Journal of Materials Chemistry B最新文献

The high glutathione (GSH) concentration and insufficient H₂O₂ content in tumor cells strongly constrict the efficacy of Fenton reaction-based chemodynamic therapy (CDT). Despite numerous efforts, it still remains a formidable challenge for achieving satisfactory efficacy using CDT alone. Herein, an intelligent tetrasulfide bond-bridged mesoporous organosilica-based nanoplatform that integrates GSH-depletion, H₂S generation, self-supplied H₂O₂, co-delivery of doxorubicin (DOX) and Fenton reagent Fe²⁺ is presented for synergistic triple-enhanced CDT/chemotherapy/H₂S therapy. Because the tetrasulfide bond is sensitive to GSH, the nanoplatform can effectively consume GSH, leading to ROS accumulation and H₂S generation in the GSH-overexpressed tumor microenvironment. Meanwhile, tetrasulfide bond-induced GSH-depletion triggers the degradation of nanoparticles and the release of DOX and Fe²⁺. Immediately, Fe²⁺ catalyzes endogenous H₂O₂ to highly toxic hydroxyl radicals (˙OH) for CDT, and H₂S induces mitochondria injury and causes energy deficiency. Of note, H₂S can also decrease the decomposition of H₂O₂ to augment CDT by downregulating catalase. DOX elicits chemotherapy and promotes H₂O₂ production to provide a sufficient substrate for enhanced CDT. Importantly, the GSH depletion significantly weakens the scavenging effect on the produced ˙OH, guaranteeing the enhanced and highly efficient CDT. Based on the synergistic effect of triple-augmented CDT, H₂S therapy and DOX-mediated chemotherapy, the treatment with this nanoplatform gives rise to a superior antitumor outcome.

Structural degeneration of a hybrid layer composed of a demineralized dentin matrix (DDM) and adhesive causes unsatisfactory functional outcomes in terms of bonding repair and caries treatment and is accompanied by high prevalence of secondary caries. Clinically, defects in the hybrid layer from insufficient adhesive infiltration, bacterial load from retained infected-dentin, and bacterial attack from the oral cavity are the main threats to degeneration. Currently, there is no strategy to simultaneously address adhesive penetration and bacterial infection. Herein, based on the core role of the strongly-polar hydrated DDM interface in dentin bonding, an interface-reconstructed bonding strategy assisted by electrostatic assembly of broad-spectrum germicidal polyhexamethylene biguanide (PHMB) is proposed that kills two birds with one stone. PHMB is absorbed onto the anionic 3D DDM forming a PHMB/DDM complex. The surface potential of the DDM increases by about 100 mV, the anion content decreases by 20%, and the interface water content decreases by nearly 40%. All of these changes contribute to the penetration of the adhesive, thereby improving the bonding strength and durability. After thermal cycling aging, the bonding strength of the PHMB group was 1.45–1.65 times that of the control group. In terms of antibacterial properties, PHMB treatment not only has a bacterial-killing ability due to the already formed biofilm but also significantly reduces the adhesion of bacteria, thereby delaying the occurrence of secondary caries. In summary, PHMB treatment reconstructed the DDM interface, resulting in a defect-low and inherent antibacterial hybrid layer that improves the bonding effect, treatment of caries and even prevention of secondary caries.

Noninvasive detection of small extracellular vesicles (sEVs) has become one of the most promising liquid biopsy methodologies for effective and timely cancer diagnosis and prognostic monitoring. Currently, accurate and sensitive detection of tumor-derived sEVs is compromised by their heterogeneous nature, and the tissue origin and parent cell cycle change may significantly affect the tumor-associated information (e.g., phenotypic proteins) of sEVs. Accordingly, many of the single-marker dependent detections on sEVs may not provide comprehensive information about the tumor, and their reliability and clinical applicability cannot be guaranteed. Herein, a strategy for constructing AND gate photoluminescence on tumor-derived sEVs is proposed. Briefly, only after co-recognition of the two epithelial phenotypic proteins (EpCAM and MUC1) on tumor-derived sEVs simultaneously, can our designed lanthanide luminescence probe precursors then assemble to form the AND gate for photoluminescence detection. Consequently, the generated AND gate photoluminescence provided time-resolved luminescence for a wide cancerous sEV linear detection range of 6.0 × 10⁴–6.0 × 10⁹ particles per mL, with a calculated detection limitation of 1.42 × 10² particles per mL. Furthermore, the AND gate photoluminescence can significantly distinguish epithelial cancer patients from healthy controls, displaying its great potential for accurate and noninvasive cancer diagnosis.

Traditional cancer therapies no longer meet the current demand for cancer precision therapy and personalized treatment and it's essential to develop new therapeutic modalities as well as to investigate new combination anti-tumor mechanisms. Therefore, amphiphilic prodrug polymer chains linking methoxy poly(ethylene glycol) (mPEG) and cinnamaldehyde (CA) with adipic acid dihydrazide (ADH) as the pH-responsive center were designed and synthesized, which could self-assemble into PAC micelles in aqueous solution. A supramolecular hydrogel was formed based on the host–guest interaction between α-cyclodextrin (α-CD) and PAC micelles. Polyetherimide (PEI) modified copper manganese sulfide nanoenzyme catalysts (PCMS NPs) were prepared by a solvothermal method, which could be uniformly dispersed in the hydrogel to form a composite supramolecular hydrogel (PCMS@PAC/α-CD Gel). Under an acidic tumor environment, pH-responsive hydrazone bonds were broken, resulting in the slow release of CA and the amplification of hydrogen peroxide (H₂O₂) levels. PCMS NPs exerted peroxidase (POD)-like activity and catalase (CAT)-like activity, which could convert H₂O₂ into hydroxyl radicals (˙OH) and oxygen (O₂) to alleviate intra-tumor hypoxia and induce apoptosis, while exerting glutathione oxidase (GPX)-like activity to consume glutathione (GSH) to further enhance the effect of chemodynamic therapy (CDT). Under near-infrared light (NIR) irradiation, PCMS NPs exhibited an excellent photothermal conversion performance, which could rapidly increase the temperature of tumor cells to above 42 °C for photothermal therapy (PTT) and convert O₂ to a superoxide anion (˙O₂⁻) by exerting oxidase (OXD)-like activity for photodynamic therapy (PDT). It was demonstrated by in vitro and in vivo experiments that the PCMS@PAC/α-CD Gel was highly cytotoxic to cancer cells and could effectively inhibit tumor growth, indicating the potential for applications in the fields of biomedicine and smart materials.

Tuberculosis (TB) remains one of the most infectious pathogens with the highest human mortality and morbidity. Biofilm formation during Mycobacterium tuberculosis (Mtb) infection is responsible for bacterial growth, communication, and, most essentially, increased resistance/tolerance to antibiotics leading to higher bacterial persistence. Thus, biofilm growth is presently considered a key virulence factor in the case of chronic disease. Metal–Organic Frameworks (MOFs) have recently emerged as a highly efficient system to improve existing antibiotics' therapeutic efficacy and reduce adverse effects. In this regard, we have synthesized Cu-MOF (IITI-3) using a solvothermal approach. IITI-3 was well characterized by various spectroscopic techniques. Herein, IITI-3 was first encapsulated with isoniazid (INH) to form INH@IITI-3 with 10 wt% loading within 1 hour. INH@IITI-3 was well characterized by PXRD, TGA, FTIR, and BET surface area analysis. Furthermore, the drug release kinetics studies of INH@IITI-3 have been performed at pH 5.8 and 7.4 to mimic the small intestine and blood pH, respectively. The results show that drug release follows first-order kinetics. Furthermore, the antimycobacterial activity of INH@IITI-3 demonstrated significant bacterial killing and altered the structural morphology of the bacteria. Moreover, INH@IITI-3 was able to inhibit the mycobacterial biofilm formation upon treatment and showed less cytotoxicity toward the murine RAW264.7 macrophages. Thus, this work significantly opens up new possibilities for the applications of INH@IITI-3 in biofilm infections in Mtb and further contributes to TB therapeutics.

Correction for ‘Injectable organo-hydrogels influenced by click chemistry as a paramount stratagem in the conveyor belt of pharmaceutical revolution’ by Abhyavartin Selvam et al., J. Mater. Chem. B, 2023, https://doi.org/10.1039/d3tb01674a.

The reasonable structure of aza-BODIPY renders it as an efficient photothermal reagent for photothermal therapy. Herein, we describe the design and synthesis of aza-BODIPY NMeBu with the free rotating tert-butyl group and the dimethylamino-substituted segment to promote the photothermal conversion via the excited state non-radiative transition. NMeBu was found to be the π–π stacking form in the unit cell based on X-ray analysis. NMeBu-NPs by self-assembly possessed a near-infrared absorption (λ_abs = 772 nm), and once activated by near-infrared light, the photothermal efficiency in aqueous solution can reach 49.3%. NMeBu-NPs can penetrate the cell and trigger cell death via the apoptosis pathway under low concentration and low light power irradiation, thereby avoiding dark toxicity. Aza-BODIPY created using this procedure has excellent photothermal efficiency and could serve as a potential candidate for the treatment of cancer cells and tumors.

Porphyrin-based metal–organic frameworks (PMOFs) are a kind of crystal hybrid material with broad application prospects in energy, catalysis, biomedicine, and other fields. In this study, the La-TCPP PMOF nanocrystal was constructed using a porphyrin ligand and La ion. This material can produce a high loading rate on doxorubicin (DOX) owing to its special porous structure. The high loading rate of drug molecules and the reactive oxygen species (ROS) of the porphyrin ligand enable La-TCPP@DOX nanocrystal to produce a powerful killing effect on cancer cells under the synergistic attack of chemotherapy (CT) and photodynamic therapy (PDT). Finally, by modifying the targeted aptamer, the actual therapeutic effect of this special La-TCPP@DOX@Apt material on tumors was confirmed by applying the established mouse tumor model. The composite nanomaterial not only avoids the side effects caused by high concentrations of chemotherapeutic drugs, but also overcomes the limitation of PDT owing to insufficient light penetration and can inhibit and kill solid tumors under the condition of synergistic attack. This study is a complement to PMOF crystal materials, and its tumor-killing ability was achieved by loading drugs and introducing targeting molecules, which proves that the synergistic attack can more effectively inhibit and treat solid tumors. These studies have a reference and guiding significance for the treatment of cancer patients.

Cancer remains the most common lethal disease in the world. Although the treatment choices for cancer are still limited, significant progress has been made over the past few years. By improving targeted drug therapy, drug delivery systems promoted the therapeutic effects of anti-cancer medications. Exosome is a kind of natural nanoscale delivery system with natural substance transport properties, good biocompatibility, and high tumor targeting, which shows great potential in drug carriers, thereby providing novel strategies for cancer therapy. In this review, we present the formation, distribution, and characteristics of exosomes. Besides, extraction and isolation techniques are discussed. We focus on the recent progress and application of exosomes in cancer therapy in four aspects: exosome-mediated gene therapy, chemotherapy, photothermal therapy, and combination therapy. The current challenges and future developments of exosome-mediated cancer therapy are also discussed. Finally, the latest advances in the application of exosomes as drug delivery carriers in cancer therapy are summarized, which provide practical value and guidance for the development of cancer therapy.

Metal–organic gels (MOGs) are a type of functional soft substance with a three-dimensional (3D) network structure and solid-like rheological behavior, which are constructed by metal ions and bridging ligands formed under the driving force of coordination interactions or other non-covalent interactions. As the homologous substances of metal–organic frameworks (MOFs) and gels, they exhibit the potential advantages of high porosity, flexible structure, and adjustable mechanical properties, causing them to attract extensive research interest in the pharmaceutical field. For instance, MOGs are often used as excellent vehicles for intelligent drug delivery and programmable drug release to improve the clinical curative effect with reduced side effects. Also, MOGs are often applied as advanced biomedical materials for the repair and treatment of pathological tissue and sensitive detection of drugs or other molecules. However, despite the vigorous research on MOGs in recent years, there is no systematic summary of their applications in the pharmaceutical field to date. The present review systematically summarize the recent research progress on MOGs in the pharmaceutical field, including drug delivery systems, drug detection, pharmaceutical materials, and disease therapies. In addition, the formation principles and classification of MOGs are complemented and refined, and the techniques for the characterization of the structures/properties of MOGs are overviewed in this review.