Latest ArticlesIn the quest for new agrochemicals and pharmaceuticals, chemists seek access to reliable and mild synthetic techniques to allow for the systematic modification of chemical structures, exploration of unexplored chemical space, and facilitation of practical synthesis in their search for novel agrochemicals and pharmaceuticals. In this regard, photocatalytic reactions enabled the synthesis of intricate and more functionalized compounds. This review overviews the developed synthetic methodologies and their utility in the chemical synthesis of pharmaceuticals. This review also offers in-depth insights into contemporary photoredox reactions such as allylic additions, cyclization, reductive cross-coupling, CH activation, ring opening, oxidative cross-coupling, dehydrogenation, desulphonation, and decarboxylation. It provides a positive outlook for the promising future of this field.
Peroxymonosulfate (PMS) activation and photocatalysis are effective technologies to remove organic pollutants, but the adsorption effect of the catalyst is usually unheeded in degradation process. Herein, a bifunctional catalyst of amorphous MoSx (a-MoSx) with 3D layer-by-layer superstructure was synthesized by assembling basic active units [Mo3S13]2- of MoS2. The large interlayer spacing and high exposure of active sites render a-MoSx to have excellent synergy of adsorption and photo-assisted PMS activation for tetracycline (TC) degradation. Experiments and DFT calculation show that TC can be efficiently enriched on a-MoSx by pore filling, π-π interaction, hydrogen bonding and high adsorption energy. Subsequently, PMS can be quickly activated through electron transfer with a-MoSx, resulting in high TC degradation efficiency of 96.6% within 20 min. In addition, the synergistic mechanism of adsorption and photo-assisted PMS activation was explored, and the degradation pathway of TC was expounded. This work is inspirational for constructing bifunctional catalysts with superior synergistic adsorption and catalytic capabilities to remove refractory organic pollutants in water.
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.
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.
Two novel fungal metabolites, asperochones A and B, were obtained from an Aspergillus sp. Their structures were determined by 1D/2D nuclear magnetic resonance (NMR) spectroscopy, high resolution electrospray ionization mass spectroscopy (HRESIMS), and single-crystal X-ray diffraction analysis. Asperochone A possesses an intriguing skeleton bearing 5/6/6/6/7/5/5/5 octacyclic ring system, and asperochone B also exhibits an unusual carbon skeleton with five stereochiral centers. Their structures were proposed as heterotrimeric and heterodimeric products of aromatic polyketides. In addition, asperochone A exhibited a potential anti-tuberculosis effect since it showed a moderate potency against Mycobacterium smegmatis.
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.
As one of the most promising adoptive T-cell therapies, chimeric antigen receptor T-cell (CAR-T) therapy has acquired Food and Drug Administration (FDA) approval for a variety of products and has been used successfully in the treatment of malignant hematological tumors. CAR-T therapy, on the other hand, faces a number of obstacles in the field of solid tumor therapy that limit its widespread clinical implementation. Significant advances in nanoparticle research in cancer therapy and immunotherapy have been made in recent years, providing novel strategies to address the challenges encountered by CAR-T therapy in the treatment of solid tumors. This review commences with a comprehensive explanation of the basic framework of CAR-T therapy as well as the challenges it faces in the treatment of solid tumors. Subsequently, we encapsulate a summary of the developmental research combining nanoparticles with CAR-T cells for the treatment of solid tumors, which includes gene transfection, cell activation and expansion, targeted infiltration, immune escape inhibition, and combination with other therapies. Coupled with the overview of the research progress, a discussion has been initiated on the challenges and perspectives of CAR-T based on nanoparticles.
Formaldehyde (HCHO) as an indoor air pollutant released by new furniture and decorative materials is of great concern. Developing a self-cleaning device to remove HCHO is an ideal way to improve indoor air quality. In this study, a self-cleaning window with a multilayered structure constructed from fluorine-doped tin oxide/bismuth tungstate/resorcinol-formaldehyde resin (FTO/Bi2WO6/RF) has been fabricated, which is capable of degrading HCHO in natural indoor condition. The as-fabricated device could utilize the natural room light and promote the generation and transfer of the photocatalytic carriers in Bi2WO6, which subsequently delivers a good catalytic oxygen reduction efficiency in RF to produce hydrogen peroxide (H2O2). The as-synthesized H2O2 could further split into hydroxyl radicals (•OH), then oxide the HCHO molecules in the air. The present study demonstrates a novel and efficient strategy to fabricate a transparent multifunctional window for self-cleaning indoor gaseous pollutants, the concept is of great importance to be expanded in a broad range of indoor furniture for in-house air pollution control.
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.
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