Latest ArticlesMetal phosphosulfides have been recognized as advanced anode materials for sodium/potassium ion batteries due to their high theoretical capacities and the incorporation of the advantage of metal sulfides and phosphates. However, they also suffer from the shortcomings of frustrating cycling stability due to the large volume expansion and unsatisfactory electrical conductivity. Herein, hexapod cobalt phosphosulfide nanodots based nanorods encapsulating into N, P, and S hetero-atoms tri-doped carbon framework (CoP/CoS2@NPSC) have been triumphantly designed and synthesized. The six nanorods constructed hexapod framework and multi-atom doped carbon matrix not only provides more active sites, but also contribute to maintain the structure integrity from avoiding the agglomeration of internal CoP and CoS2 nanodots. The synergistic effect between CoP and CoS2 components, as well as the CoP/CoS2 and the NPSC carbon framework can improve the electrochemical conductivity. Besides, the kinetics analysis demonstrated that N/P/S tri-doping could greatly increase the interlayer distance and introduce enough active sites, which effectively facilitate the transport, adsorption, insertion and diffusion of Na+ and K+. CoP/CoS2@NPSC demonstrated excellent electrochemical properties and battery performances including excellent cycle stability with 404.63 mAh/g at 5.0 A/g around 700 cycles for SIBs and 115.33 mAh/g at 5.0 A/g around 800 cycles for PIBs. This presented strategy establishes a novel and adaptable method for the integration of doped carbon with metal phosphosulfide and guides a new research approach and direction for secondary batteries electrode materials.
Established evidence has unveiled two strategies for treating cancer: depleting tumor-associated macrophages (TAMs) and reprogramming M2-like TAMs into an antitumor M1 phenotype. Here, we designed novel pH-sensitive biomimetic hybrid nanovesicles (EDHPA) loaded with doxorubicin (DOX). DOX@EDHPA can specifically target TAMs by activating macrophage-derived exosomes (M1-Exos) and anisamide (AA) as cancer-specific targeting ligands. In vitro and in vivo studies demonstrated that DOX@EDHPA could efficiently be delivered to the tumor site and taken up by cells. Meanwhile, it synergistically enhanced immunogenic cell death (ICD) and induced a subsequent antigen-specific T cell immune response. The tumor inhibitory rate of the DOX@EDHPA group was 1.42 times that of the free DOX group. Further analysis showed that the excellent antitumor effects of DOX@EDHPA should ascribe to the homing effect of M1-Exos on macrophages and the repolarization to antitumor M1 TAMs, which induced the elevated secretion of pro-inflammatory factors. Therefore, the hybrid EDHPA targeting TAMs to reshape the tumor microenvironment constituted a novel immunochemotherapy strategy to inhibit tumor growth.
Prostaglandin E2 (PGE2) serves as the ultimate mediator of fever induced by inflammatory factors. In contrast to cyclooxygenase inhibitors that suppress arachidonic acid metabolism, antipyretic herbs possess a well-established clinical history in effectively managing fever. However, the specific mechanisms underlying their efficacy remain unclear. Following the screening for lead compounds that inhibit PGE2 from antipyretic herbs, alkynylated active molecule probes were designed and synthesized to track and identify potential targets. The target investigation revealed that three antipyretic compounds, namely cinnamaldehyde, 2,4-decadienal, and perillaldehyde, containing α,β-unsaturated aldehyde groups irreversibly targeted the microsomal PGES1-TM4 helix (mPGES1-TM4) at Ser139. This specific interaction effectually inhibited PGE2 production in the cerebral vasculature, leading to exert potent antipyretic effects. α,β-Unsaturated aldehydes targeting mPGES1-TM4 offer a new approach for antipyretic effects with significant potential for various applications.
Mo2N has been identified as a highly promising carrier for electrocatalysis. However, its complex synthesis method, use of toxic gases, and serious effects on supported noble metals catalyst during high-temperature sintering processes have seriously affected its hydrogen evolution reaction (HER) activity and stability. Here, we report an efficient strategy for synthesizing Mo2N using the high temperature shock (HTS) method in just 1.67 s, while also uniformly loading Ru onto Mo2N nanosheets. The HTS enables the homogeneous dispersion of the noble metal Ru, leading to an increased electrocatalytic activity, along with a strong charge transfer between Mo2N and Ru. Ru/Mo2N exhibited an overpotential of 66 mV at 10 mA/cm2 in 1 mol/L KOH. In the evaluation of catalytic activity, Ru/Mo2N demonstrates superiority over commercial Pt/C catalysts in terms of mass activity (1.71 A/mgRu vs. 0.91 A/mgPt at 200 mV) and turnover frequency (1.41 s−1 vs. 0.18 s−1 at 100 mV). This result provides a rational and effective pathway for the preparation of efficient electrocatalysts.
The Fenton method is an effective technology for the removal of organic materials from wastewater. In this work, an induced catalyst Fe3O4 was synthesized by a hydrothermal method, and the modulation of the chemical composition of Fe3O4 crystals was achieved under the microwave shock method with the same effect as that of calcination treatment. Fe3O4 catalyst for the removal of the dye Rhodamine B (RhB) from polluted wastewater under microwave (MW), H2O2 system. The results showed that Fe3O4 nanomicrospheres prepared by microwave shock exhibited superior catalytic activity under the conditions of 500 W, 0.4 mol/L H2O2 and10 mg/L RhB, and the removal rate of RhB reached 98.5% after 10 min. The Fe3O4 catalysts also exhibited good stability and degradation efficiency. Electron paramagnetic resonance experiments confirmed that •OH plays a major role in the rapid degradation of RhB. Under microwave action, the catalyst produces electron-hole pairs, in which the holes react with OH− produced by water ionisation to form •OH, and the microwave-treated Fe3O4 produces more active species. Fe3+ and Fe2+ serve as microwave catalytic activity centers and Fenton catalytic activity centers, respectively. This research demonstrates that optimizing the Fe2+/Fe3+ ratio significantly enhances the degradation efficiency of RhB. This study presents novel views regarding the mechanism of microwave synergistic catalyst-induced Fenton.
Sulfates are always promising short-wave ultraviolet (UV) nonlinear optical (NLO) candidates, if their birefringence could be greatly improved. Here, in terms of the insufficient birefringence, the unity of heteroleptic tetrahedral groups and triangular ones was proposed and implemented. Thus, a new semi-organic crystal, [C(NH2)3]S3O6 (G2S3O6), was obtained, which is composed of [S3O6]2− and [C(NH2)3]+ groups. It exhibits excellent optical properties with a short absorption cutoff edge of 218 nm, a strong NLO response of 1.4 × KH2PO4, and more especially, a large birefringence of 0.097@546 nm. This birefringence leap makes the G2S3O6 crystal achieve a phase-matching behavior under a 532 nm laser. Thus, the synergy of [S3O6]2− and [C(NH2)3]+ groups results in excellent optical performances. This finding opens a new horizon for exploring novel UV NLO crystals.
The oxygen evolution reaction (OER) is the bottleneck in the overall photocatalytic splitting of water. The active sites (terminal titanium or bridging oxygen) and active species (molecular or dissociative water) of the initial step of the photocatalyzed OER on the prototypical photocatalyst TiO2, remain debatable. Herein, the photocatalytic chemistry of monolayer water on oxygen-pretreated TiO2(110) (o-TiO2(110)) and reduced TiO2(110) (r-TiO2(110)) surfaces initiated by 400 nm light illumination was investigated by time-dependent two-photon photoemission spectroscopy (TD-2PPE). The photoinduced reduction of the H2O/o-TiO2(110) interface rather than the H2O/r-TiO2(110) interface was detected by TD-2PPE. The difference in 2PPE originated from the presence of the terminal hydroxyl anions (OHt¯) on H2O/o-TiO2(110), as identified by X-ray photoelectron spectroscopy and temperature-programmed desorption. Therefore, the evolution of the electronic structure of H2O/o-TiO2(110) was attributed to the photocatalyzed oxidation of the terminal hydroxyl anions, which most likely formed gaseous •OH radicals, reducing the interface. This work suggested that the oxidation of hydroxyl anions on top of the terminal titanium ions on TiO2, which were excluded previously in solution, need to be considered in the mechanistic studies of the photocatalyzed OER.
Herein, we report an iron-promoted carbonylation-rearrangement of α-aminoaryl-tethered alkylidene cyclopropanes with CO2 to generate quinolinofuran derivatives. A variety of quinolinofuran derivatives are obtained in moderate to excellent yields, and two promising luminescent material molecules have been synthesized using the developed method. The Lewis acid FeCl3 was introduced into this reaction, which effectively promoted the ring opening and rearrangement of cyclopropanes. This reaction features a broad substrate scope, satisfactory functional group tolerance, facile scalability, and easy derivatization of the products.
Maintaining high metal dispersion of supported metal catalysts to achieve superior reactivity under harsh conditions poses one of the main challenges for their practical applications. Constructing and regulating the strong metal-support interactions (SMSI) by diverse methodologies has emerged as one of the promising approaches to fabricating robust supported metal catalysts. In this study, we report an L-ascorbic acid (AA)-inducing strategy to generate SMSI on a titania-supported gold (Au) catalyst after high-temperature treatment in an inert atmosphere (600 ℃, N2). The AA-induced SMSI can efficiently stabilize Au nanoparticles (NPs) and preserve their catalytic performance. The detailed study reveals that the key to realizing this SMSI is the generation of oxygen vacancies within the TiO2 support induced by the adsorbed AA, which drives the formation of the TiOx permeable layer onto the Au NPs. The strategy could be extended to TiO2-supported Au catalysts with different crystal phases and platinum group metals, such as Pt, Pd, and Rh. This work offers a promising novel route to design stable and efficient supported noble metal catalysts by constructing SMSI using simple reducing organic adsorbent.
Polyphosphazene with phenoxy or 4-ester phenoxy as pendent groups are demonstrated as both ligands and host matrices for CsPbBr3 perovskite nanocrystals (NCs). These polymers produced flexible nanocomposite films with excellent NCs dispersion, optical transparency and stability in various extreme conditions. Both films remained stable even after 30 days of air storage. CsPbBr3/poly[bis(phenoxy phosphazene)] (PBPP) delivered better air and light stability, and CsPbBr3/poly[bis(4-esterphenoxy)phosphazene] (PBEPP) exhibited superior water and heat resistance. CsPbBr3/PBEPP showed a greater increase in fluorescence intensity under 365 nm UV light and demonstrated a 10% luminescence increase after 96 h of water immersion and even at high temperature (150 ℃). These findings thus provide new insight into flexible luminescent CsPbBr3 films with high stability in optoelectronic applications.
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