Latest ArticlesDeveloping precise extracellular vesicles (EVs) labelling techniques with minimal disturbance is of great importance to the follow-up EVs detection and analysis. However, currently available methods such as using probes to conjugate phospholipids or membrane proteins have certain limitations due to EV steric hindrance, dye aggregation, etc. Here, we present a microfluidic platform to enhance EVs' labelling efficiency and improve their detection. This platform provides excellent sample throughput and high-efficiency EV labelling at lower label concentrations with an optimized flowing rate. Flow cytometry analysis (FCM) and cellular uptake results show that EV labelling by utilizing this platform possesses the merits of a higher labelling efficiency with 64.1% relative improvement than conventional co-incubation method and a lower background noise. Moreover, this technique maintains EVs' size, morphology and biological activities. After the recipient cells uptake the EVs treated by the microfluidic platform, the spatial and temporal distribution of EVs in the cells are clearly observed. These results demonstrate that our method holds great potential in efficient labelling of EVs, which is essential to subsequent EV quantification and analysis.
Establishing an effective charge transfer mechanism in carbon nitride (g-C3N4) to enhance its photocatalytic activity remains a limiting nuisance. Herein, the combination design of a single Cu atom with hollow g-C3N4 nanospheres (Cu-N3 structure) has been proven to offer significant opportunities for this crucial challenge. Moreover, this structure endows two pathways for charge transfer in the reaction, namely, the N atoms in the three-dimensional planar structure are only bonded with a single Cu atom, and charge transfer occurs between the plane and the layered structure due to the bending of the interlayered g-C3N4 hollow nanospheres. Notably, Cu-N3 and hollow nanosphere structures have been certified to greatly enhance the efficiency of photogenerated carrier separation and transfer between the layers and planes by ultrafast spectral analysis. As a result, this catalyst possesses unparalleled photocatalytic efficiency. Specifically, the hydrogen production rate up to 2040 µmol h−1 g−1, which is 51 times that of pure C3N4 under visible light conditions. The photocatalytic degradation performance of tetracycline and oxidation performance of benzene is also expressed, with a degradation rate of 100%, a conversion of 97.3% and a selectivity of 99.9%. This work focuses on the structure-activity relationship to provide the possibilities for the development of potential photocatalytic materials.
Interface engineering is of great importance to improve the photocatalytic performance. Herein, in-situ formation plasmon Bi/BiOCl nanosheets assembled heterojunction microspheres are fabricated via facile reductive solvothermal approach. The aldehyde group in the DMF structure is used to exert the weak reducing property of the solvent and thus strip out the metal Bi in BiOCl. The metal Bi is anchored on surface of BiOCl firmly due to in-situ formation engineered interface, which could realize efficient charge transfer channel. The resultant Bi/BiOCl heterojunctions assemblies with narrow bandgap of 3.05 eV and mesoporous structure extend the photoresponse to visible light region and could provide sufficient surface active sites. The visible-light-driven photocatalytic degradation of high-toxic norfloxacin for Bi/BiOCl heterojunctions is up to 95.5% within 20 min, representing several times that of pristine BiOCl nanosheets and the physical mixture. It is attributed to the in-situ formation of Bi/BiOCl heterojunctions and surface plasmon resonance (SPR) effect of plasmon Bi promoting charge transfer, and the obvious photothermal effect promoting the photocatalytic reaction, which are verified by experimental and density functional theory (DFT) calculations. This strategy provides ideal perspectives for fabricating metal/semiconductor heterojunctions photocatalysts with high-performance.
Patients with epidermal growth factor receptor (EGFR) wild-type non-small cell lung cancer (NSCLC) often show primary resistance to gefitinib therapy. It is thus necessary to study the metabolism of gefitinib in NSCLC cells to comprehensively reveal the reasons for the primary resistance of tumors. Herein, we develop a platform for studying drug metabolism heterogeneity based on single-cell mass spectrometry (sDMH-scMS) by integrating living-cell electrolaunching ionization MS (ILCEI-MS) and high-performance liquid chromatography-MS (HPLC-MS) analysis, and the primary resistance of NSCLC cells to gefitinib was studied using this platform. The ILCEI-MS analysis showed that approximately 11.9% of NSCLC single cells contained the gefitinib metabolite M11; HPLC-MS detection diluted the intensity of M11 in subpopulations and concealed the heterogeneity of drug metabolism in tumor single cells. The intensity of gefitinib in EGFR wild-type A549 cells was markedly lower than in mutant PC9 cells, and the intensity of gefitinib metabolites was significantly higher than in PC9 cells, suggesting that the primary resistance of NSCLC cells is related to gefitinib metabolism. Moreover, the combination of gefitinib and the drug-metabolizing enzyme inhibitor α-naphthoflavone was shown to overcome the primary resistance of the NSCLC cells. Overall, the results of this study are expected to be applicable for clinical drug resistance diagnosis and treatment at the single-cell level.
Owing to the large exciton binding energy (>100 meV) of most organic materials, the process of exciton dissociation into free electrons and holes is seriously hindered, which plays a key role in the photocatalytic system. In this study, a series of chalcogen (S, Se)-substituted mesoporous covalent organic frameworks (COFs) have been synthesized for enhanced photocatalytic organic transformations. Photoelectrochemical measurements indicate that the introduction of semi-metallic Se atom and the enlargement of conjugation degree can not only reduce the exciton binding energy accelerating the charge separation, but also reduce the band gap of COFs. As a result, the COF-NUST-36 with the lowest exciton binding energy (39.5 meV) shows the highest photocatalytic performance for selective oxidation of amines (up to 98% Conv. and 97.5% Sel.). This work provides a feasible method for designing COFs with high photocatalytic activity by adjusting exciton binding energy.
Rapid analysis of metal ions and organic compounds in strong acidic solutions is of sustainable interest in multiple disciplines. However, complicated and time-consuming pretreatments are always required for MS analysis of the compounds in strong acidic solutions. Otherwise, it will result in a weak signal and cause serious damage to the mass spectrometer. Herein, a simple method inherited from nano-ESI MS was developed for rapid analysis of strong acidic solutions. Nanoliter (nL) strong acidic solution was first loaded in the nano-ESI emitter, followed by evaporation to remove the H+ and leave the analytes on the wall of the nano-ESI emitter. The evaporation process can be completed within 1 min because of the extremely tiny volume (≤1 nL) of the loaded solution. Then, the dried analytes on the wall of the nano-ESI emitter were redissolved by loading a new solvent, followed by nano-ESI MS analysis. By using this method, metal ions and organic compounds in the strong acidic solution can be detected with low sample consumption (1 nL), high speed (< 2 min/sample), high sensitivity (limit of detection = 0.2 µg/L), and high accuracy (> 90%). Proof-of-concept applications of the present method have been successfully achieved for the analysis of gastric juice (pH of the sample = 1), monitoring reaction catalyzed by strong acid (pH of the system = 0), and micro-area analysis of ores (pH of the extraction solvent = 0), showing great application potential in multiple fields.
After a century of standstill, bacteria-based tumor therapy has resurged recently benefiting from the revolution of tumor immunotherapy, which provides unique solutions to tackle the obstacles of traditional tumor treatments. Obligate and facultative anaerobes with active tropism can selectively colonize at tumor sites and suppress tumor growth via different mechanisms, serving as attractive tools for tumor treatment either as a monotherapy or combining with other therapies for synergistic anti-tumor effects. In this critical review, we introduce the recent advances of bacteria-based tumor therapy from the following aspects. First, the general properties of bacteria are reviewed emphasizing on their structural components related to tumor immunotherapy, and the main bacteria that have been used in tumor therapy are listed. Then, the benefits of bacteria for tumor therapy are illustrated, such as tumor targetability, deep penetration, and facile genetic engineering for attenuation, enhanced efficacy, as well as bioimaging. Next, anti-tumor mechanisms of bacteria are summarized, which refer to intrinsic tumoricidal activities, immune activation, bacteria metabolism, and their capability to regulate gut microbiota homeostasis. Moreover, bacteria could act as carriers to deliver various types of therapeutics to achieve combination therapy with improved efficacy. In addition, several challenges for anti-tumor applications of bacteria are discussed regarding the delivery, efficacy and safety issues, and potential solutions are also provided. Finally, the possible improvements and perspectives are discussed in the end, which provide a guideline for the design of advanced bacteria-based tumor therapeutics in the future.
Achieving high activity and durability for the oxygen reduction reaction (ORR) with an ultra-low amount of platinum is significant to promote the widespread application of proton exchange membrane fuel cells (PEMFCs). Here we report a new ultrathin (~1 nm) ternary PtNiGa alloy nanowires (PtNiGa NWs) electrocatalyst, in which the presence of gallium (Ga) enhances the oxidation resistance of platinum (Pt) and nickel (Ni) and suppresses the dissolution of Ni. The mass and specific activities of PtNiGa NWs are about 11.2 and 7.6 times higher than those of commercial Pt/C catalysts for ORR. Moreover, the mass activity of PtNiGa/C NWs nanocatalyst decreased only by 12.8% and largely retained its electrochemical surface area (ECSA) after 10,000 potential cycles, compared with 38% loss of ECSA for commercial Pt/C catalyst. Therefore, this work provides a general guideline for preparing ternary alloy electrocatalysts and enhancing the activity and stability of the cathode ORR reaction of PEMFCs.
Rechargeable alkaline aqueous zinc batteries (RAZBs) have attracted increasing attention. However, most RAZBs are hindered by the limited availability of cathode materials. The practical electrochemical performance of most cathode materials is lower than the theoretical value due to their poor electrical conductivity and low utilization capacity. In this work, we develop a facile hydrothermal procedure to prepare highly uniform bimetallic sulfides as novel cathode materials for RAZBs. Copper-cobalt binary metallic oxides materials possess higher conductivity and larger capacity compared with their mono-metal oxides compounds due to bimetallic synergistic effects and multiple oxidation states. Furthermore, bimetallic sulfide compounds have smaller bond energy and longer bond length than their oxides, leading to less structural damage, faster kinetics of electrochemical reactions, and better stability. The as-prepared Co-Cu bimetallic sulfides show enhanced electrochemical performance due to various valences of Co and Cu as well as the existence of S. As a result, aqueous Zn/CuCo2S4 battery shows a high specific capacity of 117.4 mAh/g at 4 A/g and a good cycle life of over 8000 cycles. Based on PANa hydrogel electrolytes, a flexible Zn/CuCo2S4 battery demonstrates excellent cycling stability. This battery can also meet the requirements of electronic devices with different shapes and performs well in extreme environments, such as freezing, drilling, and hammering. This work opens new avenues to obtain high-rate and long-life cathode materials for RAZBs by utilizing the synergistic effects of bimetallic sulfides and provides a new platform for flexible energy storage devices.
Electrochemical nitrate reduction reaction (NITRR) is regarded as a “two birds-one stone” method for the treatment of nitrate contaminant in polluted water and the synthesis of valuable ammonia, which is retarded by the lack of highly reactive and selective electrocatalysts. Herein, for the first time, nickel foam supported Co4N was designed as a high-performance NITRR catalyst by an in-situ nonmetal leaching-induced strategy. At the optimal potential, the Co4N/NF catalyst achieves ultra-high Faraday efficiency and NH3 selectivity of 95.4% and 99.4%, respectively. Ex situ X-ray absorption spectroscopy (XAS), together with other experiments powerfully reveal that the nitrogen vacancies produced by nitrogen leaching are stable and play a key role in boosting nitrate reduction to ammonia. Theoretical calculations confirm that Co4N with abundant nitrogen vacancies can optimize the adsorption energies of NO3- and intermediates, lower the free energy (ΔG) of the potential-determining step (*NH3 to NH3) and inhibit the formation of N-containing byproducts. In addition, we also conclude that the nitrogen vacancies can stabilize the adsorbed hydrogen, making H2 quite difficult to produce, and lowering ΔG from *NO to *NOH, which facilitates the selective reduction of nitrate. This study reveals significant insights about the in-situ nonmetal leaching to enhance the NITRR activity.
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