Latest ArticlesExploring the therapeutic effect of single atom catalysts beyond reactive oxygen species (ROS) modulation would boost the prosperity of nanomedicine in cancer treatment. Autophagy as a vital therapy target offers new options for the control of renal cell carcinoma (RCC) progression. Herein, Fe single atom-decorated graphene oxide (Fe1-GO) nanosheet is developed to be a feasible autophagy inducer in RCC treatment. With the well-dispersed O−Fe1−O active sites, Fe1-GO kills ACHN cells effectively but maintains acceptable cytotoxicity to the normal podocyte and HK2 ones. In-depth analyses ascribe the inhibition of ACHN cells to the upregulated autophagy instead of the commonly known catalytic ROS generation. The in vivo therapeutic effect of Fe1-GO nanomedicine is also validated by the RCC-bearing BALB/c mice model, realizing an 89% reduction of tumor weight and good biosafety. This work provides new insights into the design of autophagy regulators as well as potential therapeutic strategies for RCC treatment.
Introducing heavy halogen atoms into organic small molecules is a practical strategy for efficient singlet oxygen (1O2) generation. Generally, bromine or iodine atoms are introduced on the aza-boron-dipyrromethene (aza-BODIPY) core, rather than on the periphery aryl rings for efficient 1O2 generation. Herein, an aza-BODIPY dye NBDPBr with unexpected bromination on the periphery aryl rings was synthesized for photoacoustic (PA) imaging-guided synergistic photothermal therapy (PTT) and photodynamic therapy (PDT) in tumor cells. Owing to unexcepted bromination at the periphery aryl rings, NBDPBr demonstrated an outstanding singlet oxygen quantum yield of 66% which was superior to similar brominated photosensitizers previously reported. After encapsulation with amphiphilic polymer F-127, hydrophilic NBDPBr nanoparticles (NPs) were fabricated and exhibited an excellent photothermal conversion efficiency (η) of 43.0% under 660 nm photoirradiation. In vivo PA imaging results demonstrated that NBDPBr NPs could specifically accumulate at tumor sites and realized the maximum tumor retention at 7 h post-injection. All the in vitro and in vivo results indicated the significant potence of NBDPBr with unexpected bis-bromination for PA imaging-guided synergetic PDT/PTT.
Elevated level of hypochlorous acid (HClO) is closely associated with cancer development. Identifying HClO level in cancer cells would provide important evidence in either early-stage cancer diagnostics or monitoring of its treatment efficiency. In this work, a new pyronine-based fluorescent probe for rapid and sensitive detection of HClO was developed by condensing meso–formyl pyronine (PyCHO) with 2-hydrazinopyridine to form meso–pyridylhydrazone-functionalized pyronine PyHP, PyHP is nonfluorescent due to the excited-state C=N isomerization nonradiative decay, whereas the HClO-triggered formation of meso–triazolopyridyl pyronine PyTP abolishes the C=N isomerization and thus greatly enhances the fluorescence. With the probe, the cancer cells/tumor were distinguished with high-contrast from normal ones by laser confocal fluorescence imaging, and the tumor-to-normal (T/N) ratios obtained exceed the clinically acceptable threshold of 2.0. Moreover, its capability of in vivo imaging tumor was also demonstrated. These results indicate the potential of PyHP as an effective tool in the early clinical diagnosis of cancers.
Lead-halide perovskites exhibit outstanding performance in X-ray detection due to their intrinsic features such as high charge carrier mobility, large atomic number, and long carrier lifetime, but the toxicity of lead is regarded as the major factor hindering their development. Here, we introduce organic molecule (R)-(-)-2-methylpiperazine (R-MPz) into the bismuth-based structure to synthesize lead-free (R)-(H2MPz)BiI5 (R-MBI). The high-quality centimeter-sized single crystals have been obtained, which show a low dark current and superior environmental stability. Particularly, the single-crystal device of R-MBI exhibits a high μτ product up to 1.88 × 10−4 cm2/V and a low trap density of 1.21 × 1010 cm−3. Further, the detector displays excellent detection sensitivity of 263.58 µC Gyair−1 cm−2 and a favorable low detection limit of 4.35 µGyair/s, both of which meet the requirement for medical diagnostics. These findings shed light on the exploration of innovative bismuth-based hybrid perovskites for high-performance X-ray detection.
The combination of horseradish peroxidase (HRP) and a fluorescence substrate has been attracting great interests in developing sensitive biochemical analysis and immunoassays. 10-Acetyl-3,7-dihydroxyphenoxazine (ADHP or Amplex red) is the most sensitive fluorogenic substrate known for HRP in current market, however, it suffers from some drawbacks, such as non-specific reactivity to carboxylesterase and limited fluorescence stability. In the present study, a novel HRP substrate 10-cyclopropylcarbonyl-dichloro-dihydroxyphenoxazine (AR-2), has been prepared, which exhibited improved sensitivity than ADHP in sensing HRP. Moreover, the fluorescence of AR-2/HRP demonstrated improved tolerance to physiological relevant pH fluctuation as compared to ADHP/HRP. Successful detection of uric acid/urate oxidase reaction indicated excellent application prospect of AR-2/HRP for monitoring H2O2-generating biochemical reactions. More interestingly, an enzyme-linked immunosorbent assay (ELISA) using AR-2 as the fluorescence reporter has been successfully used in detecting IgG against severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) from human serum samples. Overall, AR-2 exhibits improved performances over the commercial ADHP, which will be an ideal alternative to ADHP in HRP-based fluorescence biochemical analysis and immunoassays.
Heterogeneous reaction of mineral aerosols and atmospheric polluting gases play an important role in atmospheric chemistry. In this study, the reactions of NO2 with or without SO2 mixture gas on the surface of α-Fe2O3 particles under dry conditions were studied. The effects of sodium dodecyl sulfate (SDS) and the heterogeneous reaction under both dark and UV irradiation conditions were investigated. The infrared spectrum analyzed by the two-dimensional correlation spectroscopy (2D-COS) was used to obtain the products formation sequences. The results showed that UV irradiation can promote the production of nitrate. The 2D-COS analysis indicated SDS changed the sequence order of nitrate and nitrite species during reactions. In oxidation conditions, the final product of heterogeneous reaction of NO2 and α-Fe2O3 was monodentate nitrate. Only the heterogenous reaction of NO2 and α-Fe2O3 containing SDS (FOS) without UV light, the final product was bidentate nitrate. SDS was the catalysis agent supply and photoresist to the system. With surface active compounds, the environmental lifetime of heterogeneous reactions between trace gases and aerosols extends. Surfactants, ultraviolet light, and the types of gases involved in the reaction all have complex effects on the aerosol aging process. This study provided a reference for subsequent heterogeneous reaction studies and the formation of aerosols.
Carbon dots (CDs) with precise targeting function show great potential in the field of drug delivery therapeutics. In this study, the functionalized nucleus-targeting orange-emissive CDs with nuclear localization sequence (NLS) were loaded with adriamycin (DOX) to obtain a nucleus-targeting orange-emissive CDs drug delivery system (CDs-NLS-DOX), which delivered DOX to tumor cell nuclei to enhance its anti-tumor activity. The drug carrier orange-emissive CDs showed excitation-independent behavior, stable and enhanced imaging capability and good biocompatibility in vitro and in vivo. Meanwhile, the CDs-NLS could target the nuclei efficiently, and the CDs-NLS-DOX complexes had a high drug loading rate (59.4%) after loading DOX, exhibiting pH-dependent DOX release behavior through breaking acylhydrazone bond in a weak acidic environment. In addition, the CDs-NLS-DOX complexes exhibited an enhanced killing activity against human hepatoma cells (HepG2). The in vivo therapeutic effects on HepG2 nude mice transplanted tumors indicated the CDs-NLS-DOX had a stronger ability to inhibit tumor growth compared to free DOX. In short, CDs-NLS-DOX is expected to be a precise and efficient nucleus-targeting nano-drug delivery system for tumor treatment.
Membrane-based separation is a promising technology to eliminate water impurities from the oil phase. However, it remains a great challenge to separate water from highly emulsified viscous oil owing to the high stability of the water droplets in oil. Herein we report a surface wettability engineering on an alumina ceramic membrane to achieve an efficient separation of a water-in-oil (W/O) emulsion. Silanes with different carbon chain lengths and fluorinated status were introduced to endow the alumina membrane with different surface wettabilities. While all the modified membranes exhibited excellent separation of the W/O without Span 80 (surfactant), the one with amphiphobic wettability and lowest surface energy failed to separate the Span 80 stabilized W/O. The presence of Span 80 reduced the interfacial tension of water droplets, making them easier to deform and penetrate the modified membrane with the lowest surface energy. It reveals that engineering proper surface wettability is the key to separating the oil and water phases. Besides, the modified membranes maintained decent separation performance and stability under long-term run separation of the emulsified W/O.
The efficient conversion of CO2 into hydrocarbon fuels (CH4) with high selectivity is considered as a great challenge in photocatalysis owing to the multiple-electron transfer pathway and competitive H2 generation. Herein, we developed carbon dots (CDs)-modulated S-scheme heterojunction of CDs/NiAl-LDH@In2O3 (C-DH@IN) through a facile in-situ hydrothermal method. Thanks to the multi-shell nanotube structure, the C-DH@IN shows an enhanced CH4 evolution rate of 10.67 µmol h−1 g−1 and higher selectivity of CH4 (85.70%) compared with In2O3 and NiAl-LDH@In2O3 binary catalyst in the pure water without sacrificial agent. Electron spin resonance (ESR) and in situ Fourier transform infrared spectra verify that the constructed S-scheme heterojunction can possess the strong redox capability and the HCOO− and CH3O− as critical intermediates play an important role in selective CO2 reduction to generate CH4. Furthermore, CDs with superior photoabsorption can boost the electron transfer and absorb H+, thus improving the integration of H+ and CO2 molecule. Therefore, this work emphasizes a facile strategy to achieve efficient CO2-to-CH4 conversion based on construction of CDs-based heterojunction catalysts.
Single atom catalysts (SACs) have been in the forefront of catalysts research because of their high efficiency and low cost and provide new ideas for development of renewable energy conversion and storage technologies. However, the relationship between the intrinsic properties of materials such as lattice thermal conductivity and catalysis remains to be explored. In this work, the lattice thermal conductivity of BN and graphene was calculated by ShengBTE. In addition, the adsorption properties of 3d-TM (TM = V, Cr, Mn, Fe, Co, Ni) on BN and graphene were investigated using first-principles methods, and it was found that Ni atom can form relatively stable SACs compared to other TMs. The molecular dynamics (MD) simulation and migration barrier of Ni loaded on BN and graphene were calculated. Our study found that graphene has higher thermal conductivity and is easier to form SACs than BN, but the SACs formed on BN surface have higher thermodynamic stability.