Latest ArticlesHerein, vacancy engineering is utilized reasonably to explore molybdenum tungsten oxide nanowires (W4MoO3 NWs) rich in O-vacancies as an advanced electrochemical nitrogen reduction reaction (eNRR) electrocatalyst, realizing further enhancement of NRR performance. In 0.1 mol/L Na2SO4, W4MoO3 NWs rich in O vacancies (CTAB-D-W4MoO3) achieve a large NH3 yield of 60.77 µg h-1 mg-1cat. at -0.70 V vs. RHE and a high faradaic efficiency of 56.42% at -0.60 V, much superior to the W4MoO3 NWs deficient in oxygen vacancies (20.26 µg h-1 mg-1cat. and 17.1% at -0.70 V vs. RHE). Meanwhile, W4MoO3 NWs rich in O-vacancies also show high electrochemical stability. Density functional theory (DFT) calculations present that O vacancies in CTAB-D-W4MoO3 reduce the energy barrier formed by the intermediate of *N-NH, facilitate the activation and further hydrogenation of *N-N, promote the NRR process, and improve NRR activity.
The high conductivity of electrocatalyst can eliminate the Schottky energy barrier at the interface of heterogeneous phases during an electrocatalytic reaction and accelerate the rapid electron transfer to the catalytic active center. Therefore, the electronic conductivity is a vital parameter for oxygen reduction reaction (ORR). Covalent triazine frameworks (CTFs) have shown great potential application as electrocatalysts in ORR with a merit of the diverse building blocks. However, the intrinsic low conductivity and high impedance of CTFs could be significant setbacks in electrocatalytic application. Herein, CTFs were constructed by introducing F and N co-modification for efficient 2e− ORR. Compared with the pristine CTF, the co-presence of F, N could increase the conductivity obviously by 1000-fold. As a result, F-N-CTF exhibits enhanced catalytic performance of H2O2 generation and selectivity towards reaction pathways. This work reveals the importance of conductivity optimization for CTFs and provides guidance for designing high conductivity non-metallic organic semiconductor catalysts for 2e− ORR.
The synthesis of polyurethanes (PUs) from the reaction of low molecular weight poly(ethylene carbonate) diol (PECD) is rarely investigated. This work reports a novel PU with excellent mechanical properties from the solution polymerization of 4,4′-diphenylmethane diisocyanate (MDI) with PECD that was derived from the copolymerization of carbon dioxide (CO2) and ethylene oxide (EO). The tensile strength, the elongation at break and 300% constant tensile strength of the PECD-PU were up to 66 ± 2 MPa, 880% ± 50% and 13 MPa, respectively, higher than the control PUs from the reaction of MDI with commercial polyethers or polyesters. The PECD-PU with high CO2 carbonate content exhibited good solvent resistance and chemical stability. Of importance, the mechanical properties and chemical resistance of PECD-PU were significantly enhanced with the increasing content of CO2, i.e., the carbonate unit in PECD. This work provides comprehensive properties of PECD-derived PUs, indicating that PECD is a competitive precursor for the preparation of PU and has broad application prospects.
The dysbiosis of oral microbiota contributes to diseases such as periodontitis and certain cancers by triggering the host inflammatory response. Developing methods for the immediate and sensitive identification of oral microorganism is crucial for the rapid diagnosis and early interventions of associated diseases. Traditional methods for microbial detection primarily include the plate culturing, polymerase chain reaction and enzyme-linked immunosorbent assay, which are either time-consuming or laborious. Herein, we reported a persistent luminescence-encoded multiple-channel optical sensing array and achieved the rapid and accurate identification of oral-derived microorganisms. Our results demonstrate that electrostatic attractions and hydrophobic-hydrophobic interactions dominate the binding of the persistent luminescent nanoprobes to oral microorganisms and the microbial identification process can be finished within 30 min. Specifically, a total of 7 oral-derived microorganisms demonstrate their own response patterns and were differentiated by linear discriminant analysis (LDA) with the accuracy up to 100% both in the solution and artificial saliva samples. Moreover, the persistent luminescence encoded array sensor could also discern the microorganism mixtures with the accuracy up to 100%. The proposed persistent luminescence encoding sensor arrays in this work might offer new ideas for rapid and accurate oral-derived microorganism detection, and provide new ways for disease diagnosis associated with microbial metabolism.
Rational design of viable routes to obtain efficient and stable oxygen evolution reaction (OER) electrocatalysts remains challenging, especially under industrial conditions. Here, we provide a solvent-steam assisted corrosion engineering strategy to directly fabricate high-entropy NiFe-LDH with spatially resolved structural order. Ammonium fluoride in methanol steam enables the formation of nanosheets while Fe3+ effectively enhances their adhesion to the semi-sacrificial nickel-iron foam (NFF), thereby conjuring up a NiFe-LDH@NFF catalyst that exhibits remarkable adaptability to robust electrochemical activation yet with excellent stability. Comprehensive measurements reveal the in-situ formation of high-valance metal oxyhydroxide and the enhancement of adsorption-desorption process. Under the industrial condition (6 mol/L KOH, 60 ℃), the NiFe-LDH@NFF exhibits excellent activity of 50 mA/cm2 at 1.55 V and high durability of over 120 h at 200 mA/cm2. We anticipate that the steam assisted strategy could promote the development of efficient non-precious electrocatalysts for hydrogen energy.
Photocatalytic overall pure water splitting is a promising method for generating green hydrogen energy under mild conditions. However, this process is often hindered by sluggish electron-hole separation and transport. To address this, a step-scheme (S-scheme) B-doped N-deficient C3N4/O-doped C3N5 (BN-C3N4/O-C3N5) heterojunction with interfacial B-O bonds has been constructed. Utilizing Pt and Co(OH)2 as co-catalysts, BN-C3N4/O-C3N5 S-scheme heterojunction demonstrates significantly enhanced photocatalytic activity for overall pure water splitting under visible light, achieving H2 and O2 evolution rates of 40.12 and 19.62 µmol/h, respectively. Systematic characterizations and experiments revealed the performance-enhancing effects of the enhanced built-in electric field and the interfacial B-O bonding. Firstly, the strengthened built-in electric field provides sufficient force for rapid interfacial electron transport. Secondly, by reducing the transport energy barrier and transfer distance, the interfacial B-O bonds facilitate rapid recombination of electrons and holes with relatively low redox potential via the S-scheme charge-transfer route, leaving the high-potential electrons and holes available for H+ reduction and OH− oxidation reactions. Overall, the photocatalytic efficiency of BN-C3N4/O-C3N5 S-scheme heterojunction was significantly improved, making it a promising approach for green hydrogen production through overall pure water splitting.
As battery technology evolves and demand for efficient energy storage solutions, aqueous zinc ion batteries (AZIBs) have garnered significant attention due to their safety and environmental benefits. However, the stability of cathode materials under high-voltage conditions remains a critical challenge in improving its energy density. This review systematically explores the failure mechanisms of high-voltage cathode materials in AZIBs, including hydrogen evolution reaction, phase transformation and dissolution phenomena. To address these challenges, we propose a range of advanced strategies aimed at improving the stability of cathode materials. These strategies include surface coating and doping techniques designed to fortify the surface properties and structure integrity of the cathode materials under high-voltage conditions. Additionally, we emphasize the importance of designing antioxidant electrolytes, with a focus on understanding and optimizing electrolyte decomposition mechanisms. The review also highlights the significance of modifying conductive agents and employing innovative separators to further enhance the stability of AZIBs. By integrating these cutting-edge approaches, this review anticipates substantial advancements in the stability of high-voltage cathode materials, paving the way for the broader application and development of AZIBs in energy storage.
Ethylene carbonate (EC) is the conventional and promising solvent to achieve high energy lithium metal battery. However, the innate low energy level of lowest unoccupied molecular orbital (LUMO) in EC makes it incompatible with lithium metal, causing uncontrolled lithium growth and low Coulombic efficiency (CE). Herein, we introduced bis(2,2,2-trifluoroethyl) carbonate (TFEC), a carbonate with a strong electron-withdrawing effect (-CF3), which enhances the stability of EC at electrode interface by reducing ion-dipole interactions between Li+ and EC. As the interaction between Li and EC weakens, TFEC and more PF6− anions coordinate with Li+, promoting the formation of contact ion pairs (CIPs) and aggregates (AGGs), thereby increasing the inorganic composition within the solid electrolyte interphase. Additionally, the distinct solvated sheath structure favors the decomposition of fluorinated solvents and PF6− anions, forming inorganic-rich electrode-electrolyte interfaces (SEI and CEI), thereby ensuring high stability for both the Li anode and high-voltage cathode. Hence, when applied in the full-cell LiLiMn0.8Fe0.2PO4, it displays consistent cycling performance, exhibiting minimal capacity decay with a retention rate of 62.5% after 800 cycles, substantially surpassing that of cells using base electrolytes (29.8%).
Disulfidptosis, a novel mechanism of programmed cell death through the disruption of tumor metabolic symbiosis (TMS), has showed tremendous potential in cancer therapy. However, the efficacy of disulfidptosis is limited by poor permeability of drugs in solid tumors. Herein, hydrogen sulfide (H2S) and near-infrared (NIR) light-driven nanomotors (denoted as HGPP) have been constructed to efficiently penetrate tumors and induce disulfidptosis. HGPP demonstrate glutathione (GSH)-responsive release of H2S, which combined with NIR light-induced photothermal effect drive HGPP movement to facilitate deep tumor penetration. The released H2S induces tumor acidosis and disrupts TMS, where disulfide accumulation following cell starvation leads to disulfidptosis. In addition, HGPP induce hepatoma specific cellular uptake and catalyze the conversion of glucose and oxygen to produce hydrogen peroxide (H2O2), leading to glucose starvation. Overall, this study has developed a multifunctional Janus nanomotor that provides a novel strategy for disulfidptosis-based solid tumor therapy.
Photocatalytic hydrogen peroxide (H2O2) production has been considered as a promising strategy for H2O2 synthesis due to its environmentally friendly. Among various photocatalysts, carbon nitride-based materials are excellent candidates for H2O2 production because of their excellent visible-light response, low cost and high stability. In this review, we summarize in detail the research progress on the photocatalytic production of H2O2 by carbon nitride. First, we summarize the basic principles of photocatalysis and photocatalytic H2O2 production. Second, the classification and modification methods of carbon-nitride-based materials are discussed, including morphology modulation, noble metal loading, defect control, heterojunction regulation, molecular structure engineering and elemental doping. Finally, the different in-situ applications of H2O2 via photosynthesis were discussed, including disinfection and antibiotic resistant genes degradation, organic pollutants degradation, medical applications and fine chemical synthesis. This review brings great promise for in-situ H2O2 photosynthesis, which is expected to serve as a key component in future applications.
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