Latest ArticlesComprehensive surgical staging or optimal tumor cytoreductive surgery of malignant ovarian cancer directly affects disease prognosis. Therefore, a fluorescent selenium nanoparticle (Se@RGD/S2.2) decorated with cancer-targeting Arg-Gly-Asp (RGD) peptides and GCAGTTGATCCTTTGGATACCCTGG aptamer (S2.2) was developed for use as a diagnostic agent to achieve rapid, noninvasive diagnosis and visualization of microinvasive lesions during surgery for malignant ovarian cancer.
This 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.
Tyrosine sulfation is an important post-translational modification that enhances the inhibitory activity of hirudin. Herein, we developed a facile synthetic strategy to afford the sulfated hirudins with up to three modifications and in multi-milligram scales, after a single HPLC purification step. Through these synthetic proteins, a novel type of modulation mechanism exhibited by tyrosine sulfation was proposed, which would help to delineate the structure–function relationships in other sulfated proteins and more importantly, to serve as a basis for the development of related antithrombotic agents.
Novel polyoxometalate (POM) Pickering interfacial catalyst (PIC) was fabricated through loading (NH4)5H6PMo4V8O40 (PMo4V8) on both alkyl and alkyl-amino groups functionalized silica nanoparticles. PMo4V8/SiO2(C8/C8NH2 with molar ratio as 1:1) PIC system provided a new catalytic model for aerobic conversion of 5-hydroxymethylfurfural (5-HMF), as well as its recovery and product separation in H2O/methyl isobutyl ketone (MIBK) biphase reaction. Balancing the ratio of PMo4V8, C8 and C8NH2 gave rise to variety in hydrophilicity and hydrophobicity for PMo4V8/SiO2(C8/C8NH2), which enhanced the transformation of 5-HMF to 2, 5-diformylfuran (DFF) in H2O/MIBK with 73.7% yield at 81.8% conversion than in H2O or MIBK single phase.
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.
Pyrochlore-structured polyantimonic acid (PAA) is a potential high-capacity electrode material, but its innately poor electroconductivity (~10−10 S/cm) seriously impairs its electrochemical reversibility for lithium-ion storage. Herein, we report design and synthesis of a novel V-substituted PAA (PAA-V), where V5+ are introduced to partially replace Sb5+. Owing to identical valence and close ionic radius relative to Sb5+, the V5+ cation can constitute the covalent VO6 octahedra framework without changing the pyrochlore crystal structure of PAA. As a result, the V5+-substitution is capable to modulate the electronic structure of PAA with significantly improved electrical conductivity (~10−6 S/cm for PAA-V) and meanwhile decreases the size of crystals with reduced diffusion length for Li+-ions. With varying the ratio of V5+-substitution, the PAA-V with optimized substitution molar ratio (18%) exhibits the best lithium-ion storage performance, delivering a long cycling life with high reversible capacity (731 mAh/g after 1200 cycles at 1 A/g) and outstanding rate capability (279 mAh/g at 15 A/g). More importantly, by pairing the PAA-V as anode and commercial LiFePO4 as cathode, the full cell with a limited negative/positive capacity ratio of 1.2 exhibits decent cycling stability at 1 C after 150 cycles with 85.5% capacity retention.
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.
Molybdenum disulfide (MoS2) has attracted great attention in hydrogen peroxide (H2O2) activation as a Fenton-like catalyst and cocatalyst, but the distinct mechanism of generating •OH remains unclear. In this paper, the metallic 1T phase and semiconducting 2H phase of MoS2 nanosheets were prepared and applied in MoS2/H2O2 and MoS2/Fe2+/H2O2 systems with and without light irradiation. Compared with 2H-MoS2, 1T-MoS2 exhibited superior removal rates in degrading organic pollutants in the two systems under light irradiation. However, the phase had little effect on activating H2O2 in the MoS2/H2O2 system under dark conditions. This is because it was difficult for the surface •OHads generated in the MoS2/H2O2 system to diffuse into solution, while the •OHfree radicals were mainly responsible for degrading organic pollutants. When introducing light irradiation, external energy may accelerate the desorption of •OHads into •OHfree. Interestingly, the conversion between Mo4+ and Mo5+ triggered the decomposition of H2O2 in the Fenton-like reaction, while the cycle of Mo4+/Mo6+ promoted the regeneration of Fe3+ when employing 1T-MoS2 as a cocatalyst. Meanwhile, the 1T-MoS2 catalysts exhibited excellent stability and ability to degrade various organics in the two systems. This work offers deeper insight into the MoS2-based Fenton-like and cocatalytic mechanisms.
Two-photon imaging has attracted increasing attention owing to its deep tissue imaging capabilities. Therefore, many fluorophores have been developed to satisfy its requirements. However, long-wavelength emission fluorophores with an optically tunable group are rarely developed. In this study, two long-wavelength emission fluorophores with an optically tunable amino group were successfully developed by introducing strong electron acceptor and large conjugated group to the TPQL dye. TPCO2 displayed a bright red emission (λem = 638 nm, Φ = 0.15) together with high two-photon action cross section and good water solubility, which enabled higher signal-to-background ratios and deep tissue imaging. The proof-of-concept probe (TPCONO2) was successfully applied to the high signal-to-background ratio imaging of nitroreductase in liver fibrosis, further realizing diagnosis of the degree of hypoxia during liver fibrosis.
Polyoxometalates (POMs) have conducive properties such as controlled Brønsted and Lewis acidity, high thermal stability, nontoxic nature, tunable solubility, and less corrosiveness. POMs have been extensively applied in catalytic organic reactions and have an exciting prospect for industrial applications. This review summarized recent progress in the application of POMs as acid catalysts for various organic reactions including CC bond formation, CN bond formation, CO bond formation, heterocyclic synthesis reactions, cyanosilylation and hydrolysis reactions. Various POMs catalysts including heteropoly acids (HPAs) and cationic functionalized HPAs with Brønsted acidity, HPAs supported on non-precious metal support with Brønsted acidity (or both Brønsted and Lewis acidity), transition metal substituted POMs with Lewis acidity were applied in above reactions. This review attempts to provide up-to-date information about POMs acid-catalyzed organic reactions and propose future prospects.
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