期刊：
Trends in Biotechnology,2023年41(2):140-143 ISSN：0167-7799
通讯作者：
Ge-Fei Hao<&wdkj&>Guang-Fu Yang
作者机构：
[Mei, Long-Can; Hao, Ge-Fei] Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China;[Hao, Ge-Fei] State Key Laboratory Breeding Base of Green Pesticide and Agricultural Bioengineering, Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, Research and Development Center for Fine Chemicals, Guizhou University, Guiyang 550000, China. Electronic address: gefei_hao@foxmail.com;[Yang, Guang-Fu] Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China. Electronic address: gfyang@mail.ccnu.edu.cn
通讯机构：
[Ge-Fei Hao; Guang-Fu Yang] K;Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China<&wdkj&>State Key Laboratory Breeding Base of Green Pesticide and Agricultural Bioengineering, Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, Research and Development Center for Fine Chemicals, Guizhou University, Guiyang 550000, China<&wdkj&>Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China
作者机构：
[Xu, Weiqing; Zhu, Chengzhou; Wu, Yu; Jiao, Lei; Gu, Wenling; Wang, Hengjia] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Bioensing Technol &, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Jiao, Lei] Qingdao Univ, Inst Mol Metrol, Coll Chem & Chem Engn, Qingdao 266071, Peoples R China.;[Hu, Liuyong] Wuhan Inst Technol, Hubei Engn Technol Res Ctr Optoelect & New Energy, Sch Mat Sci & Engn, Hubei Key Lab Plasma Chem & Adv Mat, Wuhan 430205, Peoples R China.
通讯机构：
[Chengzhou Zhu] K;Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan, Hubei 430079, P. R. China
作者机构：
[Xu, Weiqing; Qin, Ying; Luo, Zhen; Zhu, Chengzhou; Wu, Yu; Wang, Xiaosi; Zhu, CZ; Gu, Wenling; Wang, Hengjia] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Wen, Jing; Hu, Liuyong] Wuhan Inst Technol, Sch Mat Sci & Engn, Hubei Key Lab Plasma Chem & Adv Mat, Wuhan 430205, Peoples R China.
通讯机构：
[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.
摘要：
Exploring advanced co‐reaction accelerators with superior oxygen reduction activity that generate rich reactive oxygen species (ROS) has attracted great attention in boosting luminol‐O2 electrochemiluminescence (ECL). However, tuning accelerators for efficient and selective catalytic O2 activation to switch anodic/cathodic ECL is very challenging. Herein, we report that enzyme‐inspired Fe‐based single‐atom catalysts with axial N/C coordination structures (FeN5, FeN4(C) SACs) can generate specific ROS for cathodic/anodic ECL conversion. Mechanistic studies reveal that FeN5 sites prefer to produce highly active hydroxyl radicals and afford direct cathodic luminescence by promoting the cleavage of O‐O bonds through N‐induced electron redistribution. In contrast, FeN4(C) sites tend to produce superoxide radicals, resulting in inefficient anodic ECL. Benefiting from the enhanced cathodic ECL, FeN5 SAC‐based immunosensor was constructed for the sensitive detection of cancer biomarkers.
作者机构：
[Huang, Yurou; Yang, Guang-Fu; Liu, Sheng Hua; Chen, Weijie; Yin, Jun; Liu, Jia; Ma, Xiaoxie] Minist Educ, Key Lab Pesticide & Chem Biol, Hubei Int Sci & Technol Cooperat Base Pesticide &, Wuhan, Peoples R China.;[Huang, Yurou; Yang, Guang-Fu; Liu, Sheng Hua; Chen, Weijie; Yin, Jun; Liu, Jia; Ma, Xiaoxie] Int Joint Res Ctr Intelligent Biosensing Technol &, Wuhan, Peoples R China.;[Huang, Yurou; Yang, Guang-Fu; Liu, Sheng Hua; Chen, Weijie; Yin, Jun; Liu, Jia; Ma, Xiaoxie] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
通讯机构：
[Prof. Jun Yin; Prof. Guang-Fu Yang] K;Key Laboratory of Pesticide and Chemical Biology (Ministry of Education), Hubei International Scientific and Technological Cooperation Base of Pesticide and Green Synthesis, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan, 430079 P. R. China
摘要：
The cationic nature of heptamethine cyanines gives them the capacity to form aggregates with salts by electrostatic interactions. In this work, NaCl promoted J-aggregate formation of aza-coating heptamethine cyanines is explored. NaCl can induce the N-benzyloxycarbonyl Cy-CO2Bz to assemble into a J-aggregate having an absorption at 890 nm. Its excellent fluorescence response to NaCl implies that it has great potential for use as a probe for tracing salt stress in plants. Moreover, NaCl also promotes formation of J-aggregates from the N-ethyloxycarbonyl Cy-CO2Et. The aggregate shows an intense absorption at 910 nm compared to the monomer which absorbs at 766 nm. Its J-aggregated form can serve as a photothermal agent. And the photothermal conversion efficiency is increased from 29.37 % to 57.59 %. This effort leads to the development of two applications of new cyanine J-aggregates including one for tracing salt stress of plants and the other for promoting photothermal therapy of tumors.
期刊：
Proceedings of the National Academy of Sciences of the United States of America,2023年120(21):e2220315120 ISSN：0027-8424
通讯作者：
Zhu, CZ;Guo, SJ
作者机构：
[Qin, Ying; Tang, Yinjun; Zhu, Chengzhou; Jiao, Lei; Gu, Wenling; Xu, Weiqing; Sha, Meng; Wu, Yu; Su, Rina; Zhu, CZ] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Zhong, Hong; Beckman, Scott P.] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.;[Zheng, Lirong] Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China.;[Hu, Liuyong] Wuhan Inst Technol, Sch Mat Sci & Engn, Wuhan 430205, Peoples R China.;[Guo, SJ; Zhang, Shipeng; Guo, Shaojun] Peking Univ, Sch Mat Sci & Engn, Beijing 100871, Peoples R China.
通讯机构：
[Guo, SJ ] P;[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.;Peking Univ, Sch Mat Sci & Engn, Beijing 100871, Peoples R China.
关键词：
electron transfer;metal–organic frameworks;nanozymes;photoenzymes;single-atom catalysis
摘要：
The unsatisfactory catalytic activity of nanozymes owing to their inefficient elec-tron transfer (ET) is the major challenge in biomimetic catalysis-related biomedical applications. Inspired by the photoelectron transfers in natural photoenzymes, we herein report a photonanozyme of single-atom Ru anchored on metal-organic frame-works (UiO-67-Ru) for achieving photoenhanced peroxidase (POD)-like activity. We demonstrate that the atomically dispersed Ru sites can realize high photoelectric conversion efficiency, superior POD-like activity (7.0-fold photoactivity enhancement relative to that of UiO-67), and good catalytic specificity. Both in situ experiments and theoretical calculations reveal that photoelectrons follow the cofactor-mediated ET process of enzymes to promote the production of active intermediates and the release of products, demonstrating more favorable thermodynamics and kinetics in H2O2 reduction. Taking advantage of the unique interaction of the Zr-O-P bond, we establish a UiO-67-Ru-based immunoassay platform for the photoenhanced detection of organophosphorus pesticides.SignificancePhotoinvolved redox enzymes driven by the photoinduced electron transfer (ET) can realize efficient energy conversion of green and sustainable solar energy to chemical energy. Inspired by this, nanozymes coupling with photoexcited electrons to perform the ET process are expected to serve as alternatives to enzymes and boost the inherent catalytic performance for wide application scenarios. To this end, we rationally design the metal- organic framework-supported Ru single-atom photonanozymes with excellent enzyme-like activity, photoelectronic conversion efficiency, and good catalytic specificity. The resultant photonanozymes follow an enzyme catalytic mechanism and exhibit photoenhanced peroxidase-like activity. This work not only expands the function and application scope of light -driven catalysis but also represents great opportunities for a research direction to design advanced photonanozymes.
期刊：
Water Research,2023年228(Pt A):119328 ISSN：0043-1354
通讯作者：
Hongwei Sun<&wdkj&>Zhihui Ai
作者机构：
[Liang, Chuan; Zhang, Lizhi; Sun, Hongwei; Guo, Furong; Zhang, Xu; Ai, Zhihui; Zhang, Xiang; Cao, Shiyu; Li, Meiqi] Cent China Normal Univ, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[Zhang, Lizhi; Shi, Yanbiao; Ling, Cancan] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China.;[Liu, Xiufan] Hubei Normal Univ, Hubei Key Lab Pollutant Anal & Reuse Technol, Huangshi 435002, Peoples R China.;[He, Hua] Hebei North China Pharmaceut Huaheng Pharmaceut Co, Shijiazhuang 051530, Peoples R China.
通讯机构：
[Hongwei Sun; Zhihui Ai] K;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, Central China Normal University, Wuhan 430079, China
关键词：
Biochar;Organic pollutants degradation;Peroxymonosulfate;Pharmaceutical sludge;Pyrolysis;Reactive species
摘要：
Pyrolysis of pharmaceutical sludge (PS) is a promising way of safe disposal and to recover energy and resources from waste. The resulting PS biochar (PSBC) is often used as adsorbent, but has seldom been explored as catalyst. Herein we demonstrate that PSBC (0.4 g/L) could efficiently activate peroxymonosulfate (PMS) to 100% degrade 4-chlorophenol (4-CP) with rate constants of 0.42-1.70 min(-1), outperforming other reported catalysts. Interestingly, the PMS activation pathway highly depended on PSBC pyrolysis temperature, which produced dominantly high-valent iron species (e.g., (FeO2+)-O-IV) at low temperature but more sulfate radical (SO4 center dot-) and hydroxyl radical (center dot OH) at higher temperature, e.g., 0.17, 0.23, 0.12 mmol/L of (FeO2+)-O-IV and 0.009, 0.038, 0.102 mmol/L of SO4 center dot-/center dot OH were produced within 10 min by PSBC-600/PMS, PSBC-800/PMS, and PSBC-1000/PMS, respectively. Characterization, density functional theory (DFT) simulation and Pearson correlation analysis revealed that along with the increase of pyrolysis temperatures, the active sites of PSBC gradually shifted from atomically dispersed N-coordinated Fe moieties (FeNx) to iron nitrides (FexN), which activated PMS to produce (FeO2+)-O-IV and SO4 center dot-/center dot OH, respectively. This study clarifies the structure-activity relationships of PSBC for PMS activation, and opens a new avenue for the treatment and utilization of PS as high value-added resources.
作者机构：
[Feng, Lizhen; Zhang, Lizhi; Gong, Jingming; Yuan, Yijin; Wu, Mengsi; He, Xianqin] Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensing Technol, Coll Chem,Minist Educ, Inst Environm & Appl Chem,Key Lab Pesticide & Che, Wuhan 430079, Peoples R China.
通讯机构：
[Lizhi Zhang; Jingming Gong] K;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, China
摘要：
Sulfite (S(IV)) is a promising substitute for sulfate radical-based advanced oxidation processes. Here, a composite of in-situ anchoring NiCo2O4 nanosheets on biochar (BC) was firstly employed as a heterogeneous activator for sulfite (NiCo2O4@BC-sulfite) to degrade atrazine (ATZ) in the neutral environment. The synergistic coupling of BC and NiCo2O4 endows the resulting composite excellent catalytic activity. 82% of the degradation ratio of ATZ (1 mg/L) could be achieved within 10 min at initial concentrations of 0.6 g/L NiCo2O4@BC, 3.0 mmol/L sulfite in neutral environment. When further supplementing sulfite into the system at 20 min (considering the depletion of sulfite), outstanding degradation efficiency (similar to 100%) were achieved in the next 10 min without any other energy input by the NiCo2O4@BC-sulfite system. The features of the prepared catalysts and the effects of some key parameters on ATZ degradation were systematically examined. A strong inner-sphere complexation ( Co2+/Ni2+-SO32-) was explored between sulfite and the metal sites on the NiCo2O4@BC surface. The redox cycle of the surface metal efficiently mediated sulfite activation and triggered the series radical chain reactions. The generated radicals, in particular the surface-bound radicals were involved in ATZ degradation. High performance liquid chromatography-tandem mass spectrometry (LC-MS) technique was used to detect the degradation intermediates. Density functional theory (DFT) calculations were performed to illustrate the possible degradation pathways of ATZ. Finally, an underlying mechanism for ATZ removal was proposed. The present study offered a low-cost and sustainable catalyst for sulfite activation to remove ATZ in an environmentally friendly manner from wastewater. (C) 2022 The Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences. Published by Elsevier B.V.
作者机构：
[Jake Song] Department of Materials Science and Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139 USA;Department of Bioengineering and Department of Materials Science and Engineering, Lehigh University, 27 Memorial Dr W, Bethlehem, PA, 18015 USA;[Li Rao] Department of Chemistry, Central China Normal University, Wuhan, 430079 P. R. China;Laboratory for Atomistic and Molecular Mechanics (LAMM), Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139 USA;Center for Computational Science and Engineering, Schwarzman College of Computing, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139 USA
通讯机构：
[Jake Song; Niels Holten-Andersen] D;Department of Materials Science and Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139 USA<&wdkj&>Department of Materials Science and Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139 USA<&wdkj&>Department of Bioengineering and Department of Materials Science and Engineering, Lehigh University, 27 Memorial Dr W, Bethlehem, PA, 18015 USA
关键词：
density functional theory;metal coordination;polymers;rheology
摘要：
Histidine–metal coordination complexes exhibit a metal‐dependent binding stability that remains poorly understood. Computational and experimental techniques show that the observed hierarchy of histidine–metal binding affinity can be attributed to a metal‐specific preference for different coordination numbers, where copper (Cu2+) exhibits high binding affinity at low coordination numbers and nickel (Ni2+) exhibits high binding affinity at high coordination numbers. Abstract Histidine–M2+ coordination bonds are a recognized bond motif in biogenic materials with high hardness and extensibility, which has led to growing interest in their use in soft materials for mechanical function. However, the effect of different metal ions on the stability of the coordination complex remains poorly understood, complicating their implementation in metal‐coordinated polymer materials. Herein, rheology experiments and density functional theory calculations are used to characterize the stability of coordination complexes and establish the binding hierarchy of histamine and imidazole with Ni2+, Cu2+, and Zn2+. It is found that the binding hierarchy is driven by the specific affinity of the metal ions to different coordination states, which can be macroscopically tuned by changing the metal‐to‐ligand stoichiometry of the metal‐coordinated network. These findings facilitate the rational selection of metal ions for optimizing the mechanical properties of metal‐coordinated materials.
摘要：
Pd/SSZ-13 has been proposed as a passive NO(x) adsorber (PNA) for low-temperature NO(x) adsorption. However, it remains challenging for Pd/SSZ-13 to work efficiently when suffering from phosphorus poisoning. Herein, we report a simple and efficient strategy to regenerate the phosphorus-poisoned Pd/SSZ-13 based on the cooperation between hydrothermal aging treatment and Na cocations. It was found that hydrothermal aging treatment enabled the redispersion of Pd and P-containing species in phosphorus-poisoned Pd/SSZ-13. Meanwhile, the presence of Na cocations significantly reduced the formation of AlPO(4) and retained more paired Al sites for highly dispersed Pd(2+) ions, which was of great importance for the recovery of adsorption performance. To our satisfaction, the restoration ratio of the adsorption capacity of poisoned Pd/SSZ-13 was >90% after regeneration. Strikingly, the NO(x) adsorption activities of phosphorus-poisoned Pd/SSZ-13 with phosphorus loadings of 0.2 and 0.4 mmol g(-1) almost completely recovered upon regeneration. This study demonstrates the promoting effect of Na cocations on the regeneration of phosphorus-poisoned Pd/SSZ-13 by hydrothermal aging treatment, which provides useful guidance for the design of PNA materials with excellent durability for cold-start application.
摘要：
One novel cadmium(II)-coordination polymer [Cd(3)L(2)(datrz)(H(2)O)(3)] (CP 1) is controllably synthesized by surmising the astute combination of semi-rigid tricarboxylate acid 4-(2',3'-dicarboxylphenoxy) benzoic acid (H(3)L) and auxiliary ligand 3,5-diamino-1,2,4-triazole (datrz). Structure analysis shows that CP 1 has a two-dimensional (2D) layer structure with a 5-nodal (4(3)) (4(4)·6(2)) (4(5)·6(4)·8) (4(5)·6) (4(7)·6(6)·8(2)) topology. Further investigations reveal that CP 1 shows superordinary water stability and good thermal stability. The fluorescent explorations suggest that the as-synthesized CP 1 could emit blue light centered at 485nm, attributing to ligand-based emission. In terms of sensing investigations, CP 1 could act as a fluorescent sensor for detecting hypochlorite (ClO(-)) and acetylacetone (acac) through fluorescence turn-off process in aqueous solution, and the detection limit could reach 0.18μM and 0.056μM, respectively. Further research reveals that it is more likely the N-H···O-Cl hydrogen bonds between -NH(2) groups of the triazole ligands and O atoms of ClO(-) plays the key role in the system, which may serve as a bridge for the energy transfer, leading to fluorescence quenching of the chemosensor. While the photoinduced electron transfer (PET) combined with inner filter effect (IFT) should be responsible for the turn-off fluorescence of CP 1 triggered by acac.
期刊：
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY,2023年71(5):2610-2615 ISSN：0021-8561
通讯作者：
Zhu, Xiao-Lei(xlzhu@ccnu.edu.cn)
作者机构：
[Li, Hua] Anyang Inst Technol, Henan Joint Int Res Lab Vet Biol Res & Applicat, Anyang 455000, Henan, Peoples R China.;[Li, Hua; Zhu, Xiao-Lei; Dong, Ying; Wang, Yu-Xia; Liu, Zheng] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Int Joint Res Ctr Intelligent Biosensor Technol &, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Xiao-Lei Zhu] K;Key Laboratory of Pesticide and Chemical Biology of the Ministry of Education, International Joint Research Center for Intelligent Biosensor Technology and Health, College of Chemistry, Chemical Biology Center, Central China Normal University, Wuhan, Hubei 430079, P.R. China
关键词：
Ammonia recovery;Cl-modified Cu electrode;Flow-through coupled device;Membrane-free electrolyzer;Nitrate electroreduction
摘要：
Green ammonia production from wastewater via electrochemical nitrate reduction contributes substantially to the realization of carbon neutrality. Nonetheless, the current electrochemical technology is largely limited by the lack of suitable device for efficient and continuous electroreduction nitrate into ammonia and in-situ ammonia recovery. Here, we report a flow-through coupled device composed of a compact electrocatalytic cell for efficient nitrate reduction and a unit to separate the produced ammonia without any pH adjustment and additional energy-input from the circulating nitrate-containing wastewater. Using an efficient and selective Cl-modified Cu foam electrode, nearly 100% NO(3)(-) electroreduction efficiency and over 82.5% NH(3) Faradaic efficiency was realized for a wide range of nitrate-containing wastewater from 50 to 200 mg NO(3)(-)-N L(-1). Moreover, this flow-through coupled device can continuingly operate at a large current of 800 mA over 100 h with a sustained NH(3) yield rate of 420 μg h(-1) cm(-2) for nitrate-containing wastewater treatment (50 mg NO(3)(-)-N L(-1)). When driven by solar energy, the flow-through coupled device can also exhibit exceptional real wastewater treatment performance, delivering great potential for practical application. This work paves a new avenue for clean energy production and environmental sustainability as well as carbon neutrality.
期刊：
Journal of Chemical Information and Modeling,2023年63(15):4850-4863 ISSN：1549-9596
通讯作者：
Wan, Jian;Rao, L;Xu, X
作者机构：
[Rao, Li; Shao, Xubo; Liu, Jiaqi; Wan, Jian; Ren, Yanliang] Cent China Normal Univ, Natl Key Lab Green Pesticide, Hubei Int Sci & Technol Cooperat Base Pesticide &, Key Lab Pesticide & Chem Biol,Minist Educ,Coll Che, Wuhan 43009, Peoples R China.;[Xu, Xin] Fudan Univ, Dept Chem, Shanghai Key Lab Mol Catalysis & Innovat Mat, Minist Educ MOE,Lab Computat Phys Sci, Shanghai 200433, Peoples R China.;[Xu, Xin] Fudan Univ, Dept Chem, Shanghai Key Lab Mol Catalysis & Innovat Mat, Minist Educ MOE,Lab Computat Phys Sci, Shanghai 200433, Peoples R China.;[Wan, J; Rao, L] Cent China Normal Univ, Natl Key Lab Green Pesticide, Hubei Int Sci & Technol Cooperat Base Pesticide &, Key Lab Pesticide & Chem Biol,Minist Educ,Coll Che, Wuhan 43009, Peoples R China.
通讯机构：
[Xu, X ; Wan, J; Rao, L ] ;Cent China Normal Univ, Natl Key Lab Green Pesticide, Hubei Int Sci & Technol Cooperat Base Pesticide &, Key Lab Pesticide & Chem Biol,Minist Educ,Coll Che, Wuhan 43009, Peoples R China.;Fudan Univ, Dept Chem, Shanghai Key Lab Mol Catalysis & Innovat Mat, Minist Educ MOE,Lab Computat Phys Sci, Shanghai 200433, Peoples R China.
摘要：
Accurate prediction of the protein-ligand binding affinity (PLBA) with an affordable cost is one of the ultimate goals in the field of structure-based drug design (SBDD), as well as a great challenge in the computational and theoretical chemistry. Herein, we have systematically addressed the complicated solvation and desolvation effects on the PLBA brought by the difference of the explicit water in the protein cavity before and after ligands bind to the protein-binding site. Based on the new solvation model, a nonfitting method at the first-principles level for the PLBA prediction was developed by taking the bridging and displaced water (BDW) molecules into account simultaneously. The newly developed method, DOX_BDW, was validated against a total of 765 noncovalent and covalent protein-ligand binding pairs, including the CASF2016 core set, Cov_2022 covalent binding testing set, and six testing sets for the hit and lead compound optimization (HLO) simulation. In all of the testing sets, the DOX_BDW method was able to produce PLBA predictions that were strongly correlated with the corresponding experimental data (R = 0.66-0.85). The overall performance of DOX_BDW is better than the current empirical scoring functions that are heavily parameterized. DOX_BDW is particularly outstanding for the covalent binding situation, implying the need for considering an electronic structure in covalent drug design. Furthermore, the method is especially recommended to be used in the HLO scenario of SBDD, where hundreds of similar derivatives need to be screened and refined. The computational cost of DOX_BDW is affordable, and its accuracy is remarkable.
作者机构：
[Huang, Yurou; Yang, Guang-Fu; Yin, Jun; Zeng, Xiaoyan; Liu, Sheng Hua; Li, Anning; Ma, Xiaoxie] 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：
[Yin, J ] C;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：
Cyanines in the near-infrared region are a typical example of a classic fluorescent dye that has garnered significant attention and widespread use in the life sciences and biotechnology. Their character to form assemblies or aggregates has inspired the development of various functional cyanine dye aggregates in phototherapy. This article provides a brief summary of the strategies used to prepare these cyanine dye aggregates. The reports in this concept suggest that the self-assembly of cyanine dyes can enhance their photostability, opening up new possibilities for their application in phototherapy. This concept may encourage researchers to explore the development of functional fluorescent dye aggregates further.
通讯机构：
[Hui Xu] K;Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, China
摘要：
Micro-matrix cartridge extraction coupled on-line to micro-solid phase extraction-high performance liquid chromatography-mass spectrometry (mu-MCE-online-mu-SPE-HPLC-MS) is presented. Micro-matrix cartridge extraction (mu-MCE) was applied to highly efficient desorption of adsorbed pesticides from contaminated soil with favorable extraction efficiency (100%). Novel polystyrene@hydroxypropyl-beta-cyclodextr in (PS@HPCD) electrospun nanofibers with 3D network structure were prepared to selectively capture fipronil and its metabolites. High selectivity was obtained with adsorption efficiency >= 86.64% via complexation, hydrophobic affinity, and pi-pi interactions. PS@HPCD nanofibers exhibited remarkable advantages such as excellent enrichment factors (24-55), superior permeability, and long service life (> 65 times). Under the optimum conditions, wide linear range (0.1-1000 ng g(-1)), low detection limits (0.0032-0.0067 ng g(-1)), high recoveries (84-124.5%), favorable repeatability (RSD <= 10.4%, n = 5), and reproducibility (RSD < 7.2%, n = 3) were acquired for fipronil and three metabolites. The developed method was applied to the pesticide determination in actual soils and the ISO-certified soil with satisfactory recoveries (96.5%). The method developed provides a green, efficient, and miniaturized method for the determination of trace pesticide residues in soil.
期刊：
BRIEFINGS IN BIOINFORMATICS,2022年23(4) ISSN：1467-5463
通讯作者：
Wei Huang<&wdkj&>Ge-Fei Hao<&wdkj&>Guang-Fu Yang
作者机构：
[Wang, Zhi-Zheng] Cent China Normal Univ CCNU, Coll Chem, Wuhan, Peoples R China.;[Hao, Ge-Fei] Guizhou Univ, Key Lab Green Pesticide & Agr Bioengn, Guiyang, Peoples R China.;[Yang, Guang-Fu; Wang, Ming-Shu; Shi, Xing-Xing; Huang, Wei; Wang, Fan] CCNU, Coll Chem, Wuhan, Peoples R China.;[Hao, Ge-Fei] CCNU, Key Lab Pesticide & Chem Biol, Bioinformat, Wuhan, Peoples R China.
通讯机构：
[Wei Huang; Ge-Fei Hao; Guang-Fu Yang] K;Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, International Joint Research Center for Intelligent Biosensor Technology and Health, College of Chemistry, Central China Normal University , Wuhan, 430079 , P. R. China
关键词：
fragment-based drug discovery;drug resistance;web platform;fragment growing;TRK inhibitor
摘要：
Protein kinases play crucial roles in many cellular signaling processes, making them become important targets for drug discovery. But drug resistance mediated by mutation puts a barrier to the therapeutic effect of kinase inhibitors. Fragment-based drug discovery has been successfully applied to overcome such resistance. However, the complicate kinase-inhibitor fragment interaction and fragment-to-lead process seriously limit the efficiency of kinase inhibitor discovery against resistance caused by mutation. Here, we constructed a comprehensive web platform KinaFrag for the fragment-based kinase inhibitor discovery to overcome resistance. The kinase-inhibitor fragment space was investigated from 7783 crystal kinase-inhibitor fragment complexes, and the structural requirements of kinase subpockets were analyzed. The core fragment-based virtual screening workflow towards specific subpockets was developed to generate new kinase inhibitors. A series of tropomyosin receptor kinase (TRK) inhibitors were designed, and the most potent compound YT9 exhibits up to 70-fold activity improvement than marketed drugs larotrectinib and selitrectinib against G595R, G667C and F589L mutations of TRKA. YT9 shows promising antiproliferative against tumor cells in vitro and effectively inhibits tumor growth in vivo for wild type TRK and TRK mutants. Our results illustrate the great potential of KinaFrag in the kinase inhibitor discovery to combat resistance mediated by mutation. KinaFrag is freely available at http://chemyang.ccnu.edu.cn/ccb/database/KinaFrag/.
期刊：
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2022年144(46):21347-21355 ISSN：0002-7863
通讯作者：
Xiaotian Qi<&wdkj&>Hao Xu
作者机构：
[Xu, Hao; Kong, Han-Han; Zhao, Ruinan; Qi, Xiaotian; Xu, Guang; Xiang, Hua-Ming; Yao, Chaochao; Zhu, Cuiju; Zhao, Chunhui] Wuhan Univ, Coll Chem & Mol Sci, Engn Res Ctr Organosilicon Cpds & Mat, Minist Educ, Wuhan 430072, Peoples R China.;[Xu, Hao] Cent China Normal Univ, Coll Chem, CCNU u Ottawa Joint Res Ctr, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Xiaotian Qi] E;[Hao Xu] C;Engineering Research Center of Organosilicon Compounds and Materials, Ministry of Education, College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, P. R. China<&wdkj&>CCNU-uOttawa Joint Research Centre, Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan 430079, P. R. China
摘要：
The first copper-catalyzed enantioselective [4 + 1] annulation of yne-allylic esters with 1,3-dicarbonyl compounds was realized through an elegant remote stereocontrol strategy. The very remote ε regioselective nucleophilic substitution was developed by employing a novel chiral copper-vinylvinylidene species from the new C4 synthon yne-allylic esters. Thus, greatly diverse spirocycles were obtained with ample scope and excellent levels of chemo-, regio-, and enantioselectivities. Moreover, detailed mechanistic studies suggest an yne-allylic substitution and Conia-ene cascade pathway on the remote stereochemical induction progress.
作者机构：
[Guo, Zhen-Zhong; Zhang, Ge] Wuhan Univ Sci & Technol, Hubei Prov Key Lab Occupat Hazard Identificat & Co, Wuhan 430070, Peoples R China.;[Ye, Hua-Rong; Zhang, Ge] Wuhan Univ Sci & Technol, China Resources & Wisco Gen Hosp, Dept Med Ultrasound, Wuhan 430080, Peoples R China.;[Sun, Yao] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
通讯机构：
[Yao Sun] C;[Zhen-Zhong Guo] H;College of Chemistry, Central China Normal University, Wuhan, China, 430079<&wdkj&>Hubei Province Key Laboratory of Occupational Hazard Identification and Control, Wuhan University of Science and Technology, Wuhan, China, 430070
关键词：
cancer diagnosis, cancer therapy;contrast agents;gas vesicle;microbubble;molecular imaging;nanobubble;nanodroplet;ultrasound imaging
摘要：
Ultrasound imaging is regarded as a highly sensitive imaging modality used in routine clinical examinations. Over the last several decades, ultrasound contrast agents have been widely applied in ultrasound molecular cancer imaging to improve the detection, characterization, and quantification of tumors. To date, a few new potential preclinical and clinical applications regarding ultrasound molecular cancer imaging are being investigated. This review presents an overview of the various kinds of ultrasound contrast agents employed in ultrasound molecular imaging and advanced imaging techniques using these contrast agents. Additionally, we discuss the recent enormous development of ultrasound contrast agents in the relevant preclinical and clinical applications, highlight the recent challenges which need to be overcome to accelerate the clinical translation, and discuss the future perspective of ultrasound molecular cancer imaging using various contrast agents. As a highly promising and valuable tumor-specific imaging technique, it is believed that ultrasound molecular imaging will pave an accurate and efficient way for cancer diagnosis.
作者机构：
[Xu, Weiqing; Zhu, Chengzhou; Wu, Yu; Jiao, Lei; Gu, Wenling] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Du, Dan; Lin, Yuehe] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.;[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.
通讯机构：
[Yuehe Lin] S;[Chengzhou Zhu] K;School of Mechanical and Materials Engineering, Washington State University, Pullman, WA 99164, USA<&wdkj&>Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China
通讯机构：
[Zhihui Ai] K;Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan 430079, PR China
关键词：
Chloronitrobenzenes;Environmental remediation;H(2)O(2);Reduction-oxidation coupling;Zero-valent iron
摘要：
Chloronitrobenzenes (CNBs) are typical refractory aromatic pollutants. The reduction products of CNBs often possess higher toxicity, and the electron-withdrawing substituent groups are detrimental to the ring-opening during the oxidation treatment, leading to ineffective removal of CNBs by either reduction or oxidation technology. Herein we demonstrate a controllable reduction-oxidation coupling (ROC) process composed of zero-valent iron (ZVI) and H(2)O(2) for the effective removal of CNBs from both water and soil. In water, ZVI first reduced p-CNB into 4-chloronitrosobenzene and 4-chloroaniline intermediates, which were then suffered from the subsequent oxidative ring-opening by ·OH generated from the reaction between Fe(II) and H(2)O(2). By controlling the addition time of H(2)O(2), the final mineralization rate of p-CNB reached 6.6×10(-1) h(-1), about 74 times that of oxidation alone (9.0×10(-3) h(-1)). More importantly, this controllable ROC process was also applicable for the site remediation of CNBs contaminated soil by either ex-situ treatment or in-situ injection, and, respectively decreased the concentrations of p-CNB, m-CNB, and o-CNB from 1105, 980, and 94mg/kg to 3, 1, and < 1mg/kg, meeting the remediation goals (p-CNB: < 32.35mg/kg, o-CNB and m-CNB: < 1.98mg/kg). These laboratory and field trial results reveal that this controllable ROC strategy is very promising for the treatment of electron-withdrawing groups substituted aromatic contaminates.
