Latest ArticlesDoxorubicin (DOX) is known to elicit potent antitumor immune responses through the induction of immunogenic cell death (ICD). However, its therapeutic efficacy is undermined by the adaptive upregulation of programmed cell death ligand 1 (PD-L1), which hijacked the antitumor immunity. In this study, we developed a reactive oxygen species (ROS)-responsive dihydroartemisinin (DHA) prodrug to facilitate the delivery of DOX via hydrophobic and electrostatic interactions. Upon internalization by tumor cells, the nanoparticles (NPs) preferentially accumulated in endoplasmic reticulum (ER), exacerbating ER stress and amplifying ICD to enhance tumor immunogenicity. Simultaneously, the oxidative intracellular environment trigged the degradation of NPs, releasing DHA, which downregulated PD-L1 by disrupting signal transducer and activator of transcription 3 (STAT3) phosphorylation and inactivating the nuclear factor kappa-B (NF-κB) pathway. Consequently, the effective PD-L1 blockade and robust ICD response, synergistically inhibited breast cancer progression, significantly enhancing the chemo-immunotherapy efficacy of doxorubicin.
Raw water temperature can fluctuate significantly throughout the year, with peaks above 30 ℃ in summer and below 15 ℃ in winter. Traditional desalination systems (e.g., reverse osmosis, RO) face challenges under these varying temperature conditions. Specifically, while the RO system performs well under high temperatures, its efficiency decreases sharply at lower temperatures. Membrane capacitive deionization (MCDI) is considered as an emergent and promising technology for brackish water desalination. While plenty of studies have been devoted to investigating the impacts of raw water properties (e.g., salinity, coexisting ions, and natural organic matter) on MCDI performance, the role of water temperatures during the desalination remains under-explored. In this study, we first tested and determined the optimized MCDI operation parameters, such as the cell voltage and feedwater flow rate. Key findings showed that MCDI's salt removal efficiency remains unaffected by feedwater temperature fluctuations. However, as feedwater temperature increases from 15 ℃ to 40 ℃, the specific energy consumption for desalination slightly rises by 16.3%, and current efficiency drops by 14.1%. Compared to RO systems, the resilience of MCDI to temperature fluctuations makes it a preferable choice for brackish water treatment in areas with a large temperature difference.
Peroxymonosulfate (PMS)-based advanced oxidation technology has been proven to be a viable option for the decontamination of organic pollutants from water bodies. Advanced catalyst design is essential to this technology. Herein, a vanadium-doped LaFeO3 perovskite (LFO-V) featuring asymmetric Fe-O-V sites was rationally designed. Thanks to orbital electron interaction between Fe and V atoms, the modified electronic structure elevated electron density near the Fermi energy level while reducing the energy barrier toward effective PMS activation. This facilitated concurrent PMS reduction at the Fe sites to generate SO4•- and •OH (57.7%), and PMS oxidation at V sites to produce 1O2 (42.3%). The LFO-V/PMS system demonstrated excellent tetracycline (TC) degradation performance with a 2-fold enhancement in rate constant compared to that of pristine LFO. Further, the LFO-V maintained long-term stability, and the toxicity of degradation intermediates was evaluated through microbial metabolomics. This work establishes an effective route to regulate the PMS activation pathways through precise electronic structure modulation, advancing the rational design of advanced Fenton-like catalysts.
The limited redox capability of photocatalysts often leads to harmful NO2 byproduct formation during photocatalytic NO oxidation. Herein, Bi4Ti3O12 nanosheets modified with plasmonic metallic bismuth and abundant oxygen vacancies were synthesized via an in-situ reduction method. The optimized catalyst (BTOR2, with a molar ratio of 40% NaBH4 to Bi4Ti3O12) achieved a maximum NO removal efficiency of 62.3%, significantly higher than pristine Bi4Ti3O12 (40.5%) while minimizing NO2 production. The results reveal that the synergistic effects of Bi's plasmonic resonance and oxygen vacancies enhanced visible light absorption and charge separation. The density functional theory (DFT) analysis showed electrons can transfer from Bi4Ti3O12 to Bi, promoting O2 activation to •O2- radicals. In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) confirmed that light-induced H2O adsorption was strengthened, improving •OH radical generation. These radicals promoted the selective conversion of activated NO- to NO3-, rather than NO2. This work provides valuable insights for advancing research into efficient photocatalysts for air pollution control.
Vacuum-ultraviolet (VUV) radiation is high-energy UV radiation with a wavelength of 100–200 nm capable of decomposing/mineralizing hazardous emerging organic pollutants (EPs) in water through direct photolysis and/or by generating reactive free radicals (RFRs) during photolysis. However, due to the unsatisfactory photoelectric conversion rate, strong absorption by oxygen and water molecules, and other characteristics of VUV radiation, its application and development are hindered, leading to misconceptions regarding high energy consumption and insufficient free radical yield. The objectives of our assessment in this review are as follows: The illumination of the photochemical characteristics of VUV and the reactivity of aqueous solutions. Summarization of accurate UV dose and energy evaluation criteria. Comparison and analysis of the photochemical mechanisms and reaction kinetics of different types of EPs via VUV direct photolysis, as well as the interference origins of typical substrates in water for VUV decontamination. We found that quantities typically reported in VUV photochemical reactions of engineered systems are underreported in low-pressure mercury lamp (LPUV) photochemical reactions, especially a quantitative indicator of the species or energy that induces a chemical reaction. The absence of these quantities has made it difficult to assess the fundamental performance of VUV photolysis fully compared with that of UV-C. Some studies have sought to optimize VUV-advanced reduction processes (VUV-ARP) or VUV reactor treatment of these contaminants; however, an abundant evaluation of the reaction origins and processes between VUV-derived main RFRs and reactants (H2O, O2, organic matter, inorganic ions, etc.) is essential, cause these scientific elements will provide the possibility to break the application gap for VUV in the field of EPs treating. Overall, the data compilation, analysis, and research recommendations provided in this review will form the basis for all photochemical reactions initiated by VUV radiation with water as the backing agent.
Machine learning (ML) is recognized as a potent tool for the inverse design of environmental functional material, particularly for complex entities like biochar-based catalysts (BCs). Thus, the tailored BCs can have a distinct ability to trigger the nonradical pathway in advance oxidation processes (AOPs), promising a stable, rapid and selective degradation of persistent contaminants. However, due to the inherent "black box" nature and limitations of input features, results and conclusions derived from ML may not always be intuitively understood or comprehensively validated. To tackle this challenge, we linked the front-point interpretable analysis approaches with back-point density functional theory (DFT) calculations to form a chained learning strategy for deeper sight into the intrinsic activation mechanism of BCs in AOPs. At the front point, we conducted an easy-to-interpret meta-analysis to validate two strategies for enhancing nonradical pathways by increasing oxygen content and specific surface area (SSA), and prepared oxidized biochar (OBC500) and SSA-increased biochar (SBC900) by controlling pyrolysis conditions and modification methods. Subsequently, experimental results showed that OBC500 and SBC900 had distinct dominant degradation pathways for 1O2 generation and electron transfer, respectively. Finally, at the end point, DFT calculations revealed their active sites and degradation mechanisms. This chained learning strategy elucidates fundamental principles for BC inverse design and showcases the exceptional capacity to integrate computational techniques to accelerate catalyst inverse design.
Chlorinated antibiotics pose great challenges in efficient removal, while for the first time, this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co3O4/g-C3N4 heterojunctions to improve process cost-effectiveness. The Co3O4/g-C3N4 heterojunction demonstrated an effective removal of 93.6% thiamphenicol (TAP) within 45 min, with the rate constant (0.0584 min-1) that was 2.4 and 2.8 times that of Co3O4 and g-C3N4 alone, respectively. The formation of heterojunctions facilitated electron transfer, enriched the electron density on Co3O4, and enhanced the adsorption of pollutants as well as the desorption of degradation intermediates. The enhanced production of atomic hydrogen (H*) of Co3O4/g-C3N4, which increased by 13.6–28.2 times, contributed more to pollutant removal (64.0%), much higher than that of Co3O4 (37.3%) and g-C3N4 (6.1%). The energy barrier for H2 formation on Co3O4/g-C3N4 (0.75 eV) was higher than that on Co3O4 (-1.84 eV), supporting that it could stabilize H* and inhibit the formation of H2. The Co3O4/g-C3N4 heterojunction exhibited stable performance with less impact by pH and co-existing ions, and posed effectiveness for the dechlorination of typical chlorinated antibiotics. This study offers an efficient and sustainable strategy for constructing heterojunctions to enhance the performance of non-noble metal catalysts in electrocatalytic dechlorination.
A visible-light induced cascade sulfonation/cyclization reaction of 3-allyl-2-arylquinazolinones employing water as an environmentally friendly solvent was revealed. This transition metal-free protocol, using 9-mesityl-10-methylacridinium perchlorate as the photocatalyst, represents a masterly tactic for the synthesis of sulfonated dihydroisoquinolino[1,2-b]quinazolinones featuring mild conditions, facile operation, and broad substrate scope.
ADPr-ATP is a natural nucleotide with three sugar rings and five pentavalent phosphorus, and can be produced through TIR-catalyzed ADP-ribosylation reactions for plant immunity. Here, we report the first total synthesis of ADPr-ATP (1) with a total yield of 6.4% through 14 steps, featuring late-stage P(V)−N activation reaction of pyrophosphate (4) and 5′-phosphoromorpholidate (25). The protected adenosine 5′-phosphoromorpholidate (24) was prepared on the basis of a scalable to adenosine 5′′-monophosphate (2). The construction of P(V)−N bond in phosphoramidate is esteemed as a critical step as they are sufficiently stable in deprotection reactions. The chemical synthesis of ADPr-ATP can offer an appealing alternative to traditional enzymatic synthesis and fractionation methods. Furthermore, the pRib-AMP and its prodrug are also synthesized to evaluate cytotoxicity and anti-influenza activity in vitro.
Lysine-targeting reversible covalent inhibitors, particularly salicylaldehyde-based compounds such as the Food and Drug Administration (FDA)-approved drug Voxelotor, exhibit significant therapeutic potential but are limited by challenges including instability and off-target effects. To overcome these limitations in kinase inhibitor A5, we devised a pH-responsive prodrug strategy by masking its reactive aldehyde group with an acid-labile hydrazone linkage and enhancing intracellular delivery through conjugation with FK506. The optimized prodrug demonstrated robust antitumor efficacy in K562 tumor-bearing mice. Furthermore, the incorporation of the photosensitizer chlorin e6 (Ce6) led to the formation of self-assembled nanoparticles (AKNP), which not only improved physiological stability and prolonged tumor retention but also enabled light-triggered release of A5 in conjunction with photodynamic therapy (PDT). Our study thus presents a promising prodrug self-assembly strategy that combines the on-demand release of a novel lysine-targeting, reversible covalent kinase inhibitor with PDT in clinical cancer therapy.
No. 86 Xueyuan South Road, Haidian District, Beijing
010-62662699(Operation and Technical Support)
qkjq@cast.org.cn
Copyright © 2025 China Association for Science and Technology. All rights reserved. For all open access content, the relevant licensing terms apply.
Sponsored by the Office of the Leading Group for Cybersecurity and Informatization of CAST, and supported by Science and Technology Review Publishing House
