作者机构：
School of Hydraulic and Ocean Engineering, Changsha University of Science & Technology, Changsha 410114, China;Key Laboratory of Dongting Lake Aquatic Eco-Environmental Control and Restoration of Hunan Province, Changsha 410114, China;[Yanxiao Wei] RIKEN Center for Sustainable Resource Science, 1-7-22 Suehiro-cho, Tsurumi-ku, Yokohama, Kanagawa 230-0045, Japan;[Jianhong Jiang; Qingchang Tang] China Machinery International Engineering Design & Research Institute Co., Ltd., Changsha 410007, China;[Xinying Kong] School of Chemistry and Chemical Engineering, University of South China, Hengyang, Hunan 421001, China
通讯机构：
[Hong Chen] S;School of Hydraulic and Ocean Engineering, Changsha University of Science & Technology, Changsha 410114, China<&wdkj&>Key Laboratory of Dongting Lake Aquatic Eco-Environmental Control and Restoration of Hunan Province, Changsha 410114, China
摘要：
To explore the adaptive mechanisms of the partial nitritation-anammox (PNA) process under high salinity stress during kitchen wastewater treatment, focusing on their physiological and molecular responses through metagenomic analysis. An airlift inner-circulation partition bioreactor (AIPBR) was developed, featuring an inner cylinder and a flow guide tube to create distinct oxygen gradients, facilitating the study of microbial adaptation under varying salt conditions. The AIPBR was operated with synthetic wastewater containing ammonium concentrations of 1800 ± 100 mg/L and salinity gradients ranging from 1 to 10 g/L, followed by a fixed salinity period at 6 g/L, with ammonium concentrations approximately 850 mg/L. High-throughput metagenomic analysis revealed shifts in functional genes and metabolic pathways in response to salinity stress. Anammox bacteria adapted by enriching genes involved in the synthesis of osmoprotective compounds and activating energy-producing pathways like the tricarboxylic acid cycle (TCA). These adaptations, along with modifications in membrane composition, were essential for sustaining system stability under elevated salinity. Under prolonged high salinity stress, anaerobic ammonium oxidizing (AnAOB) exhibited improved salt tolerance, maintaining a total nitrogen removal efficiency above 85 % and stabilizing after an adaptation phase. The metagenomic data revealed a marked enrichment of genes associated with ion transport, stress response mechanisms, and DNA repair pathways. Changes in microbial community composition favored salt-tolerant species, supporting system stability. These findings highlight the applicability of the developed bioreactor for scaling up the PNA process to handle high-salinity wastewater, providing a promising avenue for sustainable nitrogen removal in challenging environments.
To explore the adaptive mechanisms of the partial nitritation-anammox (PNA) process under high salinity stress during kitchen wastewater treatment, focusing on their physiological and molecular responses through metagenomic analysis. An airlift inner-circulation partition bioreactor (AIPBR) was developed, featuring an inner cylinder and a flow guide tube to create distinct oxygen gradients, facilitating the study of microbial adaptation under varying salt conditions. The AIPBR was operated with synthetic wastewater containing ammonium concentrations of 1800 ± 100 mg/L and salinity gradients ranging from 1 to 10 g/L, followed by a fixed salinity period at 6 g/L, with ammonium concentrations approximately 850 mg/L. High-throughput metagenomic analysis revealed shifts in functional genes and metabolic pathways in response to salinity stress. Anammox bacteria adapted by enriching genes involved in the synthesis of osmoprotective compounds and activating energy-producing pathways like the tricarboxylic acid cycle (TCA). These adaptations, along with modifications in membrane composition, were essential for sustaining system stability under elevated salinity. Under prolonged high salinity stress, anaerobic ammonium oxidizing (AnAOB) exhibited improved salt tolerance, maintaining a total nitrogen removal efficiency above 85 % and stabilizing after an adaptation phase. The metagenomic data revealed a marked enrichment of genes associated with ion transport, stress response mechanisms, and DNA repair pathways. Changes in microbial community composition favored salt-tolerant species, supporting system stability. These findings highlight the applicability of the developed bioreactor for scaling up the PNA process to handle high-salinity wastewater, providing a promising avenue for sustainable nitrogen removal in challenging environments.
期刊：
Dyes and Pigments,2026年245:113195 ISSN：0143-7208
通讯作者：
Yuli Yin
作者机构：
[Chao Fu; Wei Zhao; Hongmian Yu; Xiruo Li; Jiayi Li; Guoqi Chen; Yuli Yin; Rong Hu] School of Chemistry and Chemical Engineering, University of South China, Hengyang, 421001, PR China
通讯机构：
[Yuli Yin] S;School of Chemistry and Chemical Engineering, University of South China, Hengyang, 421001, PR China
摘要：
The construction of organic photosensitizers with near infrared (NIR) emission has shown great promise for precise therapeutic applications. However, fluorescence imaging and phototherapy efficacy are dependent on competitive photophysical processes, so it is still a great challenge to engineer photosensitizer with appreciable light emission especially in the NIR light region, and highly efficient energy conversion into valuable reactive oxygen species. In this paper, we report series of simple perylene diimide (PDI)-based NIR photosensitizers by regulating the position of a phenyl moiety in the donor-acceptor-donor conjugated backbone, a packing balance between the twisted molecular structure and effective π-conjugation is actualized. Photodynamic property observation reveals that the developed fluorophores present desirable photosensitizing ability with the production of both type I and II reactive oxygen species (ROS) under light irradiation, and the eradication of tumor cells is realized based on ferroptosis mechanism. Moreover, the bright emission in NIR region allows for the sensitive detection of pulmonary metastasis in vivo . These results provide an illuminating NIR photosensitizers design strategy for image-guided tumor photodynamic therapy applications.
The construction of organic photosensitizers with near infrared (NIR) emission has shown great promise for precise therapeutic applications. However, fluorescence imaging and phototherapy efficacy are dependent on competitive photophysical processes, so it is still a great challenge to engineer photosensitizer with appreciable light emission especially in the NIR light region, and highly efficient energy conversion into valuable reactive oxygen species. In this paper, we report series of simple perylene diimide (PDI)-based NIR photosensitizers by regulating the position of a phenyl moiety in the donor-acceptor-donor conjugated backbone, a packing balance between the twisted molecular structure and effective π-conjugation is actualized. Photodynamic property observation reveals that the developed fluorophores present desirable photosensitizing ability with the production of both type I and II reactive oxygen species (ROS) under light irradiation, and the eradication of tumor cells is realized based on ferroptosis mechanism. Moreover, the bright emission in NIR region allows for the sensitive detection of pulmonary metastasis in vivo . These results provide an illuminating NIR photosensitizers design strategy for image-guided tumor photodynamic therapy applications.
作者机构：
School of Chemical Engineering and Materials, Changzhou Institute of Technology, Changzhou 213022, China;[Qingqing Song; Meng Cao; Chunhong Tan; Xiao-Feng Wang; Kejie Du] School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China;[Yuheng Zhang; Yi Ding] Industrial College of Carbon Fiber and New Materials, Changzhou Institute of Technology, Changzhou 213022, China;[Yunkai Sun] School of Chemical Engineering and Materials, Changzhou Institute of Technology, Changzhou 213022, China<&wdkj&>School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China<&wdkj&>Industrial College of Carbon Fiber and New Materials, Changzhou Institute of Technology, Changzhou 213022, China;[Xiaoqiang Xue] School of Chemical Engineering and Materials, Changzhou Institute of Technology, Changzhou 213022, China<&wdkj&>Industrial College of Carbon Fiber and New Materials, Changzhou Institute of Technology, Changzhou 213022, China
通讯机构：
[Yunkai Sun; Xiao-Feng Wang; Kejie Du; Xiaoqiang Xue] S;School of Chemical Engineering and Materials, Changzhou Institute of Technology, Changzhou 213022, China<&wdkj&>School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China<&wdkj&>Industrial College of Carbon Fiber and New Materials, Changzhou Institute of Technology, Changzhou 213022, China<&wdkj&>School of Chemical Engineering and Materials, Changzhou Institute of Technology, Changzhou 213022, China<&wdkj&>Industrial College of Carbon Fiber and New Materials, Changzhou Institute of Technology, Changzhou 213022, China<&wdkj&>School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China
摘要：
Metal-organic complexes, particularly copper complexes, are emerging as promising candidates for anticancer drug due to their versatile redox states. Two copper complexes ( complex1 and complex2 ) have been designed based on the ligands for 1,10-phenanthroline (phen), 4,5-diazofluoren-9-one (DAFO) and 1,4-terephthalic acid (1,4-BDC), and the structures have been determined by X-ray single crystal analysis. The interactions of the complexes with calf thymus DNA (CT-DNA) have been investigated using UV-vis absorption and viscosity measurements. The results indicate that the complex 1 and complex 2 respectively bind to CT-DNA, and the binding mode of the former is in electrostatic binding or groove mode, while that of the latter is in insertion mode. The complex 2 had better activity to break CT-DNA than complex 1 .
Metal-organic complexes, particularly copper complexes, are emerging as promising candidates for anticancer drug due to their versatile redox states. Two copper complexes ( complex1 and complex2 ) have been designed based on the ligands for 1,10-phenanthroline (phen), 4,5-diazofluoren-9-one (DAFO) and 1,4-terephthalic acid (1,4-BDC), and the structures have been determined by X-ray single crystal analysis. The interactions of the complexes with calf thymus DNA (CT-DNA) have been investigated using UV-vis absorption and viscosity measurements. The results indicate that the complex 1 and complex 2 respectively bind to CT-DNA, and the binding mode of the former is in electrostatic binding or groove mode, while that of the latter is in insertion mode. The complex 2 had better activity to break CT-DNA than complex 1 .
期刊：
Progress in Materials Science,2026年156:101575 ISSN：0079-6425
通讯作者：
Yongli Zhou<&wdkj&>Chen Li<&wdkj&>Jianyong Ouyang<&wdkj&>Kuan Sun
作者机构：
[Yifan Wang; Ibrahim Mwamburi Mwakitawa; Hao Yang; Mingyu Song; Qian Huang; Xinzhe Li; Pengchi Zhang; Wei Fang; Yongli Zhou; Kuan Sun] MOE Key Laboratory of Low-Grade Energy Utilization Technologies and Systems, School of Energy & Power Engineering, Chongqing University, Chongqing 400044, PR China;[Lijun Hu] Hunan Key Laboratory for the Design and Application of Actinide Complexes, School of Chemistry and Chemical Engineering, University of South China, Hengyang, Hunan 421001, PR China;[Chen Li] Sibley School of Mechanical and Aerospace Engineering, Cornell University, Ithaca, NY 14853, USA;[Jianyong Ouyang] Department of Materials Science & Engineering, National University of Singapore, Singapore
通讯机构：
[Yongli Zhou; Kuan Sun] M;[Chen Li] S;[Jianyong Ouyang] D;Department of Materials Science & Engineering, National University of Singapore, Singapore<&wdkj&>MOE Key Laboratory of Low-Grade Energy Utilization Technologies and Systems, School of Energy & Power Engineering, Chongqing University, Chongqing 400044, PR China<&wdkj&>Sibley School of Mechanical and Aerospace Engineering, Cornell University, Ithaca, NY 14853, USA
摘要：
Ionic thermoelectrics (i-TEs) are emerging as a promising, sustainable technology for low-grade heat recovery, notable for their absence of moving mechanical parts. In recent years, significant advancements in i-TE materials and devices have been propelled by their advantages in thermal power generation, compatibility with room-temperature operation, and potential for integration into flexible, wearable devices. However, challenges remain to be addressed for practical future applications, primarily due to insufficient evaluations of innovative operational modes and materials. This review aims to bridge this gap by summarizing key existing theories and providing an in-depth analysis of ion migration mechanisms within i-TE capacitors. We also highlight significant contributions from leading studies, focusing on material selection, operational modes, performance characteristics, and pivotal discoveries. Ultimately, this review seeks to identify transformative approaches in i-TEs to foster innovative designs for practical applications.
Ionic thermoelectrics (i-TEs) are emerging as a promising, sustainable technology for low-grade heat recovery, notable for their absence of moving mechanical parts. In recent years, significant advancements in i-TE materials and devices have been propelled by their advantages in thermal power generation, compatibility with room-temperature operation, and potential for integration into flexible, wearable devices. However, challenges remain to be addressed for practical future applications, primarily due to insufficient evaluations of innovative operational modes and materials. This review aims to bridge this gap by summarizing key existing theories and providing an in-depth analysis of ion migration mechanisms within i-TE capacitors. We also highlight significant contributions from leading studies, focusing on material selection, operational modes, performance characteristics, and pivotal discoveries. Ultimately, this review seeks to identify transformative approaches in i-TEs to foster innovative designs for practical applications.
摘要：
Photocatalytic reduction is a promising way to remove radioactive uranium U(VI) in wastewater. Herein, an S-scheme ZnO@ZnS heterojunction with hollow structure and dual-vacancies of Zn and S (ZnV, SV) is developed. The hollow confined space enhances light trapping ability through multiple light scattering and reflection, while the existence of vacancies extends light absorption, further enhancing the utilization of solar spectrum. Furthermore, the density function theory (DFT) calculations demonstrate that co-sharing of metal atoms at the interface and the ZnV and SV dual-vacancies induce enhanced internal electric field (IEF), leading to facilitated S-scheme charge transfer, thereby resulting in improved retention of redox potential and suppressed carrier recombination dynamics. ZnO@ZnS shows a highest U(VI) removal rate of 96.48% along with a highest U enrichment of 514.33 mg/g, which is 3.6 and 2.7-folds enhanced compared to pristine ZnO and ZnS, respectively. Through various quenching experiments, a potential new mechanism for the catalytic reduction of U(VI) is proposed. Our findings reveal the involvement of h+ in the reaction, highlighting its significant catalytic role in the reduction process. Moreover, ZnO@ZnS performs excellent U(VI) extraction ability in open-air conditions without any sacrificial agents, revealing the great significance for practical applications.
Photocatalytic reduction is a promising way to remove radioactive uranium U(VI) in wastewater. Herein, an S-scheme ZnO@ZnS heterojunction with hollow structure and dual-vacancies of Zn and S (ZnV, SV) is developed. The hollow confined space enhances light trapping ability through multiple light scattering and reflection, while the existence of vacancies extends light absorption, further enhancing the utilization of solar spectrum. Furthermore, the density function theory (DFT) calculations demonstrate that co-sharing of metal atoms at the interface and the ZnV and SV dual-vacancies induce enhanced internal electric field (IEF), leading to facilitated S-scheme charge transfer, thereby resulting in improved retention of redox potential and suppressed carrier recombination dynamics. ZnO@ZnS shows a highest U(VI) removal rate of 96.48% along with a highest U enrichment of 514.33 mg/g, which is 3.6 and 2.7-folds enhanced compared to pristine ZnO and ZnS, respectively. Through various quenching experiments, a potential new mechanism for the catalytic reduction of U(VI) is proposed. Our findings reveal the involvement of h+ in the reaction, highlighting its significant catalytic role in the reduction process. Moreover, ZnO@ZnS performs excellent U(VI) extraction ability in open-air conditions without any sacrificial agents, revealing the great significance for practical applications.
作者：
Tao Huang;Xiaoxia He;Zulin Xiao;Juan Liu;Fusheng Li*
期刊：
European Journal of Organic Chemistry,2025年28(30):e202500448 ISSN：1434-193X
通讯作者：
Fusheng Li
作者机构：
[Tao Huang; Xiaoxia He; Zulin Xiao; Juan Liu; Fusheng Li] School of Chemistry and Chemical Engineering, University of South China, Hengyang, 421001 China
通讯机构：
[Fusheng Li] S;School of Chemistry and Chemical Engineering, University of South China, Hengyang, 421001 China
摘要：
α‐Allenols have become common advanced synthons for the synthesis of various of structures and are a frequent motif in natural products and pharmaceuticals. The special reactivity can occur due to the synergistic effect of the allene and hydroxy functional groups. Thus, many remarkable and elegant protocols have been explored through ionic pathways for the construction of α‐allenols. Recently, the rapid growth of radical chemistry has provided an alternative strategy to obtain α‐allenols through single‐electron transfer. As compared to the ionic pathway, the radical pathway has clear advantages, such as mild conditions, high efficiency, and excellent selectivity control. In this review, the most important contributions for the construction of α‐allenols are summarized via radical intermediates by categorizing them into different types of substrates. Additionally, mechanistic studies and synthetic challenges are highlighted.
α‐Allenols have become common advanced synthons for the synthesis of various of structures and are a frequent motif in natural products and pharmaceuticals. The special reactivity can occur due to the synergistic effect of the allene and hydroxy functional groups. Thus, many remarkable and elegant protocols have been explored through ionic pathways for the construction of α‐allenols. Recently, the rapid growth of radical chemistry has provided an alternative strategy to obtain α‐allenols through single‐electron transfer. As compared to the ionic pathway, the radical pathway has clear advantages, such as mild conditions, high efficiency, and excellent selectivity control. In this review, the most important contributions for the construction of α‐allenols are summarized via radical intermediates by categorizing them into different types of substrates. Additionally, mechanistic studies and synthetic challenges are highlighted.
期刊：
Chemical Communications,2025年61(85):16498-16511 ISSN：1359-7345
通讯作者：
Xing, H
作者机构：
[Huang, Xiaowei; Lin, Yingwu] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Xie, Wenxue; Huang, Xiaowei; Du, Jiajun; Li, Haokun; Xing, Hang] Hunan Univ, Inst Chem Biol & Nanomed, State Key Lab Chemo & Biosensing, Coll Chem & Chem Engn,Hunan Prov Key Lab Biomacrom, Changsha 410082, Peoples R China.;[Liu, Yuanyuan] Hunan Inst Drug Control, Changsha 410001, Hunan, Peoples R China.;[Xing, Hang] Hunan Univ Chongqing, Res Inst, Chongqing 401100, Peoples R China.
通讯机构：
[Xing, H ] H;Hunan Univ, Inst Chem Biol & Nanomed, State Key Lab Chemo & Biosensing, Coll Chem & Chem Engn,Hunan Prov Key Lab Biomacrom, Changsha 410082, Peoples R China.;Hunan Univ Chongqing, Res Inst, Chongqing 401100, Peoples R China.
摘要：
This highlight review article summarizes recent advances in employing HUH endonucleases as self-labeling protein tags for the sequence-specific covalent conjugation of unmodified ssDNA and examines their applications in cellular studies via engineered DNA-protein conjugates. We outline the structural basis and catalytic mechanism of the conserved HUH and Y motifs, which enable high selectivity, bioorthogonality, and robust conjugation under physiological conditions. Recent applications demonstrate the versatility of HUH-based DNA-protein conjugates in programmable cellular interface engineering, targeted therapeutic delivery, and enhancement of genome editing systems such as CRISPR-Cas. In the perspective section, we further highlight two emerging directions: computational tools such as the HUHgle platform for predictive substrate design, and directed evolution strategies extending HUH reactivity toward RNA substrates. Together, these advancements establish HUH endonucleases as powerful, programmable tools for generating DNA-protein conjugates that enable innovations in chemical biology, synthetic biology, and therapeutics.
摘要：
Research continues to be heavily focused on the synthesis of silver nanoparticles (Ag NPs) with programmable characteristics for various potential applications. In this study, a wet-chemical method was applied to synthesize Ag NPs modified with 3-aminopropyltriethoxysilane (APTES). A number of variables, including reaction time, temperature, precursor concentration, and the molar ratio of the raw components, were systematically investigated to modulate the structures and surface plasmon resonance (SPR) properties of Ag NPs. Notably, the Ag NPs demonstrated pronounced temperature- and/or time-dependent plasmonic effects owing to the transition between spherical Ag NPs capped by silanols or organosilicon oligomers and aggregated NPs coated with polysiloxane. Extending the reaction time (within a temperature range from 60 degrees C to 80 degrees C) facilitated the plasmonic coupling of spherical Ag NPs into aggregation, whereas an increase in reaction temperature promoted the formation of monodispersed spherical Ag NPs. The controllable SPR properties of Ag NPs, attributed to the transition between monodisperse and aggregated states, may prove advantageous for their prospective applications in chemical and biological sensing, analytical techniques, catalysis, as well as in diagnostic and therapeutic contexts.
期刊：
Molecular and Cellular Biochemistry,2025年480(4):2143-2157 ISSN：0300-8177
通讯作者：
Wang, J
作者机构：
[Jiang, Tingting] Univ South China, Hengyang Med Sch, Affiliated Nanhua Hosp, Dept Clin Lab, Hengyang 421000, Peoples R China.;[Zeng, Qun] Univ South China, Hengyang Med Sch, Dept Biochem & Mol Biol, Hengyang 421000, Peoples R China.;[Wang, Jing] Changsha Med Univ, Hunan Prov Key Lab Tradit Chinese Med Agr Biogenom, Changsha 410219, Peoples R China.;[Wang, Jing] Changsha Med Univ, Hunan Prov Univ Key Lab Fundamental & Clin Res Fun, Changsha 410219, Peoples R China.;[Wang, Jing] Changsha Med Univ, Clin Coll 1, Changsha 410219, Peoples R China.
通讯机构：
[Wang, J ] C;Changsha Med Univ, Hunan Prov Key Lab Tradit Chinese Med Agr Biogenom, Changsha 410219, Peoples R China.;Changsha Med Univ, Hunan Prov Univ Key Lab Fundamental & Clin Res Fun, Changsha 410219, Peoples R China.;Changsha Med Univ, Clin Coll 1, Changsha 410219, Peoples R China.
摘要：
FHL2 (Four-and-a-half LIM domain protein 2) is a crucial factor involved in cardiac morphogenesis, the process by which the heart develops its complex structure. It is expressed in various tissues during embryonic development, including the developing heart, and has been shown to play important roles in cell proliferation, differentiation, and migration. FHL2 interacts with multiple proteins to regulate cardiac development as a coactivator or a corepressor. It is involved in cardiac specification and determination of cell fate, cardiomyocyte growth, cardiac remodeling, myofibrillogenesis, and the regulation of HERG channels. Targeting FHL2 has therapeutic implications as it could improve cardiac function, control arrhythmias, alleviate heart failure, and maintain cardiac integrity in various pathological conditions. The identification of FHL2 as a signature gene in atrial fibrillation suggests its potential as a diagnostic marker and therapeutic target for this common arrhythmia.
期刊：
CURRENT ANALYTICAL CHEMISTRY,2025年20(9):1199-1212 ISSN：1573-4110
通讯作者：
Tan, Yan;Xiao, XL
作者机构：
[Chen, Zijie; Tan, Yan; Tan, Y; Xiao, Xilin; Huang, Shaorong; Wu, Qian; Xiao, XL; Liu, Zhen] Univ South China, Sch Publ Hlth, Hengyang Med Sch, Hengyang, Hunan, Peoples R China.;[Liu, Jingjing] Univ South China, Sch Chem & Chem Engn, Hengyang, Hunan, Peoples R China.;[Xiao, Xilin] Hunan Univ, State Key Lab Chemo Biosensing & Chemometr, Changsha, Hunan, Peoples R China.
通讯机构：
[Tan, Y; Xiao, XL ] U;Univ South China, Sch Publ Hlth, Hengyang Med Sch, Hengyang, Hunan, Peoples R China.
关键词：
Magnetic nanoparticles;MnFe2O4;graphene oxide;treatment;adsorption;uranium ions.
摘要：
Background: The problem of nuclear water pollution is becoming serious worldwide. Uranium, as a metal substance with long half-life radioactivity, is commonly treated by various methods. Adsorption is considered to be one of the most promising methods for treating uraniumcontaining wastewater.<&wdkj&>Method: Magnetic nanoparticles MnFe2O4 were prepared via the coprecipitation method, followed by modification of silica using the improved Stöber method. Subsequently, amino was functionalized and grafted onto graphene oxide to prepare a novel magnetic graphene oxide composite MnFe2O4@SiO2-NH2@GO.<&wdkj&>Results: The highest adsorption rate of MnFe2O4@SiO2-NH2@GO for uranium can reach 97.27% in 1 mg·L-1 uranium solution, and the adsorption process conformed to the quasi-second-order kinetic model and Langmuir adsorption isotherm model, indicating that it was a monolayer adsorption dominated by chemisorption. The adsorption thermodynamic parameters demonstrated that the adsorption process was a spontaneous endothermic reaction.<&wdkj&>Conclusion: MnFe2O4@SiO2-NH2@GO had excellent adsorption properties for uranium, which has great application potential in the treatment of low-concentration uranium-containing wastewater.
通讯机构：
[Lin, YW ; Wang, HM] U;[Xing, QY ] H;Univ South China, Sch Chem & Chem Engn, Hengyang, Peoples R China.;Hunan Inst Technol, Sch Chem & Environm Engn, Hengyang, Peoples R China.
摘要：
Aromatic organophosphorus compounds have significant applications in catalysis, organic synthesis, medicinal chemistry, and materials science. Herein, we report a metal-free, Et(3)N-mediated phosphorylation of 4-nitroisoxazoles with secondary phosphine oxides. The protocol proceeds via a unique dearomatization-elimination process, affording functionalized phosphonylated isoxazoles with good yields under mild conditions. Furthermore, some other aromatic substrates, including nitrofuran, nitroindole, nitrothiophene and nitroquinoxaline derivatives, can also undergo this reaction to afford the corresponding phosphonylated heteroarenes. Gram-scaled synthesis and synthetic transformations further suggest that this methodology has practical applicability and synthetic value. Additionally, we successfully synthesized novel phosphonylated enaminones via a one-pot cascade dearomatization/elimination/reductive ring-opening process.
摘要：
The magnetic properties of double perovskite oxide RE 2 FeCrO 6 (RE = GD, Tb, Dy, Er) were systematically studied, and the Griffiths phase evolution was observed. In Tb 2 FeCrO 6 , Dy 2 FeCrO 6 , and Er 2 FeCrO 6 , there are antiferromagnetic (AFM)-ferromagnetic (FM) first-order phase transition and the Griffiths phase with coexistence of FM and paramagnetic (PM) was observed by the EPR spectra. Gd 2 FeCrO 6 has an AFM–PM second-order phase transition, and there is no first-order phase transition in the range of ∆ H = 0–50 kOe. As the temperature decreases, all four sets of samples present χ −1 ( T ) deviates downwards from the Curie–Weiss linear behavior from 0.2 to 5 kOe, corresponding to the typical characteristics of Griffiths phase evolution. In addition, all four sets of samples have excellent magnetocaloric performance. Especially, the Gd 2 FeCrO 6 oxide has giant magnetic entropy change and relative cooling power (−∆ S M max = 30.31 J/kg K and RCP = 312.8 J/kg when ∆ H = 50 kOe). From the perspective of low-temperature magnetic refrigeration application, the present work provides important candidate references for magnetic component researchers.
摘要：
The major facilitator superfamily (MFS) type efflux pumps of Acinetobacter baumannii play important roles in antibiotic resistance. However, the molecular mechanism of these transporters remains poorly understood. To address the molecular basis of substrate polyspecificity mediated by multidrug MFS transporters, we compared the substrate binding modes of A. baumannii CraA with its well-studied homolog, Escherichia coli MdfA. MdfA and CraA share similar structural features, including a cavity accessible to drugs from the cytoplasm when these transporters adopt the inside-out conformation. This predominantly hydrophobic cavity contains several distinct titratable and hydrophilic residues. Through substitution analysis, we demonstrate that these polar residues within the CraA drug binding cavity contribute to the transport of all tested drugs, whereas mutations of hydrophobic residues result in altered drug recognition profiles. In addition to the known titratable residues E38 and D46, we identified E338 as the only titratable residue that plays a substrate-specific role, as it is required for efficient transport of norfloxacin, but not ethidium. Substitution of E338 with asparagine or glutamine changes substrate specificity, enabling specific recognition of phenicols and mitomycin C. Furthermore, we show that the aromaticity of Y42 is crucial for phenicol recognition, while general hydrophobicity at this position is critical for mitomycin C specificity. We propose that E338 and Y42 function as key substrate selectivity determinants in CraA. IMPORTANCE Multidrug efflux transporters of the major facilitator superfamily (MFS) are key contributors to antibiotic resistance, mediating the export of structurally diverse compounds across bacterial membranes. While homologous transporters such as Escherichia coli MdfA and Acinetobacter baumannii CraA share high structural similarity and overlapping substrate profiles, the molecular basis of their substrate specificity remains poorly understood. In this study, we show that structural homology among MFS transporters does not inherently imply mechanistic conservation, as species-specific variations can give rise to distinct substrate recognition profiles. Our findings reveal that CraA utilizes unique residues Y42 and E338 for substrate selectivity, while R124 and Y73 contribute to its transport activity. These findings enhance our understanding of efflux pump specificity and underscore the need to consider organism-specific features when targeting multidrug transporters in antimicrobial therapy.
The major facilitator superfamily (MFS) type efflux pumps of Acinetobacter baumannii play important roles in antibiotic resistance. However, the molecular mechanism of these transporters remains poorly understood. To address the molecular basis of substrate polyspecificity mediated by multidrug MFS transporters, we compared the substrate binding modes of A. baumannii CraA with its well-studied homolog, Escherichia coli MdfA. MdfA and CraA share similar structural features, including a cavity accessible to drugs from the cytoplasm when these transporters adopt the inside-out conformation. This predominantly hydrophobic cavity contains several distinct titratable and hydrophilic residues. Through substitution analysis, we demonstrate that these polar residues within the CraA drug binding cavity contribute to the transport of all tested drugs, whereas mutations of hydrophobic residues result in altered drug recognition profiles. In addition to the known titratable residues E38 and D46, we identified E338 as the only titratable residue that plays a substrate-specific role, as it is required for efficient transport of norfloxacin, but not ethidium. Substitution of E338 with asparagine or glutamine changes substrate specificity, enabling specific recognition of phenicols and mitomycin C. Furthermore, we show that the aromaticity of Y42 is crucial for phenicol recognition, while general hydrophobicity at this position is critical for mitomycin C specificity. We propose that E338 and Y42 function as key substrate selectivity determinants in CraA.
IMPORTANCE
Multidrug efflux transporters of the major facilitator superfamily (MFS) are key contributors to antibiotic resistance, mediating the export of structurally diverse compounds across bacterial membranes. While homologous transporters such as Escherichia coli MdfA and Acinetobacter baumannii CraA share high structural similarity and overlapping substrate profiles, the molecular basis of their substrate specificity remains poorly understood. In this study, we show that structural homology among MFS transporters does not inherently imply mechanistic conservation, as species-specific variations can give rise to distinct substrate recognition profiles. Our findings reveal that CraA utilizes unique residues Y42 and E338 for substrate selectivity, while R124 and Y73 contribute to its transport activity. These findings enhance our understanding of efflux pump specificity and underscore the need to consider organism-specific features when targeting multidrug transporters in antimicrobial therapy.
Multidrug efflux transporters of the major facilitator superfamily (MFS) are key contributors to antibiotic resistance, mediating the export of structurally diverse compounds across bacterial membranes. While homologous transporters such as Escherichia coli MdfA and Acinetobacter baumannii CraA share high structural similarity and overlapping substrate profiles, the molecular basis of their substrate specificity remains poorly understood. In this study, we show that structural homology among MFS transporters does not inherently imply mechanistic conservation, as species-specific variations can give rise to distinct substrate recognition profiles. Our findings reveal that CraA utilizes unique residues Y42 and E338 for substrate selectivity, while R124 and Y73 contribute to its transport activity. These findings enhance our understanding of efflux pump specificity and underscore the need to consider organism-specific features when targeting multidrug transporters in antimicrobial therapy.
Multidrug efflux transporters of the major facilitator superfamily (MFS) are key contributors to antibiotic resistance, mediating the export of structurally diverse compounds across bacterial membranes. While homologous transporters such as Escherichia coli MdfA and Acinetobacter baumannii CraA share high structural similarity and overlapping substrate profiles, the molecular basis of their substrate specificity remains poorly understood. In this study, we show that structural homology among MFS transporters does not inherently imply mechanistic conservation, as species-specific variations can give rise to distinct substrate recognition profiles. Our findings reveal that CraA utilizes unique residues Y42 and E338 for substrate selectivity, while R124 and Y73 contribute to its transport activity. These findings enhance our understanding of efflux pump specificity and underscore the need to consider organism-specific features when targeting multidrug transporters in antimicrobial therapy.
关键词：
2-((2-(hydroxymethyl)quinolin-8-yl)oxy)-N-(quinolin-8-yl)acetamide;density functional theory;molecular simulation;solvent systems;“five toxic” heavy metal
摘要：
Addressing severe environmental and health threats posed by mercury, cadmium, lead, chromium, and arsenic ("five toxic" heavy metals), this study employs density functional theory (DFT) calculations and molecular simulations to investigate the capture and detection mechanisms of the dual-fluorescent probe 2-((2-(hydroxymethyl)quinolin-8-yl)oxy)-N-(quinolin-8-yl)acetamide in both water solvent and dimethyl sulfoxide (DMSO). Key findings indicate that the probe forms highly stable, planar complexes with arsenic, lead, and chromium, exhibiting significant red-shifts in UV absorption bands and enhanced fluorescence intensity-strongest for arsenic in water solvent, while arsenic/chromium complexes show markedly increased fluorescence in DMSO. This work demonstrates the probe's selective recognition of As, Pb, and Cr, with solvent polarity modulating detection signals, providing a novel theoretical framework for monitoring and remediating heavy metal pollution.
作者机构：
[Chen, Qianwen; Li, Qiulin; Bao, Shu-Juan; Tan, Yangyang; Ma, Yan-Dong; He, Ruilin] Southwest Univ, Inst Clean Energy & Adv Mat, Fac Mat & Energy, Key Lab Luminescent & Real Time Analyt Chem,Minist, Chongqing 400715, Peoples R China.;[Deng, Zhiqin; Liu, Heng] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.;[Chen, Qianwen; Li, Qiulin; Bao, Shu-Juan; Tan, Yangyang; Ma, Yan-Dong; He, Ruilin] Southwest Univ, Chongqing Key Lab Battery Mat & Technol, Chongqing 400715, Peoples R China.
通讯机构：
[Bao, SJ ] S;[Liu, H ] U;Southwest Univ, Inst Clean Energy & Adv Mat, Fac Mat & Energy, Key Lab Luminescent & Real Time Analyt Chem,Minist, Chongqing 400715, Peoples R China.;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.;Southwest Univ, Chongqing Key Lab Battery Mat & Technol, Chongqing 400715, Peoples R China.
摘要：
Iron carbide assisted Fe–N–C electrocatalysts have attracted significant attention as promising candidates to enhance intrinsic activity in the oxygen reduction reaction (ORR), offering a viable alternative to Pt-based catalysts. However, their widespread development is impeded by challenges such as uncontrolled aggregation, the formation of large nanoparticles, and inefficient synthesis processes. Herein, we report a multiligand coordination self-assembly strategy to synthesize a novel metal–organic framework (MOF) precursor (FeZn-PBMI) with dual ligands and dual metals, followed by a thermal polymerization self-assembly process that successfully prepared FeN x sites and Fe x C atomic clusters decorating N-doped carbon nanotubes (Fe x C@FeNCNTs) in gram-scale quantities. The ordered distribution of Zn and Fe within the FeZn-PBMI effectively prevents Fe aggregation during high-temperature pyrolysis, resulting in uniformly dispersed approximately 10 nm Fe x C nanoparticles. As expected, the Fe x C@FeNCNTs exhibit superior ORR performance with a half-wave potential of 0.87 V, surpassing commercial Pt/C (0.85 V), and demonstrate excellent long-term stability in Zn–air batteries with 1000 cycles. This synthetic approach may facilitate the development of highly active catalysts, advancing the practical application of Fe–N–C catalysts in various energy-related technologies.
通讯机构：
[Ou, LJ ] H;[He, WM ] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Hunan Inst Technol, Sch Mat Sci & Engn, Hengyang 421002, Peoples R China.
关键词：
N -heteroarenes;fluoroalkylation;isocyanide;chloride radical;hydrogen atom transfer
摘要：
The first example of the dual-functional photocatalytic fluoroalkylation of 2-isocyanides with R f SO 2 Cl catalyzed by Yb@g-C 3 N 4 has been accomplished by simultaneously coupling the photogenerated electron-driven reductive production of fluoroalkyl radicals with the photogenerated hole-driven oxidative production of chloride radicals. This strategy not only fully utilizes photogenerated electron–hole pairs for bond formation but also avoids the use of exogenous chloride salts, additional redox reagents, and sacrificial electron donors/acceptors. A variety of fluoroalkylated N -heteroarenes were heterogeneously synthesized in good to high yields with excellent functional-group compatibility. Furthermore, applying sono-photocatalysis not only improves the energy efficiency but also increases the reaction rate and overall efficiency.
期刊：
Journal of Radioanalytical and Nuclear Chemistry,2025年334(1):709-726 ISSN：0236-5731
通讯作者：
Nie, Chang-ming;Peng, GW
作者机构：
[Peng, Guo-wen; Guo, Meng-zhen; Xiao, Xi-lin; Wang, Yun; Kong, Xiang-he; Peng, GW; Nie, Chang-ming; Wu, Can-ran; Ouyang, Wen-jun; Nie, CM] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Peng, Guo-wen; Guo, Meng-zhen; Xiao, Xi-lin; Wang, Yun; Kong, Xiang-he; Peng, GW; Nie, Chang-ming; Wu, Can-ran; Ouyang, Wen-jun; Nie, CM] Key Lab Hunan Prov Design & Applicat Nat Actinide, Hengyang 421001, Peoples R China.
通讯机构：
[Peng, GW ; Nie, CM] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Key Lab Hunan Prov Design & Applicat Nat Actinide, Hengyang 421001, Peoples R China.
关键词：
Chiral-at-uranium complex;R/S-O,O-dimethyl-S-[1,2-bis(ethoxycarbonyl)ethyl]thiophosphates (R/S-DBTPs);Complexation;Enantioseparation;Density functional theory (DFT)
摘要：
It's very important to design novel uranium(VI) complexes with enantioselectivity for identification and enantioseparation of chiral pesticides. Enantiomers of O,O-dimethyl-S-[1,2-bis(ethoxycarbonyl)ethyl]thiophosphates(DBTPs) exhibit different biological toxicities. In this work, two novel chiral-at-uranium complexes (uranyl-2-(9-(1H-indazole-1-carbonyl)-1,10-phenanthrolin-2-yl)-1H-inden-1-one (Uranyl-IPIDO) and uranyl-2-(9-(1-oxo-1H-inden-2-yl)-1,10-phenanthrolin-2-yl)naphthalene-1,4-dione (Uranyl-OPND)) were designed to selectively enantioseparate R/S-DBTPs. Based on density functional theory (DFT), complexation behaviors and enantioseparation of Uranyl-IPIDO/Uranyl-OPND with R/S-DBTPs were theoretically investigated. Through analyses of EDA, Delta G, ESP, QTAIM, EDDM, LOL, FMO, MO, IGMH, ETS-NOCV, we found that Uranyl-IPIDO/Uranyl-OPND demonstrated excellent enantioseparation performance for R/S-DBTPs, with separation factors of 110-30526 and enantioselectivity coefficients exceeding 99% in water, butanol, octanol, and propanoic acid.
作者机构：
[Zhou, Daming; Qin, AJ; Zhang, Guiquan; Qin, Anjun] South China Univ Technol, Guangdong Prov Key Lab Luminescence Mol Aggregates, State Key Lab Luminescent Mat & Devices, Guangzhou 510640, Peoples R China.;[Tang, Ben Zhong] Chinese Univ Hong Kong, Shenzhen Inst Aggregate Sci & Technol, Sch Sci & Engn, Shenzhen CUHK Shenzhen, Shenzhen 518172, Peoples R China.;[Hu, Rong; Hu, R] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
通讯机构：
[Qin, AJ ] S;[Tang, BZ ] C;[Hu, R ] U;South China Univ Technol, Guangdong Prov Key Lab Luminescence Mol Aggregates, State Key Lab Luminescent Mat & Devices, Guangzhou 510640, Peoples R China.;Chinese Univ Hong Kong, Shenzhen Inst Aggregate Sci & Technol, Sch Sci & Engn, Shenzhen CUHK Shenzhen, Shenzhen 518172, Peoples R China.
摘要：
Fluorescence imaging technology is playing increasing roles in modern personalized and precision medicine. Thanks to their excellent photophysical properties, organic luminogens featuring aggregation-induced emission (AIE) characteristics (AIEgens) have attracted considerable attention over the past two decades. Because of their superior biocompatibility, ease of processing and functionalization, excellent water solubility, high responsiveness, and exceptional signal-to-noise ratio (SNR) for biotargets, AIE bioconjugates, formed by covalently linking AIEgens with biomolecules, have emerged as an ideal candidate for bioapplications. In this review, we summarize the progress in preparation, properties, and application of AIE bioconjugates in the last five years. Moreover, the challenges and opportunities of AIE bioconjugates are also briefly discussed.
摘要：
Enhanced bulk-surface charges separation and migration are essential to maximize the photocatalytic activity. In this study, ethylenediamine (EDA)-modified Zn 0.7 Cd 0.3 S nanorods (ZCS-NR-EDA) were synthesized through an integral modification approach. After 1-hour adsorption equilibrium followed by 6-minute co-irradiation with visible light and ultrasonic waves, ZCS-NR-EDA removed 99.2 % of U(VI) from the solution, significantly better than Zn 0.7 Cd 0.3 S nanoparticles (ZCS-NP) (13.6 %) and Zn 0.7 Cd 0.3 S nanorods (ZCS-NR) (25.3 %). This catalytic performance has outperformed most reported materials. Experimental and density functional theory (DFT) calculation studies confirmed that EDA modification induced polarization to establish a bulk electric field (BEF) and modified the electron distribution at the material's surface to create localized surface electric field (LSEF), while simultaneously enhancing the material's piezoelectric properties. The synergistic effect of these triple electric fields (polarization-induced BEF, LSEF, and piezoelectric field (PF)) promoted migration of bulk-surface charges, thereby enhancing catalytic performance. When applied to uranium spiked tailing water, ZCS-NR-EDA achieved up to 98.1 % U(VI) removal within 15 min of combined visible light and ultrasonic irradiation (after adsorption equilibrium). More importantly, this “tri-electric fields synergy” strategy provides a novel approach for the design of advanced photocatalytic materials.
Enhanced bulk-surface charges separation and migration are essential to maximize the photocatalytic activity. In this study, ethylenediamine (EDA)-modified Zn 0.7 Cd 0.3 S nanorods (ZCS-NR-EDA) were synthesized through an integral modification approach. After 1-hour adsorption equilibrium followed by 6-minute co-irradiation with visible light and ultrasonic waves, ZCS-NR-EDA removed 99.2 % of U(VI) from the solution, significantly better than Zn 0.7 Cd 0.3 S nanoparticles (ZCS-NP) (13.6 %) and Zn 0.7 Cd 0.3 S nanorods (ZCS-NR) (25.3 %). This catalytic performance has outperformed most reported materials. Experimental and density functional theory (DFT) calculation studies confirmed that EDA modification induced polarization to establish a bulk electric field (BEF) and modified the electron distribution at the material's surface to create localized surface electric field (LSEF), while simultaneously enhancing the material's piezoelectric properties. The synergistic effect of these triple electric fields (polarization-induced BEF, LSEF, and piezoelectric field (PF)) promoted migration of bulk-surface charges, thereby enhancing catalytic performance. When applied to uranium spiked tailing water, ZCS-NR-EDA achieved up to 98.1 % U(VI) removal within 15 min of combined visible light and ultrasonic irradiation (after adsorption equilibrium). More importantly, this “tri-electric fields synergy” strategy provides a novel approach for the design of advanced photocatalytic materials.
