Latest ArticlesElectrosynthesis has emerged as a powerful and sustainable strategy in organic chemistry, with growing applications in carbohydrate synthesis. Herein, we report an electrochemical method for the regio- and stereo-selective O-glycosylation of exo-glycals with a wide range of substrates under mild conditions. This approach employs simple setup in an undivided cell with KOTf as electrolyte, facilitating the efficient synthesis of bioactive O-glycosides in good yields and with exclusive α-selectivity. The reaction exhibits broad substrate compatibility, accommodating both sugar- and non-sugar-based acceptors, including complex natural products and pharmaceuticals. Furthermore, gram-scale reactions proceed without loss of efficiency or stereocontrol, underscoring the practicality of this method. Mechanistic studies suggest a radical cation-based pathway. This strategy provides a robust and scalable platform for O-glycosides synthesis.
Skeletal transformations of heteroaromatic compounds via endocyclic bond cleavage have emerged as powerful tools in modern organic synthesis. Nonetheless, selective cleavage of the C2−N1 bond in indoles without the assistance of metal reagents or additives remains highly challenging, owing to the strong aromatic stabilization and intrinsic bond strength of the indole framework. Herein, we present a distinctive dimerization of C3-substituted indolyl vinyl isonitriles that proceeds through a sequential "head-to-head" cross-coupling, pyridannulation, and C2−N1 bond cleavage cascade. This transformation not only disrupts the indole core but also forges a new pyridine ring, thereby providing a metal-free and efficient route to highly functionalized 1-(2-pyridyl)-β-carbolines. Notably, an oxidative aromatic dimerization of C3- and C2-substituted heteroaryl vinyl isonitriles was developed, providing a modular route to bis-β-carbolines, bis-γ-carbolines, and their chalcogen analogues.
Palladium catalysis is regarded as a significant tool for the construction of carbon-carbon and carbon-heteroatom bond in organic synthesis. Thus the sustainable development of this type of transformations, especially designing properly, clean chemical technology, is of great importance. Recently, water as a reaction medium has been developed in both academic laboratories and in the industry, improving the reaction activity and selectivity of the organic reaction through its own properties (such as polarity, high dielectric constant). This review focuses on palladium-catalysed organic synthesis using water as solvent, summarizing relevant articles published from 2015 to 2025. Meanwhile, mechanistic studies, supported by experimental investigations, are thoroughly reviewed to elucidate the interplay between water and palladium species in facilitating bond-forming processes. Furthermore, practical applications of these aqueous-phase methodologies in the synthesis of complex natural products and pharmaceutical intermediates are showcased, underscoring their potential for scalable and sustainable chemical manufacturing.
Constructing high-contrast mechanochromic luminescent (MCL) materials with a wide range of emission color variations remains challenging. Herein, a host-guest strategy is proposed to optimize molecular MCL behavior. Two pyridinium-functionalized carbazole derivatives only exhibit a slight red-shifted fluorescence under mechanical stimulation. By forming host-guest complexes with cucurbit[n]urils (CB[n]s, n = 8 or 10), the complexes demonstrate more significant fluorescence wavelength changes after grinding. Mechanistic studies reveal that the crystallization and CB[n]’s confinement effect, synergistically induce more twisted molecular conformations and facilitate the planarization of guests under mechanical stimulation. Moreover, the host-guest complexes also exhibit outstanding MCL property in the polyvinyl alcohol (PVA) film. This strategy is both conceptually and synthetically simple and provides a promising method for preparing high-contrast MCL materials.
Porous organic polymers (POPs) are promising candidates for CO2 capture and conversion, yet the integration of direct air capture (DAC) and in situ conversion presents a fundamental challenge. Here, we report six novel water-dispersible cyclen-based POPs for efficient atmospheric CO2 capture and photoreduction. The resulting POPs (POP-1~6) exhibit exceptional aqueous-phase CO2 uptake (264–569 mg/g) with DAC capacities reaching 11–49 mg g−1 d−1. When integrated with an iron porphyrin catalyst (Fe-P) and a ruthenium-based photosensitizer, these POPs enable efficient photocatalytic atmospheric CO2-to-CO conversion with rates of 1.4–4.5 µmol g−1 h−1 and a yield up to 93% in water. These findings provide valuable insights for the further exploration of POP materials for atmospheric CO2 capture and photoreduction.
The development of novel catalysts with both robust activity and long-term stability is significant but remains a critical challenge for the degradation of emerging pollutants. Herein, CoSe nanocrystal-embedded amorphous carbon (CoSe/MC) was rationally designed and synthesized via an in situ selenization strategy. Interestingly, the unique hierarchical architecture featuring CoSe nanocrystal cores and carbon shells simultaneously exposes abundant accessible active sites and enhances stability during the Fenton-like process. Under ambient conditions, CoSe/MC achieves 97% tetracycline (TC) degradation within 2 min, with a rate constant of 3.74 × 10–2 s-1, which is 7.3-fold faster than Co3O4/C. Furthermore, CoSe/MC exhibits remarkable versatility across a wide pH range (3–11), various water sources (e.g., river/lake water), and diverse pollutants (e.g., antibiotics/dyes). Continuous-flow tests confirm long-term stability (>95% efficiency over 300 min) with negligible metal leaching (<0.1 mg/L Co). Mechanistic studies reveal a synergistic radical/non-radical pathway dominated by 1O2 generation, validated by EPR spectroscopy and quenching experiments. Density functional theory (DFT) calculations further elucidate the key role of CoSe in activating PMS by elongating O–O bonds considerably and accelerating electron transfer, which synergistically promotes O–O cleavage and the generation of reactive oxygen species during TC degradation.
The structure of photocatalysts largely determines the selectivity of CO2 conversion products in CO2 photoreduction reaction, while it is dynamic during the photoreaction. Therefore, how the dynamic structure affecting photoactivity deserves further investigation. Herein, with defective oxygen vacancies BiOCl/C3N5 nanosheets heterojunction (BiO1-xCl/C3N5) as model photocatalyst, the structure dynamic evolution in CO2 photoreduction reaction and its influence on the CO2-to-CO directional conversion were investigated. Specially, in BiO1-xCl/C3N5, the exposed Bi atoms adjected oxygen vacancies interacted with N atoms of C3N5 via the strong electrostatic effect, resulting in the shrinking crystalline structures. Once illuminated, the photogenerated electrons enriched on Bi active sites, which further strengthened the interfacial interaction between BiO1-xCl and C3N5 to a quasi-bonding state. The resulting changes in electronic structure destroyed the linear structure of CO2 molecule pre-adsorbed on Bi sites, accompanying with transformation of Bi atom valence states and heterostructure restoration. As a result, the *CO2 molecule activation and *CO intermediate desorption barrier energies both reduced, promoting the CO2-to-CO directional conversion with a CO evolution rate of 207.3 μmol g−1 h−1. This work demonstrated the importance of studying the structural dynamics evolution in photoreactions, which may be beneficial for future photocatalyst design.
Thrombin can participate in many physiological and pathological processes so that its sensitive determination is important in diagnostic and pharmaceutical fields. The content of hirudin in leech is a key criterion for determining the quality of leech. In this work, a dual-modal biosensor was constructed based on fluorescence resonance energy transfer between UCNPs and Cy5 via a thrombin-responsive peptide as a linker. Thrombin cleaved the peptide and Cy5 released, leading to the fluorescence recovery of UCNPs at a specific wavelength, which enabled the successful ratiometric fluorescence detection of thrombin. Simultaneously, Cy5 in the supernatant allowed a colorimetric detection. Hirudin inhibited the activity of thrombin, causing the intensity reduction of the corresponding fluorescence and absorbance signals. The linear ranges of the fluorescence and colorimetric detection for thrombin were 10−9 ~ 10−4 U/mL with a detection limit of 1.15 × 10−10 U/mL and 0.0025–5 U/mL with a detection limit of 1.12 × 10−3 U/mL, respectively. The linear ranges of the fluorescence and colorimetric detection for hirudin were 10−8–10−4 U/mL with a detection limit of 6.026 × 10−9 U/mL and 0.005–5 U/mL with a detection limit of 2.82 × 10−3 U/mL, respectively. This developed biosensor was further applied to the detection of anti-thrombin components in leech extract and the results showed that it had an excellent analytical performance, indicating this dual-modal biosensor provided a new specific and sensitive method for the detection of anti-thrombin components in practical sample, which is significant in quality evaluation of traditional Chinese medicine.
Direct methanol fuel cell (DMFC) is a clean energy technology that integrates high-efficiency energy conversion with environmental benefits. However, its industrial application is hindered by the sluggish kinetics of the cathode oxygen reduction reaction (ORR). This key scientific challenge has driven diversified advances in high-performance ORR electrocatalysts. This review systematically outlines the reaction mechanisms and ORR pathways in DMFC. Furthermore, it comprehensively summarizes recent advances in multi-scale modification strategies, including methanol tolerance optimization, rational design of active sites, electronic structure tailoring, surface/interface micro-environment engineering, and additional modulation approaches for enhancing ORR performance. Additionally, the mechanisms for enhancing intrinsic catalytic activity are discussed in depth, along with the elucidation of the structure-activity relationship governing catalyst performance in terms of activity, selectivity, and stability. Finally, in light of the critical challenges currently facing DMFC cathode catalysts, future directions and development pathways for catalyst design are proposed.
At present, the practical application of photocatalysis is still limited by poor charge carrier separation efficiency. The incorporation of a piezoelectric polarization field is an effective strategy to enhance the photogenerated charge transport rate and strengthen the photocatalytic activity. In this work, a NaNbO3/AgI (NBO/AgI) heterojunction was fabricated for the efficient piezo-photocatalytic degradation of sulfamethoxazole (SMZ). 91.6% of SMZ was degraded within 30 min, which far surpasses degradation under individual photocatalysis or piezocatalysis. Density functional theory (DFT) calculations reveal that electron cloud interactions form interfacial cascade channels at the NBO/AgI heterojunction interface, facilitating charge transport. Meanwhile, the piezoelectric polarization field promotes the separation and migration of photogenerated charges, inducing high-efficiency piezo-photocatalytic performance. The piezo-photocatalytic mechanism was explored by electron paramagnetic resonance, piezo-response force microscopy. Intermediate analysis confirmed the degradation pathways and reduced ecological risks of intermediates. This study provides new insights for the design of piezo-photocatalytic materials, as well as a fresh perspective on the treatment of pollutants in wastewater.
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