Latest ArticlesThe application of DNA hybridization technology, grounded in Watson-Crick base pairing, has facilitated the rational design of framework nucleic acids (FNAs) featuring adaptable shapes and dimensions. These nanostructures exhibit remarkable stability and reproducibility, making them promising candidates for biomedical applications. Among various FNAs, tetrahedral FNAs (tFNAs), first introduced by Turberfield, are nanoscale assemblies of oligonucleotides that possess unique physical, chemical, and biological properties. Previous studies have demonstrated that tFNAs exhibit excellent cellular uptake, enhanced tissue permeability, and strong capabilities to promote cell migration, proliferation, and differentiation. Moreover, the intrinsic ability of tFNAs to efficiently penetrate cell membranes allows tFNAs to serve as versatile carriers for small-molecule drugs or functional oligonucleotides, thereby exerting significant anti-inflammatory, antioxidant, antibacterial, and immunomodulatory effects. These features highlight the therapeutic potential of tFNA-based complexes in skin, mucosal, and barrier tissue repair and regeneration. This review provides a comprehensive analysis of recent advances in the application of tFNAs for the prevention and treatment of skin, mucosal, and barrier tissue diseases, with a focus on their mechanisms of action and future prospects in regenerative medicine and targeted therapies.
Polymer-electrolyte-based solid-state Li metal batteries with high-voltage Ni-rich cathodes are promising energy storage technologies owing to their favorable security and high energy densities. However, operating in wide temperature range and at high voltage is a tough challenge for them. Herein, F/N donating fluorinated-amide-based plasticizers regulated polymer electrolyte capable of enabling high-voltage Li||LiNi0.8Co0.1Mn0.1O2 (NCM811) batteries with excellent performance in wide temperature range is developed. F/N donating fluorinated-amide-based plasticizers significantly improve ionic conductivity (1.52 mS/cm at 30 ℃), enhance oxidation stability (5.0 V vs. Li+/Li) and fabricate robust LiF/Li3N-rich electrode-electrolyte interphases, which significantly improve the interface stability of Li metal anode and NCM811 cathode. The designed polymer electrolyte is nonflammable and has excellent dimensional stability at 200 ℃. Capitalizing on these advantageous attributes, the Li||NCM811 cells show excellent cycle stability and rate capability from −20 ℃ to 60 ℃ at high voltages (~4.6 V), and under high-loading full cell condition, which display impressive capacity retention of 84.4% after 1000 cycles and ultrahigh capacity of 154.8 mAh/g at 10 C. This work provides a rational design strategy of polymer electrolytes for wide-temperature high-energy solid-state Li metal batteries.
Organic pollutants, a pivotal factor in water pollution, have persistently menaced the aquatic ecosystem, as well as the sustainable development of human health, economy, and society. Consequently, there is an urgent need for advanced techniques to efficiently eliminate organic micropollutants from water. Here, we present the synthesis of three nonporous cavitand-crosslinked polymers capable of adsorbing diverse organic pollutants from aqueous solutions. These polymeric adsorbents exhibit outstanding adsorptive performance towards the tested micropollutants, characterized by high apparent adsorption rate constants (kobs) and maximum adsorption capacities (qmax, e). Notably, Compound NCCP-1 demonstrated a remarkable qmax, e of 459 mg/g for bisphenol A (BPA), ranking among the highest values reported for organic polymer adsorbents. In-depth investigation of the adsorption mechanism of the nonporous polymer revealed that it involves the recognition of pollutants by the deep cavities of the cavitand moieties and the interstitial spaces between them, primarily mediated by the hydrophobic effect. Furthermore, NCCP-1 was applied in situ water purification simulations and was proven to maintain its removal efficiency over more than four cycles, highlighting its potential for practical applications in water treatment.
Carbenes as one of the most important class of intermediates have been widely utilized in various organic synthetic transformations. Carbene insertion-initiated ring-opening reactions of cyclic ethers offer a valuable strategy for constructing new carbon-oxygen bonds. In comparison with traditional thermal or metal-mediated carbene transfer reactions, visible-light-promoted multi-component reaction strategy provides a mild and eco-friendly approach to access densely functionalized molecules. Recently, visible-light-induced multi-component carbene transfer reactions of diazo compounds have been rapidly developed and attracted a great deal of research interest of chemists owing to their advantages of simple operation, mild condition, high atom economy and rich structural diversity. This paper summarizes the recent research progress on the visible-light-promoted multi-component carbene transfer reactions of diazo compounds via ring-opening of cyclic ethers with various nucleophiles. The reaction patterns of different nucleophiles and their corresponding mechanism are described in this review. The future research direction and challenges in this area are also discussed.
Catalytic CO2-to-methanol conversion presents a synergistic approach for concurrent greenhouse gas abatement and sustainable energy carrier synthesis. Single-atom catalysts (SACs) with maximized atomic utilization, tailored electronic configurations and unique metal-support interactions, exhibit superior performance in CO2 activation and methanol synthesis. This review systematically compares reaction mechanisms and pathways across thermal, photocatalytic and electrocatalytic systems, emphasizing structure-activity relationships governed by active sites, coordination microenvironments and support functionalities. Through case studies of representative SACs, we elucidate how metal-support synergies dictate intermediate binding energetics and methanol selectivity. A critical analysis of reaction parameters (e.g., temperature, pressure) reveals condition-dependent catalytic behaviors in thermal system, with fewer studies in photo/electrocatalytic systems identified as key knowledge gaps. While thermal catalysis achieves industrially viable methanol yields, the scalability is constrained by energy-intensive operation and catalyst sintering. Conversely, photo/electrocatalytic routes offer renewable energy integration but suffer from inefficient charge dynamics and mass transport limitations. To address the challenges, we propose strategic research priorities on precise design of active sites, synergy of multiple technological pathways, development of intelligent catalytic systems and diverse CO2 feedstock compatibility. These insights establish a framework for developing next-generation SACs, offering both theoretical foundations and technological blueprints for developing carbon-negative catalytic technologies.
Pseudomonas aeruginosa is an opportunistic pathogen responsible for severe nosocomial infections. This multidrug-resistant bacterium can cause pneumonia and cystic fibrosis, both of which are associated with high morbidity and mortality rates. The lipopolysaccharide of P. aeruginosa serves as an attractive target for the development of effective glycoconjugate vaccines. In this article, we report the first chemical synthesis of the highly challenging tetrasaccharide repeating unit of the P. aeruginosa serotype O3 O-antigen using a two-directional [1+(2 + 1)] glycosylation strategy. The synthesis is particularly challenging due to the poor nucleophilicity of the axial C4 hydroxyl group of L-galactose and the steric hindrance imposed by the 3S-hydroxybutyryl (Hb) chain. Furthermore, the presence of an acetyl group at the ortho position relative to the glycosylation site on L-galactose can lead to undesirable acetyl migration. Additionally, it is noteworthy that the selective removal of a 2-naphthylmethyl ether (Nap) during the late stages of synthesis, particularly in the presence of multiple benzyl groups, can be somewhat challenging to predict. Through the careful selection of synthetic strategies, building blocks, and optimized reaction conditions, we achieved the stereoselective glycosylations, selective oxidation of primary alcohols, remarkable enhancement of acceptor activity, and efficient introduction of the 3S-Hb group. The synthetic methodology presented in this work serves as a valuable reference for the preparation of structurally related oligosaccharides. By incorporating an aminopropyl linker, the target tetrasaccharide facilitates glycan microarray preparation and in vivo immunological assessments, thereby accelerating progress toward a synthetic glycoconjugate vaccine for P. aeruginosa.
Portable ratiometric fluorescent platforms have emerged as promising tools for multifarious detection, yet remain unexplored for point-of-care monitoring doxorubicin (DOX), one of clinically antineoplastic drugs. To this end, we herein develop a portable self-calibrating platform namely carbon dots (C-dots)-embedded hydrogel sensors with a smartphone-assisted high-throughput imaging device, for DOX sensing. The prepared green-emitting (λem = 508 nm) and negatively-charged C-dots (−11.40 ± 1.21 mV), which have sufficient spectral overlap with the absorption band of DOX (~500 nm), can strongly bind with positively-charged DOX molecules by electrostatic attraction effects. As a result, DOX molecules are selectively and rapid (20 s) determined with a detection limit of 10.26 nmol/L via Förster resonance energy transfer processes, demonstrating a remarkably chromatic shift from green to red. Further integrated with a 3D-printed smartphone-assisted device, the platform enabled high-throughput quantification, achieving recoveries of 96.40%–101.85% in human urine/serum (RSDs < 2.94%, n = 3). Notably, the dual linear detection ranges of the platform align with the reported clinical DOX concentrations in urine and plasma (0–4 h post-administration), validating their capability for direct quantification of DOX in clinical samples without special pre-treatment processes. By virtue of attractive analytical performances and robust feasibility, this platform bridges laboratory precision and point-of-care testing needs, offering promising potential for personalized chemotherapy and multiplexed analyte screening.
The hydrogen evolution reaction (HER) is crucial for hydrogen production and sustainable energy storage. Molybdenum disulfide (MoS2), a representative transition metal dichalcogenides (TMDs), shows potential as an HER catalyst but suffers from limited performance due to poor charge transfer and interfacial effects. Here, we report a salt-assisted chemical vapor deposition (CVD) method for synthesizing high-quality tungsten ditelluride (WTe2) with tunable morphologies using alkali halides (NaCl, KCl and LiCl). The prepared WTe2 nanoribbons and hexagonal nanosheets exhibit morphology-dependent electrical conductivity, with nanosheets showing superior performance. To evaluate WTe2 as a contact electrode, WTe2−MoS2 heterostructures were fabricated and compared with graphene-MoS2 counterparts. The WTe2−MoS2 heterostructure exhibits a superior Tafel slope of 111.57 mV/dec and an overpotential of 298 mV at -10 mA/cm2, significantly outperforming graphene-based electrodes. This improvement is attributed to the excellent conductivity of WTe2 and reduced interfacial Schottky barriers. Moreover, we systematically investigate the influence of WTe2 thickness on HER performance and assess the electrochemical durability and structural stability of the heterostructure, further confirming the effectiveness of WTe2 as a contact electrode for enhancing the HER activity of MoS2. This study offers a novel approach for enhancing the HER performance of MoS2 through controlled WTe2 growth and application as a contact electrode. Our findings provide valuable insights into the synthesis of high-quality WTe2 and broaden the potential applications of two-dimensional materials in energy catalysis.
Cu electrocatalysts have been demonstrated to have unique ability to reduce CO2 to various high value-added C2 products like ethylene and alcohols. However, realizing high selectivity of C2 products are still a main challenge due to complex CO2 electroreduction pathways and small opportunity of C–C coupling reactions. Here, we found the origin of enhanced CO2 electroreduction reaction activity and product selectivity towards C2 products and C–C coupling mechanism at halogen atoms-adsorbed Cu/H2O interfaces, the corresponding CO2 electroreduction evolution mechanisms at the halogen atoms-modified Cu/H2O interfaces are systematically studied via theoretical modeling and calculations. The calculated results indicate that halide anions modifications are beneficial to CO dimerization into OCCO dimer, especially Cl−-adsorbed Cu(111)/H2O interface has the optimum activity and selectivity towards OCCO dimer, subsequent Cl-adsorbed Cu(111)/H2O interface can selectively reduce CO2 into C2H4 product. The function relationship between adsorption free energy of Cl atom and electrode potential explain why the adsorption of Cl− can enhance selectivity of C2H4 product. The determinations of onset potentials indicate that electroreduction pathways of CO2 towards C2H4 product are facile to take place and further explain the origin of the significantly enhanced CO production activity and C2H4 product selectivity. This work on selective realization of CO2 electroreduction towards C2H4 product via Cl−-modified Cu(111)/H2O interface provide a theoretical guideline for how to selectively realize other high value-added C2 products.
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