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Symmetry 15 (2): 403 (2023)
University of British Columbia. Nanomaterials and Polymer Nanocomposites Laboratory
Valizadeh Harzand, Farrokhfar
Mousavi Nejad, Seyyed Navid
Babapoor, Aziz
Mousavi, Seyyed Mojtaba
Hashemi, Seyyed Alireza
Gholami, Ahmad
Chiang, Wei-Hung
Buonomenna, Maria Giovanna
Lai, Chin Wei
Metal-organic frameworks (MOFs) are a new class of porous crystalline materials composed of metal and organic material. MOFs have fascinating properties, such as fine tunability, large specific surface area, and high porosity. MOFs are widely used for environmental protection, biosensors, regenerative medicine, medical engineering, cell therapy, catalysts, and drug delivery. Recent studies have reported various significant properties of MOFs for biomedical applications, such as drug detection and delivery. In contrast, MOFs have limitations such as low stability and low specificity in binding to the target. MOF-based membranes improve the stability and specificity of conventional MOFs by increasing the surface area and developing the possibility of MOF-ligand binding, while conjugated membranes dramatically increase the area of active functional groups. This special property makes them attractive for drug and biosensor fabrication, as both the spreading and solubility components of the porosity can be changed. Asymmetric membranes are a structure with high potential in the biomedical field, due to the different characteristics on its two surfaces, the possibility of adjusting various properties such as the size of porosity, transfer rate and selectivity, and surface properties such as hydrophilicity and hydrophobicity. MOF assisted asymmetric membranes can provide a platform with different properties and characteristics in the biomedical field. The latest version of MOF materials/membranes has several potential applications, especially in medical engineering, cell therapy, drug delivery, and regenerative medicine, which will be discussed in this review, along with their advantages, disadvantages, and challenges.
Citation: Valizadeh Harzand, F.;Mousavi Nejad, S.N.; Babapoor, A.;Mousavi, S.M.; Hashemi, S.A.;Gholami, A.; Chiang, W.-H.;Buonomenna, M.G.; Lai, C.W. RecentAdvances in Metal-OrganicFramework (MOF) AsymmetricMembranes/Composites forBiomedical Applications. Symmetry2023, 15, 403. https://doi.org/10.3390/sym15020403Academic Editors: Chong Liu andStefano SuperchiReceived: 25 December 2022Revised: 19 January 2023Accepted: 30 January 2023Published: 3 February 2023Copyright: © 2023 by the authors.Licensee MDPI, Basel, Switzerland.This article is an open access articledistributed under the terms andconditions of the Creative CommonsAttribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).symmetryS SReviewRecent Advances in Metal-Organic Framework (MOF)Asymmetric Membranes/Composites forBiomedical ApplicationsFarrokhfar Valizadeh Harzand 1 , Seyyed Navid Mousavi Nejad 2, Aziz Babapoor 1, Seyyed Mojtaba Mousavi 3,*,Seyyed Alireza Hashemi 4, Ahmad Gholami 5 , Wei-Hung Chiang 3,* , Maria Giovanna Buonomenna 6and Chin Wei Lai 7,*1 Department of Chemical Engineering, University of Mohaghegh Ardabili, Ardabil 56199-11367, Iran2 Department of Clinical Biochemistry, School of Medicine, Shahid Beheshti University of Medical Sciences,Tehran 15167-45811, Iran3 Department of Chemical Engineering, National Taiwan University of Science and Technology,Taipei 106335, Taiwan4 Nanomaterials and Polymer Nanocomposites Laboratory, School of Engineering,University of British Columbia, Kelowna, BC V1V 1V7, Canada5 Biotechnology Research Centre, Shiraz University of Medical Sciences, Shiraz 71348-14336, Iran6 Ordine dei Chimici e Fisici della Campania (OCF) and MIUR, 80134 Napoli, Italy7 Nanotechnology & Catalysis Research Centre, University of Malaya, Kuala Lumpur 50603, Malaysia* Correspondence: mousavi.nano@gmail.com (S.M.M.); whchiang@mail.ntust.edu.tw (W.-H.C.);cwlai@um.edu.my (C.W.L.)Abstract: Metal-organic frameworks (MOFs) are a new class of porous crystalline materials composedof metal and organic material. MOFs have fascinating properties, such as fine tunability, large specificsurface area, and high porosity. MOFs are widely used for environmental protection, biosensors,regenerative medicine, medical engineering, cell therapy, catalysts, and drug delivery. Recent studieshave reported various significant properties of MOFs for biomedical applications, such as drugdetection and delivery. In contrast, MOFs have limitations such as low stability and low specificity inbinding to the target. MOF-based membranes improve the stability and specificity of conventionalMOFs by increasing the surface area and developing the possibility of MOF-ligand binding, whileconjugated membranes dramatically increase the area of active functional groups. This specialproperty makes them attractive for drug and biosensor fabrication, as both the spreading andsolubility components of the porosity can be changed. Asymmetric membranes are a structure withhigh potential in the biomedical field, due to the different characteristics on its two surfaces, thepossibility of adjusting various properties such as the size of porosity, transfer rate and selectivity, andsurface properties such as hydrophilicity and hydrophobicity. MOF assisted asymmetric membranescan provide a platform with different properties and characteristics in the biomedical field. Thelatest version of MOF materials/membranes has several potential applications, especially in medicalengineering, cell therapy, drug delivery, and regenerative medicine, which will be discussed in thisreview, along with their advantages, disadvantages, and challenges.Keywords: metal-organic frame works; MOF membrane; drug delivery; cancer therapy;asymmetric membranes1. IntroductionAll types of cancer and bacterial infections are serious threats to global health. Accord-ing to reports until 2018, nearly 18 million people die annually due to cancer and bacterialinfection [1]. The development of nanotechnology has experienced exponential growth inrecent years and has led to entry into interdisciplinary branches of various sciences, such asbiomedicine, bio-nano-technology, nanobiotechnology, and nanomedicine. NanostructuresSymmetry 2023, 15, 403. https://doi.org/10.3390/sym15020403 https://www.mdpi.com/journal/symmetrySymmetry 2023, 15, 403 2 of 22are designed with acceptable biocompatibility and efficiency. This class of materials hasattracted researchers and scientists to explore nanostructures as innovative and efficientnanoplatforms for anticancer drug/gene delivery and nanocarriers, as well as promisingdevices for various bioassay and diagnostic applications (especially for therapy/diagnosisof cancer) to be used [2–4]. Metal-organic frameworks (MOFs) are organic-inorganic hybridmaterials that have been rapidly developed for various applications such as clean energy,storage of gases such as hydrogen and methane, catalytic processes, and drug deliveryplatforms [3,5]. MOFs are composed of organic ligands as bases and clusters of suitablemetal ions as nodes. MOFs with different properties can be obtained by adjusting thealmost infinite combination of metal nodes and organic ligands. The wide range in thechoice of ingredients of MOFs makes it possible to adjust the different sizes of their poresfrom micropores to mesopores or macropores. Like other nanomaterials, one of the maincharacteristics of MOFs is their high surface area. In addition, by modifying the surface ofMOFs, their performance increases. These properties make MOFs suitable candidates forbiomedical applications such as drug delivery and magnetic resonance imaging (MRI) [6–8].The high specific surface area and large pore size of MOFs facilitate the encapsulation ofdrugs with drug loads, and besides, the structural and functional flexibility of MOFs allowsthem to be adapted to shape size, and function [9,10]. Modifying the surface of MOFs withdifferent chemical groups makes it possible to carry various drugs and can simultaneouslyact as MRI contrast agents. MOFs perform both diagnosis and treatment goals at the sametime. According to the mentioned contents, MOFs offer new advantages in the field ofbiomedicine, including the fields of monitoring, diagnosis, and treatment [11,12]. TheMOFs show greater than 90% porosity at physiological conditions, as well as a high degreeof stability, whereas the MOFs have a high potential for biomolecular in situ functional-ization with metals or organic molecules. Additionally, flexible membranes enable thedesign of bioactive substrates effectively. In addition, by using different metal groups andmultiple organic molecules, structures with a tunable pore size (typically 0.4–6 nm) andspecific surface area (500–4500 m2/g) of MOFs can be obtained [13–15]. ZIF-8 is one ofthe types of MOFs. In 2020 Ejeian, and colleagues [16,17], used polypropylene, polyurea,and ZIF-8 (PP/PDA/ZIF-8) as a selective thin film to support the essential activities ofcells using dental pulp stem cells (DPSCs). The results of this study indicated that ZIF-8nanostructures offer new opportunities for the surface functionalization of polypropylenemembranes as nanomedicines with significant therapeutic benefits. The researchers testedthe primary cell attachment, proliferation rate, and multilineage differentiation of cells onthis platform. guided bone regeneration (GBR). In the continuation of this review, someapplications of MOFs in the biomedical field and recent developments in this field havebeen discussed.2. MOF SynthesisIn the still relatively young field of MOF synthesis, the chemistry of the solid stateand zeolites have been recognized as forming the basis of this field [18]. As coordinationpolymers are formed by connecting metal ions with organic ligands as linkers, coordinationchemistry has investigated compounds labeled as coordination polymers for years. Eventhough Prussian blue compounds and Hofmann clathrates showed reversible sorptionproperties, interest in porous coordination polymers emerged much later [19]. A layeredco-trimester that demonstrated reversible sorption properties was first called MOF by Yaghiet al. around 1995 [20]. HKUST-1 and MOF-5, which were synthesized in 1999, becameamong the most studied MOFs in the following years [21,22].Hydrothermal or solvothermal synthesis routines have traditionally been used to pre-pare MOFs on small scales through electrical heating, which can take several hours or daysto complete. To prepare high-quality single crystals suitable for structural analysis in diluteliquid phase conditions, efforts were primarily focused on preparing high-quality singlecrystals. Later, microwave-assisted synthesis, sonochemical synthesis, electrochemicalsynthesis, and mechanochemical synthesis methods were used to shorten the synthesisSymmetry 2023, 15, 403 3 of 22time. Several studies were conducted on the scale-up of MOF synthesis conditions toobtain high yields of solid products for industrial applications; some of these studies alsoinvestigated the optimization of MOF synthesis conditions to achieve high yields [23,24].A variety of elements, including zinc, copper, chromium, aluminum, and zirconium,are commonly used to form frameworks containing bivalent or trivalent aromatic carboxylicacids or aromatics that contain N [25].According to Table 1, the MOF structures were synthesized using the following meth-ods and the key findings of these studies are presented.Table 1. Some of the MOFs and synthesis methods.Sample Ligand Metal Synthesis Method RefZIF-8 2methyl imidazole Zn(NO3)2·6H2O Microwave-assisted [26]IRMOF-3 2-amino-1,4-benzene dicarboxylic acid Zn(NO3)2·6H2O Microwave-assisted [27]UiO-66 1,4-benzenedicarboxylic acid ZrCl4Conventional solvothermalheating [28]Fe-MIL-100 1,3,5-benzenetricarboxylic acid Metallic iron (Fe0)Conventional solvothermalheating [29]MOF-5 1,4-benzenedicarboxylic acid Zn(NO3)2·4H2O Conventional solvothermalheating [30]MOF-5 1,4-benzenedicarboxylic acid Zn(NO3)2·4H2O Microwave-assisted [31]ZIF-8 2methyl imidazole ZnO Mechanochemical synthesis [32]ZIF-4 Imidazole ZnO Mechanochemical synthesis [32]Al-MIL-100 1,3,5-benzenetricarboxylic acid Al(NO3)3·9H2O Electrochemical [33]Mg-MOF-74 2,5- 4 dihydroxy-1,4-benzenedicarboxylicacid Mg(NO3)·6H2O Sonochemical [34]Cr-MIL-101 1,4-benzenedicarboxylic acid Cr(NO2)3·9H2O Microwave-assisted [35]3. MOF MembranesMOF membranes are widely employed in the food industry, gas separation, drugdelivery, and cancer therapy. various protocols have been applied for the design of MOFmembranes. Thereby produced various types of MOF membranes with unique propertiessuch as amorphous and low-crystalline MOF membranes, stimuli-responsive MOF mem-branes, ultra-thin MOF membranes, oriented MOF membranes, and pilot scale-up of MOFmembranes. MOFs are gaining attention since they have regular nanopores and are highlyselective in gas separation membranes. MOFs can be integrated into membrane materialsin two different ways. In one way, MOF particles can be blended with a polymer matrix toform mixed matrix membranes (MMMs), while in another, dense MOF films can be grownon porous substrates. It is important in both cases to ensure the compatibility of MOFswith polymer matrixes and substrates at the interface [36,37].3.1. Asymmetric MembranesAsymmetric membranes were first manufactured out of cellulose acetate in the late1950s by Loeb and Sourirajan and were used in reverse osmosis [38,39]. Since then, asym-metric membranes have been used in various fields of separation processes such as ultrafil-tration, microfiltration, dialysis, gas separation, and wastewater treatment.In addition to the mentioned applications, asymmetric membranes have also beenused as wound dressings to treat skin injuries [40]. The first efforts of scientists in thefield of regenerative medicine began with the development of occlusive wound dressings.Failure to absorb exudate in occlusive wound dressings such as Opsite®, Omiderm®, orSpandre® results in delayed healing in resuscitation medicine. Despite their effectiveness,these dressings did not prevent the penetration of microorganisms and dehydration ofSymmetry 2023, 15, 403 4 of 22wounds. Researchers later concluded that a combination of both systems (occlusive as wellas macroporous) would be ideal, since the bacteria could not penetrate both structures andexudate could be absorbed and gas exchanged simultaneously [41].The first wound dressings used in regenerative medicine were impermeable and pre-vented exudate from being absorbed through the wound, causing the healing process to bedelayed. Eventually, microporous constructs (e.g., Coldex®, Surfasoft®) were developedthat allowed wound exudate to be better drained. Although these dressings preventedmicrobial penetration and wound dehydration, they were incapable of preventing penetra-tion of microorganisms. The researchers concluded that combining both systems (occlusiveand macroporous structures) would be the best option since it would prevent bacteria fromentering while allowing exudate to be absorbed and gaseous exchange to occur. In order toimprove blood flow, dressings were developed with a macroporous sublayer or a hydrogellinked to a dense or hydrophobic microporous top layer. These types of dressings includeLyofoam®, Epigard®, and Duoderm®. Although they were effective, they also had somedisadvantages. For example, they had limited drainage capacity, exudate accumulation,and frequent replacements, which meant more wound infections. In the 1990s, Hinrichset al., following Loeb and Sourirajan’s work, developed for the first time an asymmetricpolyurethane membrane (PU) [39]. Based on in vitro bacterial testing using P. aeruginosa,the asymmetric PU membrane exhibited an interconnected microporous top layer (pore size0.7 m), which prevented wound dehydration and bacterial penetration. The sublayer alsopossesses a sponge-like structure that contains micropores (pore size: ten micrometers) andmacropores (pore size: 50–100 µm) that enhance tissue regeneration and absorption capaci-ties. Moreover, both layers acted as drug release reservoirs, allowing controlled gaseousexchange in a way that surpasses the limitations of Lyofoam®, Epigard®, and Duoderm®described in the previous paragraph. The use of chitosan (CS) membranes in asymmetricalforms has also been demonstrated. Due to its intrinsic properties, such as antimicrobialactivity, biocompatibility, biodegradability and hemostatic properties, CS, a natural poly-mer derived from deacetylation of chitin, has been extensively used for wound dressingproduction. A platelet recognizes the CS surface and initiates coagulation in a matter ofseconds by attracting the negatively charged residues on red blood cell membranes withits protonated amine groups, leading to a strong agglutination, thrombin production, andfibrin mesh synthesis within the microenvironment created by this polysaccharide [39,42].Considering the various properties of MOFs, the use of these materials with asymmetricmembranes have shown a high potential in separating different materials, especially gases,with the help of membranes [43]. However, the use of these two-dimensional materials andasymmetric membranes in the biomedical field, especially in the field of wound dressing,still has room for improvement.3.2. ElectrospinningNormally, polymer melts or solutions are electrospun by either pressing them througha needle, coating them on a wire, rotating a cylinder, etc., or introducing them into a strongelectric field. Generally, a strong electric field is used to melt or introduce the polymer solu-tion [44,45]. Its higher production performance can be attributed to needleless technology,which can usually be scaled up from the laboratory to the industrial level. A biotechnologyor medical application often uses nanofiber mats of this type [44,46]. Nanofiber matsare typically produced with incidentally oriented nanofibers using a static collector plate.Biotechnology and biomedicine often use these kinds of nanofiber mats. Nanofiber matsaligned in a particular direction are beneficial for cell growth [44,47,48]. A rapidly rotatingcollector and blades can be used to prepare them. A conductive substrate with groundingcan be used in orienting nanofiber mats, including magnetic nanofibers, allowing fiberalignment. Dielectric coatings can also be applied to parts of the substrate to modify theelectric field during electrospinning. In their study, Nguyen et al. study a cylinder collectorshielded by two dielectric films that rotate at a high speed. A thin gap between these twocylinders amplifies the electronic field, which controls fiber alignment and position throughSymmetry 2023, 15, 403 5 of 22diverting airflow due to cylinder rotation [49,50]. It is possible, as well, to create one ormore layers with different mechanical properties by partially growing nanofiber layerson conductive structures and partly consolidating them. Different polymers and polymerblends can be used for electrospinning nanofiber mats. An electrospinning process canbe carried out using aqueous solutions for some polymers. This method is simple andenvironmentally friendly. To use nanofiber mats in humid environments, a crosslinkingstep is required. The majority of water-resistant polymers must be electrospun usingtoxic or corrosive solvents, as opposed to electrospinning with low-toxic solvents suchas dimethyl sulfoxide (DMSO). Electrospinning often uses polyacrylonitrile (PAN) dueto its spinnability from DMSO. Another reason PAN is often electrospun is that it can beused as a precursor for carbon nanofibers. There is a wide range of materials that can bespun and co-spun into nanofiber mats, making them attractive for applications in manyfields, including biotechnology and biomedicine. It is, however, for this discussion that wewill be focusing on materials that are suitable for tissue engineering as well as other typesof cell growth that apply to this discussion [51,52]. It is highly desirable for biomedicaland biotechnological applications due to its low toxic nature and ability to be electrospunfrom dimethyl sulfoxide (DMSO). Its use for tissue engineering is less frequent, howeverthan that of other polymers. Scientists found that electrospun nanofiber mats with lowFe-MOF levels were highly porous, had an appropriate fiber diameter, and were chemicallystable [53,54]. Fe-MOF scaffolds showed better attachment, proliferation, and spreadingof human umbilical vein endothelial cells (HUVEC) than pure PAN nanofiber mats, asshown in Figure 1. It was possible to exclude cytotoxic effects for Fe-MOF in low quantities;in vivo implantation did not result in any inflammatory response. The optimal concentra-tion of Fe-MOF is the concentration that has a balance between scaffold degradation andan increase in cytotoxicity. A negative effect of Fe-MOF is that it negatively impacts cellactivity, but it positively impacts pH values at the biointerface [54–56].Symmetry 2023, 15, x FOR PEER REVIEW 6 of 23 Figure 1. Various scaffolds after seeding HUVEC are shown in scanning electron micrographs. (a) Placing HUVEC on a PAN scaffold, (b) placing HUVEC on a PAN/5% FeMOF scaffold, (c) placing HUVEC on a PAN/10% FeMOF scaffold, and (d) placing HUVEC on a PAN/20% FeMOF scaffold. Reprinted from [54]. Copyright © 2021, MDPI. 4. Biomedical Applications In coordination chemistry, open framework materials such as zeolites have been cru-cial since their discovery. In a wide range of applications, including catalysis, ion ex-change, and gas separation, porous solids have been developed with targeted topology, architecture, crystallinity, and porosity [6,57,58]. Crystallized MOFs are open framework materials composed of metal nodes and organic ligands. The large surface area and well-defined pore distribution of MOFs have made them a valuable material for a wide range of applications since they were discovered at the end of the 1990s [59]. As well as tuning their chemical functionality during synthesis, they are capable of modifying their physical properties [60,61]. There has however been considerable effort made to improve the re-sistance of MOFs to degradation under different/harsh chemical conditions because of their chemical, thermal, and mechanical stability [62,63]. 4.1. Biosensors Biosensors allow for molecular interactions to be detected and converted into an elec-trical signal that can be detected [64,65]. An electrochemical, optical, piezoelectric, acous-tic, or calorimetric biosensor involves the combination of biological elements, such as en-zymes, DNA, RNA, metabolites, cells, and oligonucleotides [66–68]. An important char-acteristic of biosensors is their ability to convert biochemical interactions into electric sig-nals that can be measured and quantified. Further, it is imperative that the minute changes that occur during biological processes, such as the interaction of various biomolecules, are analyzed efficiently. Therefore, biosensors are being developed to diagnose diseases, en-sure food quality, and monitor the environment. As far as medical applications are con-cerned, biosensors are designed to detect tumors, bacteria, toxins, and biomarkers early Figure 1. Various scaffolds after seeding HUVEC are shown in scanning electron micrographs.(a) Placing HUVEC on a PAN scaffold, (b) placing HUVEC on a PAN/5% FeMOF scaffold, (c) placingHUVEC on a PAN/10% FeMOF scaffold, and (d) placing HUVEC on a PAN/20% FeMOF scaffold.Reprinted from [54]. Copyright © 2021, MDPI.Symmetry 2023, 15, 403 6 of 224. Biomedical ApplicationsIn coordination chemistry, open framework materials such as zeolites have beencrucial since their discovery. In a wide range of applications, including catalysis, ionexchange, and gas separation, porous solids have been developed with targeted topology,architecture, crystallinity, and porosity [6,57,58]. Crystallized MOFs are open frameworkmaterials composed of metal nodes and organic ligands. The large surface area andwell-defined pore distribution of MOFs have made them a valuable material for a widerange of applications since they were discovered at the end of the 1990s [59]. As well astuning their chemical functionality during synthesis, they are capable of modifying theirphysical properties [60,61]. There has however been considerable effort made to improvethe resistance of MOFs to degradation under different/harsh chemical conditions becauseof their chemical, thermal, and mechanical stability [62,63].4.1. BiosensorsBiosensors allow for molecular interactions to be detected and converted into an elec-trical signal that can be detected [64,65]. An electrochemical, optical, piezoelectric, acoustic,or calorimetric biosensor involves the combination of biological elements, such as enzymes,DNA, RNA, metabolites, cells, and oligonucleotides [66–68]. An important characteristic ofbiosensors is their ability to convert biochemical interactions into electric signals that canbe measured and quantified. Further, it is imperative that the minute changes that occurduring biological processes, such as the interaction of various biomolecules, are analyzedefficiently. Therefore, biosensors are being developed to diagnose diseases, ensure foodquality, and monitor the environment. As far as medical applications are concerned, biosen-sors are designed to detect tumors, bacteria, toxins, and biomarkers early in the onset ofvarious disorders. Several factors have contributed to the popularity of biological sensors,including their low manufacturing costs, rapid response time, portability, high specificity,and high sensitivity, along with their ability to determine minute changes in biologicalelements [64,69–71]. Detecting biomolecules intracellularly presents a challenging tasksince non-specific targets can bind to biosensors [70,72]. To overcome this defect, structuredmaterials from the Institute Lavoisier (MIL) family of metal-organic frameworks (MOF) arebeing utilized. In particular, a combination of MILs and fluorescence was used to detectintracellular ATP molecules. An indicator of active metabolism is the concentration of ATPswithin the cell, which is the cellular energy currency [70,73]. As ATP aptamers (Apt-F)labeled with carboxyfluorescein (FAM) were linked to MIL-100, and thus quenched byPET (photoinduced electron transfer), Apt-F is bound to the ATP molecules at this point,thereby restoring FAM fluorescence. Using a chemiluminescent sensor, microfluidics-basednanosensors have been developed for identifying CD4 cells in the presence of HIV. Basedon previous research, CD4+ and CD8+ T-helper cells are thought to play a role in woundhealing, and so immunosensors can be used to monitor wound healing [64,74,75]. Due tothe difficulty of finding water-soluble photosensitizer molecules that can bind selectivelyto tumor tissues that have a wide range of characteristics and are water-soluble (for highcell uptake), nanoscale agents are generally used for delivering photosensitizer molecules(molecules that destruct tumors upon exposure to light) [64,71]. With their high porosity,large surface area, and high tunability, MOFs can be used as nanocarriers for the treatmentof sick tissue. The size, stability, half-life, and biocompatibility of these nano-carriers mustalso be monitored to increase their specificity to tumor tissue [76,77].4.2. Drug DeliveryIt has been proven that drug delivery systems (DDSs) consist of a carrier and a drug.Conventional DDSs such as tablets, capsules, and granules have several limitations anddisadvantages such as high doses needed, poor bioavailability issues, and side effects.Due to various limitations of conventional DDSs, new DDSs have been created and de-signed in the last decade. Recently, numerous DDSs have been developed to reduce sideeffects and increase therapeutic efficacy. Therefore, inorganic materials such as carbonSymmetry 2023, 15, 403 7 of 22nanotubes, graphene, magnetic nanoparticles (NPs) of iron oxide, and gold nanoparticleswere used. MOF membranes are a fascinating and versatile class of NPs, assembled frommetal ions/clusters and organic linkers. MOF membranes have various properties, such ashigh porosity and surface area and special chemical and thermal stability. They have beenapplied in diverse applications, such as gas storage, photochemistry, catalysis, separationprocesses, adsorption properties, diagnostic, and antimicrobial properties, and deliveryof a large variety of active drugs, biological gases, and cosmetics. Due to these properties,MOF membranes have become a good candidate for therapeutic and medicinal targets.The properties, such as low side effects, stimulus-based delivery systems, and multipledrugs loaded properties, have popularized the use of MOFs in drug delivery in the lastdecade. MOF membranes have been synthesized by diverse methods such as solvother-mal, sonochemical, mechanochemical, and electrochemical. Drug release is controlled byMOFs, which have a high loading capacity, and targeting capabilities thanks to their highspecific surface area, adjustable structure, modifications, and biodegradability [78]. Theirphysicochemical properties change as a result of being absorbed by proteins and cellularcomponents [79,80]. This makes it extremely problematic for nanomaterials to have lowtherapeutic efficacy, poor targeting, and adverse side effects, which are all the result of theirnano size. It is still possible to modify biomaterials (PEG, polymers, liposomes, hyaluronicacid, proteins, peptides, etc.) with MOF surfaces to some extent, despite MOFs’ propertiesof biocompatibility, active/passive targeting, and long circulation. However, there are stillsome limitations, such as easy degradation, immune recognition, and low targeting effi-ciency [81–85]. Moreover, the immune system can easily recognize and eliminate syntheticcomposites as foreign materials. Hence, most synthetic MOF carriers have a short half-life,which makes it difficult for them to accumulate in diseased parts of the body [86,87].Theideal drug carrier should therefore be biocompatible, stable, and able to target drugs.Physiochemically and biologically, biomimetic nanomaterials are derived from cell mem-branes [88–90]. Thus, they can avoid detection and elimination by the immune system aswell as perform functions such as long circulation, targeted delivery, and controlled release.To achieve bionic camouflage, cell membrane biomimetic technology entraps MOFs andtransfers their natural properties to the surface of MOFs using cell membrane biomimetictechnology. Multifunctional MOF carriers can be designed easily using this method [91,92].Since cell membrane-cloaked MOFs have similar properties to membrane-extracted sourcecells, they are capable of long circulation and disease-related targeting. Nano-carriers arecurrently made from various plasma membranes and cancer cell membranes, includingthose from blood-circulating cells [93,94]. The MOF platform has already been used tomodify red blood cells (RBCs), platelets, neutrophils, macrophages, dendritic cells, andvarious cancer cell membranes to achieve biological camouflage [95–98]. The combinationof enhanced bio-functions with improved drug delivery properties can be exhibited in abiomimetic MOF carrier. Considering the mentioned advantages of MOFs, the synergy ofthese properties with the capabilities that membranes bring can be considered a promisingoption in the field of controlled drug delivery [99]. Researchers are investigating porouspolymers for applications apart from commercial applications, such as in catalysis andphoto energy conversion [46,100]. For porous polymeric membranes, the most commercialpotential may be found in the area of biomedicine, particularly in drug delivery, tissueengineering, bio-separation, and hemodialysis. Biodegradability and easy dissolution incertain solvents make these materials ideal for biomedical applications [85,101,102]. Bio-logical scaffolds fabricated in vivo from membranes require controlled biodegradability,for example, for tissue engineering [103,104]. The development of porous polymeric mem-branes with diverse designs was enabled by selective solubility in polymer fabricationtechniques such as electrospinning or block copolymer self-assembly [105]. The second halfof this review discusses the use of porous polymeric membranes in biomedical applications.Detailed discussions of membrane properties, and features, including pore diameter ranges,porosity, and mechanical strength, will guide drug delivery techniques, including tissueengineering, biosensing, and bio-separation [87,106].Symmetry 2023, 15, 403 8 of 224.2.1. Biomaterial TypesTissue engineering uses synthetic biodegradable polymers and acellular tissue ma-trixes such as decellularized tissues and organs [107,108]. These include natural polymers(such as collagen and alginate), acellular tissue matrixes, and synthetic biodegradablepolymers (such as poly (glycolic acid) (PGA), poly (lactic acid) (PLA), and their copoly-mers) [109,110]. A biochemical, biomechanical, and biological evaluation of these bio-materials has been conducted. There are several differences between natural polymersand synthetic polymers, including their mechanical strength, degradation rate, and repro-ducible microstructures [46,111]. By electrospinning, nanofibers with unique propertiessuch as high porosity, high permeability, and large surface area can be produced fromnatural and synthetic polymers. According to previous studies, a composite made ofpolycaprolactone (PCL) and collagen combines the excellent mechanical properties of PCLwith excellent biocompatibility of collagen, making the composite a tissue engineeringsubstrate for nerves, skin, bones, vascular scaffolds, etc. As a result, the electrospinningof PCL/Collagen can serve as an effective tissue-engineered substrate [112,113]. Since 2Dnanomaterials possess unique physical, electronic, and chemical characteristics, they tendto possess remarkable properties compared to 1D and 3D nanomaterials [114]. In additionto having outstanding physical and chemical properties, 2D nanomaterials are also verybiocompatible and biodegradable, which means they can be used in tissue or organ con-struction by combining them with cell biology [115,116]. Furthermore, 2D nanomaterialshave high aspect ratios (surface area to volume ratios), which makes them suitable foruse in drug delivery systems, as they can encapsulate a large number of molecules andprovide superior control over the release of those molecules [117]. A variety of methodscan be used to prepare MOFs, including solvochemical, electrochemical, mechanochemi-cal, and sonochemical methods [23,77,118]. MOFs have proved a promising platform forbiomedical applications due to their unique structure, large surface area, tunable poresizes, and biodegradability. Rather than bridging metal ions with organic ligands, MOFsconsist of organic bonds [119,120]. A polymer fibrous mat can have increased porosity byadding MOFs as high-porosity compounds. There are many composites of these porousmaterials reported that consist of fibers or monoliths of MOFs embedded in a polymermatrix [121,122].4.2.2. Osmotic and Diffusion-Controlled MembranesOsmotic-Controlled MembranesA porous polymeric membrane diffuses drug molecules through its pores. The proper-ties of the membrane are adjusted to control the permeation and release of drug molecules.As far as membrane systems go, there are two main types: (1) membrane systems con-trolled by osmosis, and (2) membrane systems controlled by diffusion [123,124]. A polymermembrane reservoir is usually used for osmotic systems, which are capable of permeatingwater but not drugs. This approach involves pore-forming agents being added to themembranes to create pores in situ. Meanwhile, diffusion-controlled membranes transportdrugs across the membrane via drug diffusion, swelling of polymers, and degradation ofthe polymers [125,126]. Porous polymeric membranes are critical for the delivery of drugsbecause they must remain chemically and mechanically stable till the drug cargo reachesthe target point, they must be uniform in size to control drug permeability and they shouldbe easily adjustable to fit the drug’s size. Block copolymer self-assembly methods havegained popularity for drug delivery applications due to their ability to control pore sizes inthe nanometer range and low fabrication costs [126–128].Diffusion-Controlled MembranesCompared to intravenous and oral drug delivery methods, transdermal drug deliverygenerally offers several advantages. In contrast to intravenous and oral DDS that requirethe internalization of membranes, the membranes do not need to be internalized in thebody, thereby removing many barriers, such as controlled drug release or discomfortSymmetry 2023, 15, 403 9 of 22from needles [129–131]. It can be achieved by either injecting the drugs directly into thestratum corneum (SC) or by injecting them directly into the hair follicles and sweat ducts.To prevent drugs from leaking out of the transdermal drug delivery membrane, a drugimpermeable layer is placed on top of it. In the case of porous polymer matrixes, anadhesive layer is used to attach the polymer matrix to the skin, followed by a drug reservoirand porous membrane to control drug release [132,133]. It has been demonstrated that awide range of polymers can be used to produce transdermal drug delivery membranes,including gelatin, semi-synthetic polymers like hydroxypropyl cellulose, nitrocellulose,or cellulose, as well as synthetic polymers such as polysiloxane, polyisoprene, polyester,polyurethane, polyethylene vinyl acetate, polyacrylamide, and PVA [134,135]. Using alow current, the charged drug molecules pass through the body safely without causingphysiological damage. Iontophoresis is a commonly used technique for this system thathas been widely studied. Artificial membranes made of biocompatible materials are themain component of almost all iontophoresis patches. A significant improvement in drugpenetration is possible due to active transport because: (1) without releasing the druginto the bloodstream, the superficial distribution of the drugs can be controlled; and(2) rather than releasing drugs into the bloodstream, the superficial distribution of thedrugs can be controlled. The versatility of MOFs, their porosity, their large surface areas,and their high drug uptake have made them popular as DDSs in recent years [134,136].The bioactive molecules can be incorporated into MOF materials in different ways. Aone-pot synthesis and loading method takes advantage of the coordinative properties ofthe bioactive molecule by soaking the MOF system in a saturated solution of the bioactivemolecule. The limitations of these methods are related to poor solubility of the bioactivemolecules, competition with solvent molecules, or the absence of coordinative properties ofthe molecules. Mechanochemical methods are an alternative strategy. An environmentallyfriendly method for synthesizing MOFs and immobilizing catalysts has been reportedbased on mechanochemical synthesis [137,138].4.3. MOFs for Cardio-Vascular ImplantsThe prevalence of coronary artery disease (CAD) in industrialized societies is ap-proximately 4%. The traditional treatment for artery occlusions is the administration ofanti-thrombotic medications and small molecular weight nitric oxide donors [139]. Theartery may also be blocked permanently by implanting a drug-eluting stent. The use ofcopper-based MOFs in antithrombotic coatings for cardio-vascular implants has recentlybecome more prevalent. Using Cu-BTC as a catalyst, it has been established that blood-borne s-nitroso-cysteine can be converted into cysteine and nitric oxide in vitro [140,141].S-Ntirosoglutathione can also be catalyzed by more complex Cu-MOFs. MOF/polymercomposite materials show promise as lead materials for novel implants due to their nitricoxide release properties. In addition to these preliminary studies, Cu-BTC was directlygrown on stent surfaces and demonstrated acceptable hemocompatibility in vitro. The MIL-101 (Fe) polycaprolactone composite, which was evaluated as an effective non-copper-basedMOF for cardiovascular implants, used the MOF as mechanical reinforcement, a sustaineddrug release vehicle, as well as an MRI contrast agent. The interactions between MOFsand cardiomyocytes are also poorly studied [140,142]. A coating of Cu-BTC combined withpolydopamine demonstrated effective surface modification of cardiovascular stents in vivo.The reduction of protein absorption, thrombus formation, platelet adhesion, and increasedvasodilation, especially with nitric oxide donors that require catalytic degradation, resultedin a significant reduction in protein absorption, thrombus formation, and platelet adhesion(Figure 2). Other studies have reported that 3-(1H-tetrazole-5-yl) isophthalic acid-basedMOFs reduced sympathetic excitability and prevented arrhythmia. In the future, MOFswill need to be compared to clinically used materials to determine their effectiveness andsafety [120,140,143].Symmetry 2023, 15, 403 10 of 22Symmetry 2023, 15, x FOR PEER REVIEW 11 of 23 Figure 2. By continuously releasing earth-alkaline ions from MOFs, bone implants are improved, increasing bone regeneration and biomineralization (A). By enhancing osteoinduction and integra-tion of relevant genes in the presence of specific MOFs (B), and by improving tissue integration and antibacterial effects (C), MOFs facilitate osteoinduction and integration. Reprinted from [140]. Cop-yright © 2021, Frontiers. 4.3.1. Tissue Engineering Despite donor availability, the need for organ and tissue transplantation is still con-sidered one of the biggest challenges in the medical field [144,145]. Tissue engineering scaffolds are materials that, by mimicking the extracellular matrix environment (ECM), enable connection to the cells of living tissues and can be implanted in the tissues of living organisms [146,147]. Tissue engineering scaffolds must have characteristics such as bio-compatibility and high mechanical properties. On the other hand, the scaffold should have a suitable biodegradability speed for optimal tissue regeneration and match the new tissue regeneration speed [148–151]. The goal of regenerative medicine is to restore and maintain the normal function of injured or diseased tissues through the use of biological substitutes that mimic native tissues’ anatomical and functional characteristics. Engineer-ing, cell biology, and materials science principles are used in this approach [152,153]. To-day, tissue engineering is largely based on cell-based approaches and scaffold-based ap-proaches [154,155]. Traditionally, tissues are engineered using natural and synthetic scaf-fold materials. For proper direction and orientation of new tissue in growth, scaffold-based tissue engineering relies more on the body’s natural ability to regenerate [53,156,157]. By mechanically and chemically removing cellular components from tissues, collagen-based tissue matrices can be prepared by constructing artificial microenviron-ments from natural or synthetic materials [158,159]. During cell ingrowth, extracellular matrix proteins replace scaffold materials that slowly degrade following implantation [160,161]. The field of tissue engineering, despite its challenges and versatility, has estab-lished itself as a very important discipline that combines alternative materials as replace-ments for damaged tissue and stimulates natural regeneration [155]. Modern science has made tissue engineering a dominant technique for overcoming transplantation limita-tions, graft rejections, and complexities in restoring function [162,163]. In addition to Figure 2. By continuously releasing earth-alkaline ions from MOFs, bone implants are improved,increasing bone regeneration and biomineralization (A). By enhancing osteoinduction and integra-tion of relevant genes in the presence of specific MOFs (B), and by improving tissue integrationand antibacterial effects (C), MOFs facilitate osteoi duction and integratio . Reprinted from [140].Copyright © 2021, Frontiers.4.3.1. Tissue EngineeringDespite donor availability, the need for organ and tissue transplantation is still con-sidered one of the biggest challenges in the medical field [144,145]. Tissue engineeringscaffolds are materials that, by mimicking the extracellular matrix environment (ECM),enable connection to the cells of living tissues and can be implanted in the tissues of livingorganisms [146,147]. Tissue engineering scaffolds must have characteristics such as biocom-patibility and high mechanical properties. On the other hand, the scaffold should have asuitable biodegradability speed for optimal tissue regeneration and match the new tissue re-generation speed [148–151]. The goal of regenerative medicine is to restore and maintain thenormal function of injured or diseased tissues through the use of biological substitutes thatmimic native tissues’ anatomical and functional characteristics. Engineering, cell biology,and materials science principles are used in this approach [152,153]. Today, tissue engi-neering is largely based on cell-based approaches and scaffold-based approaches [154,155].Traditionally, tissues are engineered using natural and synthetic scaffold materials. Forproper direction and orientation of new tissue in growth, scaffold-based tissue engineeringrelies more on the body’s natural ability to regenerate [53,156,157]. By mechanically andchemically removing cellular components from tissues, collagen-based tissue matrices canbe prepared by constructing artificial microenvironments from natural or synthetic materi-als [158,159]. During cell ingrowth, extracellular matrix proteins replace scaffold materialsthat slowly degrade following implantation [160,161]. The field of tissue engineering, de-spite its challenges and versatility, has established itself as a very important discipline thatcombines alternative materials as replacements for damaged tissue and stimulates naturalregeneration [155]. Modern science has made tissue engineering a dominant techniquefor overcoming transplantation limitations, graft rejections, and complexities in restoringfunction [162,163]. In addition to nanotechnology and biosensors, tissue engineering hasexpanded into the design of organs on chips, clinical trials on chips, microfluidics, geneticSymmetry 2023, 15, 403 11 of 22manipulation, and more. Deciphering etiologies and repairing damaged tissues is possibleusing this technique [164,165]. With the growing clinical need to repair critical-sized bonydefects, guided bone biomaterials have been developed for bone tissue engineering [54]. Arange of treatment approaches can be used to achieve bone regeneration, including guidedbone regeneration (GBR), especially in the maxillofacial region [166,167]. An osseous injurycannot be penetrated by rapidly growing fibroblasts because of a barrier between gingivalconnective tissue and alveolar bone tissue. Osteoblasts can selectively repopulate bonedefects during healing by maintaining a secluded space during this process [16,168]. Thereare two main types of GBR membranes: non-resorbable and resorbable materials [16,169].Collagen (Col) membranes are advantageous for biomedical applications since they arebiocompatible and biodegradable, eliminating the need for a second surgery. Col mem-branes, however, exhibit unsatisfactory mechanical properties and rapidly degrade, makingthem unsuitable for medical applications [170,171]. A MOF has the potential to make apromising biomedical platform because of its unusual pore structure, large surface area,and ability to be functionalized in a variety of ways [172–174]. The solution to designingbioactive substrates is to immobilize enzyme MOFs onto porous and flexible membranes.A MOF is also suitable for combining short peptides, antibodies, and nucleic acids. MOFlayers have therefore been successfully used to support cellular behavior in vitro as wellas in vivo [140,173]. Multifunctional MOF-based biomaterials are being designed andsynthesized at an accelerated pace. Due to its excellent chemical and thermal stability, pHsensitivity, and negligible cytotoxicity, zeolitic imidazolate framework-8 (ZIF-8) is an idealcandidate for use in bone regeneration processes [172] (Figure 3).Symmetry 2023, 15, x FOR PEER REVIEW 12 of 23 nanotechnology and biosensors, tissue engineering has expanded into the design of or-gans on chips, clinical trials on chips, microfluidics, genetic manipulation, and more. De-ciphering etiologies and repairing damaged tissues is possible using this technique [164,165]. With the growing clinical need to repair critical-sized bony defects, guided bone biomaterials have been developed for bone tissue engineering [54]. A range of treatment approaches can be used to achieve bone regeneration, including guided bone regeneration (GBR), especially in the maxillofacial r gion [166,167]. An osseou injury cannot be pene-trated by rapidly growing fibroblasts because of a barrier between gingival connective tissue and alveolar bone tissue. Osteoblasts can selectively repopulate bone defects during healing by maintaining a secluded space during this process [16,168]. There are two main types of GBR membranes: non-reso bable and resor bl mat rials [16,169]. Collagen (Col) membranes are advantageous for biomedical applications since they are biocompat-ible and biodegradable, eliminating the need for a second surgery. Col membranes, how-ever, exhibit unsatisfactory mechanical properties and rapidly degrade, making them un-suitable for me ical applications [170,171]. A MOF has the potential to make a promising iomedical platform because f its unusual pore structure, large surface area, and ability to be functionalized in a variety of ways [172–174]. The solution to designing bioactive substrates is to immobilize enzyme MOFs onto porous and flexible membranes. A MOF is also suitable for co bining short peptides, antibodies, and nucleic acids. MOF layers have theref re been successfully used to support cellular behavior in vitro as well as in vivo [140,173]. Multifunctional MOF-based biomaterials are being designed and synthe-sized at an accelerated pace. Due to its excellent chemical and thermal stability, pH sensi-tivity, and negligible cytotoxicity, zeolitic imidazolate framework-8 (ZIF-8) is an ideal can-didate for use in regeneration processes [172] (Figure 3). Figure 3. ZIF-8 base Polymeric bone regenerative platform. Reprinted from [172]. Copyright © 2021, Wiley. Figure 3. ZIF-8 base Polymeric bone regenerative platform. Reprinted from [172]. Copyright ©2021, Wiley.Symmetry 2023, 15, 403 12 of 224.3.2. Bone AdhesivesBone adhesives with properties such as biocompatibility and prevention of shapechanges in drugs used in the reconstruction of bone defects play an important role in bonegraft repair surgery [175]. A multifunctional hydrogel containing catechol and chitosanmodified with ZIF-8 nanoparticles (CA-CS/Z) was produced by Y. Liu et al. to stabilize graftenvironment, accelerate bone regeneration, promote osteogenic differentiation, and expandblood supply [176]. By chemically converting catechol and ZIF-8, they developed hydrogelswith excellent wet adhesion. An analyses of the characterization data demonstrated thatCA-CS/Z hydrogels were synthesized successfully, displaying reliable mechanical strength,excellent rheological properties, and excellent adhesion for clinical application. In rat bonemarrow mesenchymal stem cells (rBMSCs), their superior biocompatibility allows them toprovide blood supply through paracrine production of vascular endothelial growth factor(VEGF). Furthermore, ZIF-8 nanoparticles released from the hydrogels could enhanceosteogenic differentiation of rBMSCs by up-regulating the secretion and production ofcollagen 1, osteocalcin, and alkaline phosphatase. Additionally, CA-CS/Z had antibacterialproperties. CA-CS/Z also demonstrated an important effect on vascularized osteogenesisby stabilizing bone graft materials and thereby accelerating bone regeneration when appliedto wound areas [175,176].4.4. Cancer TherapyDifferent synthetic methods have been used to prepare MOFs for a variety of uses,including catalysis, separations, sensing, drug delivery, optics, and many biomedical ap-plications. Annually, millions of people die from cancer, one of the most serious threatsto human health [177,178]. The most common method of treatment is chemotherapy. Inaddition to undesirable side effects, poor pharmacokinetics, and poor biodistribution,therapeutic drugs cannot be administered directly to patients. To decrease side effects andenhance therapeutic efficacy, research efforts have focused on controllable drug deliveryvehicles [179]. Over the past few decades, various nanocarriers have been developed,including organic micelles, liposomes, and dendrimers, as well as inorganic mesoporoussilica and quantum dots. These carriers, however, do have limitations in bio application,such as a low loading capability of liposomes, micelles, or dendrimers, and undesirabletoxicity and degradation properties of inorganic materials. The following basic require-ments must be met in a drug-loading system: a large loading capacity is important forintravenous drug administration; carriers must be nanoscale to allow intravenous drugadministration; carriers must also be biocompatible, i.e., not toxic, and easily degraded bythe body [179,180]. It is also possible to control the release of drugs from a vehicle loadedwith drugs. Therefore, controlled drug release systems have been extensively investigatedin cancer chemotherapy. A multimodal treatment system is also being developed to meetthe ever-growing demand for effective therapeutic interventions [181]. Janus nanocompos-ites made of Au nanorods (NRs) and ZIF-8 were developed by Han and colleagues for CTimaging and synergistic chemo-photothermal treatment of BALB/c mice bearing the H22gene (see Figure 4) [182,183]. MOFs have the following obvious advantages over traditionaldrug carriers, as discussed above: with a variety of morphologies, compositions, sizes, andchemical properties, MOFs have a variety of multi-functionalities and stimuli-responsivedrug release mechanisms. In addition, MOF-based materials retain their desirable physico-chemical characteristics after modification without significantly altering their controlledsize, shape, or uniformity. The properties described above make MOFs beneficial as deliverysystems for drugs, clinical tumor therapies, and other diseases [184]. Table 2 summarizes afew of the most important applications of MOF composites in biomedical fields.Symmetry 2023, 15, 403 13 of 22Symmetry 2023, 15, x FOR PEER REVIEW 14 of 23 Table 2. MOF/Matrix applications in biomedical fields and preparation methods. MOF-Type Matrix/MOF-Based Material Preparation Method Application Ref ZIF-11 Dimethylformamide Electrospinning Integrated restoration of the ten-don-to-bone interface. [106] ZIF-8 Alumina membranes Electrochemical depo-sition Homologous-targeted therapeu-tic applications. [185] Cobalt-based MOF PLA/PVP Electrospinning Antibacterial applications. [186] ZIF-8 Double-layer PCL/Col mem-brane Electrospinning Osteogenesis and angiogenesis applications. Bone regeneration, bone tissue engineering. [172] CuBTTri Medical tubing Tubing Coating Method/chemical va-por deposition (CVD) Antibacterial coating for medical devices. [187] ZIF-8 PCL- PPCL- TAEG-PDA melt-blown Electro-spinning Day ligDaylight recyclable anti-bacterial masks, medical protec-tive clothing, and bactericidal air purification filter application. [188] ZIF-67 Au@Pt One-pot synthesis ul-trasound-assisted method Electrochemical sensing of H2O2 in living cells [189] MOF-199,MOF-74,MOF-5, MIL-53 Cotton In situ cotton-MOF synthesis Antimicrobial activity against nosocomial bacteria [190] MOF-5 Ag Green and mild method Antibacterial activity [191] Fe(III) metal-or-ganic frameworks PAN Electrospinning Tissue engineering investigations [173] Figure 4. LA-AuNR/ZIF-8 and its application for CT imaging-guided tumor treatment. Reprintedfrom [182]. Copyright © 2020, Wiley.Table 2. MOF/Matrix applications in biomedical fields and preparation methods.MOF-Type Matrix/MOF-Based Material Preparation Method Application RefZIF-11 Dimethylformamide Electrospinning Integrated restoration of thetendon-to-bone interface. [106]ZIF-8 Alumina membranes Electrochemical deposition Homologous-targetedtherapeutic applications. [185]Cobalt-based MOF PLA/PVP Electrospinning Antibacterial applications. [186]ZIF-8 Double-layer PCL/Colmembrane ElectrospinningOsteogenesis andangiogenesis applications.Bone regeneration, bonetissue engineering.[172]CuBTTri Medical tubing Tubing Coating Method/chemicalvapor deposition (CVD)Antibacterial coating formedical devices. [187]ZIF-8 PCL- PPCL- TAEG-PDA melt-blown ElectrospinningDay ligDaylight recyclableantibacterial masks, medical protectiveclothing, and bactericidal airpurification filter application.[188]ZIF-67 Au@Pt One-pot synthesisultrasound-assisted methodElectrochemical sensing of H2O2 inliving cells [189]MOF-199,MOF-74,MOF-5,MIL-53Cotton In situ cotton-MOF synthesis Antimicrobial activity againstnosocomial bacteria [190]MOF-5 Ag Green and mild method Antibacterial activity [191]Fe(III) metal-organicframeworks PAN Electrospinning Tissue engineering investigations [173]5. ChallengesDuring the past decade, membrane surface engineering has become increasinglypopular due to the use of mussel-inspired surface chemistry. The use of membranes indifferent processes and different membrane preparations have been extensively investigatedand applied, but there are still several key challenges to be overcome in this field, whichSymmetry 2023, 15, 403 14 of 22represent interesting future research opportunities. A common property of such coatingsshould be considered more closely. In membrane fabrication, mussel-inspired coatings mayplay a more diverse role due to their hydrophilicity. Multilayer composite membranes madefrom thin film composite membranes have shown excellent interfacial compatibility whenthey contain mussel-inspired interlayers. In this review, the latest applications of MOFs andmembranes based on them in the biomedical field have been discussed. Because of theiradaptability, excellent surface areas, high porosity, crystallinity, great loading capacities,improved thermal/chemical stability, and variable affinity, MOFs are most commonlyused in biomedicine as multifunctional supports. Biomedical applications for MOF-basedcomposites still face critical challenges despite significant advances in laboratory research.As a first step, toxicity issues regarding MOFs need to be addressed before or during clinicaltrials. The variety of MOF structures, species, sizes, and stabilities, along with the complexenvironment organisms live in, make MOFs toxic not only because of their composition,morphology, size, or stability, but also because of the environments they live in. As a result,a comprehensive assessment of MOF toxicity is necessary. To date, considerable researchhas been conducted on the toxicity of MOF scaffolds, with most experiments focusing onshort-term in vivo or acute toxicity. However, the most important aspect of MOF scaffoldsfor biomedical applications is long-term toxicity, which has rarely been addressed. In vivoor acute toxicity studies of MOFs have been conducted in many excellent studies so far.Despite the critical aspect of long-term toxicity that must be considered if MOF scaffoldsare to be outstanding biomedical candidates, few studies have been conducted to date. Toevaluate MOFs’ toxicity comprehensively, extensive in vivo studies and long-term tissueaccumulation monitoring is urgently needed. A ligand with strong biocompatibility andmetal ion nodes with high biocompatibility can also be used to create functional MOFswhile avoiding toxicity associated with MOFs. Considering the potential properties ofMOFs, their use in the construction of MOF-based membranes has become a promisingoption in the biomedical field. Because the synergism of the properties of MOFs with thecharacteristics of membranes that can be produced from various materials such as polymerscan facilitate the controlled and stable release of drugs. In addition, the use of membranesbased on tissue engineering has paved the way for many treatments. In recent years,advances in nanotechnology and the understanding of biosensors have allowed tissueengineering to be applied to designing organs on chips, conducting clinical trials on chips,using microfluidics, manipulating genetics, and so on, for the puerto decodend repairingdrepairssues. Considering the variety of materials that can be used with MOFs, the fieldof application of these materials in biomedical field is even wider, while among thesematerials, there are plenty of materials that solve problems such as the low biocompatibilityof MOFs. However, due to the novelty of this aspect of 2D materials, there are manyundiscovered applications that need to be investigated.6. Perspective and ConclusionsIn this review, the latest applications of MOFs and membranes based on them in thebiomedical field have been discussed. Because of their adaptability, excellent surface areas,high porosity, crystallinity, great loading capacities, improved thermal/chemical stability,and variable affinity, MOFs are most commonly used in biomedicine as multifunctionalsupports. Biomedical applications for MOF-based composites still face critical challengesdespite significant advances in laboratory research. As a first step, toxicity issues regardingMOFs need to be addressed before or during clinical trials. The variety of MOF structures,species, sizes, and stabilities, along with the complex environment organisms live in, makeMOFs toxic not only because of their composition, morphology, size, or stability, butalso because of the environments they live in. As a result, a comprehensive assessmentof MOF toxicity is necessary. To date, considerable research has been conducted on thetoxicity of MOF scaffolds, with most experiments focusing on short-term in vivo or acutetoxicity. However, the most important aspect of MOF scaffolds for biomedical applicationsis long-term toxicity, which has rarely been addressed. In vivo or acute toxicity studies ofSymmetry 2023, 15, 403 15 of 22MOFs have been conducted in many excellent studies so far. Despite the critical aspectof long-term toxicity that must be considered if MOF scaffolds are to be outstandingbiomedical candidates, few studies have been conducted to date. To evaluate MOFs’toxicity comprehensively, extensive in vivo studies and long-term tissue accumulationmonitoring is urgently needed. A ligand with strong biocompatibility and metal ion nodeswith high biocompatibility can also be used to create functional MOFs while avoidingtoxicity associated with MOFs. Considering the potential properties of MOFs, their usein the construction of MOF-based membranes has become a promising option in thebiomedical field. Because the synergism of the properties of MOFs with the characteristicsof membranes that can be produced from various materials such as polymers can facilitatethe controlled and stable release of drugs. In addition, the use of membranes based ontissue engineering has paved the way for many treatments. In recent years, advances innanotechnology and the understanding of biosensors have allowed tissue engineeringto be applied to designing organs on chips, conducting clinical trials on chips, usingmicrofluidics, manipulating genetics, and so on, for the purpose of decoding etiology andrepairing damaged tissues. Considering the variety of materials that can be used withMOFs, the field of application of these materials in biomedical field is even wider, whileamong these materials, there are plenty of materials that solve problems such as the lowbiocompatibility of MOFs. However, due to the novelty of this aspect of 2D materials, thereare many undiscovered applications that need to be investigated.Author Contributions: S.N.M.N., A.B. and S.M.M. developed the idea and structure of the reviewarticle; S.A.H. and F.V.H. wrote the manuscript and collected the materials from databases; A.G. andM.G.B. revised and improved the manuscript; S.M.M., C.W.L. and W.-H.C. supervised the manuscript.All authors have read and agreed to the published version of the manuscript.Funding: This research work was financially supported by Fundamental Research Grant SchemeFRGS/1/2020/TK0/UM/02/8 (NO.FP023-2020), and Global Collaborative Programme—SATU JointResearch Scheme (No. ST004-2021).Institutional Review Board Statement: Not applicable.Informed Consent Statement: Not applicable.Data Availability Statement: All data generated or analyzed during this study are included in thispublished article.Conflicts of Interest: The authors declare no conflict of interest.References1. 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metal-organic frame works
MOF membrane
drug delivery
cancer therapy
asymmetric membranes
Recent Advances in Metal-Organic Framework (MOF) Asymmetric Membranes/Composites for Biomedical Applications
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