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• W2078656392 abstract "NanomedicineVol. 8, No. 2 EditorialFree AccessNanohydrogels as a prospective member of the nanomedicine familyZhi-Yong Qian, Shao-Zhi Fu & Si-Shen FengZhi-Yong QianState Key Laboratory of Biotherapy, West China Hospital, West China Medical School, Sichuan University, Chengdu, 610041, PR ChinaSearch for more papers by this author, Shao-Zhi FuState Key Laboratory of Biotherapy, West China Hospital, West China Medical School, Sichuan University, Chengdu, 610041, PR ChinaSearch for more papers by this author & Si-Shen Feng* Author for correspondenceDepartment of Chemical & Biomolecular Engineering, National University of Singapore, Block E5, 02–11, 4 Engineering Drive 4, Singapore 117576, Singapore. Search for more papers by this authorEmail the corresponding author at chefss@nus.edu.sgPublished Online:8 Feb 2013https://doi.org/10.2217/nnm.13.1AboutSectionsPDF/EPUB ToolsAdd to favoritesDownload CitationsTrack CitationsPermissionsReprints ShareShare onFacebookTwitterLinkedInRedditEmail Keywords: anticancer drugbiodegradable polymerdrug deliverydrug formulationdrug targetingnanobiotechnologyMolecular biomaterials, such as synthetic or natural biodegradable polymers, are the material basis of nanomedicine [1]. Among them, hydrophilic polymers, such as poly(ethylene glycol) (PEG), can be crosslinked to form a hydrogel, which is a 3D network that may absorb water in quantities from a few percent to thousands of times their dry weight. The amount of expansion is determined by the number of crosslinked molecules and the type of composite hydrophilic polymers or copolymers. Hydrogels can be either physical (reversible) gels, when the networks are held together by molecular entanglements and/or secondary forces including ionic or hydrophobic forces, or chemical (permanent) gels, when they are covalently crosslinked networks. Since the 1960s, hydrogels have had wide applications in biomedical engineering, especially in local drug delivery and tissue engineering for tissue repair and regeneration [2]. Recently, nanohydrogels, in other words hydrogel nanoparticles in the nanometer scale from tens to hundreds of nanometers, have become a member of great potential in the nanomedicine family. Among the various nanomedicine formulations, nanohydrogels have shown great advantages for delivery of hydrophilic small-molecule drugs and protein/peptide therapeutics due to their huge loading capacity of water-soluble compounds. Nanohydrogels combine the advantages of hydrogels and nanoparticles for drug formulation and delivery, which include controllable drug release, high stability in physiological media, distinct responsiveness to environmental factors such as pH and temperature, high cellular uptake due to the endocytosis mechanisms, long half-life in circulation by appropriate surface modification (to escape from recognition by the reticuloendothelial system) and drug targeting by conjugation of ligand onto the surface of hydrogel nanoparticles to aim the corresponding biomarkers that are overexpressed in the cancer cell membrane. In the past decade, nanohydrogels have been under intensive investigation as a versatile tool for the delivery of advanced biological therapeutics such as proteins, peptides and carbohydrates. Even for oligonucleotides, a few attempts have been made for the delivery of siRNA [3–6].Physical hydrogels and their biomedical applications have been intensively investigated in recent years. Fang et al. fabricated a honokiol (HK) nanoparticles loaded thermosensitive PEG-poly(ε-caprolactone) (PCL)-PEG (PECE) hydrogel (HK-hydrogel), and demonstrated that such a hydrogel composite has outstanding therapeutic effects on malignant pleural effusion. Compared with the use of HK nanoparticles alone, blank hydrogel or normal saline, the HK-hydrogel system has distinct advantages in reducing the number of pleural tumor foci, prolonging survival time and inhibiting angiogenesis of pleural tumors [7]. Yang et al. also found that the thermosensitive PECE hydrogel has a notable efficacy in preventing post-surgical abdominal adhesions [8]. Additionally, Fu et al. tried to enlarge the application of PECE hydrogel in the bone tissue engineering field. Nano-hydroxyapatite or acellular bone matrix were incorporated into a PECE hydrogel to form an injectable thermoresponse nano-hydroxyapatite or acellular bone matrix/PECE hydrogel composite [9].Chemical hydrogels are commonly water-swollen networks of hydrophilic homopolymers or copolymers. They can be prepared by crosslinking water-soluble polymers or by conversion of hydrophobic polymers to hydrophilic polymers plus crosslinking to form a network. Normally, the biodegradability, swelling properties, elasticity and hydrophilicity of chemical hydrogels can be easily tailored by simply changing the synthetic parameters, such as block length, monomer ratio, crosslinker ratio and other factors (e.g., time of heating and illumination). Park et al. fabricated the biodegradable elastic hydrogel scaffolds based on hydrophilic PEG and hydrophobic PCL and investigated them as a delivery vehicle for rabbit chondrocytes for the formation of neocartilage [10]. Wang et al. prepared a biodegradable pH-sensitive poly(caprolactone-methylacrylic acid-ethylene glycol) hydrogel based on PCL, PEG and methylacrylic acid through UV-initiated free radical polymerization, and a pH-sensitive hydrogel composed of methoxyl PEG-PCL-acryloyl chloride [11]. In order to improve the biodegradability of thermoresponse copolymers, a variety of polyester blocks, such as PCL, poly(D, L-lactic acid-co-glycolic acid) (PLGA) and poly(L-lactic acid) (PLLA), have been successfully introduced into the polymer backbones to form various biodegradable di- or tri-block polyester–polyether-based copolymers [12,13].Nanohydrogels can be made by various self-assembly nanoparticle technologies such as solvent emulsion, diffusion and precipitation methods. Nanohydrogels possess the advantages of both hydrogels (i.e., a high loading ratio and high encapsulation efficiency in formulation of hydrophilic diagnostic and therapeutic agents) and nano-sized drug carriers (i.e., high cellular uptake due to the bulky size, which is suitable for internalization by the cells via endocytosis). In the process of endocytosis, the nanoparticles detach a small disk of bilayer from the cell membrane by sacrificing their surface energy to provide the edge energy of the disk, which is then converted to the bending energy to allow the bilayer disk to be curved to envelope the nanoparticles and bring them into the cytoplasm. It has been shown by experiments, theoretical analysis and computer simulation that nanoparticles of 100–200 nm in size could have the highest cellular uptake efficiency. Therefore, it is easy to understand that nanoparticles that are too small may not have sufficient surface energy to overcome the bending energy needed for endocytosis. Moreover, too small nanoparticles would result in low drug encapsulation efficiency and fast drug release kinetics [14]. The effect of size on cellular uptake of nanoparticles was confusing for many years. It was not until recently that the optimal size of nanoparticles for cellular drug delivery was shown to be 100–200 nm in diameter, which was concluded by experimental measurement, theoretical analysis by membrane mechanics and thermodynamics [15–17]. Endocytosis as a transportation mechanism has much higher efficiency than individual drug molecules for crossing the cell membrane. In fact, the bilayer membrane is a physical barrier to stop hydrophilic molecules from getting into cells. Nanohydrogels thus have all the advantages of other types of nanoparticles, such as micelles, liposomes, dendrimers, solid lipid nanoparticles and nanoparticles of biodegradable polymers, regarding efficient cellular delivery of diagnostic and therapeutic agents. Moreover, nanohydrogels are especially suitable for efficient delivery of hydrophilic small-molecule drug, as well as biological drugs such as therapeutic proteins and peptides.Nanohydrogels, especially those sensitive to environmental changes, such as pH, temperature and other stimuli, have been under intensive investigation due to their great potential [18,19]. Lim et al. used a new injectable bone morphogenic proteins-loaded alginate nanohydrogel to enhance osteoblastic growth and differentiation of human bone marrow stromal cells [20]. Hong et al. used amine-terminated PEG thin films on silicon substrates to generate PEG nanohydrogels, which can bind different proteins covalently to create multifunctional surfaces for applications in emerging bio/proteomic and sensor technologies [21]. Additionally, the most popular temperature-sensitive nanohydrogels based on poly(N-isopropylacrylamine) (PNIPAAm) have gathered great interest. PNIPAAm hydrogels are known for their reversible swelling–deswelling behavior in response to temperature changes. When the temperature of their aqueous solution is below their lower critical solution temperature, nanohydrogels can keep in a state of swelling and have the ability to circulate within the bloodstream. However, the nanohydrogels become hydrophobic, aggregate easily and deposit in heated tissues when the temperature increases [22]. The temperature sensitivity is due to the unique amphiphilic structure of the main monomer NIPA. The thermally targeted behavior gives the ability to use PNIPAAm nanohydrogel as a thermally targeted carrier for the delivery of genes or drugs, especially for anticancer drugs. It is well known that tumors usually have a higher temperature than surrounding tissue, particularly in the peripheral region of the tumor, owing to the higher metabolic rates of growing tumor cells compared with those of normal tissues. Thus, anti-tumor drugs or diagnostic agents can be loaded in a smart nanohydrogel system and then released at hyperthermic tumor sites through the passive targeted behavior and intelligently thermal-responsive properties of the nanohydrogel. Therefore, diagnosing tumors in their early stage, and monitoring and prognosing therapy processes can be achieved. More importantly, a smaller amount of drug will be necessary to obtain a therapeutic effect, and the severe side effects due to systemic administration can be reduced [19]. Some researchers have carried out very important work on the applications of NIPA-based nanohydrogels into intelligently controlled drug release systems. For example, the group led by Gu prepared thermally responsive poly(N-isopropylacrylamide-co-acrylamide) nanohydrogels by free radical precipitation polymerization, and used in vivo florescence imaging on S180 tumor-bearing denuded mice with or without hyperthermia treatment to evaluate the thermally targeted behavior of the nanohydrogels [22]. In vivo noninvasive optical imaging of near-infrared organic dye encapsulated in nanohyrogel and anti-tumor efficacy of docetaxel-loaded nanohydrogel is also studied in their other works [23].The most common method of PNIPAAm nanohydrogel synthesis is the free radical polymerization of NIPAAm in water in the presence of different additives, such as surfactants, stabilizers and crosslinkers, under emulsion polymerization conditions [20]. However, the use of surfactants or crosslinkers may cause the widely acknowledged concerns about biocompatibility and toxicity. Therefore, in order to avoid the presence of surfactants but retain colloidal stability of PNIPAAm nanohydrogels, Mendrek et al. prepared new core-shell nanohydrogels with a crosslinked PNIPAAm core and hydrophilic poly(glycidol) shell under additive-free conditions [24]. This work provides a beneficial foundation for designing and synthesis of novel PNIPAAm-based nanohydrogels with good biocompatibility and less toxicity. Other types of nanohydrogels responsive to stimuli, such as pH and light, as well as nanohydrogels for siRNA delivery, ligand conjugation for targeting and diagnostic imaging can be found in the recent literature [25–28].Financial & competing interests disclosureThis work was supported by the Singapore–China Cooperative Research Project between the Agency of Science, Technology and Research (A*STAR), Singapore, and Chinese Ministry of Science and Technology (MOST; R-398-000-077-305); and the NUS FSF grant R-397-000-136-731 and FRC grant R-397-000-136-112). The authors have no other relevant affiliations or financial involvement with any organization or entity with a financial interest in or financial conflict with the subject matter or materials discussed in the manuscript apart from those disclosed.No writing assistance was utilized in the production of this manuscript.References1 Zhang ZP, Tan SW, Feng SS. Vitamin E TPGS as a molecular biomaterial for drug delivery. Biomaterials33(19),4783–4974 (2012).Crossref, Medline, Google Scholar2 Hoffman AS. Hydrogels for biomedical applications. Adv. Drug Deliv. Rev.54,3–12 (2002).Crossref, Medline, CAS, Google Scholar3 Kabanov AV, Vinogradov SV. Nanogels as pharmaceutical carriers: finite networks of infinite capabilities. Angew. Chem. Int. Ed. Engl.48(30),5418–5429 (2009).Crossref, Medline, CAS, Google Scholar4 Hamidi M, Azadi A, Rafiei P. Hydrogel nanoparticles in drug delivery. Adv. Drug Deliv. Rev.60,1638–1649 (2008).Crossref, Medline, CAS, Google Scholar5 Oishi M, Nagasaki Y. 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The authors have no other relevant affiliations or financial involvement with any organization or entity with a financial interest in or financial conflict with the subject matter or materials discussed in the manuscript apart from those disclosed.No writing assistance was utilized in the production of this manuscript.PDF download" @default.
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