Latest ArticlesNasopharyngeal carcinoma (NPC), a malignant tumor originating from the nasopharynx, is one of the common malignant tumors of the head and neck. There are significant geographical differences in the incidence of nasopharyngeal carcinoma, with a high incidence in China and Southeast Asian countries. Herein, we designed and synthesized a novel near-infrared fluorescent (NIRF) probe to detect glutathione (GSH) in cellular and tumor environments using semi-naphthofluorescein (SNAFL) as the fluorescent molecular backbone and 2-fluoro-4-nitrobenzenesulfonate as the recognition moiety. Upon reaction with GSH, SNAFL-GSH emitted a fluorescence signal, and its emission wavelength at 650 nm was remarkably enhanced. The results of selectivity experiments indicated that SNAFL-GSH was able to discriminate GSH from Cys, Hcy, and H2S. Moreover, SNAFL-GSH could image both endogenous and exogenous GSH and distinguish normal and cancer cells by fluorescence signal difference. At the cellular level, cisplatin (DDP)-induced ferroptosis and inhibition of proliferation of various NPC cell lines (CNE2, CNE1, 5–8F cells) by erastin combined with DDP were visualized with the help of SNAFL-GSH. In a mouse tumor xenograft model, we successfully employed SNAFL-GSH for the evaluation of the efficacy of erastin combined with DDP in the treatment of NPC. More importantly, the probe could image cancerous tissue sections from NPC patients with an imaging depth of approximately 80 µm. It was foreseen that SNAFL-GSH offered great potential for application in the diagnosis and evaluation of the therapeutic efficacy of NPC, and these results would also provide new ideas for the clinical treatment of NPC.
Nanoemulsions are widely used as advanced pharmaceutical delivery systems in biomedical field, due to their high encapsulation efficiency and good therapy efficacy. Nanoemulsification techniques that produce nanoemulsions with controllable sizes and compositions are promising for creating advanced nanoemulsion systems for pharmaceutical delivery. This review summarizes recent advances on low-energy emulsification techniques for producing nanoemulsions, and the use of these nanoemulsions as advanced pharmaceutical delivery systems and as templates to create drug-loaded functional particles for biomedical application. First, nanoemulsification techniques that utilize elaborate interfacial physics/chemistry and micro-/nano-fluidics, featured with relatively-low energy input, to produce nanoemulsions with controllable sizes and compositions, are introduced. Uses of these nanoemulsions to create nanoemulsion-incorporated milli-particles, drug-loaded nanoparticles and nanoparticle-incorporated microparticles with sizes ranging from several millimeters to sub-10 nm are emphasized. Flexible and efficient use of the nanoemulsions, functional nanoparticles and milli-/micro-particles integrated with nanoemulsions or nanoparticles for advanced pharmaceutical delivery in biomedical field are highlighted, with focus on how the interplay between their sizes and compositions achieve desired pharmaceutical-delivery performances. Finally, perspectives on further advances on the controllable production of nanoemulsions are provided.
Due to their excellent fluorescence properties and biological function, cyanine dyes have been widely applied in biological imaging. Heptamethine cyanine (Cy7) dyes, as a type of classic near-infrared (NIR) fluorescent dyes, are considered as one of the effective fluorescent tools in the living organisms due to their good biocompatibility and very low background interference. Bioorthogonal reactions performed in living cells and tissues have developed by leaps and bounds in recent years. The NIR fluorescent labeling technique involving cyanine has attracted widespread attention. This review summarizes their recent application in the field of bioorthogonal imaging, mainly concluding Cy7-type dyes, labeling strategy, bioimaging application, etc. We expect this work can provide some helps for the studies of NIR bioorthogonal reaction in vivo.
Targeting delivery of tumor-associated carbohydrate antigen (TACA)-based vaccine to antigen-presenting cells (APCs) mediated by endogenous antibodies can improve the immunogenicity of TACA. However, an essential requirement of this approach is to generate high titers of endogenous antibodies in vivo through pre-immunization, which complicates the immunization procedure and may cause side effects. Herein, we report a new generation of APC-targeting TACA-based supramolecular complex vaccine, assembled by sialyl Thomsen-nouveau-bovine serum albumin-adamantine (sTn-BSA-Ada) and heptavalent rhamnose (Rha)-modified β-cyclodextrin (β-CD) via host–guest interaction. The complex vaccine retained anti-Rha antibodies recruiting capability and facilitated the APCs uptake of the vaccine via the interaction of the Fc-domain with the Fc receptors on APCs. We demonstrate that direct immunization of complex vaccine elicited anti-Rha and anti-sTn specific immune response synchronously, generating a novel self-enhancement effect that can improve the antigen delivery to APCs in high efficacy. The structure–activity relationship (SAR) study proved that complex vaccine 4 with polyethylene glycol 6 (PEG6) linker in host molecule provoked a robust and specific sTn immune response comparable to the pre-immunization approach. The antisera induced by complex vaccine, either through direct immunization or pre-immunization, exhibited equal potency of cytotoxicity against the sTn expression cancer cells. This study provides a general platform for TACA-based vaccines with self-enhancement effects without the need for pre-immunization.
Improving the performance of all-small-molecule organic solar cells (ASM-OSCs) largely depends on the design and application of novel donors with appropriate crystallinity. Extending molecular conjugation is an effective method for regulating molecular stacking and crystallinity. In this work, we successfully designed and synthesized two novel acceptor-donor-donor-donor-acceptor (A-D-D-D-A) type oligomeric donors with three dithieno[2,3-d:2’,3’-d’]benzo[1,2-b:4,5-b’]dithiophene (DTBDT) as the central unit, named as 3DTBDT-Cl and 3DTBDT, depending on with and without chlorine substitution on the thiophene side chains. We found that the introduction of chlorine atoms makes the blend films display stronger crystallinity but with large-scale phase separation morphology and more defects, which eventually leads to a power conversion efficiency (PCE) of only 10.83%, whereas the blend films based 3DTBDT with appropriate crystallinity achieved 13.74% PCE. Compared with 3DTBDT-Cl/L8-BO, the 3DTBDT/L8-BO films exhibited a nanoscale bi-continuous interpenetrating network morphology with a smaller domain size and more suitable crystallinity, which guarantees the corresponding devices obtained more efficient exciton dissociation, efficient charge transport, reduced bimolecular recombination, and performed more balanced carrier mobility. These results demonstrated that regulating the crystallinity of oligomeric donors to obtain the desired phase separation morphology in the blend films could facilitate further improving the performance of ASM-OSCs.
Enzyme prodrug therapies (EPTs) have been intensively explored as attractive approaches to selective activation of systemically administered benign prodrugs by the exogenous enzymes or enzymes expressed at the desired target site, thus achieving localized, site-specific therapeutic effect. Many effective strategies (e.g., antibody-, viral-, gene-, as well as polymer-directed EPT) have been developed for enzyme localization to locally activate systemically administered benign prodrugs. Nevertheless, intrinsic limitations (e.g., complex intracellular environment and catalyst instability) make the practical application of EPT strategies a task that presents itself as highly challenging. As a promising alternative to natural enzyme, nanozyme has attracted substantial attention since its discovery in 2007, mainly due to the advantages of robust catalytic activity, high stability, low cost, and facile synthesis. Recently, nanozyme-activated prodrug strategies bring a new opportunity for targeted therapy, referred to as nanozyme-activating prodrug therapies. This review focuses on recently reported nanozyme-activated prodrug strategies, aiming to provide some new insights into the potential applications in site-specific drug synthesis.
Passive daytime radiative cooling (PDRC) technology is emerging as one of the most promising solutions to the global problem of spacing cooling, but its practical application is limited due to reduced cooling effectiveness caused by daily wear and tear, as well as dirt contamination. To tackle this problem, we report a novel strategy by introducing a renewable armor structure for prolonging the anti-fouling and cooling effectiveness properties of the PDRC coatings. The armor structure is designed by decorating fluorinated hollow glass microspheres (HGM) inside rigid resin composite matrices. The HGM serve triple purposes, including providing isolated cavities for enhanced solar reflectance, reinforcing the matrices to form robust armored structures, and increasing thermal emittance. When the coatings are worn, the HGM on the surface expose their concave cavities with numerous hydrophobic fragments, generating a highly rough surface that guarantee the superhydrophobic function. The coatings show a high sunlight reflectance (0.93) and thermal emittance (0.94) in the long-wave infrared window, leading to a cooling of 5 ℃ below ambient temperature under high solar flux (~900 W/m2). When anti-fouling functions are reduced, they can be regenerated more than 100 cycles without compromising the PDRC function by simple wearing treatment. Furthermore, these coatings can be easily prepared using a one-pot spray method with low-cost materials, exhibit strong adhesion to a variety of substrates, and demonstrate exceptional environmental stability. Therefore, we anticipate their immediate application opportunities for spacing cooling.
Activated hepatic stellate cells (aHSCs), the main source of extracellular matrix deposition, are key targets in liver fibrosis. However, no effective drug specific to aHSCs has been clinically applied due to poor drug delivery efficiency. Herein, we designed a CXC chemokine receptor 4 (CXCR4)-targeted reactive oxygen species (ROS)-responsive platform AMD-Dex-ROS-responsive-sorafenib (ARS) based on natural polysaccharide and thioctic acid frame, which can deliver anti-fibrosis drug represented by sorafenib specifically to aHSCs on account of CXCR4 over-expression on aHSCs, and smartly disassemble via ROS-responsive thioketal rupture relying on high intracellular ROS in HSCs, realized on-demand drug release and effective liver fibrosis reversion. Notably, in this platform, the CXCR4 antagonist AMD3100 not only enhanced aHSCs targeting efficiency of sorafenib but also effectively magnified the aHSCs elimination of sorafenib by blocking stroma cell derived factor-1 (SDF-1)/CXCR4-induced aHSCs protection, resulting in synergistic anti-fibrosis effect. The platform provided a new approach for drug delivery system design and liver fibrosis treatment.
Calcium dibutyryladenosine cyclophosphate is a widely used cardiovascular drug. The traditional batch synthesis process suffers from long reaction times, tedious operations, and unstable yields. Herein, a sequential continuous flow synthesis combined with a multistage in-line purification process of calcium dibutyryladenosine cyclophosphate was developed. The acylation reaction was completed in a continuous coil reactor at 160 ℃ in 20 min. And the high toxic solvent pyridine was replaced by acetonitrile. Furthermore, the multistage in-line purification process was integrated into the homemade 3D circular cyclone-type micromixer chip. Combining with the membrane phase separators, the residence time of the purification step was 30 s. The isolated yield of this sequential continuous process was 92% with 99% purity.
The efficiency of photocatalytic CO2 reduction reaction (PCRR) is restricted by the low solubility and mobility of CO2 in water, poor CO2 adsorption capacity of catalyst, and competition with hydrogen evolution reaction (HER). Recently, hydrophobic modification of the catalyst surface has been proposed as a potential solution to induce the formation of triple-phase contact points (TPCPs) of CO2 (gas phase), H2O (liquid phase), and catalysts (solid phase) near the surface of the catalyst, enabling direct delivery of highly concentrated CO2 molecules to the active reaction sites, resulting in higher CO2 and lower H+ surface concentrations. The TPCPs thus act as the ideal reaction points with enhanced PCRR and suppressed HER. However, the initial synthesis of triple-phase photocatalysts tends to possess a lower bulk density of TPCPs due to the simple structure leading to limited active points and CO2 adsorption sites. Here, based on constructing a hydrophobic hierarchical porous TiO2 (o-HPT) with interconnected macropores and mesopores structure, we have significantly increased the density of TPCPs in a unit volume of the photocatalyst. Compared with hydrophobic macroporous TiO2 (o-MacPT) or mesoporous TiO2 (o-MesPT), the o-HPT with increased TPCP density leads to enhanced photoactivity, enabling a high methanol production rate with 1111.5 µmol g−1 h−1 from PCRR. These results emphasize the significance of high-density TPCPs design and propose a potential path for developing efficient PCRR systems.
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