作者机构：
[Liu, Ying; Yang, Shu; Hou, Shenghuai; Bai, Yuxuan; Qiao, Zhaoyu; Zhen, Shuang] Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, 430079, China;[Xu, Hui] Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, 430079, China. Electronic address: huixu@ccnu.edu.cn
通讯机构：
[Xu, Hui] K;Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, 430079, China. Electronic address:
关键词：
Fipronil and its metabolites;Soil;Spherical fluorinated covalent organic polymers;μ-Matrix cartridge extraction-online-μ-solid phase extraction
摘要：
Covalent organic polymers (COPs) have garnered considerable attention as promising adsorbents of online solid phase extraction (online SPE). Morphology modulation provides an appealing solution to enhance adsorption efficiency and reduce back-pressure in the absorbent. However, the synthesis of COPs with regular geometric shapes and specific adsorption selectivity remains challenging. In this study, a uniform spherical fluorinated COP (F-sCOP, average diameter: 2.14μm) was successfully synthesized by Schiff base reaction of 1,3,5-triformylphoroglucinol (TP) and 2,2(')-bis(trifluoromethyl)benzidine (TFMB). The F-sCOP had a large surface area (BET: 346.2m(2)g(-1)), remarkable enrichment capacity (enrichment factors: 186-782), high selectivity toward fipronil and its metabolites (adsorption efficiency >93.1%), and admirable service life (>60 times). Based on the adsorbent, a novel μ-matrix cartridge extraction-online-μ-solid phase extraction-high performance liquid chromatography-mass spectrometry (μ-MCE-online-μ-SPE-HPLC-MS) method was constructed and used to track trace fipronil and its metabolites in soil. The proposed method exhibited a wide linear range (0.05-1000ngg(-1)), low quantitation limits (LOQs: 0.0027-0.011ngg(-1)), high recoveries (90.1-119.6%) and good repeatability (RSD ≤10.5%, n=3) for fipronil analysis. This study paves the way for pesticide analysis in soil risk assessment.
关键词：
Photocatalysis;H2O2;g-C3N4;Excitons dissociation;Reactive oxygen species
摘要：
Solar-driven hydrogen peroxide (H2O2) production offers a sustainable strategy to address the ever-growing demand of eco-friendly oxidant and clean fuel, while its efficiency highly relies on the generation of desired reactive oxygen species (ROSs). Herein, we demonstrate that introducing boron-nitrogen vacancy (B-N-V) associates in g-C3N4 enables to weaken the robust excitonic effect and promote bound excitons spontaneously dissociating into free charge carriers under ambient conditions. Specifically, the doped B atoms introduced a donor state below the conduction band of g-C3N4, which disturbs charge distribution around heptazine rings and further destabilizes excitons. The concomitant N-V, serving as an accepter state locating above the valence band, cooperates with the doped B atoms to form B-N-V associates that simultaneously downshifts the conduction band and valence band of g-C3N4. Distinct from the counterpart preferring to activate O-2 into O-1(2) via an energy-transfer-involved pathway, g-C3N4 featuring with B-N-V associates displayed a superior photoactivity of visible-light-driven two-electron oxygen reduction reaction for H2O2 production with a yield of 182 mu mol h(-1) and selectivity of 100%. The produced H2O2 could effectively degrade organic contaminants and kill typical bacteria. This study highlights the importance of ROSs generation in two-dimensional photocatalysts for sustainable solar-to-chemical conversion and on site environmential governance.
期刊：
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY,2024年72(13):7021-7032 ISSN：0021-8561
通讯作者：
Feng, LL
作者机构：
[Zuo, Lingzi; Fan, Yuxuan; Feng, LL; Feng, Lingling; He, Yanlin; Cheng, Cai; Zhang, Liexiong; Guo, Xiaoliang; Cheng, Guonian; Yu, Jie; Tang, Guangmei; Huang, Shi; Chen, Ruiqing] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & chem Biol CCNU, Minist Educ, Wuhan 430079, Peoples R China.;[Liu, Yanyang; Feng, LL; Feng, Lingling] Wuhan Inst Photochem & Technol, Wuhan 430083, Hubei, Peoples R China.;[Feng, LL; Feng, Lingling] Cent China Normal Univ, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构：
[Feng, LL ] C;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & chem Biol CCNU, Minist Educ, Wuhan 430079, Peoples R China.;Wuhan Inst Photochem & Technol, Wuhan 430083, Hubei, Peoples R China.;Cent China Normal Univ, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
关键词：
Active substructure splicing;DFT;Harmful cyanobacteria blooms;SAR;algicide;thioacetamide derivatives
摘要：
Lakes and reservoirs worldwide are experiencing a growing problem with harmful cyanobacterial blooms (HCBs), which have significant implications for ecosystem health and water quality. Algaecide is an effective way to control HCBs effectively. In this study, we applied an active substructure splicing strategy for rapid discovery of algicides. Through this strategy, we first optimized the structure of the lead compound S5, designed and synthesized three series of thioacetamide derivatives (series A, B, C), and then evaluated their algicidal activities. Finally, compound A3 with excellent performance was found, which accelerated the process of discovering and developing new algicides. The biological activity assay data showed that A3 had a significant inhibitory effect on M. aeruginosa. FACHB905 (EC(50) = 0.46 μM) and Synechocystis sp. PCC6803 (EC(50) = 0.95 μM), which was better than the commercial algicide prometryn (M. aeruginosa. FACHB905, EC(50) = 6.52 μM; Synechocystis sp. PCC6803, EC(50) = 4.64 μM) as well as better than lead compound S5 (M. aeruginosa. FACHB905, EC(50) = 8.80 μM; Synechocystis sp. PCC6803, EC(50) = 7.70 μM). The relationship between the surface electrostatic potential, chemical reactivity, and global electrophilicity of the compounds and their activities was discussed by density functional theory (DFT). Physiological and biochemical studies have shown that A3 might affect the photosynthesis pathway and antioxidant system in cyanobacteria, resulting in the morphological changes of cyanobacterial cells. Our work demonstrated that A3 might be a promising candidate for the development of novel algicides and provided a new active skeleton for the development of subsequent chemical algicides.
关键词：
ammonia recovery;atomic hydrogen;electrocatalytic nitrate reduction;fluorine modification;neutral media
摘要：
Electrocatalytic nitrate reduction to ammonia (NITRR) offers an attractive solution for alleviating environmental concerns, yet in neutral media, it is challenging as a result of the reliance on the atomic hydrogen (H*) supply by breaking the stubborn HO-H bond (similar to 492 kJ/mol) of H2O. Herein, we demonstrate that fluorine modification on a Cu electrode (F-NFs/CF) favors the formation of an O-H center dot center dot center dot F hydrogen bond at the Cu-H2O interface, remarkably stretching the O-H bond of H2O from 0.98 to 1.01 & Aring; and lowering the energy barrier of water dissociation into H* from 0.64 to 0.35 eV at neutral pH. As a benefit from these advantages, F-NFs/CF could rapidly reduce NO3- to NH3 with a rate constant of 0.055 min(-1) and a NH3 selectivity of similar to 100%, far higher than those (0.004 min(-1) and 9.2%) of the Cu counterpart. More importantly, we constructed a flow-through coupled device consisting of a NITRR electrolyzer and a NH3 recovery unit, realizing 98.1% of total nitrogen removal with 99.3% of NH3 recovery and reducing the denitrification cost to $5.1/kg of N. This study offers an effective strategy to manipulate the generation of H* from water dissociation for efficient NO3--to-NH3 conversion and sheds light on the importance of surface modification on a Cu electrode toward electrochemical reactions.
摘要：
Spinel cobalt oxide (Co3O4), consisting of tetrahedral Co2+ (CoTd) and octahedral Co3+ (CoOh), is considered as promising earth-abundant electrocatalyst for chlorine evolution reaction (CER). Identifying the catalytic contribution of geometric Co site in the electrocatalytic CER plays a pivotal role to precisely modulate electronic configuration of active Co sites to boost CER. Herein, combining density functional theory calculations and experiment results assisted with operando analysis, we found that the CoOh site acts as the main active site for CER in spinel Co3O4, which shows better Cl- adsorption and more moderate intermediate adsorption toward CER than CoTd site, and does not undergo redox transition under CER condition at applied potentials. Guided by above findings, the oxygen vacancies were further introduced into the Co3O4 to precisely manipulate the electronic configuration of CoOh to boost Cl- adsorption and optimize the reaction path of CER and thus to enhance the intrinsic CER activity significantly. Our work figures out the importance of geometric configuration dependent CER activity, shedding light on the rational design of advanced electrocatalysts from geometric configuration optimization at the atomic level. (c) 2023 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press
期刊：
CHEMICAL SOCIETY REVIEWS,2024年53(1):137-162 ISSN：0306-0012
通讯作者：
Zhu, CZ;Lin, YH
作者机构：
[Xu, Weiqing; Zhu, Chengzhou; Wu, Yu; Zhu, CZ; Gu, Wenling] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Lin, YH; Du, Dan; Lin, Yuehe] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.
通讯机构：
[Lin, YH ] W;[Zhu, CZ ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.
摘要：
Natural metalloenzymes with astonishing reaction activity and specificity underpin essential life transformations. Nevertheless, enzymes only operate under mild conditions to keep sophisticated structures active, limiting their potential applications. Artificial metalloenzymes that recapitulate the catalytic activity of enzymes can not only circumvent the enzymatic fragility but also bring versatile functions into practice. Among them, metal-organic frameworks (MOFs) featuring diverse and site-isolated metal sites and supramolecular structures have emerged as promising candidates for metalloenzymes to move toward unparalleled properties and behaviour of enzymes. In this review, we systematically summarize the significant advances in MOF-based metalloenzyme mimics with a special emphasis on active pocket engineering at the atomic level, including primary catalytic sites and secondary coordination spheres. Then, the deep understanding of catalytic mechanisms and their advanced applications are discussed. Finally, a perspective on this emerging frontier research is provided to advance bioinspired catalysis. This review systematically summarizes the significant advances in MOF-based metalloenzyme mimics for bioinspired catalysis with a special emphasis on active pocket engineering at the atomic level.
摘要：
The contamination of drinking water by microbes is a critical health concern, underscoring the need for safe, reliable, and efficient methods to treat pathogenic microorganisms. While most sterilization materials are available in powder form, this presents safety risks and challenges in recycling. Herein, this study reports the preparation of an innovative copper oxide supported silver monolithic nanoarray mesh with abundant oxygen vacancies (Ag/CuO-V(O)) by laser ablation. The instantaneous high temperature caused by laser ablation preserves the material's original structure while generating oxygen vacancies on the CuO surface. The Ag/CuO-V(O) mesh demonstrated a remarkable ability to inactivate over 99% of Escherichia coli (E. Coli) within 20min. The oxygen vacancies in the Ag/CuO-V(O) enhance interactions between oxygen species and the Ag/CuO-V(O), leading to the accumulation of large amounts of reactive oxygen species (ROS). The generated ROS effectively disrupt both layers of the bacterial cell wall - the peptidoglycan and the phospholipid - as confirmed by Fourier Transform Infrared (FTIR) spectroscopy, culminating in cell death. This research presents a monolithic material capable of inactivating pathogenic microorganisms efficiently, offering a significant advancement in water sterilization technology.
作者机构：
[Guan-Zhu Wang; Xue Wu] National Key Laboratory of Green Pesticide, Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, Center for Research and Development of Fine Chemicals Guizhou University, Guiyang, 550025, China;National Key Laboratory of Green Pesticide, College of Chemistry, Central China Normal University, Wuhan, 430079, China;[Ge-Fei Hao] National Key Laboratory of Green Pesticide, Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, Center for Research and Development of Fine Chemicals Guizhou University, Guiyang, 550025, China<&wdkj&>National Key Laboratory of Green Pesticide, College of Chemistry, Central China Normal University, Wuhan, 430079, China
通讯机构：
[Ge-Fei Hao] N;National Key Laboratory of Green Pesticide, Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, Center for Research and Development of Fine Chemicals Guizhou University, Guiyang, 550025, China<&wdkj&>National Key Laboratory of Green Pesticide, College of Chemistry, Central China Normal University, Wuhan, 430079, China
摘要：
Auxin is an important phytohormone that regulates a string of vital rapid responses, and its signaling perception mechanism has been one of the hot spots of research. It has been shown that the ABP1/TMKs module is involved in regulating extracellular auxin signaling, however, the role of ABP1 as an auxin receptor is highly controversial. Therefore, the mechanism of quintessential TMKs sense extracellular auxin remains unresolved. Recently, a study identified two new auxin-binding proteins, ABL1 and ABL2, which directly interact with TMKs to perceive apoplast auxin. This groundbreaking research unravels the mystery surrounding how plants perceive extracellular auxin signals.
期刊：
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024年146(2):1410-1422 ISSN：0002-7863
通讯作者：
Xiao, Wen-Jing;Chen, JR
作者机构：
[Zhao, Ke; Qu, Wen-Yuan; Xiao, Wen-Jing; Chen, Jia-Rong; Mao, Zhi-Cheng; Zhang, Bin; Xiao, WJ; Li, Tian-Tian; Zhang, Zhihan; Chen, JR] Cent China Normal Univ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.;[Jiang, Min] Hangzhou Normal Univ, Coll Mat Chem & Chem Engn, Hangzhou 310036, Peoples R China.;[Xiao, Wen-Jing; Chen, Jia-Rong; Xiao, WJ; Chen, JR] Wuhan Inst Photochem & Technol, Wuhan 430082, Hubei, Peoples R China.
通讯机构：
[Xiao, WJ; Chen, JR ] C;Cent China Normal Univ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.;Wuhan Inst Photochem & Technol, Wuhan 430082, Hubei, Peoples R China.
摘要：
Alkene radical ions constitute an integral and unique class of reactive intermediates for the synthesis of valuable compounds because they have both unpaired spins and charge. However, relatively few synthetic applications of alkene radical anions have emerged due to a dearth of generally applicable and mild radical anion generation approaches. Precise control over the chemo- and stereoselectivity in alkene radical anion-mediated processes represents another long-standing challenge due to their high reactivity. To overcome these issues, here, we develop a new redox-neutral strategy that seamlessly merges photoredox and copper catalysis to enable the controlled generation of alkene radical anions and their orthogonal enantioselective cyanofunctionalization via distonic-like species. This new strategy enables highly regio-, chemo-, and enantioselective hydrocyanation, deuterocyanation, and cyanocarboxylation of alkenes without stoichiometric reductants or oxidants under visible light irradiation. This protocol provides a new blueprint for the exploration of the transformation potential of alkene radical anions.
摘要：
Highly efficient three‐component coupling of organic halides, sodium cyanate and amines or alcohols was achieved with a nickel/photoredox dual catalysis system. Significant N‐containing functional compounds, ureas and carbamates, were produced under green and sustainable conditions. Comprehensive Summary Ureas are widely used in drugs, materials and catalysts because of their diamide structure, which can form strong hydrogen bonds. Therefore, it is of great scientific significance to develop efficient and green methods for the synthesis of urea compounds, especially unsymmetrical ureas. Here, we have disclosed novel and highly efficient three‐component coupling reactions of organic halides, sodium cyanate and amines enabled by nickel/photoredox dual catalysis for the preparation of unsymmetrical ureas. The reaction features simple and safe operations, broad substrate scopes, and product diversities. It allows the facile synthesis of N‐aryl/vinyl ureas from readily available, user‐friendly feedstocks under mild conditions (27 examples, 36%—98% yields). In addition, this method is further derived to alcohols as nucleophiles to synthesize a series of carbamates (15 examples, 40%—95% yields). The mechanism experiment shows that the isocyanate produced by the coupling of halide and sodium cyanate may be the key intermediate in this reaction.
摘要：
Nanozymes with peroxidase (POD)-like activity have garnered significant attention due to their exceptional performance in colorimetric assays. However, nanozymes often possess oxidase (OD) and POD-like activity simultaneously, which affects the accuracy and sensitivity of the detection results. To address this issue, inspired by the catalytic pocket of natural POD, a single-atom nanozyme with FeN(5) configuration is designed, exhibiting enhanced POD-like activity in comparison with a single-atom nanozyme with FeN(4) configuration. The axial N atom in FeN(5) highly mimics the amino acid residues in natural POD to optimize the electronic structure of the metal active center Fe, realizing the efficient activation of H(2)O(2). In addition, in the presence of both H(2)O(2) and O(2), FeN(5) enhances the activation of H(2)O(2), effectively avoiding the interference of dissolved oxygen in colorimetric sensing. As a proof-of-concept application, a colorimetric detection platform for uranyl ions (UO(2)(2+)) in seawater is successfully constructed, demonstrating satisfactory sensitivity and specificity.
作者机构：
[Zhu, Chengzhou; Gu, Wenling; Li, Jingshuai; Xi, Mengzhen] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Hu, Liuyong] Wuhan Inst Technol, Hubei Engn Technol Res Ctr Optoelect & New Energy, Hubei Key Lab Plasma Chem & Adv Mat, Wuhan 430205, Peoples R China.;[Sun, Hongcheng] Hangzhou Normal Univ, Coll Mat Chem & Chem Engn, Key Lab Organosilicon Chem & Mat Technol, Minist Educ, Hangzhou 311121, Peoples R China.;[Gu, Wenling] Key Lab Opt Elect Sensing & Analyt Chem Life Sci, MOE, Qingdao 266042, Peoples R China.
通讯机构：
[Gu, WL ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;Key Lab Opt Elect Sensing & Analyt Chem Life Sci, MOE, Qingdao 266042, Peoples R China.
摘要：
Improving the sensitivity in electrochemiluminescence (ECL) detection systems necessitates the integration of robust ECL luminophores and efficient signal transduction. In this study, we report a novel ECL nanoprobe (Zr-MOF) that exhibits strong and stable emission by incorporating aggregation-induced emission ligands into Zr-based metal-organic frameworks (MOFs). Meanwhile, we designed a high-performance signal modulator through the implementation of a well-designed controlled release system with a self-on/off function. ZnS quantum dots (QDs) encapsulated within the cavities of aminated mesoporous silica nanoparticles (NH(2)-SiO(2)) serve as the ECL quenchers, while adenosine triphosphate (ATP) aptamers adsorbed on the surface of NH(2)-SiO(2) through electrostatic interaction act as "gatekeepers." Based on the target-triggered ECL resonance energy transfer between Zr-MOF and ZnS QDs, we establish a coreactant-free ECL aptasensor for the sensitive detection of ATP, achieving an impressive low detection limit of 0.033 nM. This study not only demonstrates the successful combination of ECL with controlled release strategies but also opens new avenues for developing highly efficient MOFs-based ECL systems.
通讯机构：
[Zhang, CH ] S;[Wang, HL; Liu, CR ] C;Shanxi Univ, Sch Chem & Chem Engn, Taiyuan 030006, Peoples R China.;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
摘要：
Abnormal lipid droplets (LDs) are known to be intimately bound with the occurrence and development of cancer, allowing LDs to be critical biomarkers for cancers. Aggregation-induced emission luminogens (AIEgens), with efficient reactive oxygen species (ROS) production performance, are prime photosensitizers (PSs) for photodynamic therapy (PDT) with imaging. Therefore, the development of dual-functional fluorescent probes with aggregation-induced emission (AIE) characteristics that enable both simultaneous LD monitoring and imaging-guided PDT is essential for concurrent cancer diagnosis and treatment. Herein, we reported the development of a novel LD-targeting fluorescent probe (TDTI) with AIE performance, which was expected to realize the integration of cancer diagnosis through LD visualization and cancer treatment via PDT. We demonstrated that TDTI, with typical AIE characteristics and excellent photostability, could target LDs with high specificity, which enables the dynamic tracking of LDs in living cells, specific imaging of LDs in zebrafish, and the differentiation of cancer cells from normal cells for cancer diagnosis. Meanwhile, TDTI exhibited fast ROS generation ability (achieving equilibrium within 60 s) under white light irradiation (10 mW/cm(2)). The cell apoptosis assay revealed that TDTI effectively induced growth inhibition and apoptosis of HeLa cells. Further, the results of PDT in vivo indicated that TDTI had a good antitumor effect on the tumor-bearing mice model. Collectively, these results highlight the potential utility of the dual-functional fluorescent probe TDTI in the integrated diagnosis and treatment of cancer.
摘要：
Picolinamide fungicides, structurally related to UK-2A and antimycin-A, bind into the Qi-site in the bc(1) complex. However, the detailed binding mode of picolinamide fungicides remains unknown. In the present study, antimycin-A and UK-2A were selected to study the binding mode of picolinamide inhibitors with four protonation states in the Qi-site by integrating molecular dynamics simulation, molecular docking, and molecular mechanics Generalized Born surface area (MM/GBSA) calculations. Subsequently, a series of new picolinamide derivatives were designed and synthesized to further understand the effects of substituents on the tail phenyl ring. The computational results indicated that the substituted aromatic rings in antimycin-A and UK-2A were the pharmacophore fragments and made the primary contribution when bound to a protein. Compound 9g-hydrolysis formed H-bonds with Hie201 and Ash228 and showed an IC(50) value of 6.05 ± 0.24 μM against the porcine bc(1) complex. Compound 9c, with a simpler chemical structure, showed higher control effects than florylpicoxamid against cucumber downy mildew and expanded the fungicidal spectrum of picolinamide fungicides. The structural and mechanistic insights obtained from the present study will provide a valuable clue for the future designing of new promising Qi-site inhibitors.
通讯机构：
[Li, DF ] C;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
摘要：
The research on electron transfer coupled spin transition regulating the valence state and spin state transition of metal ions is promising and challenging. Herein, we report a cyano-bridged {(Fe2Fe2II)-Fe-III} molecular square complex, {[Fe(Tp)(CN)(3)](2) [Fe(bnbpen)](2)}(ClO4)(2)<middle dot>8CH(3)OH (1<middle dot>8CH(3)OH, bnbpen = N,N '-bis-(2-naphthylmethyl)-N,N '-bis(2-picolayl)-ethylenediamine), and its free of solvents form (1). Combined single-crystal X-ray diffraction, temperature-dependent infrared (IR) spectra, magnetic measurements, and M & ouml;ssbauer spectra reveal that 1<middle dot>8CH(3)OH and 1 exhibit reversible one-step and two-step electron transfer coupled spin transition (ETCST) with temperature change, between the low-temperature state {Fe-II,Fe-LS(mu-CN)Fe-III,Fe-LS}(2) (LS = low spin, HS = high spin) and the high-temperature state {Fe-III,Fe-LS(mu-CN)Fe-II,Fe-HS}(2), respectively.
期刊：
Sensors and Actuators B-Chemical,2024年406:135432 ISSN：0925-4005
通讯作者：
Feng, GQ
作者机构：
[Zheng, Zhoupeng; Feng, Guoqiang; Feng, GQ; Zhang, Jinzheng; Liu, Yijia; Gong, Shenyi] Cent China Normal Univ, Coll Chem, 152 Luoyu Rd, Wuhan 430079, Peoples R China.
通讯机构：
[Feng, GQ ] C;Cent China Normal Univ, Coll Chem, 152 Luoyu Rd, Wuhan 430079, Peoples R China.
关键词：
Dual -channel fluorescent probe;Viscosity;Peroxynitrite;Mitochondria;Diabetes;In vivo imaging
摘要：
Diabetes is a common metabolic disease worldwide, which often has serious complications and seriously threatens human health. Abnormal viscosity and peroxynitrite (ONOO-) concentration are closely related to diabetes. Herein, we report a fluorescent dual response probe AO, which can simultaneously detect the changes of viscosity and ONOO- in diabetes at dual fluorescence channels. AO sensitively responds to viscosity and ONOO- with significant emission signal changes at 710 nm and 645 nm, respectively. Moreover, AO selectively targets mitochondria and generates a new compound when detecting ONOO-, which can spontaneously target and light up another type of organelle (lipid droplets), thus showing spatially separated dual -channel fluorescence signals. More notably, AO was successfully used to simultaneously detect the viscosity and ONOO- variations in hyperglycemic cells, diabetes and its complications (using mice models) for the first time, which may lead to a better understanding of the physiological and pathological phenomena of diabetes.
期刊：
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024年 ISSN：0002-7863
作者机构：
[Zhou, Yan; Luo, Zhen; Zhu, Chengzhou; Wu, Yu; Li, Jingshuai; Xi, Mengzhen; Gu, Wenling; Ling, Ling] State Key Laboratory of Green Pesticide, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China;[Hu, Liuyong] Hubei Key Laboratory of Plasma Chemistry and Advanced Materials, Hubei Engineering Technology Research Center of Optoelectronic and New Energy Materials, Wuhan Institute of Technology, Wuhan 430205, P. R. China;[Wang, Canglong] Institute of Modern Physics, University of Chinese Academy of Sciences, Lanzhou 730000, P. R. China
摘要：
The development of potential-resolved electrochemiluminescence (ECL) systems with dual emitting signals holds great promise for accurate and reliable determination in complex samples. However, the practical application of such systems is hindered by the inevitable mutual interaction and mismatch between different luminophores or coreactants. In this work, for the first time, by precisely tuning the oxygen reduction performance of M-N-C single-atom catalysts (SACs), we present a dual potential-resolved luminol ECL system employing endogenous dissolved O(2) as a coreactant. Using advanced in situ monitoring and theoretical calculations, we elucidate the intricate mechanism involving the selective and efficient activation of dissolved O(2) through central metal species modulation. This modulation leads to the controlled generation of hydroxyl radical (·OH) and superoxide radical (O(2)(·-)), which subsequently trigger cathodic and anodic luminol ECL emission, respectively. The well-designed Cu-N-C SACs, with their moderate oxophilicity, enable the simultaneous generation of ·OH and O(2)(·-), thereby facilitating dual potential-resolved ECL. As a proof of concept, we employed the principal component analysis statistical method to differentiate antibiotics based on the output of the dual-potential ECL signals. This work establishes a new avenue for constructing a potential-resolved ECL platform based on a single luminophore and coreactant through precise regulation of active intermediates.
期刊：
JOURNAL OF ORGANIC CHEMISTRY,2024年89(6):3941-3953 ISSN：0022-3263
通讯作者：
Wang, JG;Wu, AX
作者机构：
[Wang, Jun-Gang; Ma, Lin-Lin] Guizhou Minzu Univ, Sch Chem Engn, Guiyang 550025, Guizhou, Peoples R China.;[Wang, Zheng-Hao; Tang, Yong-Xing; Wu, An-Xin; Zhou, You; Chen, Ting; Wu, Yan-Dong] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构：
[Wu, AX ] C;[Wang, JG ] G;Guizhou Minzu Univ, Sch Chem Engn, Guiyang 550025, Guizhou, Peoples R China.;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
摘要：
An efficient synthetic method for constructing 2,3- and 2,4-disubstituted pyrimidio[1,2-b]indazole skeletons through I(2)-DMSO-mediated and substrate-controlled regioselective [4 + 2] cyclization is reported. The reaction conditions are mild, its operation is simple, and the substrate scope is wide. More than 60 pyrimidio[1,2-b]indazole derivatives have been synthesized, providing a new methodology for constructing related molecules and potentially enriching bioactive-molecule libraries.
作者机构：
[Lin, Jinying] Jilin Univ, Sch Stomatol, Dept Oral Implantol, Jilin Prov Key Lab Tooth Dev & Bone Remodeling, Changchun 130021, Peoples R China.;[Ding, Qihang] Korea Univ, Dept Chem, Seoul 02841, South Korea.;[Sun, Yao] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构：
[Sun, Y ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
期刊：
Sensors and Actuators B-Chemical,2024年405 ISSN：0925-4005
通讯作者：
Xu, Miao;Gu, WL;Ye, HR
作者机构：
[Xu, Weiqing; Chen, Yifeng; Zhu, Chengzhou; Xu, Miao; Sha, Meng; Zou, Chufan; Gu, Wenling; Chen, Guo] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Ye, Huarong; Ye, HR] China Resources & Wisco Gen Hosp, Wuhan 430080, Peoples R China.;[Zhu, Chengzhou] Hangzhou Normal Univ, Coll Mat Chem & Chem Engn, Key Lab Organosilicon Chem & Mat Technol, Minist Educ, Hangzhou 311121, Peoples R China.;[Gu, Wenling] Hubei Univ, Sch Life Sci, State Key Lab Biocatalysis & Enzyme Engn, Wuhan 430062, Peoples R China.
通讯机构：
[Xu, M; Gu, WL ; Ye, HR ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;China Resources & Wisco Gen Hosp, Wuhan 430080, Peoples R China.;Hubei Univ, Sch Life Sci, State Key Lab Biocatalysis & Enzyme Engn, Wuhan 430062, Peoples R China.
摘要：
The fragility inherent in enzymes can be overcome by immobilizing them within nano-carriers, which offer designability and controllability and serve as a promising strategy for overcoming the inherent fragility of enzymes. While enzyme immobilization enhances enzyme stability and reusability, it can potentially hinder their bioactivity and catalytic efficiency. In this study, we present an enzyme-directed biomimetic mineralization approach for the in situ encapsulation of horseradish peroxidase (HRP) within hydrogen-bonded organic frameworks (HOFs) to obtain HOF@HRP nanocomposites. Remarkably, the HOF@HRP nanocomposites exhibit an ultrahigh protein content and demonstrate comparable catalytic activity to that of the free enzyme. Moreover, the HOFs act as protective shields, safeguarding the internal enzymes against various environmental disturbances. Leveraging the unique properties of HOF@HRP, we propose a dual-modal enzyme-linked immunosorbent assay for the sensitive detection of prostate-specific antigen in human serum. The resultant biosensor exhibits a good linear range, excellent sensitivity, and selectivity, showcasing its promising potential and clinical application in the field of diagnostic medicine.
