Latest ArticlesSemiconductor-molecule surface-enhanced Raman scattering (SERS), especially the stronger interfacial charge transfer process (ICTP), represents a frontier in the field of SERS with spectral reproducibility and unparalleled selectivity. Herein, through a laser microfabrication method in situ, the free-standing, super hydrophilic and vacancy-rich TiO2-x/Ti is successfully synthesized. Using blue TiOx/Ti (B-TiOx/Ti) as pre-concentrated substrate, a nanomolar-level limit of detection of 12 nmol/L at 1385 cm–1, is confirmed using crystal violet (CV) bacteriostat as a model under 532 nm excitation. Furthermore, the results demonstrate that the SERS enhancement mechanism is via the moderate adulteration of oxygen vacancy, which leads to a narrow value of band gap and increases the ICTP of substrate to molecules. Using a hand-held extractor assembled with B-TiOx/Ti microfiber, the operando analysis of mixtures distributed information excited in different parts of Asian carp is facilely achieved. This work guides the controlled synthesis of vacancy-rich TiO2-x/Ti nanostructure and its application in ultrasensitive extraction-SERS detection. It also provides the direction for the rapid and operando transmission of biological information with temporal and spatial concentration distribution in human tissues by highly sensitized materials.
In this work, we established an exceptionally facile method for the preparation of Ni-CeO2 nanorods in a kind of deep eutectic solvents (DESs) composed of L-proline and Ce(NO3)3·6H2O. First, Ni-CeO2 nanorods were successfully prepared by adding Ni(NO3)3·6H2O to DESs. Then, we found that Ni-CeO2 nanorods prepared in DESs have more prominent oxidase-like activity than pure CeO2. The outstanding catalytic activity of Ni-CeO2 could be ascribed to its high Ce3+/Ce4+ ratio. As a proof-of-concept application, the Ni-CeO2 nanorods were successfully acted as a colorimetric platform for the sensitive determination of ascorbic acid and α-glucosidase activity, which displays excellent analytical performance. Moreover, this sensing platform was applied for screening natural α-glucosidase inhibitors, such as terpenoids from natural products. The results indicated that ursolic acid and oleanolic acid had good inhibitory rates. This strategy not only provides a new way to construct more kinds of nanomaterials from DESs, but also offers a facile and effective tool to screen the α-glucosidase natural inhibitors as potential anti-diabetic drugs.
The Na-deficient P3-type layered oxide cathode material usually experience complex in-plane Na+/vacancy ordering rearrangement and undesirable P3-O3 phase transitions in the high-voltage region, leading to inferior cycling performance. Additionally, they exhibit unsatisfactory stability when exposed to water for extended periods. To address these challenges, we propose a Cu/Ti co-doped P3-type cathode material (Na0.67Ni0.3Cu0.03Mn0.6Ti0.07O2), which effectively mitigates Na+/vacancy ordering and suppresses P3-O3 phase transitions at high voltages. As a result, the as-prepared sample exhibited outstanding cyclic performance, with 81.9% retention after 500 cycles within 2.5–4.15 V, and 75.7% retention after 300 cycles within 2.5–4.25 V. Meanwhile, it demonstrates enhanced Na+ transport kinetics during desodiation/sodiation and reduced growth of charge transfer impedance (Rct) after various cycles. Furthermore, the sample showed superb stability against water, exhibiting no discernible degradation in structure, morphology, or electrochemical performance. This co-doping strategy provides new insights for innovative and prospective cathode materials.
Covalently bonded bridging between different semiconductors is a remarkable approach to improve the transfer of charge carriers at interfaces. In this study, we designed a ternary heterojunction (MBG) combining of molybdenum diselenide (MoSe2), black phosphorus nanosheets (Bpn) and graphitic carbon nitride (GCN). Among this MBG of MoSe2/Bpn/GCN, (ⅰ) the covalently bonded bridging effect between Bpn/GCN facilitates directional charge carrier transfer, meanwhile (ⅱ) a Z-scheme heterojunction is formed between MoSe2/GCN to enhance the separation of photogenerated carriers. Furthermore, (ⅲ) this composite exhibits an increased absorption for visible light. Using this MBG, photocatalytic degradation of over 98% of moxifloxacin is achieved within 20 min, with O2•− confirmed as the primary photocatalytic active species. These findings provide novel insights into the construction of efficient heterojunction by covalently bonded bridging.
Nitrogen-doped carbon loaded single-atom catalysts (SACs) are promising candidates for electrocatalytic conversion of CO2 into high-valuable chemicals, and the modification of catalysts by heteroatom-doping strategy is an effective approach to enhance the CO2 reduction performance. However, the large difference exists in atomic radius between nitrogen atoms and the doped heteroatoms may lead to the poor stability of active sites. In this study, we have synthesized a Ni single atom catalyst with S doping at the second-shell on the ultrathin carbon nanosheets support (Ni-N4-SC) by solid-phase pyrolysis. The S atom in the second-shell contributes to the higher efficiency of CO2 conversion at lower potentials while the Ni-N4-SC can be more stable. The experimental results and theoretical calculations indicate that the S atom in second-shell breaks the uniform charge distribution and reduces the free energy of hydrogenation, which can increase the adsorption of CO2, accelerate charge transfer, and reduce the reaction energy barrier. This work reveals the close relationship between the second-shell and the electrocatalytic activity of single atom sites, which also provides a new perspective to design efficient single atom catalysts.
Macrophages, as a subset of innate immune cells, play a pivotal role in the initiation, maintenance, and resolution of inflammatory responses during tissue damage repair, defense against infections, and tumor progression. However, the mechanisms by which macrophages regulate inflammation in acute myeloid leukemia (AML) and their involvement in the chemotherapeutic effect remain elusive. In this study, we have identified that AML cells stimulate macrophage expansion by activating the colony-stimulating factor 1 receptor (CSF1R) pathway. The expanded macrophages activate nuclear factor kappa-B (NFκB) to induce the expression of inflammatory factors, thereby maintaining leukemic cell quiescence and promoting cell survival following chemotherapy. Furthermore, we have successfully utilized a poly(ferulic acid) nanocarrier to selectively target macrophages for inhibiting the NFκB-mediated inflammation, ultimately enhancing chemotherapy efficacy against AML. Taken together, our findings highlight the crucial role of macrophage-induced inflammation in conferring chemoresistance to AML, and demonstrate the potential of a targeted nanocarrier specifically designed for inflammatory macrophages to improve the AML chemotherapeutic outcomes.
Water contamination by tetracycline (TC) has emerged as an environmental concern owing to its widespread use and antibiotic resistance. Application of peracetic acid (PAA) in the water and wastewater treatment has recently been proposed and demonstrated to be effective for TC abatement, yet the underlying reaction kinetics between the PAA and TC are not yet clear. To explore the reaction kinetics, the effect of solution pH on TC abatement by PAA is studied and the species-specific rate constants are calculated. The ability to donate and accept electrons for different species of TC and PAA is evaluated via density functional theory (DFT) calculations. The pH-dependent apparent second-order rate constants of TC abatement by PAA exhibits the parabolic shape with the maximum at pH 8.5 (9.75 L mol−1 s−1). This phenomenon is closely related to the speciation of TC and PAA, in which the reaction between PAAH and TTC2− possesses the highest species-specific rate constants according to the kinetic simulation. Further DFT calculations suggest that the HOMO of TTCH+, TTC, TTC−, TTC2− and the LUMO of PAAH and PAA− are –6.40, –6.26, –5.10, –4.94 eV and –0.24, 0.60 eV, respectively. According to the DFT calculations, deprotonation of TC and PAA leads to an increase of the HOMO value of TC and the LUMO value of PAA. Furthermore, the HOMOTC–LUMOPAA values is in good agreement with the trend of species-specific rate constants, which can be used to evaluate the reactivity between PAA and TC with different species. This study provides the kinetic data and theoretical basis for the reaction of PAA and TC, which is critical for the application of PAA in the treatment of water and wastewater.
Enones are widely explored in synthetic chemistry as fundamental building blocks for a wide range of reactions and exhibit intriguing biological activities that are pivotal for drug discovery. The development of synthetic strategies for highly efficient preparation of enones thereby receives intense attention, in particular through the transition metal-catalyzed coupling reactions. Here, we describe a carbene-catalyzed cross dehydrogenative coupling (CDC) reaction that enables effective assembly of simple aldehydes and alkenes to afford a diverse set of enone derivatives. Mechanistically, the in situ generated aryl radical is pivotal to "activate" the alkene by forming an allyl radical through intermolecular hydrogen atom transfer (HAT) pathway and thus forging the carbon-carbon bond formation with aldehyde as the acyl synthon. Notably, our method represents the first example on the enone synthesis through coupling of "non-functionalized" aldehydes and alkenes as coupling partners, and offers a distinct organocatalytic pathway to the transition metal-catalyzed coupling transformations.
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