Latest ArticlesCyclin-dependent kinases 4 and 6 inhibitors (CDK4/6i) have been demonstrated to trigger antitumor immunity for tumor regression. However, the therapeutic performance of CDK4/6i-meadiated cancer immunotherapy was impaired by the immunosuppressive tumor microenvironment (ITM) due to overexpression of programmed death ligand 1 (PD-L1) on the surface of cancer cell membrane. To improve the immunotherapeutic performance of CDK4/6i, we herein developed endosomal acid-activatable micelleplex for siRNA delivery and PD-L1 knockdown in the tumor cells in vitro and in vivo. We further demonstrated that the combination of PD-L1 knockdown and CDK4/6 inhibition facilitated intratumoral infiltration of cytotoxic T lymphocytes (CTLs), and elicited protective immune response and efficiently suppressed tumor growth in vivo. This study revealed the importance of molecular design of the micelleplex for highly efficient siRNA delivery, which might provide a novel insight for RNAi-based cancer immunotherapy.
A novel diselenide-containing crown ether (BC7Se2) was fabricated, which can polymerize to form cyclic oligomers through intermolecular dynamic covalent reaction by irradiation of visible light. The size and distribution of oligomers are related to the monomer concentration. The decomposition reaction of oligomers is controlled by topology and solvents. Furthermore, potassium cation can inhibit the polymerization of BC7Se2 and accelerate the decomposition of oligomers.
An efficient and eco-friendly protocol for synthesizing difluoromethylated oxindoles through a visible-light induced one-pot tandem reaction of N-arylacrylamides, difluoroacetic acid and PhI(OAc)2 was developed. This reaction proceeded in the absence of any additive, base, metal-catalyst and external photosensitizer, using cheap and easily available CHF2CO2H as the difluoromethylation reagent and bulk biomass-derived 2-MeTHF as the sole solvent. 26 Examples of N-arylacrylamide substrates were investigated, and all of them successfully underwent difluoromethylation to deliver the target products in good to excellent yields.
The sensitive and rapid detection of blood glucose is very important for monitoring and managing diabetes. Herein, a fluorescent/magnetic bimodal sensing strategy is proposed for glucose detection using a multifunction-responsive nanocomposite (MoS2 QDs-MnO2 NS). MoS2 QDs act as fluorescent probes, and MnO2 nanosheets are used as both quenchers and recognizers in this sensing platform. In the presence of glucose-mediated enzyme product (H2O2), MnO2 nanosheet is etched, thus releasing MoS2 QDs and Mn2+ ions, which causes the significantly enhancement of fluorescent and magnetic signals. Furthermore, MoS2 QDs-MnO2 NS-based fluorescent test paper is constructed for H2O2 sensing with the naked eyes. Under optimal conditions, the dual linear ranges of 20-300 μmol/L and 40-250 μmol/L toward glucose detection are obtained for the fluorescent and magnetic mode, respectively. Furthermore, this bimodal assay exhibits good reproducibility and acceptable accuracy in glucose detection of clinical samples, demonstrating great versatility and flexibility of multifunctional probes in glucose detection.
The flourishing development in flexible electronics has provoked intensive research in flexible strain sensors to realize accurate perception acquisition under different external stimuli. However, building hydrogel-based strain sensors with high stretchability and sensitivity remains a great challenge. Herein, MXene nanosheets were composited into polyacrylamide-sodium alginate matrix to construct mechanical robust and sensitive double networked hydrogel strain sensor. The hydrophilic MXene nanosheets formed strong interactions with the polymer matrix and endowed the hydrogel with excellent tensile properties (3150%), compliant mechanical strength (2.03 kPa−1 in Young's Module) and long-lasting stability and fatigue resistance (1000 dynamic cycles under 1, 600% strain). Due to the highly oriented MXene-based three dimensional conductive networks, the hydrogel sensor achieved extremely high tensile sensitivity (18.15 in gauge factor) and compression sensitivity (0.38 kPa−1 below 3 kPa). MXene hydrogel-based strain sensors also displayed negligible hysteresis in electromechanical performance, typical frequent-independent feature and rapid response time to external stimuli. Moreover, the sensor exhibited accurate response to different scales of human movements, providing potential application in speech recognition, expression recognition and handwriting verification.
Photocatalytic water splitting utilizing solar energy is considered as one of the most ideal strategies for solving the energy and environmental issues. Recently, two-dimensional (2D) materials with an intrinsic dipole show great chance to achieve excellent photocatalytic performance. In this work, blue-phase monolayer carbon monochalcogenides (CX, X = S, Se) are constructed and systematically studied as photocatalysts for water splitting by performing first-principles calculations based on density functional theory. After confirming the great dynamical, thermal, and mechanical stability of CX monolayers, we observe that they possess moderate band gaps (2.41 eV for CS and 2.46 eV for CSe) and high carrier mobility (3.23 × 104 cm2 V-1 s-1 for CS and 4.27 × 103 cm2 V-1 s-1 for CSe), comparable to those of many recently reported 2D photocatalysts. Moreover, these two monolayer materials are found to have large intrinsic dipole (0.43 D for CS and 0.51 D for CSe), thus the build-in internal electric field can be selfintroduced, which can effectively drive the separation of photongenerated carriers. More importantly, the well-aligned band edge as well as rather pronounced optical absorption in the visible-light and ultraviolet regions further ensure that our proposed CX monolayers can be used as high efficient photocatalysts for water splitting. Additionally, the effects of external strain on the electronic, optical and photocatalytic properties of CX monolayers are also evaluated. These theoretical predictions will stimulate further work to open up the energy-related applications of CX monolayers.
Red emissive carbon dots (CDs) powder was synthesized on a large scale from phloroglucinol and boric acid by a novel solid state reaction with yield up to 75%. This method is safe and convenient, for it needs neither high pressure reactors nor complicated post-treatment procedures. The as-prepared carbon dots powder exhibited strong red fluorescence with excitation-independent behavior. XPS measurement and PL spectra suggest that such red fluorescence arise from boron-doped structures in CDs, which increases along with the boron concentration on CDs surface but decreases when the concentration quenching effect takes place. To overcome the aggregation induced fluorescence quenching of the solid CDs powder, the conventional methods are dispersing CDs into a large amount of inert substrates. But our present work provides a new strategy to realize strong red fluorescence of CDs in solid state. As a result, such carbon dots powder works well for latent fingerprint identification on various material surfaces.
The rapid development of internet and internet of things brings new opportunities for the expansion of intelligent sensors, and acetone as a major disease detection indicator (i.e., diabetes) making it become extremely important clinical indicator. Herein, uniform mesoporous ZnO spheres were successfully synthesized via novel formaldehyde-assisted metal-ligand crosslinking strategy. In order to adjust the pore structure of mesoporous ZnO, various mesoporous ZnO spheres were synthesized by changing weight percentage of Zn(NO3)2·6H2O to tannic acid (TA). Moreover, highly active heterojunction mesoporous ZnO/Co3O4 has been fabricated based on as-prepared ultra-small Co3O4 nanocrystals (ca. 3 nm) and mesoporous ZnO spheres by flexible impregnation technique. Profit from nano-size effect and synergistic effect of p-n heterojunction, mesoporous ZnO/Co3O4 exhibited excellent acetone sensing performance with high selectivity, superior sensitivity and responsiveness. Typically, 5 wt% Co3O4 embedded mesoporous ZnO sphere showed prominent acetone response (ca. 46 for 50 ppm), which was about 11.5 times higher than that in pure ZnO sensing device, and it was also endowed high cyclic stability. The nanocrystals embedded hybrid material is expected to be used as promising efficient material in the field of catalysis and gas sensing.
The construction of nanostructured ion-transport channels is highly desirable in the design of advanced electrolyte materials, as it can enhance ion conductivity by offering short ion-transport pathways. In this work, we present a supramolecular strategy to fabricate a nanocomposite electrolyte containing highly ordered lamellar proton-conducting nanochannels, by the electrostatic self-assembly of a polyoxometalate H3PW12O40 (PW) and a comb copolymer poly(4-methlstyrene)-graft-poly(N-vinyl pyrrolidone). PW can effectively regulate the self-assembling order of polymer moieties to form a large-range lamellar structure, meanwhile, introducing protons into the nanoscale lamellar domains to build proton transport channels. Moreover, the rigid PW clusters contribute a remarkable mechanical reinforcement to the nanocomposites. The lamellar nanocomposite exhibits a conductivity of 4.3×10-4 S/cm and a storage modulus of 1.1×107 Pa at room temperature. This study provides a new strategy to construct nanostructured ion-conductive pathways in electrolyte materials.
The high specific capacitance along with good cycling stability are crucial for practical applications of supercapacitors, which always demands high-performance and stable electrode materials. In this work, we report a series of ternary composites of CoO-ZnO with different fractions of reduced graphene oxide (rGO) synthesized by in-situ growth on nickel foam, named as CZG-1, 2 and 3, respectively. This sort of binder-free electrodes presents excellent electrochemical properties as well as large capacitance due to their low electrical resistance and high oxygen vacancies. Particularly, the sample of CZG-2 (CoO-ZnO/rGO 20 mg) in a nanoreticular structure shows the best electrochemical performance with a maximum specific capacitance of 1951.8 F/g (216.9 mAh/g) at a current intensity of 1 A/g. The CZG-2-based hybrid supercapacitor delivers a high energy density up to 45.9 Wh/kg at a high power density of 800 W/kg, and kept the capacitance retention of 90.1% over 5000 charge-discharge cycles.
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