摘要：
The rapid and selective identification of microorganisms is of great significance for clinical therapy applications. To develop high performance probes for microbe determination, we systemically constructed series aggregation-induced emission (AIE) luminogens by modulating the structural planarity, the basicity of functional group, the length of linker moiety and the hydrophobicity based on our previous work. The detail structure-property relationship study based on experimental and theoretical observation revealed that: i) the planar skeleton is essential for probe insertion towards the cell wall via van n der Waals' force. ii) the basic function group enable the anchoring on the membrane by binding with acidic biomolecules. iii) the shortened alkyl chain is in favor of the efficient binding of basic groups with microbes and endows the desirable hydrophobicity. Based on the developed probes, the successful detection of the pathogens in clinic samples was achieved in highly sensitive and simple way. This work provides a reliable strategy for designing intelligent luminogens for microorganism discrimination and identification in efficient and sensitive way for in vitro diagnosis applications, especially point-of-care testing (POCT).
The rapid and selective identification of microorganisms is of great significance for clinical therapy applications. To develop high performance probes for microbe determination, we systemically constructed series aggregation-induced emission (AIE) luminogens by modulating the structural planarity, the basicity of functional group, the length of linker moiety and the hydrophobicity based on our previous work. The detail structure-property relationship study based on experimental and theoretical observation revealed that: i) the planar skeleton is essential for probe insertion towards the cell wall via van n der Waals' force. ii) the basic function group enable the anchoring on the membrane by binding with acidic biomolecules. iii) the shortened alkyl chain is in favor of the efficient binding of basic groups with microbes and endows the desirable hydrophobicity. Based on the developed probes, the successful detection of the pathogens in clinic samples was achieved in highly sensitive and simple way. This work provides a reliable strategy for designing intelligent luminogens for microorganism discrimination and identification in efficient and sensitive way for in vitro diagnosis applications, especially point-of-care testing (POCT).
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.
通讯机构：
[Tan, N ] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
摘要：
The stealth segment poly(2-ethyl-2-oxazoline) (PEOX) was attempted to be grafted onto the surface of an andrographolide-imprinted polymer (ADR-MMIP) invented in our laboratory to obtain a new intelligent stimuli-responsive drug carrier with better controllable ADR release, anti-cancer, and stealth (ability to evade the immune system) properties. Serial characterization using modern instrumental analysis techniques, including Fourier-transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), vibrating sample magnetometry (VSM), transmission electron microscopy (TEM) as well as Brunauer–Emmett–Teller (BET) and zeta potential (ZP) analyses, confirmed that the novel target ADR/PEOX-MMIP was successfully prepared. Material performance tests showed that ADR/PEOX-MMIP had favourable stability and exhibited a mere decrease of 14.83% in adsorption capacity after five adsorption–desorption cycles, good selectivity adsorption for ADR with a relative selectivity coefficient of 1.4375, an acceptable ADR loading capacity of 11.46 mg g −1 , and satisfactory ADR-controllable release with a maximum cumulative drug release rate of 73.10% in response to pH/redox/light stimulation in vitro and a slower release time of 210 h compared with ADR-MMIP (60 h). Notably, ADR/PEOX-MMIP possessed definite A549 lung cancer cell cytotoxicity, with a maximum cell inhibition rate of 36% at a concentration of 160 μg mL −1 and excellent stealth performance for escaping the non-specific effects of macrophages, which indicate that it should be able to effectively improve the present therapeutic defects of ADR, both in theory and real-world practice, and provide a new idea for the development of intelligent drug carriers in the future. The adsorption mechanism of the prepared target material is also discussed in detail in this study.
通讯机构：
[Gu, YL ] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421000, Hunan, Peoples R China.
关键词：
Composite transparent polyimide film;Flexible display;Finite element analysis
摘要：
Polyimide is a high-performance polymer material that is widely used in the manufacture of printed circuit boards, cable insulation, and other electronic components because of its excellent electrical insulation properties and thermal stability. In this study, a transparent polyimide composite film material (5% CPI/OAPOSS@Al2O3) made from octaaminophenylpolysilsesquioxane (OAPOSS)-modified Al2O3 (in which the OAPOSS-modified Al2O3 filler content is 5%) homogeneously dispersed in a transparent polyimide (CPI) was used, and a foldable screen model made from the polyimide material was designed. A folding screen model made of this polyimide material was designed, and its performance in a complex mechanical environment was analyzed by detailed finite element simulation, to obtain the comprehensive performance of the composite folding screen model in a complex environment, and to try to analyze the law of the material performance in terms of the microscopic molecular structure. The simulation results show that the maximum equivalent stress of the composite CPI material in the folded screen model increases from 33.431 Mpa to 109.640 Mpa under the bending angles of 15 degrees, 45 degrees, 90 degrees, 135 degrees and 180 degrees; the elastic strain increases from 0.010131 mm/mm to 0.033224 mm/mm; and the total deformation increases from 1.762 mm to 71 mm. 1.762 mm to 71.439 mm, indicating that the 5% CPI/OAPOSS@Al2O3 composite CPI material has excellent mechanical strength and toughness, can be reversibly deformed in a wide range, and can withstand a certain degree of plastic deformation in the case of exceeding the elastic limit; the coefficient of safety is reduced from 2.5784 to 0.7862, which indicates that it can absorb enough energy during bending and has a certain plastic deformation ability, and is not prone to brittle fracture; the fatigue life of the composite material is 250,370 times when it is folded for many cycles under the condition that the bending angle is 180 degrees, i.e., the material is able to withstand many times of bending in the model of the folded screen without any significant damage or destruction. The results show that the folding screen model made of the composite material has excellent performance in all aspects, indicating that the 5% CPI/OAPOSS@Al2O3 material is fully capable of being applied in the folding screen cell phone screen, and the application of this series of polyimide-modified materials as flexible displays has a very bright future.
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.
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.
摘要：
Surface microstructure of grains vastly decides the electrochemical performance of nickel-rich oxide cathodes, which can improve their interfacial kinetics and structural stability to realize their further popularization. Herein, taking the representative LiNi(0.8)Co(0.15)Al(0.05)O(2) (NCA) materials as an example, a surface heterojunction structure construction strategy to enhance the interface characteristics of high-nickel materials by introducing interfacial ZnO sites has been designed (NCA@ZnO). Impressively, this heterointerface creates a strong built-in electric field, which significantly improves electron/Li-ion diffusion kinetics. Concurrently, the ZnO layer acts as an effective physical barrier against electrolyte corrosion, notably suppressing interfacial parasitic reactions and ultimately optimizing the structure stability of NCA@ZnO. Benefiting from synchronous optimization of interface stability and kinetics, NCA@ZnO exhibits advanced cycling performance with the capacity retention of 83.7% after 160 cycles at a superhigh rate of 3 C during 3.0-4.5 V. The prominent electrochemical performance effectively confirms that the surface structure design provides a critical approach toward obtaining high-performance cathode materials with enhanced long-cycling stability.
摘要：
The development of efficient gamma-ray shielding materials is crucial for addressing increasingly complex radiation environments. In this study, (BiO) 4 CO 3 (OH) 2 (BCH) and (BiO) 4 CO 3 (OH) 2 @Gd 2 O(CO 3 ) 2 ·H 2 O (BG) fillers were synthesized via a hydrothermal method. After being dispersed into epoxy resin by mechanical stirring, the mixtures were molded using a vacuum-assisted thermal curing process. Under 59.5 keV gamma irradiation, the linear attenuation coefficient (LAC) of BG/EP-50 reached 5.8 cm −1 , representing an 84% increase compared to BCH/EP-50 (3.15 cm −1 ) and about 33 times that of pure EP (0.17 cm −1 ). In addition, the temperature at 50% weight loss (T 50% ) of BG/EP-50 increased to 637.9〬C, which is 60.9% higher than that of the epoxy matrix, indicating improved thermal stability. The BG filler, constructed through a simple two-step hydrothermal route, demonstrated a synergistic effect between Bi and Gd components, which not only compensated for the limitations of Bi in the low-energy region but also enhanced the gamma shielding capability of the epoxy resin at higher energies. Compared to several shielding materials reported in recent years, BG/EP-50 shows superior performance and offers a promising strategy for lightweight and environmentally friendly polymer-based gamma shielding materials.
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.
作者机构：
[Yang, Minghui; Chen, Fei; Liu, You-Nian; Deng, Liu] Cent South Univ, Coll Chem & Chem Engn, Hunan Prov Key Lab Micro & Nano Mat Interface Sci, Changsha 410083, Hunan, Peoples R China.;[Chen, Fei] Xinjiang Med Univ, Coll Pharm, Xinjiang Key Lab Nat Med Act Components & Drug Rel, Urumqi 830017, Xinjiang, Peoples R China.;[Wang, Liqiang] Zhengzhou Univ, Henan Prov Ind Technol Res Inst Resources & Mat, Sch Mat Sci & Engn, Zhengzhou 450001, Henan, Peoples R China.;[He, Haichuan] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.;[Liu, You-Nian] Hangzhou Normal Univ, Coll Mat Chem & Chem Engn, Hangzhou 311121, Zhejiang, Peoples R China.
通讯机构：
[He, HC ] U;[Liu, YN ] C;Cent South Univ, Coll Chem & Chem Engn, Hunan Prov Key Lab Micro & Nano Mat Interface Sci, Changsha 410083, Hunan, Peoples R China.;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.;Hangzhou Normal Univ, Coll Mat Chem & Chem Engn, Hangzhou 311121, Zhejiang, Peoples R China.
摘要：
Carbon-supported non-noble metal-based catalysts display remarkable catalytic activity and cost-effectiveness in electrochemical CO2 reduction reaction (eCO2RR). However, precise control of the crystal facet of metal catalysts and prevention of deactivation caused by agglomeration remain challenges. Herein, a novel dual-function customized strategy is presented for the preparation of the N-doped carbon-supported Ni-based porous catalyst with carbon-encapsulated Ni(111) nanoparticles (Ni(111)@C-NDPC), through carbonizing the self-assembly of protein-Ni-ions networks and ethylenediaminetetraacetic acid (EDTA)-chelated Ni-ions (EDTA-Ni). High exposure of the (111) surface of carbon-encapsulated nickel nanoparticles is achieved through strong coordination between EDTA-Ni, thereby synergistically integrating the advantages of highly active Ni(111) and stable carbon-encapsulated structure formed by protein-Ni-ions networks. Theoretical calculations reveal that Ni(111) facilitates the formation of *COOH and inhibits the hydrogen evolution reaction. The as-prepared Ni(111)@C-NDPC electrocatalyst exhibits an excellent CO Faradaic efficiency (FECO) of 96.3% and stability over 50 h while maintaining FECO above 90% in a wide current density range of 50-300 mA cm-2. This work provides a new strategy for precisely customizing highly selective and durable carbon-supported metal eCO2RR electrocatalysts.
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：
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.
作者：
Ji, Hong-Tao;Lu, Yu-Han;Liu, Yan-Ting;Huang, Yu-Lin;Tian, Jiang-Feng;...
期刊：
中国化学快报(英文),2025年36(2):110568 ISSN：1001-8417
通讯作者：
Zhang, YH;He, WM
作者机构：
[Liu, Yan-Ting; Liu, Feng; Ji, Hong-Tao; Huang, Yu-Lin; Zhang, Yong-Hong] Univ South China, Affiliated Nanhua Hosp, Hengyang Med Sch, Dept Ophthalmol, Hengyang 421001, Peoples R China.;[Zeng, Yan-Yan; Lu, Yu-Han; He, Wei-Min; Tian, Jiang-Feng; Ji, Hong-Tao; He, WM] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Yang, Hai-Yan] Cent South Univ, Hunan Canc Hosp, Affiliated Canc Hosp,Xiangya Sch Med, Dept Lung Canc & Gastroenterol, Changsha 410013, Peoples R China.
通讯机构：
[Zhang, YH ; He, WM ] U;Univ South China, Affiliated Nanhua Hosp, Hengyang Med Sch, Dept Ophthalmol, Hengyang 421001, Peoples R China.;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
关键词：
Dual catalysis;Semiconductor;Chlorine;Redox catalyst;Hydrogen atom transfer
摘要：
The first example of Nd@C3N4-photoredox/chlorine dual catalyzed alkylation with unactivated alkanes as the alkyl sources has been developed, which allows for the synthesis of various 4-alkylated cyclic sulfonyl ketimines. In this process, chlorine functions as both a redox and hydrogen atom transfer catalyst. The synergism of the reversible Nd2+/Nd3+ and Cl¯/Cl˙ redox pairs significantly enhances overall photocatalytic efficiency. The in vitro anticancer activity of 4-alkylated products was evaluated by using the CCK8 assay against both human choroidal melanoma (MUM-2B) and lung cancer (A549) cell. Compound 3da showed approximately triple the potency of 5-fluorouracil.
The first example of Nd@C3N4-photoredox/chlorine dual catalyzed alkylation with unactivated alkanes as the alkyl sources has been developed, which allows for the synthesis of various 4-alkylated cyclic sulfonyl ketimines. In this process, chlorine functions as both a redox and hydrogen atom transfer catalyst. The synergism of the reversible Nd2+/Nd3+ and Cl¯/Cl˙ redox pairs significantly enhances overall photocatalytic efficiency. The in vitro anticancer activity of 4-alkylated products was evaluated by using the CCK8 assay against both human choroidal melanoma (MUM-2B) and lung cancer (A549) cell. Compound 3da showed approximately triple the potency of 5-fluorouracil.
摘要：
The formation of aggregate always limits the reactive oxygen species generation efficacy of photosensitizer (PS). Developing PS with high performance under physiological environment is essential for the widespread application of photodynamic therapy (PDT) in clinic. In this work, platinum-based photosensitizers with adaptive confinement effect are designed and prepared for enhanced tumor PDT treatments. By introducing pyridinothiadiazole with sp 2 nitrogen hybridization and strong electron-withdrawing properties as the ligand, spin-orbit coupling (SOC) could be efficiently enhanced, accelerating intersystemic scampering (ISC) and ultimately improving the generation efficiency of reactive oxygen species (ROS). Firstly, the developed complexes effectively reduce the photosensitizing inhibition with the formation of aggregate, enabling more efficient photodynamic activity under physiological conditions. Secondly, both experimental and simulative investigations support the high affinity of Pt-based PSs towards biomacromolecules, which allows for the acquisition of confinement effect. The relatively high binding affinity with biomacromolecules enables the improved photosensitizing ability of PSs compared to the individual ones, which is highly desirable for practical therapy applications. Finaly, in vitro cytotoxicity exploration reveals that Pt-based complexes will trigger the oxidative stress and further induce ferroptosis of tumor cells to eradicate tumor cell upon white light irradiation. The desirable tumor inhibition in vivo is also achieved. This work provides a reliable strategy to construct PSs with high performance to address the various demands PDT treatments in clinical.
The formation of aggregate always limits the reactive oxygen species generation efficacy of photosensitizer (PS). Developing PS with high performance under physiological environment is essential for the widespread application of photodynamic therapy (PDT) in clinic. In this work, platinum-based photosensitizers with adaptive confinement effect are designed and prepared for enhanced tumor PDT treatments. By introducing pyridinothiadiazole with sp 2 nitrogen hybridization and strong electron-withdrawing properties as the ligand, spin-orbit coupling (SOC) could be efficiently enhanced, accelerating intersystemic scampering (ISC) and ultimately improving the generation efficiency of reactive oxygen species (ROS). Firstly, the developed complexes effectively reduce the photosensitizing inhibition with the formation of aggregate, enabling more efficient photodynamic activity under physiological conditions. Secondly, both experimental and simulative investigations support the high affinity of Pt-based PSs towards biomacromolecules, which allows for the acquisition of confinement effect. The relatively high binding affinity with biomacromolecules enables the improved photosensitizing ability of PSs compared to the individual ones, which is highly desirable for practical therapy applications. Finaly, in vitro cytotoxicity exploration reveals that Pt-based complexes will trigger the oxidative stress and further induce ferroptosis of tumor cells to eradicate tumor cell upon white light irradiation. The desirable tumor inhibition in vivo is also achieved. This work provides a reliable strategy to construct PSs with high performance to address the various demands PDT treatments in clinical.
摘要：
The exploration of multiphases and 0D/2D heterojunction in transition metal phosphides (TMPs) and transition metal sulfides (TMDs) is of major interest for hydrogen evolution reaction (HER). Herein, a novel combination route where 0D mixed-phased 1T/2H molybdenum sulfide quantum dots (MoS 2 QDs) are uniformly anchored on the 2D CoP x nanosheets is developed. MoS 2 QDs and CoP x were prepared via hydrothermal method and mixed with different ratios (Mo:Co ratios of 2:1, 1:1, and 1:2) and annealed under different temperatures to modulate their application in acidic HER processes. Specifically, 2Mo/1Co exhibited advanced performance for HER in 0.5 M H 2 SO 4 solution and required 14 mV to deliver 10 mA cm −2 and revealed a descended Tafel slope of 75.42 mV dec −1 with 240 h stability except obvious deactivation. The successful design and construction of 0D/2D mixed-dimensional materials would broaden the application of MoS 2 and CoP x for electrocatalytic hydrogen evolution.
The exploration of multiphases and 0D/2D heterojunction in transition metal phosphides (TMPs) and transition metal sulfides (TMDs) is of major interest for hydrogen evolution reaction (HER). Herein, a novel combination route where 0D mixed-phased 1T/2H molybdenum sulfide quantum dots (MoS 2 QDs) are uniformly anchored on the 2D CoP x nanosheets is developed. MoS 2 QDs and CoP x were prepared via hydrothermal method and mixed with different ratios (Mo:Co ratios of 2:1, 1:1, and 1:2) and annealed under different temperatures to modulate their application in acidic HER processes. Specifically, 2Mo/1Co exhibited advanced performance for HER in 0.5 M H 2 SO 4 solution and required 14 mV to deliver 10 mA cm −2 and revealed a descended Tafel slope of 75.42 mV dec −1 with 240 h stability except obvious deactivation. The successful design and construction of 0D/2D mixed-dimensional materials would broaden the application of MoS 2 and CoP x for electrocatalytic hydrogen evolution.
摘要：
With Ag/g‐C 3 N 4 semiconductor as the heterogeneous photocatalyst, the visible light promoted heterogeneous synthesis of unsymmetric diaryl chalcogenides could be achieved under additive‐free and mild conditions. A series of unsymmetric diaryl chalcogenides were generated in good to excellent yields with high functional group tolerance. The Ag/g‐C 3 N 4 photocatalyst is easily recovered from the reaction mixture and reused at least 5 times, opening the way for larger‐scale industrial applications of this type of photocatalytic bond‐forming reactions.
With Ag/g‐C 3 N 4 semiconductor as the heterogeneous photocatalyst, the visible light promoted heterogeneous synthesis of unsymmetric diaryl chalcogenides could be achieved under additive‐free and mild conditions. A series of unsymmetric diaryl chalcogenides were generated in good to excellent yields with high functional group tolerance. The Ag/g‐C 3 N 4 photocatalyst is easily recovered from the reaction mixture and reused at least 5 times, opening the way for larger‐scale industrial applications of this type of photocatalytic bond‐forming reactions.
作者机构：
[Chen, Qianwen; Li, Qiulin; Bao, Shu-Juan; Tan, Yangyang; Bao, SJ; 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; Bao, SJ; 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.
摘要：
In this paper, a novel bifunctional molecule dialkyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DAHAOEP) containing both phosphoryl and hydroxamic groups was designed and synthesized, and used as a uranium extractant. The extraction properties of DAHAOEP were focused. Dihexyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DHHAOEP) was shown to have a better extraction effect on uranyl ions than dibutyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DBHAOEP) and diethyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DEHAOEP). Under the optimal extraction conditions, the extraction efficiency of DHHAOEP on uranyl ions could reach up to 98 %. Extraction saturation capacity, reusability and selectivity results indicated that the saturation capacity of DHHAOEP continuous extraction can reach 596 % after 10 times of extraction, DHHAOEP had been recycled more than 5 times, and exhibited a superior selectivity for uranyl ions. Slope method showed that DHHAOEP mainly coordinated with uranyl ions in a 1:2 coordination, i.e., monomolecular bidentate coordination M2L. FTIR and XPS analysis further confirmed that DHHAOEP combined with uranyl ions through it’s -C(=O)-NHOH and P = O groups to form a five-membered ring and P-O-U configuration, respectively.
In this paper, a novel bifunctional molecule dialkyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DAHAOEP) containing both phosphoryl and hydroxamic groups was designed and synthesized, and used as a uranium extractant. The extraction properties of DAHAOEP were focused. Dihexyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DHHAOEP) was shown to have a better extraction effect on uranyl ions than dibutyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DBHAOEP) and diethyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DEHAOEP). Under the optimal extraction conditions, the extraction efficiency of DHHAOEP on uranyl ions could reach up to 98 %. Extraction saturation capacity, reusability and selectivity results indicated that the saturation capacity of DHHAOEP continuous extraction can reach 596 % after 10 times of extraction, DHHAOEP had been recycled more than 5 times, and exhibited a superior selectivity for uranyl ions. Slope method showed that DHHAOEP mainly coordinated with uranyl ions in a 1:2 coordination, i.e., monomolecular bidentate coordination M2L. FTIR and XPS analysis further confirmed that DHHAOEP combined with uranyl ions through it’s -C(=O)-NHOH and P = O groups to form a five-membered ring and P-O-U configuration, respectively.
摘要：
The sensitive detection of the radioactive thorium (Th) ion with an oxidation state of +4 (Th(4+)) is of great significance for environmental protection and life safety. In this study, five fluorescence sensors with regulated donor-acceptor (D-A) interactions were constructed for Th(4+) detection based on intramolecular charge transfer and aggregation-induced emission mechanisms. Among the developed sensors, TPE-D bearing electron-deficient π-bridge and weak D-A interactions presented ratiometric fluorescence detection behavior toward Th(4+) in aqueous solution due to its aggregation-induced emission characteristics and unique D-A-D structures. Moreover, TPE-D showed excellent selectivity and sensitivity for Th(4+) detection, and the detection limit was as low as 8.1 × 10(-8) M. The sensing mechanism observation revealed that Th(4+) could coordinate with the hydroxyl, imine, and carbonyl groups of TPE-D accompanied by an electron transfer process. In addition, TPE-D could selectively be enriched in the lysosome. Both the detection of Th(4+) in the lysosome and liver of mice and zebrafish were realized based on this strategy, and a mobile-assisted detection approach toward Th(4+) in actual water samples was also established with high sensitivity. This is the first report for Th(4+) detection in organelles and organs, which provides a great significance and reliable strategy for radionuclide toxicology detection and analysis applications.
