Latest ArticlesThis work describes a bifunctional oxygen catalyst made of cobalt disulfide encapsulated in N, S co-doped mesoporous carbon with a novel three-dimensional micro-nano crosslinking structure. The proposed composite materials exhibit promising oxygen electrocatalytic activity and stability. The composite assembled rechargeable zinc-air battery can achieve a high power density of 208.9 mW/cm2, and can be stably cycled for more than 160 h. Additionally, the all-solid zinc-air battery assembled with the electrocatalyst also performs admirably. The micro-nano crosslinking and high porosity structure, as well as the large number of active sites generated by the synergy of N, S doping and the close interface between carbon matrix and CoS2, contribute to the composite's exceptional electrochemical performance. This study's rational strategy lays the path for the development of other high-performance bifunctional electrocatalysts.
Bacteria producing β-lactamases have become a major issue in the global public health field. To restrain the development of drug resistance and reduce the abuse of antibiotics, it is very important to rapidly identify bacteria producing β-lactamases and put forward a reasonable treatment plan. Here, an integrated microfluidic chip-mass spectrometry system was proposed for rapid screening of β-lactamase-producing bacteria and optimization of β-lactamase inhibitor dosing concentration. The concentration gradient generator followed by an array of bacterial culture chambers, as well as micro-solid-phase extraction columns was designed for sample pretreatment before mass analysis. By using the combination system, the process of the hydrolysis of antibiotics by β-lactamase-producing bacteria could be analyzed. To validate the feasibility, four antibiotics and two antibiotic inhibitors were investigated using three strains including negative control, SHV-1 and TEM-1 strains. SHV-1 and TEM-1 strains were successfully distinguished as the β-lactamase producing strains. And the acquired optimal concentrations of β-lactamase inhibitors were in accordance with the results by that obtained from the traditional microdilution broth method. The total analysis time only needed around 2 h, which was faster than conventional methods that require a few days. The technique presented herein provides an easy and rapid protocol for β-lactamase resistance related studies, which is important for the inhibition of antimicrobial resistance development and the reduction of antibiotics abuse.
Halide electrolytes in solid-state batteries with excellent oxidative stability and high ionic conductivity have been well reported recently. However, the high-cost rare-earth elements and long duration of high-rotation milling procure are the major obstacles. Herein, we have successfully synthesized the low cost Li2.25Zr0.75Fe0.25Cl6 electrolyte consisting of abundant elements with comparable Li-ion conductivity in a short milling duration of 4 h. Phase transition of the annealed sample was also carefully investigated. LiNi0.6Co0.2Mn0.2O2/Li2.25Zr0.75Fe0.25Cl6/Li5.5PS4.5Cl1.5/In-Li batteries using different halide electrolytes were constructed and cycled at different voltage windows. Solid-state battery using Li2.25Zr0.75Fe0.25Cl6 electrolyte obtained from long milling duration delivers higher discharge capacities and superior capacity retention than shorter milling time between 3.0 and 4.3 V. It delivers much higher discharge capacity when cycled at elevated temperature (60 ℃) and suffers fast capacity degradation when the upper cut-off voltage increases to 4.5 V at the same current density. This work provides an efficiency synthesis strategy for halide solid electrolyte and studies its applications in all-solid-state batteries in a wide temperature range.
Inhibitor targeting immune checkpoint is a promising new anticancer therapy. Blocking the interaction between PD-1 and PD-L1 can reverse the immunosuppression state and improve the lethality of immune cells to tumor cells. Here, we report PROTAC-based PD-L1 degraders to enhance T cell killing activity against melanoma. Four series of PD-L1 degraders were designed and synthesized to VHL, CRBN, MDM2 or cIAP E3 ligase system, in which CRBN-ligand-based compound BMS-37-C3 was identified as the most active PROTAC molecule. BMS-37-C3 also significantly enhanced the killing ability of T cells in a co-culture model of A375 and T cells. Furthermore, western blot data and flow cytometry demonstrated that BMS-37-C3 could reduce the protein levels of PD-L1 in dose and time dependent manner, which may provide a new therapeutic method for tumor immunotherapy.
Intramedullary spinal cord tumor (IMSCT) is comparatively rare malignant tumor in the central nervous system and is very difficult accessible by conventional chemotherapy regimen. Currently, there are very limited researches for IMSCT treatment using nanomedicine. To fill this gap, we originally reported a targeted strategy by leveraging nano-engineered mesenchymal stem cells (MSCs) for synergistic anti-IMSCT treatment. In this study, two mode drugs paclitaxel (PTX) and metformin (MET) were co-loaded in maleimide-modified poly(lactic-co-glycolicacid) (PLGA-MAL) nanoparticles, which were further conjugated onto MSCs surface via the thioether bond formed between PLGA-MAL and MSCs without affecting the migration ability of MSCs. Owing to the excellent tumor tropism and penetrability of MSCs and good biodegradability of PLGA, the designed drug delivery platform could accurately target IMSCT sites to exert long-term synergistic antitumor efficacy, exhibiting promising research value for alternative IMSCT management beyond surgery.
The accessibility and mass transfer between catalytic sites and substrates/intermediates are essential to a catalyst's overall performance in oxygen electrocatalysis based energy devices. Here, we present an "in-situ self-sacrifice template etching strategy" for reconstructing MOF-derived M-N-C catalysts, which introduces micro‑meso-macro pores with continuous apertures in a wide range and a central hollow-out structure to optimize the electrochemical oxygen redox kinetics. It is realized via one-step pyrolysis of ZIF-8 single crystal epitaxially coating on a multi-functional template of the Fe, Co co-loaded mesoporous ZnO sphere. The ZnO core is reduced during the general pyrolysis of ZIF-8 into M-N-C and acts as a pore former to etch the surrounding ZIF-8 shell into diverse channels anchoring highly exposed Fe and Co-based active sites with edge enrichment. The redesigned catalyst reveals apparent structural benefits towards enhanced oxygen redox kinetics as bifunctional cathode catalysts of rechargeable zinc-air battery compared with the primitive bulk M-N-C catalysts and the mixture of commercial Pt/C and Ir/C. The unique structure-based activity advantages, the omitted template removal step and good template compatibility during synthesis make the strategy universal for the channel engineering of electrocatalysts.
Zn-gas batteries have attracted great attention in the area of energy conversion and storage owing to their high theoretical energy density in the past decades. In addition to the most widely researched Zn-air/oxygen battery, other novel Zn-gas batteries such as Zn-CO2, Zn-N2 and Zn-NO batteries as "killing two birds with one stone" strategy have emerged to provide energy power and upgrade the pollutant/useless gases simultaneously. This technology becomes more appealing as a low-cost and controllable method to produce value-added chemicals and fuels (such as CO, HCOO−, CH4, NH3) at the cathode driven by surplus electricity. However, there is an absence of a guide for the selection of catalyst and the construction of energy system. Herein, we overview recent achievements in typical Zn-gas batteries beyond Zn-air/oxygen, mainly including Zn-CO2, Zn-N2 and Zn-NO batteries. The energy storage mechanism of these novel Zn-gas batteries has been clearly elaborated. Then, the produced value-added chemicals and the design of cathodic catalyst materials are summarized. Lastly, the remaining challenges and possible directions of Zn-gas batteries, such as highly reduced products, high yield rate and remarkable battery performance, in the future are discussed.
Plant-parasitic nematodes are major threat for crop protection. The lack of nematicides with new mode of action and increasing resistance raises the need for novel nematicides. In order to seek new nematicidal lead, originating from the structure of chalcone, a series of fused ring compounds was obtained by ring closure design strategy. These compounds were modified further. The nematicidal activity against M. incognita of synthesized compounds was evaluated. The bioassay showed that compound 3 and some of its derivatives such as compounds 18, 19, 21, 22, 23, 24 and 26 exhibited excellent nematicidal activity. Among them, compound 23 exhibited significant bioactivity. The LC50/72 h value reached 3.20 mg/L in vitro and the inhibition rate was 100.00% at 40 mg/L in the matrix. The structure-activity relationship of synthesized compounds was discussed in details. The influence of compound 23 on egg hatching, motility, and feeding behavior of C. elegans was also evaluated.
Electrochemical is considered an attractive approach to recycling the pollution NO (NORR) and producing the valuable NH3, which could simultaneously solve the two challenging problems, i.e., NO removal and NH3 synthesis. Current research efforts focus less on NORR due to the lack of effective catalysts. Herein, based on DFT calculation, we try to explore effective pyrrole-type TM-N4 (TM = V, Cr, Mn, Fe, Co, Ni, Cu, Ru, Rh, Ta) catalysts for achieving the direct NORR. Among the investigated systems, Fe-N4 exhibits excellent catalytic activity and high NH3 selectivity. Moreover, the free energy of adsorption of N* has been proposed as a descriptor to predict and screen the effective TM-N4 catalyst for NORR and the crystal orbital halmilton populations (COHP) is used to describe the intrinsic relationship between metal atoms and the adsorption free energy of N* intermediate. This work has provided a theoretical picture of TM-N4 catalyzing NO to NH3, which will establish guidelines for the rational design of NORR catalysts and other electrochemical reactions.
Metal-free heterogeneous photocatalysts provide an environmental-friendly and cost-efficient avenue for green organic synthesis. Covalent organic frameworks (COFs) as heterogeneous photocatalysts showcase promising potential in the field of photocatalytic organic reactions due to their high porosity, insolubility and tailor-made functions. However, thus far, COF-based catalysts only mediated a few types of reactions. Herein, we developed a series of isoreticular nitrogen-rich covalent organic frameworks (N-COFs) with comparable porous structures as photocatalysts which effectively mediated the borylation of aryl iodides with broad substrate scope. Remarkably, 6N-COF exhibits excellent photocatalytic efficiency and superior recyclability. It suggests a new pathway to construct efficient heterogeneous photocatalysts for the borylation of aryl halides.
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