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The application of nanomaterials in intelligent drug delivery is developing rapidly for treatment of cancers. In this paper, we fabricated a new kind of protease/redox/pH stimuli-responsive biodegradable nanohydrogels with methacrylic acid (MAA) as the monomer and N,N-bis(acryloyl)cystamine (BACy) as the cross-linker through a facile reflux-precipitation polymerization. After that, the polyethylene glycol (PEG) and folic acid (FA) were covalently grafted onto the surface of the nanohydrogels for enhancement of their long in vivo circulation lifetime and active targeting ability to the tumor cells and tissues. This kind of nanohydrogels could be disassembled into short polymer chains (Mn < 1140; PDI < 1.35) both in response to glutathione (GSH) through reduction of the sensitive disulfide bonds and protease by breakage of the amido bonds in the cross-linked networks. The nanohydrogels were utilized to simultaneously load both hydrophilic drug doxorubicin (DOX) and hydrophobic drug paclitaxel (PTX) with high drug loading efficiency. The cumulative release profile showed that the drug release from the drug-loaded nanohydrogels was significantly expedited by weak acidic (pH 5.0) and reducing environment (GSH), which exhibited an distinct redox/pH dual stimuli-responsive drug release to reduce the leakage of drugs before they reach tumor site. In addition, the in vitro experiment results indicated that the multidrug-loaded system had synergistic effect on cancer therapy. Meanwhile, the acute toxicity and intravital fluorescence imaging studies were adopted to evaluate the biocompatibility and biotoxicity of the nanohydrogels, the experimental results showed that the PEG modification could greatly enhance the long in vivo circulation lifetime and reduce the acute toxicity (LD50: from 138.4 mg/kg to 499.7 mg/kg) of the nanohydrogels.
In this work, a multifunctional ratiometric fluorescence (FL) nanohybrid (CSCDs@DC) was synthesized from chitosan based carbon dots (CSCDs) and dansyl chloride (DC) at room temperature. The CSCDs@DC revealed strong FL intensity, great stability and excellent anti-photobleaching properties. Herein, CSCDs@DC was responsive to pH value in the range of 1.5–4.0 and exhibited color-switchable FL properties between acidic and alkaline environments. In addition, CSCDs@DC showed good selectivity and sensitivity towards Fe3+ ions. A good linear relationship for the Fe3+ ion detection was obtained in the range from 0 μM to 100 μM, with a detection limit of 1.23 μM. What's more, CSCDs@DC can be used as a fluorescent ink. It expressed superior optical properties after 3 months of storage or continuous exposure to UV light for 24 h. This study suggested that CSCDs@DC had potential in the detection of pH and metal ions, as well as showing promising application in the anti-counterfeiting field.
Diabetes, particularly Type 2 Diabetes Mellitus (T 2 DM), is a chronic metabolic disorder with high and increasing global prevalence, characterized by insulin resistance and inadequate insulin secretion. Despite advancements in novel drug delivery systems, widespread and systematic treatment of advanced glycation end products (AGEs) remains challenging due to issues like drug toxicity, low water solubility, and uncontrolled release. Thus, developing nanoplatforms with controlled release capabilities has become a major research focus. Due to its excellent biocompatibility and drug delivery properties, chitosan has attracted considerable attention as a typical biopolymer. In this study, we designed and synthesized an intelligent fluorescence-pH sensitive nanopolymer material using chitosan. We loaded drug 1 and chromium phthalocyanine (CrPc) into folic acid-conjugated carboxymethyl chitosan (FA-CMCS) nanocarriers, forming FA-CMCS@1-CrPc. Comprehensive characterization of FA-CMCS@1-CrPc was conducted using Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), thermal gravimetric analysis (TGA), and gas adsorption analysis (BET). The results indicate that the nanomaterial was successfully synthesized and exhibits excellent specific surface area, biocompatibility, and fluorescence response. Further research revealed that FA-CMCS@1-CrPc not only achieved controlled drug release but also could regulate drug release by adjusting pH. Additionally, due to its strong fluorescence performance, the nanomaterial demonstrated higher detection sensitivity, especially for monitoring the release of 5% trace drugs. An in vitro model of insulin-resistant cells was established to evaluate the effects of the drug delivery system on glucose degradation and AGE-RAGE regulation, providing a foundation for the development of new T 2 DM drugs. Graphical Abstract
In this study, well-defined double-hydrophilic triblock copolymers , consisting of hydrophilic poly(ethylene glycol) (PEG) and hydrophobic poly( N , N -diethylamino-2-ethylmethacrylate) (PDEAEMA), were synthesized and characterized. The molecular weights of the copolymers were controllable. In the basic environments, the copolymers can self-assemble into the PDEAEMA core and PEG corona micelles in aqueous solution with an average size of 40–180 nm. The low critical micelle concentration (CMC, about 10 − 3 mg mL − 1 ) of copolymers investigated in pH 7.4 aqueous solution confirmed the adequate thermodynamic stability of their self-assembly. As shown in the cytotoxicity assay, the copolymers have good biocompatibility. Doxorubicin (DOX) was encapsulated into the triblock copolymer micelles . The drug loading efficiency and entrapment efficiency values of DOX-loaded micelles reached 8.14% and 88.6%, respectively. The DOX release of the drug-loaded micelles depends on the pH values. These phenomena indicated that the double-hydrophilic PDEAEMA – PEG – PDEAEMA triblock copolymers have a potential application in the drug delivery.
Currently, smart and functional textiles have attracted increasing attention for the research on their application in various fields. In this paper, perfluorooctyltriethoxysilane (FAS13)-loaded silica nanocapsules taken as the Pickering emulsifier was applied to stabilize O/W emulsion for obtaining pH-responsive dual-compartmental microcapsules which show a strawberry-like structure with jasmine essence as the core and pH-responsive polymers and silica nanocapsules as the shell. These microcapsules could endow it with multifunctions by functionalizing the fabric, while the preparation and functionalization process is effortless and environmental friendly. Not only does the treated fabric demonstrate the self-healing superhydrophobicity and ultraviolet (UV) resistance because of the hydrophobic FAS13 getting loaded into silica nanocapsules and the surface modification of UV absorbent, it is also capable of the pH control jasmine essence-releasing performance, which allows over 40% of the fragrance to be preserved for three months through the controlled release of jasmine essence from the microcapsules.
As a new kind of drug carries, pH-sensitive liposomes have been widely studied in tumor therapy for their advantages of target ability and sustained-release. Here, we synthesized a pH-sensitive material, N-(3-Aminopropyl)imidazole-cholesterol (IM-Chol) and prepared a novel pH-sensitive liposomes using IM-Chol and phosphatidylcholine . IM-Chol was synthesized through amidation reaction between the amino group of N-(3-Aminopropyl)imidazole and acyl chloride group of cholesteryl chloroformate in a weak base solution. Optimal conditions to prepare liposomes were obtained by the orthogonal experiment with the higher encapsulation efficiency as the evaluation indicator. The properties of liposomes, such as particle size, zeta potential , morphology, encapsulation efficiency, drug release behavior and in vitro cell toxicity were evaluated by transmission electron microscopy (TEM), dynamic light scattering (DLS) and MTT assay respectively. The results showed that the average particle size of IM-Chol liposomes was 141 nm (PDI 0.323). Liposomes can assemble into uniform spheres at pH 7.4, but under the condition of pH 5.0, the spherical structure of IM-Chol liposomes was broken, exhibiting pH-sensitive property. In vitro drug releasing studies demonstrated the controlled-release behavior of the curcumin (CUR) in the IM-Chol liposomes. The cumulative release of CUR reached to 72.5% in the first 24 h at pH 5.0, faster than that at pH 7.4, which confirmed that the drug carrier displayed pH-sensitive release behaviors. In addition, the MTT assay was employed to test the cytotoxicity of IM-Chol liposomes and CUR IM-Chol liposomes. All cell viabilities were greater than 80% after incubating for 24 h, even up to the highest dose of 500 mg/L, indicating that IM-Chol liposomes had good biocompatibility . The tumor inhibitory results towards EC109 cells of free CUR and CUR-loaded IM-Chol liposomes indicated that IM-Chol liposomes indeed enhanced the cell killing effect of CUR. These results showed that the novel IM-Chol liposomes prepared in this paper had pH-sensitive property and were expected to play a huge potential in tumor treatment.
As a typical biofilm disease, dental caries is a public healthcare problem and high sugar diets increase the risk of dental caries. Cationic nanomaterials play an important role in targeting and removing of biofilms, but their negative effects on normal cells have always caused widespread concern. In this work, pH-triggered charge-switching nanoparticles (SC&CS NPs) with selectable targeting were skillfully constructed by electrostatic adsorption and chemical cross-linking of sodium caseinate (SC) and chitosan (CS) to develop functional foods. SC&CS NPs were negatively charged and stable at pH 7.4. Once encountering in acidic microenvironment below pH 5.7, the potential of SC&CS NPs converted to positive. Based on this property, SC&CS NPs could identify the infected sites of biofilms to selectively target bacteria, while not interacting with cells in the normal physiological environment, thereby avoiding damage to normal cells. Besides, SC&CS NPs were excellent delivery systems that could effectively encapsulate bioactive ingredients with high loading efficiency (12.16 ± 0.04%) and release bioactive ingredients on demand. Moreover, after being encapsulated by SC&CS NPs, the antibacterial and anti-biofilm activities of bioactive ingredients were significantly improved. The charge-switching nanomaterials are expected to provide a safer, more effective, and smarter strategy for functional foods.
The development of stimuli-responsive materials with the ability of controllable oil/water separation is crucial for practical applications. Here, a novel pH responsive nonfluorine-containing copolymer was designed. The copolymer together with silica can be dip-coated on different materials including cotton fabric, filter paper, and polyurethane foam. The coated materials exhibit switchable superhydrophilicity and superhydrophobicity and can be applied in continuous separation of oil/water/oil three phase mixtures, different surfactant stabilized emulsion (oil-in-water, water-in-oil, and oil-in-acidic water) as well as oil uptake and release via in situ and ex situ pH change. We expect that the coatings highlight the practical applications because of the cost-effective preparation process and fluorine-free strategy.
Alaska pollock proteins (PPs) are aquatic proteins with a compact structure, which leads to poor solubility and limited application in food industries. This study explored the structural assembly and gelation behavior of the PP-soluble aggregates prepared by the refolding processing of acidic (pH 1.5–7) or alkaline (pH 12–7) pH-shifting treatment. PPs refolded at alkali pHs produced more soluble aggregates than at acid pHs. Lots of myosin heavy lights (MHCs) could interact with actin to form soluble aggregates at high pH rather than low pH. When shifting back to pH 7, the solubility of alkaline-shifted PPs was boosted to over 60% with a more flexible structure, while acidic-shifted PPs showed reduced solubility (29%) with increased rigidity. Molecular characteristics results indicated that alkaline-shifted PPs comprising MHCs and actin exhibited higher surface hydrophobicity and sulfhydryl groups. These structural modifications induced by alkaline pH-shifting contributed to improving the gelling, emulsifying and foaming properties of PPs. Intriguingly, both acidic- and alkaline-shifted PPs showed a retarded digestive behavior. These novel insights may be adaptable to other animal proteins for modulating the protein structure-functionality, expanding their applications in food industries.
Real-time monitoring of the lysosomal microenvironment using small-molecule probes is critical for understanding the complex interactions between organelles and diseases associated with lysosomal dysfunction. Most traditional fluorescent-dye-based lysosome probes rely on the protonation of the nitrogen atom in the morpholine unit to visualize the lysosomal microenvironment by inhibiting the photoinduced electron transfer (PET) effect. However, these probes often face selectivity issues within the complex cellular microenvironment. For instance, classic hemicyanine dyes (HD) show nonspecific fluorescence responses in the liver due to inappropriate pKa value, leading to low imaging contrast and the risk of false positives. Herein, a series of novel pH/viscosity-activatable, lysosomal-targeted near-infrared (NIR) fluorescent probes were developed by incorporating naphthalimide dye with hemicyanine dyes. These probes exhibit no fluorescence at physiological pH and weak fluorescence under acidic conditions (key 1), with substantial fluorescence activation triggered by abnormal viscosity in pathological tissues (key 2). Notably, NpCy-4 demonstrated a superior signal-to-background ratio (SBR) for cellular imaging and proved effective for real-time in situ diagnosis of acute gastritis.
A smart and environmentally friendly pesticide system was developed that could respond to environmental stimuli while mitigating environmental risks. In this study, thiabendazole (Thi), an effective fungicide, was loaded onto zeolitic imidazolate framework-8 (ZIF-8) using the impregnation method to fabricate a pH-responsive nano hybrid delivery system (Thi@ZIF-8). The results demonstrated that Thi@ZIF-8 had a rhombic dodecahedral morphology and a loading capacity of approximately 25%. Notably, the amount of Thi released from Thi@ZIF-8 at a pH of 5.0 reached 79.54%, which was higher than that at pH 7.0 and 9.0, for 251 h. Such pH-responsive release characteristics of Thi@ZIF-8 were probably related to the pH-dependent structure stability of ZIF-8. The release mechanism of Thi@ZIF-8 conformed to non-Fickian diffusion. Additionally, Thi@ZIF-8 showed a higher control efficacy againstB. cinereacompared with Thi alone. Importantly, the ZIF-8 carrier could effectively reduce the leaching loss of Thi in soil and showed no negative effects on the three varieties of tomato seedlings, implying good biocompatibility. This work provides a novel and eco-friendly approach to control B. cinerea effectively that has great potential in modern sustainable agriculture.
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