Latest ArticlesNitrate (NO3−) electroreduction reaction (NO3−RR) provides an attractive and sustainable route for NO3− pollution mitigation or energy-saved ammonia (NH3) synthesis. In this work, high-quality B and Fe co-doped Co2P hollow nanocubes (B/Fe-Co2P HNCs) are successfully synthesized though simultaneous boronation-phosphorization treatment, which reveal outstanding selectivity, activity, stability for the NO3− to NH3 conversion in neutral electrolyte because of big surface area, fast mass transport, superhydrophilic surface, and optimized electronic structure. B/Fe-Co2P HNCs can achieve the high NH3 yield rate (22.67 mg h−1 mgcat−1) as well as Faradaic efficiency (97.54%) for NO3−RR, greatly outperforming most of non-precious metal based NO3−RR electrocatalysts.
Deoximation is an important transformation in synthetic industry. It can be employed in protection, characterization and purification of the carbonyls, and in the synthesis of ketones from non-carbonyl molecules. In the field, oxidative deoximation reaction can utilize the driving force caused by the oxidation process so that the reaction can occur under relatively mild conditions. Recently, we designed and prepared polyaniline-supported molybdenum (Mo@PANI) just by immersing PANI into the EtOH/H2O solution of MoCl5. The material was successfully applied as the efficient catalyst for oxidative deoximation reactions, which were performed in ethanol using H2O2 as the clean oxidant. The substrate scope of the reaction was wide. It could be applied on heterocycle-containing substrates, making this protocol preferable for pharmaceutical intermediate synthesis. Since Mo is a necessary trace element for both animals and plants, this method is environment-friendly and is suitable for large-scale preparation. This work as the first example of Mo-catalyzed oxidative deoximation reaction may inspire novel ideas for both catalyst design and synthetic process development.
Multifunctional molecules with both optical signal and pharmacological activity play an important role in drug development, disease diagnosis, and basic theoretical research. Aminopeptidase N (APN), as a representative tumor biomarker with anti-tumor potential, still lacks a high-precision theranostic probe specifically targeting it. In this study, a novel quaternity design strategy for APN theranostic probe was developed. This proposed strategy utilizes advanced machine learning and molecular dynamics simulations, and cleverly employs the strategy of conformation-induced fluorescence recovery to achieve multi-objective optimization and integration of functional fragments. Through this strategy, a unique "Off–On" theranostic probe, ABTP-DPTB, was ingeniously constructed to light up APN through fluorescence restoration, relying on conformation-induced effects and solvent restriction. Differ from the common diagnostic probes, the intelligent design with non-substrated linkage makes ABTP-DPTB for long-term in-situ imaging. The fabricated probe was used for detecting and inhibiting APN in various environments, with a better in vitro inhibitory than golden-standard drug bestatin.
Cyclic polymers are a class of polymers that feature endless topology, and the synthesis of cyclic polymers has attracted the attention of many researchers. Herein, cyclic polymers were efficiently constructed by self-folding cyclization technique at high concentrations. Linear poly((oligo(ethylene glycol)acrylate)-co-(dodecyl acrylate)) (P(OEGA-co-DDA)) precursors with different ratios of hydrophilic and hydrophobic moieties were synthesized by reversible addition-fragmentation chain transfer (RAFT) polymerization using a bifunctional chain transfer agent with two anthryl end groups. The amphiphilic linear precursors underwent the self-folding process to generate polymeric nanoparticles in water. By irradiating the aqueous solution of the nanoparticles with 365 nm UV light, cyclic polymers were synthesized successfully via coupling of anthryl groups. The effects of the ratios of hydrophilic and hydrophobic moieties in linear P(OEGA-co-DDA) copolymers and polymer concentration on the purity of the obtained cyclic polymers were explored in detail via 1H nuclear magnetic resonance (1H NMR), dynamic light scattering (DLS), UV‒visible (vis) analysis, three-detection size exclusion chromatography (TD-SEC) and transmission electron microscopy (TEM). It was found that by adjusting the content of the hydrophilic segments in linear precursors, single chain polymeric nanoparticles (SCPNs) can be generated at high polymer concentrations. Therefore, cyclic polymers with high purity can be constructed efficiently. This method overcomes the limitation of traditional ring-closure method, which is typically conducted in highly dilute conditions, providing an efficient method for the scalable preparation of cyclic polymers.
Enaminones, which possesses both the nucleophilic enamine as well as electrophilic enone structures, are well known versatile building blocks in organic synthesis. Meanwhile, visible light-mediated reactions have emerged as useful synthetic strategy with enhanced sustainability. Around the last decade, various photochemical transformations of enaminones have been developed to construct cyclic or acyclic compounds. In this review, we describe the recent advances in visible light-mediated chemical transformations of enaminones. Detailed discussion on the reaction mechanism of the related reactions is given to provide guide to the reader. Finally, a summary on the existing challenges and the future outlook towards the development of practical photocatalytic reactions of enaminones is also presented.
A charge transfer complex (CTC)-enabled photoreduction of ether phosphonium salts for the generation of oxyalkyl radicals was described. The photoreduction provides a convenient method to achieve selective oxyalkylation of enamides with broad substrate scope. The method features operational simplicity, mild and inherent green conditions.
Modulating surface charge redistribution based on interface and defect engineering has been considered as a resultful means to boost electrocatalytic activity. However, the mechanism of synergistic regulation of heterojunction and vacancy defects remains unclear. Herein, a Vs-CoP-CoS2/C n-n heterojunction with sulfur vacancies is successfully constructed, which manifests superior electrocatalytic activity for oxygen evolution, as demonstrated by a low overpotential of 170 mV to reach 10 mA/cm2. The experimental results and density functional theory calculations testify that the outstanding OER performance of Vs-CoP-CoS2/C heterojunction is owed to the synergistic effect of sulfur vacancies and built-in electric field at n-n heterogeneous interface, which accelerates the electron transfer, induces the charge redistribution, and regulates the adsorption energy of active intermediates during the reaction. This study affords a promising means to regulate the electrocatalytic performance by the construction of heterogeneous interfaces and defects, and in-depth explores the synergistic mechanisms of n-n heterojunction and vacancies.
Saccharide sensing is a very meaningful research topic as saccharides are involved in many biological activities. However, it is challenging to design molecular sensors for saccharides because this family of compounds is hydromimetic in aqueous solutions and shares a similar chemical structure. In this review, research progress in the development of porphyrin-based saccharide sensors is described with representative examples. We focus on using porphyrin as the signal reporter because porphyrins exhibit unique advantages in high chemical stability, long emission wavelength, and multiple structural modification strategies. Reported literature results have been classified into mainly two sections according to the general working principles of the porphyrin sensor molecules. In the first section, recognition unit, design strategy and sensing performance of traditional porphyrin-based selective saccharide sensors are discussed. While in the second section, development of porphyrin-based sensor arrays for pattern recognition of saccharides has been summarized. Looking through the design strategy and sensing performance of reported achievements, it is reasonable to anticipate a bright future for designing practical porphyrin-based saccharide sensors.
Improving the performance of all-small-molecule organic solar cells (ASM-OSCs) largely depends on the design and application of novel donors with appropriate crystallinity. Extending molecular conjugation is an effective method for regulating molecular stacking and crystallinity. In this work, we successfully designed and synthesized two novel acceptor-donor-donor-donor-acceptor (A-D-D-D-A) type oligomeric donors with three dithieno[2,3-d:2’,3’-d’]benzo[1,2-b:4,5-b’]dithiophene (DTBDT) as the central unit, named as 3DTBDT-Cl and 3DTBDT, depending on with and without chlorine substitution on the thiophene side chains. We found that the introduction of chlorine atoms makes the blend films display stronger crystallinity but with large-scale phase separation morphology and more defects, which eventually leads to a power conversion efficiency (PCE) of only 10.83%, whereas the blend films based 3DTBDT with appropriate crystallinity achieved 13.74% PCE. Compared with 3DTBDT-Cl/L8-BO, the 3DTBDT/L8-BO films exhibited a nanoscale bi-continuous interpenetrating network morphology with a smaller domain size and more suitable crystallinity, which guarantees the corresponding devices obtained more efficient exciton dissociation, efficient charge transport, reduced bimolecular recombination, and performed more balanced carrier mobility. These results demonstrated that regulating the crystallinity of oligomeric donors to obtain the desired phase separation morphology in the blend films could facilitate further improving the performance of ASM-OSCs.
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