Latest ArticlesAs the main organ of gas exchange, the lungs are susceptible to various exogenous attacks, and pneumonia is one of the major inflammatory diseases that threaten human health. Generally, pneumonia is a disease that occurs in the alveoli and respiratory bronchioles induced by pathogens and further causes local and systemic inflammatory responses. The development of pneumonia can bring various serious complications, including lung abscess, sepsis, meningitis, brain damage and hearing loss. Over the past few decades, the mortality rate of pneumonia patients has remained high. While lung cancer is another lung-related malignant tumors worldwide, with a low 5 year survival rate. Exploring the mechanisms of their occurrence and interaction between pneumonia and lung cancer is a challenging and meaningful task. The abnormalities of lipid droplets (LDs) polarity have been found strongly accompanied by many diseases, especially cancer, inflammation, and metabolic diseases. However, their exact role is not yet clear. Hence, it is significant to develop a novel detection method to observe the polarity changes of LDs, which would help to reveal the development process of diseases pneumonia and lung cancer. In this work, a new polarity-sensitive LDs-targeted near-infrared probe BFZ up to 712 nm was designed, according to the intramolecular charge transfer mechanism, which displayed high fluorescence intensity in low polarity while showing decreased fluorescence intensity in high-polarity conditions with a significant redshift. The BFZ was successfully applied to the change of LDs polarity in lipopolysaccharide (LPS)-stimulated A549 cells, and a mouse model of lung inflammation. It also tells the polarity differences between normal and tumor cells and between normal and tumor tissues. Moreover, the correlations between pneumonia and polarity changes were observed through the imaging experiments, which may provide an insightful method for the early diagnosis of pneumonia and lung cancer.
Efficient yield of 1O2 determines the photocatalytic degradation rate of antibiotics, but the regulatory mechanism for 1O2 selective generation in O2 activation is still lacking exploration. Herein, oxygen vacancy (OV) modification strategy of MIL-125 was successfully practiced to promote the selective generation of 1O2. Multiple characterizations including extended X-ray absorption fine structure (EXAFS) and electron paramagnetic resonance spectra (EPR) confirmed the formation of oxygen vacancy in OV-MIL-125. The synthesized OV-MIL-125 exhibited greatly enhanced 1O2 selective (~90%) and antibiotics removal rate in water with high mineralization rate. Dynamics analysis of excitons by transient-steady state fluorescence and phosphorescence, transient absorption spectra (TAS) revealed that oxygen vacancy greatly enhanced the intersystem crossing (ISC) of singlet exciton, promoting triplet exciton generation. Density functional theoretical (DFT) calculation also proved the reduced gap of intersystem (ΔEST) and the modulated highest occupied molecular orbital (HOMO)-lowest unoccupied molecular orbital (LUMO) population which was conducive to intersystem crossing process. Calculation of transition state further confirmed the lower energy barrier for π* orbital spin flip of O2 adsorbed on OV-MIL-125. The Dexter energy transfer involving triplet annihilation dominated the O2 activation mechanism to generate 1O2 instead of the charge transfer to generate O2•− which happened in MIL-125. This study provides new thinking for photocatalytic activation of molecular oxygen and is expected to guide the design of MOF-based catalysts for water treatment.
Zeolites are crystalline porous materials that are used in the chemical industry for adsorption, separation and catalytic reactions. Chiral zeolites have shown promise in enantioselective adsorption and catalytic organic reactions, attracting significant research interest. Recent advances have been made in the rational design, computational prediction and hydrothermal synthesis of using chiral organic structure-directing agents. Additionally, newly developed electron microscopic techniques have been utilized to analyze the structure and determine absolute configuration. The following review aims to provide an overview of the development history of chiral zeolites, examine several prominent chiral zeolite structures discovered so far, discuss the recent progress in characterization methods and explore their potential applications.
Higher initial (de)hydrogenation temperature and sluggish kinetics are the main bottlenecks to develop Mg-based hydrogen storage alloys with high hydrogen capacity. One of the effective methods of solving these problems is introducing additives to enhance (de)hydrogenation kinetics and decrease particle sizes to lower (de)hydrogenation temperatures. In this work, Mg85-Ni10-La4.5-Y0.5 alloy doped with Cu@C nanoparticles is prepared, which could enhance (de)hydrogenation kinetics via introducing Cu nanoparticles as a catalyst and reduce the alloy particle sizes via acting as a grinding agent to lower (de)hydrogenation temperature. The results indicate the dehydrogenation temperature of the modified Mg85-Ni10-La4.5-Y0.5 composite could be decreased to 308.5 ℃, absorb 4.73 wt% H2 at 220 ℃ within 1 min and release 5.01 wt% H2 within 4 min at 300 ℃. Moreover, the capacity retention could be maintained around 98.8% after 10 cycles at 300 ℃, superior than those of Mg85-Ni10-La4.5-Y0.5 and milled-Mg85-Ni10-La4.5-Y0.5. DFT results and characterizations suggest that in-situ formed Mg2Cu could accelerate the dissociation of Mg-H bonds and the presence of amorphous carbon in Mg-Ni-La-Y-Cu system will further synergistically improve the (de)hydrogenation kinetics of Mg85-Ni10-La4.5-Y0.5. Reduced particle sizes under the aid of carbon frameworks also help introduce boundaries of the particles and shorten hydrogen diffusion pathways.
The carboxylation of readily available organo halides with CO2 represents a practical strategy to afford valuable carboxylic acids. However, efficient carboxylation of inexpensive unactivated alkyl chlorides is still underdeveloped. Herein, we report the electro-reductive carboxylation of CCl bonds in unactivated chlorides and polyvinyl chloride with CO2. A variety of alkyl carboxylic acids are obtained in moderate to good yields under mild conditions with high chemoselectivity. Importantly, the utility of this electro-reductive carboxylation is demonstrated with great potential in polyvinyl chloride (PVC) upgrading, which could convert discarded PVC from hydrophobic to hydrophilic functional products. Mechanistic experiments support the successive single electron reduction of unactivated chlorides to generate alkyl anion species and following nucleophilic attack on CO2 to give desired products.
BiVO4 is a promising semiconducting photoanode for photoelectrochemical (PEC) water splitting due to its suitable bandgap. However, the dissolution of V5+ and sluggish reaction kinetics at the surface in the oxygen evolution reaction (OER) limit its applications. Herein, we report a convenient strategy to change the microenvironment by adding Fe(Ⅲ) into the electrolyte. During the PEC process, Fe(Ⅲ) ions not only improve the current density, but also show excellent stability toward BiVO4. Consequently, the current increases by more than 1.7 times compared to that without Fe(Ⅲ). Photoelectrochemical, morphological, and structural characterizations reveal that the FeOOH co-catalyst produced in situ on the BiVO4 photoanode by cyclical formation of the intermediates at the electrode/electrolyte interface during OER accelerates the OER kinetics and prevents photo-corrosion by suppressing the dissolution of V5+. The results reveal a new strategy for the multifunctional modification of photoanodes for efficient solar conversion.
Organic semiconductors are promising candidates as active layers in flexible and biocompatible electronics owing to their solution processability and molecular design flexibility. However, it remains necessary to establish a green processing approach to acquire desirable electrical properties for scalable industrial applications. Here, a highly efficient and environmentally friendly post-treatment method using liquid nitrogen as a cooling bath is developed to optimize the aggregation structure and electrical performance of organic semiconductors. The carrier mobility has increased by nearly 60% with this treatment, achieving a performance boost comparable to that of traditional annealing methods. This performance improvement is attributable to the denser aggregation structure and enhanced molecular ordering compared with those of as-cast semiconducting polymer films. Impressively, the entire process can be completed within a few minutes without additional vacuum or high-temperature conditions, offering an economical and efficient alternative to traditional methods. Furthermore, the enhancement effect and long-term stability of this treatment are validated across a wide range of organic semiconductors, positioning this green and versatile approach as a promising substitute for conventional post-treatment, thereby facilitating the development of next-generation sustainable electronics.
A dimeric Y(Ⅲ)-containing antimonotungstate [Y4(H2O)8(mal)2(OAc)O(Sb2WⅤ2WⅥ19O72)2]21− (Y4mal2, H3mal = DL-malic acid), resembling a “handshake” configuration, was synthesized and characterized. The polyanion of Y4mal2 consists of two Dawson-derived {Y2Sb2W21} moieties that are further linked by two mal ligands and one μ2-bridging acetate to form an asymmetric polyanion. Notably, the chiral configuration induced by the D- or L-configuration of the mal ligand results in both {Y2Sb2W21} moieties within one polyanion exhibiting identical chirality, leading to the racemate crystallization of Y4mal2. Moreover, Y4mal2 exhibits excellent Lewis acid catalytic activity for environmentally friendly synthesis of imidazoles.
Photocatalytic hydrogen peroxide (H2O2) synthesis, driven by solar energy, offers a sustainable and cleaner alternative for producing green H2O2 from water and oxygen. 2D photocatalysts have emerged as powerful materials for this purpose due to their unique physiochemical properties such as a flexible planar structure and large surface area. This review provides a comprehensive overview of the latest advances in 2D photocatalytic materials employed in H2O2 synthesis, including metal oxides, metal chalcogenides, bismuth-based materials, graphitic carbon nitrides (g-C3N4), metal−organic frameworks (MOFs), and covalent organic frameworks (COFs). Beginning with an extensive introduction to possible reaction routes for photocatalytic H2O2 synthesis, we summarize the common methods for H2O2 detection, crucial for obtaining reliable results in H2O2 studies. Additionally, we highlight molecular-level modification strategies for 2D photocatalysts, such as surface modification, ion doping, defect engineering, and heterojunction construction, which promote high-efficiency solar-to-chemical conversion for sustainable H2O2 photosynthesis. Furthermore, we discuss key issues and provide perspective outlooks for the efficient and sustainable generation of H2O2 in scale-up industrial production. This review offers in-depth insights into different reaction pathways of H2O2 synthesis and provides design principles for 2D photocatalysts to enhance H2O2 production, guiding the development of efficient photocatalysts for H2O2 synthesis.
Carbon nitride, a typical low-dimensional conjugated polymer photocatalyst, features a high exciton binding energy due to the weak dielectric screening and the strong Coulombic attraction of photogenerated electrons and holes. The reduction of the exciton binding energy of carbon nitride to promote the conversion from excitons into free carriers is the first priority for the improvement of charge-transfer-dependent photocatalytic reaction activity. In this paper, by introducing a variety of polar metal cations to carbon nitride, it is demonstrated that the charge distribution of the heptazine ring can be improved by ion polarization, which effectively promotes the dissociation of excitons into electrons and holes. The sodium ion shows the best modification effect, which enhances the rate of both photocatalytic hydrogen and hydrogen peroxide production by about 50%. Characterization shows that the introduction of strongly polar metal cations contributes to the reduction of the exciton dissociation energy of carbon nitride. This study provides a new perspective and a convenient method for the exciton modulation engineering of low-dimensional photocatalysts.
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