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.
In 2021, The MOE Key Laboratory of Macromolecular Synthesis and Functionalization in Zhejiang University had achieved several important results. First, a series of versatile organoboron catalysts were synthesized for ring-opening (co)polymerizations. Second, a catalyst-free polycondensation mechanism was proposed for the production of polyesters with high molecular weights. Third, a co-assembly method that can fabricate films and coatings with controllable structures and properties on various substrates was demonstrated, providing a platform for the construction of novel surface coatings. Forth, facile methods for producing high-productivity poly(propylene carbonate) and semicrystalline polyester have been discovered. And linear non-conjugated polyesters exhibiting yellow-green clusteroluminescence were developed for the first time. Fifth, a supramolecular prodrug nano-assembly strategy has been developed for reactive nitrogen species potentiated chemotherapy. Sixth, a series of tough and stiff supramolecular hydrogels with shape memory properties have been used for information encryption. Seventh, reversible fusion and fission of wet-spun graphene oxide fibers has been successfully achieved. Eighth, three non-conjugated polypeptides were synthesized and the mechanism of clusteroluminescence was studied. Ninth, a series of conducting covalent organic frameworks with high electrical conductivity and carrier mobility have been used as high-performance chemiresistor, electrocatalyst, and organic field-effect transistor. Tenth, the exploration of non-fused electron acceptors, and their photostable mechanism are exemplified for developing high-performance, low-cost and eco-friendly polymer solar cells. Finally, gel-grown long-range ordering bulk-heterojunctions has achieved improved X-ray detector performance.
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.
In order to balance the conductivity and flexural strength of graphite composite bipolar plates, the influence of conductive filler on the properties of graphite composite bipolar plate was comprehensively studied by using phenolic resin as binder, natural flake graphite as conductive substrate and functional carbon materials with different structures as auxiliary filler. The results show that the particle size of conductive substrate has an important influence on the conductivity enhancement of auxiliary filler. The influence of conductive particle size on auxiliary filler electrical conductivity improvement was first investigated in this research. The effects of various auxiliary filler concentrations on improving electrical conductivity and flexural strength were then examined. This research has substantial implications for the balance of electrical conductivity and flexural strength of graphite composite bipolar plates.
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.
The supercapacitive properties of manganese oxides (MnOx) are strongly affected by their crystal structure. Nevertheless, the relationship between the crystal structure and supercapacitive performance of MnOx is elusive. Herein, a temperature-controlled fabrication method was developed to achieve MnO2, Mn3O4, MnO and Mn2O3 microspheres with various crystal structure as electrode materials tunable for supercapacitors. The detailed material and electrochemical characterizations revealed the structure-activity relationship of MnOx microspheres by systematically investigating the effect of valence state, specific surface area, conductivity and morphology on supercapacitive performance. Among these MnOx materials, nanoneedle-like MnO2 delivered a relatively high specific capacitance of 274.1 F/g at 1 A/g due to a high Mn valence state of +4, a large specific surface area of 113.4 m2/g and a desirable electronic conductivity of 1.73 × 10–5 S/cm. Furthermore, MnO2 presented a remarkable cycle stability with 115% capacitance retention after 10,000 cycles owing to the enhancement of wettability. This work not only provides a facile strategy to modulate MnOx crystal structure, but also offers a deep understanding of structure-dependent supercapacitive performance of MnOx.
Stable solid-electrolyte interphase (SEI) is crucial for advanced development of lithium metal batteries. However, the continuous collapse and reconstruction of SEI will deplete fresh Li and electrolytes upon cycling, leading to irreversible capacity loss. Herein, we addressed this issue by pre-formation of artificial robust hybrid interphase on a 3D layered graphene/lithium metal framework, in which is constructed by LiF associated with Li2TiF6 generated by the in-situ reaction between the surfacial lithium and titanium fluoride contained electrolytes. The as-obtained interphase can maintain the structure integrality and avoid continuous consumption of the fresh Li and electrolytes. As a consequence, the Li symmetric cells achieve high-efficiency Li deposition and stable cycling over 3600 h. When paired with LiFePO4 cathodes, the coin cells exhibit long lifespan (> 800 cycles) with almost 88.3% retention of the initial capacity.
Understanding the negative thermal expansion (NTE) mechanism is of great importance. In this work, we consider the new NTE compound GdFe(CN)6 (αv = −34.2×10-6 K-1) as a case study to investigate the NTE mechanism from the perspective of the lattice vibrational dynamics. The atomic mean-square displacements suggest that the NTE of GdFe(CN)6 comes from the strong tension effect induced by the transverse vibrations of the atomic –Fe–C≡N–Gd– linkages, with the largest contribution given by N atoms. Lattice dynamics calculations show that three low-frequency optical modes at about 50 cm-1 show the largest negative Grüneisen parameters thus providing the largest contribution to the NTE. The existence of these unusual low-frequency vibrational modes can be ascribed to the presence of GdN6 trigonal prisms in the framework structure of GdFe(CN)6.
As the greenhouse effect concerns increases, the development of new materials for the efficient capture and separation of CO2 gas from gas mixtures has become a matter of urgency. In this study, we performed density functional theory (DFT) calculations to investigate the adsorption and separation behavior of CO2/CH4/H2 on the surface of two-dimensional (2D) Al2C materials under positive/negative applied electric fields. In the absence of an electric field CO2 is weakly physisorbed on the Al2C surface, but with the application of an applied electric field, the adsorption state of CO2 gradually changes from physical to chemisorption (adsorption energy changes from −0.29 eV to −3.61 eV), while the negative electric field has little effect on the adsorption of CO2. We conclude that the C=O bond in adsorbed CO2 can be activated under an external electric field (maximum activation of 15% under an external electric field of 0–0.005 a.u.). Only in the presence of an applied electric field of 0.0033 a.u. and temperatures above 525 K/675 K can the adsorption/separation reaction of CO2 single adsorption and CO2/CH4/H2 mixture be spontaneous. The adsorption/desorption of CO2 on Al2C nanosheet in an electric field of 0.003–0.0033 a.u. is all exothermic, which can be easily controlled by switching on/off the electric field without any energy barriers. The capacity of Al2C to capture CO2 per unit electric field decreases with increasing CO2 concentration, but still has efficient gas separation properties for CO2/CH4/H2. Our theoretical results could provide guidance for designing high-capacity and high-selectivity CO2 capture materials.
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