Latest ArticlesThe cycloaddition of epoxides and CO2 has been achieved by using the designed upper-rim functionalized calix[4]arene organocatalyst in aqueous at a mild temperature under normal pressure. The upper rim of this novel calix[4]arene organocatalyst contains two hemisquaramides at the 1,4-positions. A variety of cyclic carbonate derivatives were obtained in good yields, demonstrating excellent compatibility with various functional groups. The π···π supramolecular interaction between the calixarene cavity and epoxide substrate may also play a significant role in facilitating this cycloaddition process. Additionally, this novel reaction offers a valuable complementary approach to synthesizing cyclic carbonates from epoxides and CO2.
Here, Friedel–Crafts (FC) reaction is used to synthesize a purely organic cage in a one-pot manner. The trigonal prismatic cage is composed of two trisfuran platforms, bridged by three phenanthrene pillars each bearing two methoxy (OMe) units. The organic cage exhibited good kinetic inertness, allowing for a synthetic post-functionalization. During this transforming process, the electron-donating methoxy (OMe) groups were converted into electron-withdrawing carbonyl groups without any degradation on the cage framework. The cage exhibits multiple guest recognition modes. The oxygen atoms as the Lewis base present in either methoxy or carbonyl before and after post-functionalization, endow the cage with the ability to recognize Lewis acidic guests such as alkali cations. The OMe and carbonyl units grated on the phenanthrene pillars endow the cage with an π-electron-rich and π-electron-deficient cavity, respectively, where π-electron-deficient and π-electron-rich guests can be accommodated.
Polyfunctionalized axial-chiral 2-arylpyridines are important class of chiral entities in organic synthesis and drug discovery. However, practical synthesis of such structures remains underdeveloped. Herein, we report a novel synthetic method via simple cobalt-catalyzed [2 + 2 + 2] cycloaddition reactions of easily accessible diynes with nitriles. A wide range of polyfunctionalized axial-chiral 2-arylpyridine derivatives were obtained with high enantioselectivities and atom economy by using 2-methyl tetrahydrofuran (2-MeTHF) as a green solvent. Notably, the axial-chiral 2-arylpyridine N-oxide compounds and chiral bispyridine derivatives have been accessible in high efficiency using this simple protocol. The mechanism and origin of regioselectivity of this reaction was revealed using DFT calculation profiles.
Core-shell magnetic polymer microspheres with mesoporous organic shells hold immense potential in diverse applications, encompassing adsorption, separation, delivery/immobilization of guest molecules in catalysis and controlled drug release. Herein, magnetic mesoporous melamine-formaldehyde resin microspheres (Fe3O4@SiO2@mMF) are constructed via a nanoemulsion-assisted interfacial co-assembly and polymerization strategy, using Pluronic F127 as a template agent and soluble melamine-formaldehyde (MF) oligomer as the precursor. The resulting microspheres possess radially oriented mesopores, superparamagnetic properties, and abundant N-containing active sites (nitrogen content: 15.02 wt%). The as-synthesized Fe3O4@SiO2@mMF microspheres as ideal catalyst supports, exhibit exceptional loading capacity for phosphotungstic acid (PTA). The as-formed Fe3O4@SiO2@mMF/PTA composites demonstrate not only good catalytic performance in the esterification reaction of n-butanol and acetic acid with a high conversion of 92% (to acetic acid) but also excellent antimicrobial performance against Staphylococcus aureus and Escherichia coli with viabilities of 11.58% and 7.35%, respectively.
The deficiency of reliable and physiologically relevant distal lung models has been regarded as a crucial issue for drug research on non small cell lung cancer (NSCLC). In this study, an inverse opal structure-based lung-on-a-chip was established to replicate the geometric dimensions and topography of the native lung alveoli, and two lateral microchambers were designed to induce pressure-driven stretching for the simulation of respiratory movement. Further, a concentration gradient generator was applied to connect with lung-on-a-chip for the creation of different enzyme environments to mimic the individual variability of P450s enzymes in lung patients. Based on this microfluidic platform, the Osimertinib implications in NSLC was investigated from the aspect of metabolism and adapted resistance. The results suggested that Osimertinib exhibited discernible difference in metabolism under diverse enzyme condition. Additionally, in contrast with the control group, all groups with Osimertinib treatment triggered the alterations of amino acid metabolisms and energy supply, indicating that targeting energy supply process might be an effective measure to prevent tumor cells from generating drug resistance.
Carbon nitride (CN)-based photocatalytic processes hold promise for water decontamination, during which the widely acknowledged charge transfer pathway is unfortunately characterized by severe chemical stability challenges. Herein, the intensive yet underestimated energy transfer pathway is achieved in CN nanosheets for durable, efficient, and sustainable water purification. Upon simple oxygen activation in air, the synthesized nanosheets come with an optimal pollutant removal rate constant of 0.18 min−1 under visible light irradiation, far exceeding that of state-of-the-art photocatalysts. It is revealed that the enhanced exciton binding energy inside the CN nanosheets triggers strong exciton effects, promoting the accumulation of triplet-state excitons by regulating the energy gap. The accumulated triplet excitons almost accomplish the transition from oxygen exclusively to singlet oxygen via the energy transfer pathway, which ultimately contributes to the robust degradation of the pollutants. This work proposes a viable strategy to enhance the exciton effect within CN, upon which efficient water treatment technology driven by energy transfer pathways can be expected.
Cervical cancer remains a leading cause of cancer-related mortality in women, underscoring the urgent need for advanced diagnostic and therapeutic strategies. Current imaging techniques face significant limitations, including radiation exposure, high costs, and inadequate sensitivity for detecting early metastases, particularly in imaging and diagnosing tumor metastatic lesions. To overcome these challenges, we developed a multimodal imaging strategy that combined near-infrared fluorescence (NIRF, 750–1700 nm) imaging with X-ray imaging, with assistance of innovative nanomaterial to achieve precise tumor targeting and comprehensive diagnostic. Specifically, we synthesized a folate acid-functionalized polydopamine-modified ICG-Bi2Se3 nanocomposite (FA-PDA@ICG-Bi2Se3, FPBI), which integrated the complementary advantages of NIRF, X-ray, and computerized tomography imaging. The FPBI nanocomposite leveraged the targeting capability of folate acid for specific identification of cervical cancer lesions and metastatic lymph node. Furthermore, it demonstrated robust photothermal therapeutic efficacy under near-infrared (808 nm) excitation, achieving significant tumor ablation effects. This work provides an innovative nanoplatform based strategy for multimodal imaging, precise diagnosis, and targeted therapy of cervical cancer, paving the way for improved detection and management of metastatic lesions.
Photovoltaic micron-silicon scrap (m-Si) has attracted attention as an anode material for lithium-ion batteries due to its high purity and low cost. However, its large particle size hinders the practical application. Herein, we propose an electrochemical etching process in molten KCl-LiCl to reduce its size. A novel electrode pair was developed by combining m-Si (anode) and spent lithium iron phosphate (LFP, cathode) material from spent lithium-ion batteries (LIBs). The m-Si was reduced from 10 µm to <5 µm at a cell voltage of 3.0 V by electrochemical etching without chlorine gas and was porous. The obtained e-Si-50 anode exhibits a high specific capacity of 1061.2 mAh/g at 2.0 A/g after 800 cycles in lithium-ion batteries. The Li3PO4, Fe, and carbon are derived by the electrochemical reduction of the LFP, and are efficiently separated via magnetic separation in water without acid/base treatment. This process combines the recycling of photovoltaic micro-silicon scrap and spent LIBs, providing both environmental and economic benefits.
Supramolecular architectures exhibiting cascade energy transfer characteristics represent pivotal model systems for advancing biomimetic light-harvesting systems (LHS) that emulate the natural photosynthesis. To now, the engineering of aqueous-phase artificial LHS with optimized energy transfer cascades is still a challenge. In this study, we designed and synthesized two tetraphenylethylene (TPE)-based macrocyclic compounds (namely TPE-1 and TPE-2) with different cavity sizes as supramolecular scaffolds to study their energy transfer behaviors. As a control model, a linear molecule TPE-3 was also prepared. The bigger-cavity macrocycle TPE-1 can emit green fluorescence and self-assemble into nanospherical structures in aqueous media, acting as an energy donor. Through self-assembly with eosin Y (EY) and a red-emitting fluorophore (TPE-Se), a sequential Förster resonance energy transfer (FRET) cascade: TPE-1→EY→TPE-Se was achieved thanks to their excellent spectral overlap and proximity between the donor and acceptors. The optimized ternary system (TPE-1/EY/TPE-Se) with a ratio of 1000:90:60 afforded a high energy transfer efficiency (ΦET) of 95%. Then, the artificial LHS platform catalyzed the oxidative coupling of benzylamines with 93% yield in aqueous media. Moreover, the system demonstrated broad catalytic utility oxidation reactions, the good conversion of methylthiobenzyl ester to methylbenzene sulfoxide and the aerobic cross-dehydrogenation coupling reaction of N-phenyltetrahydroisoquinoline with indole. These results robustly demonstrate the promising potential of this artificial LHS in the field of aqueous photocatalysis.
The design of covalent organic frameworks (COFs) with strong fluorescence in both solid and solution states present a significant challenge for white-light-emitting diode (WLED) applications, primarily due to the difficulty of balancing aggregation-induced emission (AIE) and aggregation-caused quenching (ACQ). Here, we report the synthesis of a 7-fold interpenetrated three-dimensional COF (3D COF) with a pts topology, termed ZJUT-M, constructed by co-condensation of a T4-symmetric monomer with two D2h-symmetric fluorophores exhibiting distinct emission behaviors. ZJUT-M displays robust fluorescence in both solid and solution states, enabling its use in WLEDs. Mechanistic studies reveal that the dual-mode emission is driven by the synergistic integration of high-degree-of-freedom chromophores, which promote AIE emission in the solid state, and conformationally restricted fluorophores, which suppress ACQ effect in solution. These findings provide a strategic pathway for achieving multi-state emissive COFs, opening avenues for their application in advanced optoelectronic devices, including next-generation LEDs.
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