], with permission from Elsevier. (II) Full thickness induced wound demonstrating the effect of NFC wound dressing. (a) Covering of treated wounds with NFC dressing (on the right) while the control (on the left) was left untreated. (b) The NFC wound dressing separated itself after 8–9 days. (c,d) Photomicrographs of the control and injury treated with NFC dressing after being stained with hematoxylin and eosine [235].

Interestingly, functionalized CNFs dressings have also been investigated in clinical trials to help in skin healing and regeneration for burn victims. Compared to the commercial products existing in the market, such as Suprathel R, cellulose dressings have outstanding features. Despite the dressing not being antibacterial, it prevented any bacterial growth and second infection. The mechanical and physical properties of the dressings can be readily tailored to suit a patient’s requirements. Upon application on the wound, the dressing can be easily attached and then detaches smoothly on its own following the complete regeneration of the skin (Figure 6II) [235].

5.5. Surgical Uses

In the preceding paragraphs, the extensive discussion was focused on cellulose applications in the tissue regeneration field as antimicrobial or antiviral preparations or as wound dressings. However, cellulose fibers also play a crucial role in the surgical field due to their hemostatic activity [236]. Specifically, oxidized cellulose fibers are utilized for this purpose [112]. As of today, the hemostatic mechanism of textiles based on oxidized cellulose remains not fully understood. Presumably, a physical process is involved. When these textiles are applied to a bleeding site, they extract water from the blood and entrap blood corpuscular elements (platelets, red blood cells, and other active components), thereby increasing the concentration of coagulation factors [237].

Currently, various products with hemostatic activity, comprising oxidized cellulose, are available in the market. These include woven or nonwoven fabrics [238], films [239], powders [240], gauzes, or multilayer filaments with excellent hemostatic results [241]. Presently in clinical applications, the most commonly used materials based on oxidized cellulose are woven or nonwoven fabrics [242].

Moreover, tissue adhesives and sealants are becoming increasingly popular for wound closure and healing applications, particularly when traditional approaches, such as sutures, are ineffective as they are of high cost, can cause discomfort in handling, and are prone to infections. Tissue adhesives and sealants have shown great efficiency in avoiding blood loss that might occur as a result of major injuries or during surgeries [243]. Although there are various commercially available bioadhesives, none of them are suitable for the reparation of elastic and soft tissues. The crucial trade-off is between mechanical characteristics and biocompatibility. Another disadvantage of most commercially available products is their poor performance in moist and highly dynamic media in the presence of blood [244,245].Cellulose fibers can be incorporated in composite bioadhesive matrices to achieve high mechanical strength combined with biocompatibility and other desirable properties. This integration can increase cohesiveness by reinforcement of the polymeric matrix. Fiber-reinforced polymers have many potential uses in medical applications [246].

Cellulosic fibers were integrated into a gelatin/alginate hydrogel and resulted in a composite bioadhesive matrix with high mechanical and physical properties [247]. It was concluded that the fibers’ geometry had a significant effect on the mechanical properties of the preparation. Fibers with a high aspect ratio (ratio between length and diameter) have been shown to be more effective for reinforcement of materials compared to those with a low aspect ratio [248].

6. Regulatory and Safety Considerations Associated with the Use of Cellulose Textiles in Pharmaceutical Products

The pharmaceutical industry operates under stringent regulatory standards to ensure the safety and efficacy of medicinal products. As previously mentioned, cellulose textiles are commonly utilized in various pharmaceutical applications, necessitating meticulous attention to regulatory and safety considerations to meet compliance requirements.

The principal Regulatory Standards are as follows.

Regarding the safety considerations, the following should be addressed.

7. Challenges and Future Directions

As explained above, cellulose is a reliable and abundant polymer with renewable sources. The latest developments in the cellulose-based textile industry involve the use of more sustainable processes for a fast and highly demanding pharmaceutical market.

Despite the merits of using cellulose in the manufacture of pharmaceutical and medical textiles like its biocompatibility, moisture absorbability, and sustainability, some limitations and challenges may hinder its development.

One of the main challenges facing the production and commercialization of cellulose is the methods of production. As it is from a natural source, the diversity of the structures of raw materials, which are primarily species-dependent, represents a major obstacle in terms of creating a unique method for cellulose fibers production. Another limitation is that as it is a natural polymer, cellulosic textiles may suffer from short lifespans due to lower durability compared to synthetic textiles. Moreover, the extraction and chemical treatment methods using different solvents can have several environmental implications if not well-managed. Ameliorating the fabrication techniques and application of new protocols are demanding prerequisites in order to maintain the consistency of the fiber properties from one batch to another as well as reducing the needed chemicals, equipment, and time, thus minimizing rejections of the final product and decreasing the production costs and final price. Trials to decrease costs are directed towards using non-wood species for production or further developing already existing functionalization techniques to increase the charge density of fibers. At the same time, it is also necessary to find new approaches to overcome the risk of clustering and aggregation within fiber walls during drying, consider the clogging problems of the equipment, and use less aggressive chemicals and more straightforward green strategies.

Although enhanced moisture absorbance is a unique property of cellulosic textiles, in some cases, it may not be favored when quick drying is required.

Furthermore, the mechanical properties of cellulose fibers may not always meet the specific requirements of pharmaceutical textiles. For example, they may lack the desired strength, flexibility, or moisture absorption properties needed for certain applications. Developing cellulose fibers with tailored properties to meet these requirements can be a challenge.

Moreover, regulatory considerations and standards can pose additional challenges for meeting the necessary regulatory requirements for safety, efficacy, and quality control.

While we have made significant progress in the area of cellulosic textiles, it is important to acknowledge that the journey of developing this field is far from complete. Scientists should continually find ways to address the limitations and improve the outcomes of using cellulosic textiles. Addressing these challenges requires ongoing research, development, and collaboration between factories concerned with cellulose preparation, textile manufacturers, pharmaceutical companies, and regulatory bodies to ensure the successful integration of cellulose fibers in pharmaceutical textiles. Finally, exploring new applications of cellulose fibers is urgently required for making their production and commercialization industrially worthwhile.

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Reproduced from:https://www.mdpi.com/1999-4923/15/12/2738
Cellulose, the most abundant biopolymer in nature, is derived from various sources. The production of pharmaceutical textiles based on cellulose represents a growing sector. In medicated textiles, textile and pharmaceutical sciences are integrated to develop new healthcare approaches aiming to improve patient compliance. Through the possibility of cellulose functionalization, pharmaceutical textiles can broaden the applications of cellulose in the biomedical field. This narrative review aims to illustrate both the methods of extraction and preparation of cellulose fibers, with a particular focus on nanocellulose, and diverse pharmaceutical applications like tissue restoration and antimicrobial, antiviral, and wound healing applications. Additionally, the merging between fabricated cellulosic textiles with drugs, metal nanoparticles, and plant-derived and synthetic materials are also illustrated. Moreover, new emerging technologies and the use of smart medicated textiles (3D and 4D cellulosic textiles) are not far from those within the review scope. In each section, the review outlines some of the limitations in the use of cellulose textiles, indicating scientific research that provides significant contributions to overcome them. This review also points out the faced challenges and possible solutions in a trial to present an overview on all issues related to the use of cellulose for the production of pharmaceutical textiles.
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