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Osteoarthritis (OA) is the most prevalent chronic joint disorder and is a major cause of disability among the elderly population. The degeneration and damage of articular cartilage associated with OA can result in a diminished range of motion in joints, subsequently impacting fundamental activities such as ambulation, standing, and grasping objects. In severe cases, it may culminate in disability. Traditional pharmacological treatments are often accompanied by various side effects, while invasive surgical procedures increase the risk of infection and thrombosis. Consequently, identifying alternative new methods for OA treatment remains a formidable challenge. With advancements in responsive hydrogel drug delivery platforms, an increasing number of strategies have emerged to enhance OA treatment protocols. Injectable response hydrogel drug delivery platforms show many advantages in treating OA, including improved biocompatibility, prolonged drug release duration, elevated drug loading capacity and enhanced sensitivity. This article reviews the recent progress of injectable responsive hydrogel drug delivery platform for OA treatment over the past few years. These innovative methodologies present new strategies and directions for future OA treatment while summarizing a series of challenges faced during the clinical transformation of injectable response hydrogel drug delivery platforms. Overall, injectable responsive hydrogel drug delivery platforms show great potential in treating OA, especially regarding improving drug retention time and stimulus-responsive release at the lesion sites. These innovative methods provide new hope for future OA treatment and point the way for clinical applications. [ABSTRACT FROM AUTHOR]

Four-dimensional printing refers to a process through which a 3D printed object transforms from one structure into another through the influence of an external energy input. Self-folding structures have been extensively studied to advance 3D printing technology into 4D using stimuli-responsive polymers. Designing and applying self-folding structures requires an understanding of the material properties so that the structural designs can be tailored to the targeted applications. Poly(N-iso-propylacrylamide) (PNIPAM) was used as the thermo-responsive material in this study to 3D print hydrogel samples that can bend or fold with temperature changes. A double-layer printed structure, with PNIPAM as the self-folding layer and polyethylene glycol (PEG) as the supporting layer, provided the mechanical robustness and overall flexibility to accommodate geometric changes. The mechanical properties of the multi-material 3D printing were tested to confirm the contribution of the PEG support to the double-layer system. The desired folding of the structures, as a response to temperature changes, was obtained by adding kirigami-inspired cuts to the design. An excellent shape-shifting capability was obtained by tuning the design. The experimental observations were supported by COMSOL Multiphysics® software simulations, predicting the control over the folding of the double-layer systems. [ABSTRACT FROM AUTHOR]

In cancer therapy, it is essential to selectively release cytotoxic agents into the tumor to prevent the adverse effects associated with anticancer drugs. Thus, in this study, a stimuli-sensitive polymer–drug conjugate was synthesized for selective drug release. Doxorubicin (DOX) and docetaxel (DTX) were conjugated onto novel poly(jasmine lactone) based copolymer via a thioketal (TK) linker. In addition, a photosensitizer (chlorin e6) was attached to the polymer, which served as a reactive oxygen species generator to cleave the TK linker. The conjugate is readily self-assembled into micelles less than 100 nm in size. Micelles demonstrate a notable increase in their ability to cause cell death when exposed to near-infrared (NIR) light on MDA-MB-231 breast cancer cells. The increase in cytotoxicity is higher than that observed with the combination of free DOX and DTX. The accumulation of DOX in the nucleus after release from the micelles (laser irradiation) was also confirmed by confocal microscopy. In the absence of light, micelles did not show any toxicity while the free drugs were found toxic irrespective of the light exposure. The obtained results suggest the targeted drug delivery potential of micelles regulated by the external stimuli, i.e., NIR light. [ABSTRACT FROM AUTHOR]

Monoolein cubic phase incorporating poly(dimethylaminoethyl methacrylate-co-phenyl vinyl sulfide) (P(DMAEMA-co-PVS)) and indocyanine green (ICG, a photosensitizer) was prepared as a multiple-responsive carrier. P(DMAEMA-co-PVS), prepared by a free radical polymerization, was air/water interface-active and it exhibited lower critical solution temperature (LCST). The polymer increased in its LCST by H2O2 treatment, possibly because of the hydrolytic detachment of DMAEMA pendant, evidenced by 1H NMR and FT-IR spectroscopy. Water channels surrounded by lipid matrix, characteristic of cubic phase, was observed on TEM photos and the inclusion of the additives (e.g., P(DMAEMA-co-PVS) had little effect on the structure. The cubic phases increased their thermal stability upon the inclusion of the polymer chains and they maintained their integrity once the temperature was kept below 60 °C, supported by the polarized optical microscopy and the differential scanning calorimetry. The release of a cargo (i.e., fluorescent dextran) was suppressed at body temperature (37 °C) at the H2O2 concentration of normal tissue (e.g., 0.000002%), possibly due to an entangled network structure formed by the thermally induced inter/intramolecular hydrophobic interaction of the polymer chains. The release was markedly promoted at the H2O2 concentration of tumor tissue (e.g., 0.0034%), possibly because the thermally induced hydrophobic interaction can be weakened by the hydrolytic degradation. In addition, the release was significantly enhanced by NIR irradiation. The cubic phase would be used as a drug carrier which releases its payload at a target site in a selected manner in answering to H2O2 and NIR irradiation. [ABSTRACT FROM AUTHOR]

Hydrogels comprise of a group of crosslinked hydrophilic polymeric materials which are capable of absorbing and holding large quantities of water in their three-dimensional network structure without undergoing dissolution. More importantly, the ability of 'smart' hydrogels to respond to certain environmental changes e.g. pH, heat, light, magnetic field, biomolecules have set them apart as a unique class of materials. A combination of several such useful and unique properties have resulted in a tremendous progress toward development of advanced hydrogel-based materials, as is evident from an explosive amount of research publications available in this area over the last few decades. Owing particularly to their biocompatibility and biodegradability, hydrogels have become a material of prime importance in context to a wide range of applications starting from simple contact lenses to more complex ones e.g. in tissue repair, drug delivery, sensors, 3D bioprinting, soft robotics and agriculture. This review includes i) an overview of hydrogels and its classifications based on source, structure, crosslinking mechanism and stimuli responsiveness, ii) detailed discussion on some of the most advanced research works being carried out in the field over the last few years in context to few smart applications that have become the need of the hour, particularly in the domain of biomedical applications. [ABSTRACT FROM AUTHOR]

This work demonstrates our effort to develop stimuli responsive cellulose films for the detection of dimethyl amines, a biogenic amine, released during food decomposition. Herein, we demonstrate that thin layer deposition of polydiacetylene‐zinc oxide nanosheets (PDA‐ZnO) on cellulose (CE) paper yields a stimuli responsive strip exhibiting strong thermochromism and solvatochromism against dimethyl amine. The incorporation of Zn nanoclusters within the composite plays an essential role in achieving reversible thermochromism while strong intermolecular interactions promote adsorption of PDA‐ZnO on cellulose paper. X‐ray diffraction and infrared spectroscopy reveal that the Zn2+ ions intercalate with PDA bilayer and strongly interact with the carboxylate headgroup of PDA. Furthermore, the reversible thermochromism persist when the nanosheets are deposited on cellulose (CE) paper when assembling PDA‐ZnO−CE paper. In addition, PDA‐ZnO−CE displayed selective solvatochromism allowing the utilization of the paper in the detection of dimethyl amine as it displayed a distinct and remarkable purple to orange colour transition. In particular, the response of the PDA‐ZnO−CE paper in several other organic solvents was poor as no transitions were observed hence its selectivity towards dimethylamine. In conclusion, the incorporation of PDA‐ZnO on cellulose paper is a step forward towards designing of a stimuli responsive packaging material that can detect biogenic amines released during food decomposition thereby preventing food poisoning. [ABSTRACT FROM AUTHOR]

Osteoarthritis (OA) is the most prevalent chronic joint disorder and is a major cause of disability among the elderly population. The degeneration and damage of articular cartilage associated with OA can result in a diminished range of motion in joints, subsequently impacting fundamental activities such as ambulation, standing, and grasping objects. In severe cases, it may culminate in disability. Traditional pharmacological treatments are often accompanied by various side effects, while invasive surgical procedures increase the risk of infection and thrombosis. Consequently, identifying alternative new methods for OA treatment remains a formidable challenge. With advancements in responsive hydrogel drug delivery platforms, an increasing number of strategies have emerged to enhance OA treatment protocols. Injectable response hydrogel drug delivery platforms show many advantages in treating OA, including improved biocompatibility, prolonged drug release duration, elevated drug loading capacity and enhanced sensitivity. This article reviews the recent progress of injectable responsive hydrogel drug delivery platform for OA treatment over the past few years. These innovative methodologies present new strategies and directions for future OA treatment while summarizing a series of challenges faced during the clinical transformation of injectable response hydrogel drug delivery platforms. Overall, injectable responsive hydrogel drug delivery platforms show great potential in treating OA, especially regarding improving drug retention time and stimulus-responsive release at the lesion sites. These innovative methods provide new hope for future OA treatment and point the way for clinical applications.

Nanotechnology-enabled pesticide delivery systems have been widely studied and show great prospects in modern agriculture. Nanodelivery systems not only achieve the controlled release of agrochemicals but also possess many unique characteristics. This study presents the development of a pH-responsive pesticide nanoformulation utilizing hollow mesoporous silica nanoparticles (HMSNs) as a nanocarrier. The nanocarrier was loaded with the photosensitive pesticide prochloraz (Pro) and then combined with ZnO quantum dots (ZnO QDs) through electrostatic interactions. ZnO QDs serve as both the pH-responsive gatekeeper and the enhancer of the pesticide. The results demonstrate that the prepared nanopesticide exhibits high loading efficiency (24.96%) for Pro. Compared with Pro technical, the degradation rate of Pro loaded in HMSNs@Pro@ZnO QDs was reduced by 26.4% after 24 h ultraviolet (UV) exposure, indicating clearly improved photostability. In a weak acidic environment (pH 5.0), the accumulated release of the nanopesticide after 48 h was 2.67-fold higher than that in a neutral environment. This indicates the excellent pH-responsive characteristic of the nanopesticide. The tracking experiments revealed that HMSNs can be absorbed by rice leaves and subsequently transported to other tissues, indicating their potential for effective systemic distribution and targeted delivery. Furthermore, the bioactivity assays confirmed the fungicidal efficacy of the nanopesticide against rice blast disease. Therefore, the constructed nanopesticide holds great prospect in nanoenabled agriculture, offering a novel strategy to enhance pesticide utilization. [ABSTRACT FROM AUTHOR]

Cancer therapy currently focuses on personalized targeted treatments. A promising approach uses stimuli-responsive biomaterials for site-specific drug release, such as pH- and redox-triggered polymer nanocomposites. These materials respond to the tumor microenvironment, enhance efficacy, and reduce off-target effects. Cancer cells with anomalous properties such as acidic cytosolic pH and elevated redox potential are targeted by these biomaterials. An imbalance in ions and biological thiols in the cytoplasm contributes to tumor growth. Functionalized polymer nanocomposites with large surface areas and specific targeting outperform conventional small-molecule materials. To overcome problems such as low bioavailability, uncontrolled drug release, and poor cell penetration, multifunctional nanomaterials make it easier for drugs to enter certain cellular or subcellular systems. High therapeutic efficacy is achieved through surface functionalization, site-specific targeting, and the use of stimuli-responsive components. In particular, pH and redox dual-stimuli-based polymeric nanocomposites for cancer therapeutics have scarcely been reported. This article provides recent progress in pH- and redox-responsive polymer nanocomposites for site-specific drug delivery in cancer therapy. It explores the design principles, fabrication methods, mechanisms of action, and prospects of these dual-stimuli-responsive biomaterials. [ABSTRACT FROM AUTHOR]

Abstract Smart molecules have attracted increasing attention due to their transformative role in creating the next generation of smart structures and devices. Smart bistable coordination complexes are a class of functional complexes which have two stable states that can be reversibly switched in response to external stimuli. Such bistable molecules play a vital role in various applications, such as sensors, data storage, spintronics, smart windows, optical switches, information encryption and decryption, displays, actuators, etc. Herein, the recent research studies into the development of these smart bistable metal coordination complexes are reviewed. According to the different external stimuli, these smart bistable coordination systems have been classified and summarized, including light‐responsive systems, thermally‐responsive systems, electrically‐responsive systems, mechanically‐responsive systems, and some other cases. These systems are further subdivided according to the changes in signals (e.g., color, fluorescence, spin state, crystalline phase) under external stimuli. The design principles of each type of smart bistable metal complexes as well as their broad and innovative applications are comprehensively described. Finally, the challenges and opportunities in this field are briefly analyzed and discussed.

Abstract Chirality is a fundamental property in nature, which is essential for the existence and survival of living organisms. Smart responsive chiroptical materials have garnered increasing attention due to their unique structural characteristics and potential applications. Among these, azobenzene (Azo), as a typical photoresponsive chromophore, plays a crucial role in constructing and controlling chiral structures. The unique cis‐trans isomerization, liquid crystallinity, and other physicochemical properties allow for a wide range of tunability in stimuli‐responsive chiroptical materials. Herein, we review the research studies in the field of chiral/achiral Azo building blocks for multilevel chiral generation as well as chiral switching, and summarize the recent advances on the applications of the chiral Azo structures from micro to macro levels. Finally, we aim to provide an overview of the potential challenges and new research opportunities for the development of novel smart responsive chiroptical materials.

In cancer therapy, it is essential to selectively release cytotoxic agents into the tumor to prevent the adverse effects associated with anticancer drugs. Thus, in this study, a stimuli-sensitive polymer–drug conjugate was synthesized for selective drug release. Doxorubicin (DOX) and docetaxel (DTX) were conjugated onto novel poly(jasmine lactone) based copolymer via a thioketal (TK) linker. In addition, a photosensitizer (chlorin e6) was attached to the polymer, which served as a reactive oxygen species generator to cleave the TK linker. The conjugate is readily self-assembled into micelles less than 100 nm in size. Micelles demonstrate a notable increase in their ability to cause cell death when exposed to near-infrared (NIR) light on MDA-MB-231 breast cancer cells. The increase in cytotoxicity is higher than that observed with the combination of free DOX and DTX. The accumulation of DOX in the nucleus after release from the micelles (laser irradiation) was also confirmed by confocal microscopy. In the absence of light, micelles did not show any toxicity while the free drugs were found toxic irrespective of the light exposure. The obtained results suggest the targeted drug delivery potential of micelles regulated by the external stimuli, i.e., NIR light.

Addressing the challenge of poor wound healing in chronic wounds remains complex, as the underlying physiological mechanisms are still not fully understood. Traditional wound dressings often fail to meet the specific needs of the chronic wound healing process. Recently, considerable interest has shifted toward employing biomacromolecule-based smart wound dressings to facilitate wound healing. These stimuli-responsive dressings have undergone substantial development to manage local drug delivery, demonstrating promising therapeutic effects in treating chronic wound defects. They have displayed improved drug release profiles both in vitro and in vivo. Recently, there have been advancements in the development of innovative dual and multi-stimuli responsive dressings that react to combinations of signals including pH-temperature, pH-enzyme, pH-ROS, pH-glucose, pH-NIR, and multiple stimuli. This paper offers an in-depth review of recent progress in responsive wound dressings based on biomacromolecules, with a specific focus on their design, drug release capabilities, and therapeutic advantages. [ABSTRACT FROM AUTHOR]

Bilirubin (BR) is among the most potent endogenous antioxidants that originates from the heme catabolic pathway. Despite being considered as a dangerous and cytotoxic waste product at high concentrations, BR has potent antioxidant effects leading to the reduction of oxidative stress and inflammation, which play an important role in the development and progression of cancer. The purpose of this study is to introduce PEGylated BR nanoparticles (NPs), themselves or in combination with other anti-cancer agents. BR is effective when loaded into various nanoparticles and used in cancer therapy. Interestingly, BRNPs can be manipulated to create stimuli-responsive carriers providing a sustained and controlled, as well as on-demand, release of drug in response to internal or external factors such as reactive oxygen species, glutathione, light, enzymes, and acidic pH. This review suggests that BRNPs have the potential as tumor microenvironment-responsive delivery systems for effective targeting of various types of cancers. [Display omitted] [ABSTRACT FROM AUTHOR]

Spinal cord injury (SCI) is a debilitating condition that can result in significant functional impairment and loss of quality of life. There is a growing interest in developing new therapies for SCI, and hydrogel-based multimodal therapeutic strategies have emerged as a promising approach. They offer several advantages for SCI repair, including biocompatibility, tunable mechanical properties, low immunogenicity, and the ability to deliver therapeutic agents. This article provides an overview of the recent advances in hydrogel-based therapy strategies for SCI repair, particularly within the past three years. We summarize the SCI hydrogels with varied characteristics such as phase-change hydrogels, self-healing hydrogel, oriented fibers hydrogel, and self-assembled microspheres hydrogel, as well as different functional hydrogels such as conductive hydrogels, stimuli-responsive hydrogels, adhesive hydrogel, antioxidant hydrogel, sustained-release hydrogel, etc. The composition, preparation, and therapeutic effect of these hydrogels are briefly discussed and comprehensively evaluated. In the end, the future development of hydrogels in SCI repair is prospected to inspire more researchers to invest in this promising field. Various types of hydrogels, including phase-change hydrogels, self-healing hydrogel, oriented fibers hydrogel, and self-assembled microspheres hydrogel, as well as different functional hydrogels such as conductive hydrogels, stimuli-responsive hydrogels, are employed as biological scaffolds, combined with stem cells, exosomes, and neurotrophic factors, in the treatment of SCI. [Display omitted] [ABSTRACT FROM AUTHOR]

Ionic liquids (ILs) play a crucial role in the design of novel materials. The ionic nature of ILs provides numerous advantages in drug delivery, acting as a green solvent or active ingredient to enhance the solubility, permeability, and binding efficiency of drugs. They could also function as a structuring agent in the development of nano/micro particles for drug delivery, including micelles, vesicles, gels, emulsion, and more. This review summarize the ILs and IL-based gel structures with their advanced drug delivery applications. The first part of review focuses on the role of ILs in drug formulation and the applications of ILs in drug delivery. The second part of review offers a comprehensive overview of recent drug delivery applications of IL-based gel. It aims to offer new perspectives and attract more attention to open up new avenues in the biomedical applications of ILs and IL-based gels. [Display omitted] • Discussion on the classification and properties of ionic liquids, along with their key roles in drug formulation. • Identification of the properties and applications of ionic liquids and ionogels in various delivery methods. • Exploration of the classification, preparation, processing methods, and biomedical characteristics of ionogel. • Highlighting the challenges associated with ionic liquids and ionogels in drug delivery. [ABSTRACT FROM AUTHOR]

α-cyanostilbene derivatives, known as AIE molecules, have the potential to serve as optical recorders and vapor sensor by altering the molecular aggregation and / or stacking models. Despite the significant scientific and technological importance of the correlation between molecular stacking modes and modulated optical properties, relevant research remains scarce. Herein, two thermodynamically stable crystalline phase (BCr and GCr) were found for a biphenyl-based cyanostilbenic compound, DSB-SQ , condensed from its solution. Uniquely, the BCr demonstrated reversible mechanochromism and irreversible thermalchromism, whereas GCr remained unaffected by exposure to light, heat, grinding, etc. The discoloration process was correlated with the variation of local dipole coupling modes during the phase transition, leading to a significant change in π-π overlap and delocalization of excited states. Finally, the BCr was doped with polyvinyl alcohol (PVA) to prepare a composite membrane with dynamic information storage and encryption function. [Display omitted] [ABSTRACT FROM AUTHOR]

The design of novel drug delivery systems is exceptionally critical in disease treatments. Among the existing drug delivery systems, mesoporous silica nanoparticles (MSNs) have shown profuse promise owing to their structural stability, tunable morphologies/sizes, and ability to load different payload chemistry. Significantly, the presence of surface silanol groups enables functionalization with relevant drugs, imaging, and targeting agents, promoting their utility and popularity among researchers. Stimuli-responsive silanol conjugates have been developed as a novel, more effective way to conjugate, deliver, and release therapeutic drugs on demand and precisely to the selected location. Therefore, it is urgent to summarize the current understanding and the surface silanols' role in making MSN a versatile drug delivery platform. This review provides an analytical understanding of the surface silanols, chemistry, identification methods, and their property-performance correlation. The chemistry involved in converting surface silanols to a stimuli-responsive silica delivery system by endogenous/exogenous stimuli, including pH, redox potential, temperature, and hypoxia, is discussed in depth. Different chemistries for converting surface silanols to stimuli-responsive bonds are discussed in the context of drug delivery. The critical discussion is culminated by outlining the challenges in identifying silanols' role and overcoming the limitations in synthesizing stimuli-responsive mesoporous silica-based drug delivery systems., (© 2023 The Authors. Small published by Wiley‐VCH GmbH.)

Objective: To design and evaluate a matrix metalloproteinase 9 (MMP-9)-responsive hydrogel for vital pulp therapy., Methods: A peptide linker with optimized sensitivity toward MMP-9 was crosslinked with 4-arm poly (ethylene glycol)-norbornene (PEG-NB) by thiol-norbornene photo-polymerization. This resulted in the formation of a hydrogel network in which the peptide IDR-1002 was incorporated. Hydrogel characterization and gelation kinetics were examined with Fourier-transform infrared spectroscopy, scanning electron microscopy, rheological testing, and swelling evaluation. Hydrogel degradation was examined through multiple exposure to pre-activated MMP-9, to simulate flare-ups of dental pulp inflammation. The IDR-1002 released from degraded hydrogels was measured with high-performance liquid chromatography. Effect of IDR-1002 released from hydrogels on one-week-old multispecies oral biofilms was evaluated using confocal laser scanning microscopy., Results: MMP-9-responsive, injectable, and photo-crosslinkable hydrogels were successfully synthesized. When hydrogel degradation and release of IDR-1002 were examined with exposure to pre-activated MMP-9, IDR-1002 release was significantly correlated with elevated levels of MMP-9 (p < 0.05). The effectiveness of IDR-1002 in killing bacteria in multispecies oral biofilms was significantly enhanced when the hydrogels were immersed in 10 nM or 20 nM pre-activated MMP-9, compared to immersion in phosphate-buffered saline (p < 0.05)., Conclusions: The MMP-9-responsive hydrogel is a promising candidate for on-demand delivery of bioactive agent in vital pulp therapy., Clinical Significance: MMP-9 is one of the most important diagnostic and prognostic biomarkers for pulpitis. An MMP-9-responsive hydrogel has potential to be used as an in-situ on-demand release system for the diagnosis and treatment of dental pulp inflammation., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Published by Elsevier Ltd.)

[Display omitted] The advent of 3D printing technology in the 1980s enabled the fabrication of patient-specific products with precise shape, size, and complexity. A variety of 3D printing techniques, such as direct ink writing by extrusion, particle fusion printing, light-induced printing, volumetric bioprinting, and inkjet printing, have been explored recently for the purpose of developing desired 3D printed objects. Among these techniques, direct ink writing has been used extensively due to its affordability, ease of use, potential for scaling up, and faster speed. This approach saves time and resources while allowing for the flexible use of various materials. The lack of a variety of varied printing inks, however, continues to be an impediment to its widespread commercial use. Owing to their quick gelling behaviour, extrudability, and shape fidelity, injectable hydrogels have become interesting alternatives for printing inks. Hydrogel inks can be developed by either natural or synthetic polymers, or a combination of the both, to achieve the desired rheological and mechanical properties utilizing various strategies of crosslinking and incorporation of nanoparticles like nanoclay, bioactive glass, graphene oxide and silica nanoparticles. Further, various stimuli responsive hydrogel inks responding to various external stimuli (such as temperature, pH, magnetic field) can be developed to prepare engineered biostructures that can be used in healthcare sector. This review provides a spotlight on recent advancement in developing hydrogel inks and their different physicochemical aspects for developing desired engineered biostructures. Finally, we discuss the opportunities of 4D printing, current difficulties and future prospects for hydrogel inks-based 3D printing to emphasize the significant scope for future innovations. [ABSTRACT FROM AUTHOR]