Latest ArticlesTwenty-four novel neonicotinoid analogues with nitromethylene and five-membered aromatic heterocycles were designed and synthesized. All target molecular structures have been confirmed by analytical and spectral data. Some compounds exhibited notable insecticidal activities against aphid (Aphis medicaginis) and brown planthopper (Nilaparvata lugens). The aqueous stability test confirmed that the stabilities of those compounds were superior to the leading compound, and the photostability was even better than that of imidacloprid.
Schisandrin A is a natural dibenzocyclooctene lignan with potent neuroprotective activity. However, the specific mechanisms or direct target proteins have not been clarified up to now. In this study, we designed and synthesized the probes of schisandrin A with photoreactive diazirine and clickable alkyne to identify its direct target in SH-SY5Y cells by employing activity-based protein profiling (ABPP) technique. Ykt6 was prominent among the 13 proteins obtained with high confidence and we confirmed Ykt6 as the direct target of schisandrin A by CETSA, IF, SPR and knockdown assay. Functionally, schisandrin A protected the cells against the injury induced by glutamate by regulating autophagy via Ykt6. This discovery may provide a novel therapeutic option for various neuronal cell damage-mediated diseases.
Nitrogen electro-reduction reaction (NERR) is a promising alternative method for ammonia production to the Haber–Bosch approach due to mild reaction conditions and free harmful by-product emission. A formidable challenge in bringing NERR closer to the practical application is developing an electro-catalyst which can simultaneously improve the Faraday efficiency and reduce the reaction over-potential. Herein, we fabricated a catalyst of nitrogen-doped carbon dots modified copper-phosphate nanoflower petals (CuPo-NCDs NF) via a self-assembly method. The flower structure endowed the CuPo-NCDs NF with large specific surface area, and thus enabled more active sites to be exposed. In particular, we demonstrated that the NCDs modified CuPo petals with flower-like structure can accelerate the interfacial proton-electron transfer, suppressing the competing hydrogen evolution reaction and promoting the desired NERR process. Ultimately, for the CuPo-NCDs NF catalyzed NERR, the FENH3 and the reaction potential both were boosted, the resultant energy efficiency of NERR reached a record-breaking value of 56.5%, and the NH3 yield rate increased by 7 times compared to NCDs. This study provides a novel catalyst with a new pathway to boost the NERR.
Various phototheranostics have recently been developed for phototherapy. Through proper molecular design, the photochemical and photophysical properties of these phototheranostics can be promoted. Herein, an acceptor-donor-acceptor (A-D-A)-structured dye, BTP-4F-DMO, was synthesized and prepared into water-soluble nanoparticles (NPs). The obtained BTP-4F-DMO NPs had strong absorption from 650 nm to 850 nm and a fluorescence emission peak at ~900 nm that tailed to ~1100 nm. The NPs showed a superhigh photothermal conversion efficiency of 90.5% ± 5% and could simultaneously generate •OH and 1O2 with a 1O2 generation quantum yield of 4.6% under 808 nm laser irradiation. Due to these advanced properties, BTP-4F-DMO NPs can switch the role of autophagy from pro-survival to pro-death, thereby further promoting cancer cell death. These features make BTP-4F-DMO NPs a promising multifunctional phototheranostic agent for NIR-Ⅱ fluorescence/photoacoustic dual-mode imaging-guided synergetic photodynamic/photothermal therapy. In general, this work provides a strategy for expanding the biomedical applications of organic A-D-A-structured phototheranostics.
The massive use of polyhexamethylene guanidine (PHMG), as a typical bactericidal agent, raised environmental concerns to the public. This work comprehensively revealed the hormesis effects of PHMG occurred in waste activated sludge (WAS) on the generation of volatile fatty acids (VFAs) during anaerobic fermentation. The low level of PHMG (100 mg/g TSS) significantly promoted the VFAs generation (1283 mg COD/L, compared with 337 mg COD/L in the control) via synchronously facilitating the solubilization, hydrolysis, and acidification steps but inhibiting methanogenesis. Metagenomic analysis showed that the functional anaerobe (i.e., Bacteroides, Macellibacteroide and Parabacteroide) and corresponding genetic expressions responsible for extracellular hydrolysis (i.e., clpP), membrane transport (i.e., ffh and gspF), intracellular substrates metabolism (i.e., ald and paaF) and VFAs biosynthesis (i.e., ACACA and FASN) were enhanced in the optimal presence of PHMG. Moreover, the anaerobic species could respond and adapt to low PHMG stimuli via quorum sensing (i.e., cqsA, rpfC and rpfG), and thus maintain the high microbial metabolic activities. However, they were unable to tolerate the toxicity of excessive PHMG, resulting in the extremely low VFAs production. This work enlightened the effects of emerging pollutants on WAS fermentation at the genetic levels, and provided guidance on the WAS treatment and resource recovery.
Conductive hydrogels have shown great prospects as wearable flexible sensors. Nevertheless, it is still a challenge to construct hydrogel-based sensor with great mechanical strength and high strain sensitivity. Herein, an ion-conducting hydrogel was fabricated by introducing gelatin-dialdehyde β-cyclodextrin (Gel-DACD) into polyvinyl alcohol-borax (PVA-borax) hydrogel network. Natural Gel-DACD network acted as mechanical deformation force through non-covalent cross-linking to endow the polyvinyl alcohol-borax/gelatin-dialdehyde β-cyclodextrin hydrogel (PGBCDH) with excellent mechanical stress (1.35 MPa), stretchability (400%), toughness (1.84 MJ/m3) and great fatigue resistance (200% strain for 100 cycles). Surprisingly, PGBCDH displayed good conductivity of 0.31 S/m after adding DACD to hydrogel network. As sensor, it showed rapid response (168 ms), high strain sensitivity (gage factor (GF) = 8.57 in the strain range of 200%-250%) and reliable sensing stability (100% strain for 200 cycles). Importantly, PGBCDH-based sensor can accurately monitor complex body movements (knee, elbow, wrist and finger joints) and large-scale subtle movements (speech, swallow, breath and facial expressions). Thus, PGBCDH shows great potential for human monitoring with high precision.
Rational regulation of stable graphitic carbon nitride (CN) for superior peroxymonosulfate (PMS) activation is important in the catalytic degradation of water contaminants. In this work, the copper oxide and oxygen co-doped graphitic carbon nitride (CuO/O-CN) was prepared via one-step synthesis and applied in activating PMS for oxytetracycline (OTC) degradation, displaying superior catalytic performance. Systematic characterization and theoretical calculations indicated that the synergistic effect between the oxygen site of CN and CuO can modulate the electronic structure of the whole composite further facilitating the formation of non-radical 1O2 and various reactive radicals. Results of the influencing factor experiments revealed that CuO/O-CN has a strong resistance to the environmental impact. The degradation efficiency of OTC in the real water environment even exceeded that in the deionized water. After four successive runs of the optimal catalyst, the OTC removal rate was still as high as 91.3%. This work developed a high-efficiency PMS activator to remove refractory pollutants via both radical pathway and non-radical pathway, which showed a promising potential in the treatment of wastewaters.
Glioma is a malignant primary brain tumor that is extremely harmful to human beings. Therefore, studying the invasiveness of glioma cells is of great significance for the diagnosis and treatment of glioma. In this work, TiO2/Nb2C was prepared as a SERS substrate and combined with microfluidic chip to construct an invasion model capable of monitoring glioma invasion in real time. Both experimental data and density function theory (DFT) calculations showed that the significant SERS-enhancing effect of TiO2/Nb2C on methylene blue (MB) originated from the chemical magnification (CM) mechanism when MB was used as the adsorbed molecule. Based on this, we achieved a highly sensitive and targeted detection of vascular endothelial growth factor (VEGF), a biomarker for glioma with a low detection limit of 3.7 pg/mL, then quantified the invasive process in real time by detecting VEGF. Meanwhile, the depletion of reactive oxygen species (ROS) by TiO2/Nb2C can inhibit the invasion of glioma cells. For the first time, the invasion model combines SERS technology with microfluidic technology, while monitoring the cell invasion process in real time, the invasion process can be quantified by detecting the VEGF secreted by glioma cells during the invasion process, realizing the integration of diagnosis and treatment, and establish a new model for the biomedical analysis, clinical diagnosis and treatment of glioma.
The construction of highly active catalysts for methanol oxidation reaction (MOR) is central to direct methanol fuel cells. Tremendous progress has been made in transition metal phosphides (TMPs) based catalysts. However, TMPs would be partially damaged and transformed into new substances (e.g., Pt-M-P composite, where M represents a second transition metal) during Pt deposition process. This would pose a large obstacle to the cognition of the real promoting effects of TMPs in MOR. Herein, Co2P co-catalysts (Pt-P/Co2P@NPC, where NPC stands for N and P co-doped carbon) and Pt-Co-P composite catalysts (Pt-Co-P/NPC) were controllably synthesized. Electrocatalysis tests show that the Pt-Co-P/NPC exhibits superior MOR activity as high as 1016 mA/mgPt, significantly exceeding that of Pt-P/Co2P@NPC (345 mA/mgPt). This result indicates that the promoting effect is ascribed primarily to the resultant Pt-Co-P composite, in sharply contrast to previous viewpoint that Co2P itself improves the activity. Further mechanistic studies reveal that Pt-Co-P/NPC exhibits much stronger electron interaction and thus manifesting a remarkably weaker CO absorption than Pt-P/Co2P@NPC and Pt/C. Moreover, Pt-Co-P is also more capable of producing oxygen-containing adsorbate and thus accelerating the removal of surface-bonded CO*, ultimately boosting the MOR performance.
Development of high-performance solid state luminescent carbon-based nanomaterials remains challenging. Here, strong blue-green fluorescent carbonized polymer dots (CPDs) from o-aminobenzenethiol and thiosalicylic acid (oABT-TSA-CPDs) with an absolute photoluminescence quantum yield (PLQY) of 76% in solid state without matrix were synthesized. Through adjusting the reaction temperature and time, the PL centers were proved to be carbon core state and surface state associated to carbonyl group which was the source of strong fluorescence emission in solid state. The mechanism of the unique phenomenon of enhanced emission from ethanol solution (PLQY = 7%) to powder (PLQY = 76%) was investigated by analyzing the chemical properties and structures of oABT-TSA-CPDs at different temperatures and oABT-TSA-CPDs/PVC composites, and was confirmed as fixation of PL centers.
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