期刊：
Pesticide Biochemistry and Physiology,2024年199:105769 ISSN：0048-3575
通讯作者：
Sun, Y;Zhang, AD
作者机构：
[Zhou, Yaqing; Wang, Jili; Sun, Yong; Sun, Y; Zhou, Xin; Wu, Wenhai] Hanjiang Normal Univ, Coll Chem & Environm Engn, Shiyan 442000, Peoples R China.;[Zhang, Aidong; Han, Mengying] Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构：
[Zhang, AD ] C;[Sun, Y ] H;Hanjiang Normal Univ, Coll Chem & Environm Engn, Shiyan 442000, Peoples R China.;Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
摘要：
The discovery of safe, effective, and selective chemical algicides is the stringent need for the algicides development, and it is also one of the effective routes to control cyanobacteria harmful algal blooms and to meet the higher requirements of environmental and ecological. In this work, a series of novel bromo-N-phenyl-5-ohydroxyphenylpyrazole-3-carboxyamides were rationally designed as pseudilin analogs by bioisosteric replacement and molecular hybridization strategies, in which the pyrrole unit of pseudilin was replaced with pyrazole and further combined with the dominant structural fragments of algicide diuron. The synthesis was carried out by a facile four-step routeincluding cyclization, amidation, transanulation, and halogenation. The biological activity evaluation on AtIspD, EcIspD, Synechocystis sp. PCC6803 and Microcystis aeruginosa FACHB905 revealed that most compounds had good EcIspD and excellent cyanobacteria inhibitory activity. In particular, compound 6bb exhibited potent algicidal activity against PCC6803 and FACHB905 with EC50 = 1.28 mu M and 0.37 mu M, respectively, 1.4-fold and 4.0-fold enhancement compared to copper sulfate (EC50 = 1.79 and 1.49 mu M, respectively), and it also showed the best inhibitory activity of EcIspD. The binding of 6bb to EcIspD was explored by molecular docking, and it was confirmed that 6bb could bind to the EcIspD active site. Compound 6bb was proven to be a potential structure for the further development of novel algicides that targets IspD in the MEP pathway.
期刊：
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY,2024年72(8):3884-3893 ISSN：0021-8561
通讯作者：
Lin, Hong-Yan;Wang, DW
作者机构：
[Ye, Bao-Qing; Yang, Guang-Fu; Cai, Zhuo-Mei; Chen, Li-Jun; Wang, Da-Wei; Dong, Jin; Huang, Guang-Yi; Lin, Hong-Yan; Lin, HY] Cent China Normal Univ, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Ye, Bao-Qing; Yang, Guang-Fu; Cai, Zhuo-Mei; Chen, Li-Jun; Wang, Da-Wei; Dong, Jin; Huang, Guang-Yi; Lin, Hong-Yan; Lin, HY] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Wuhan 430079, Peoples R China.
通讯机构：
[Wang, DW ; Lin, HY] C;Cent China Normal Univ, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Wuhan 430079, Peoples R China.
摘要：
4-Hydroxyphenylpyruvate dioxygenase (HPPD, EC 1.13.11.27) is one of the most valuable herbicide targets due to its unique biological functions. In search of HPPD inhibitors with promising biological performance, we designed and synthesized a series of novel tetrazolamide-benzimidazol-2-ones using a structure-based drug design strategy. Among the synthesized compounds, 1-(2-chlorobenzyl)-3-methyl-N-(1-methyl-1H-tetrazol-5-yl)-2-oxo-2,3-dihydro-1H-benzo[d]imidazole-4-carboxamide, <bold>25</bold>, IC50 = 10 nM, was identified to be the most outstanding HPPD inhibitor, which showed more than 36-fold increased Arabidopsis thaliana HPPD (AtHPPD) inhibition potency than mesotrione (IC50 = 363 nM). Our AtHPPD-<bold>25</bold> complex indicated that one nitrogen atom on the tetrazole ring and the oxygen atom on the amide group formed a classical bidentate chelation interaction with the metal ion, the benzimidazol-2-one ring created a tight pi-pi stacking interaction with Phe381 and Phe424, and some hydrophobic interactions were also found between the ortho-Cl-benzyl group and surrounding residues. Compound <bold>32</bold> showed more than 80% inhibition against all four tested weeds at 150 g ai/ha by the postemergence application. Our results indicated that the tetrazolamide-benzimidazol-2-one scaffold may be a new lead structure for herbicide discovery.
摘要：
Cancer cells need a greater supply of glucose mainly due to their aerobic glycolysis, known as the Warburg effect. Glucose transport by glucose transporter 1 (GLUT1) is the rate-limiting step for glucose uptake, making it a potential cancer therapeutic target. However, GLUT1 is widely expressed and performs crucial functions in a variety of cells, and its indiscriminate inhibition will cause serious side effects. In this study, we designed and synthesized a photocaged GLUT1 inhibitor WZB117-PPG to suppress the growth of cancer cells in a spatiotemporally controllable manner. WZB117-PPG exhibited remarkable photolysis efficiency and substantial cytotoxicity toward cancer cells under visible light illumination with minimal side effects, ensuring its safety as a potential cancer therapy. Furthermore, our quantitative proteomics data delineated a comprehensive portrait of responses in cancer cells under glucose deprivation, underlining the mechanism of cell death via necrosis rather than apoptosis. We reason that our study provides a potentially reliable cancer treatment strategy and can be used as a spatiotemporally controllable trigger for studying nutrient deprivation-related stress responses.
通讯机构：
[Pan, FF ] C;[Dong, XY ] H;Henan Polytech Univ, Coll Chem & Chem Engn, Jiaozuo 454000, Peoples R China.;Zhengzhou Univ, Coll Chem, Zhengzhou 450001, Peoples R China.;Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
摘要：
Materials exhibiting X-ray-induced photochromism have consistently piqued the interest of researchers. Exploring the photochromic properties of such materials is valuable for understanding the structural changes and electron transfer processes that occur under high energy radiation, such as X-ray irradiation. Here, a crystalline silver(I) nanocluster synthesized from tert-butylacetylene silver was found to have the ability to exhibit color and photoluminescence changes upon exposure to X-ray radiation. The responsive behavior was observed across a wide temperature range of 100-300 K, with the ability to respond particularly well to soft X-rays (lambda > 1 & Aring;) and exhibit light responsiveness to hard X-rays (lambda < 1 & Aring;). By combining experimental findings including X-ray diffraction, X-ray photoelectron spectroscopy, electron spin resonance, etc. with theoretical calculations, we have proposed that X-ray irradiation induces electron transfer from chloride (Cl-) located in the center of the silver(I) nanocluster to the surrounding Ag-14 in the skeleton. This represents the first documented example in which electron transfer induced by X-ray excitation has been observed, accompanied by a photochromism process, in silver nanoclusters. This study contributes to our understanding of X-ray-induced photochromism and the electron transfer process in silver cluster compounds. It also provides valuable insights and potential design strategies for applications such as photochromism, photoluminescence color change, and photoenergy conversion.
摘要：
Developing green composite with high biomass content is one crucial way to realize the strategy of 'carbon reduction'. The type of polyurethane prepolymer and its soft segment's structure have an important influence on the structure and properties of composite materials. This work focused on preparing different kinds of wood powder-polyurethane prepolymer (WCLPU) composite with high biomass content to study the effects of the molecular weight of the soft segment of the polyurethane prepolymer (PCLPU) on the structure and properties of the composites. The results showed that the composite materials with 70 wt% wood content exhibited high strength and good bending performance. Specifically, with decreasing molecular weight of the PCLPU soft segment, the bending strength and bending modulus of the modified WCLPU composite also increased. This work has laid a foundation for studying the effects of the molecular weight of the PCLPU soft segment on the structure and properties of composite materials.
摘要：
Organic molecules bearing chiral sulfur stereocenters exert a great impact on asymmetric catalysis and synthesis, chiral drugs, and chiral materials. Compared with acyclic ones, the catalytic asymmetric synthesis of thio-heterocycles has largely lagged behind due to the lack of efficient synthetic strategies. Here we establish the first modular platform to access chiral thio-oxazolidinones via Pd-catalyzed asymmetric [3+2] annulations of vinylethylene carbonates with sulfinylanilines. This protocol is featured by readily available starting materials, and high enantio- and diastereoselectivity. In particular, an unusual effect of a non-chiral supporting ligand on the diastereoselectivity was observed. Possible reaction mechanisms and stereocontrol models were proposed.
期刊：
JOURNAL OF MEDICINAL CHEMISTRY,2024年67(8):6822-6838 ISSN：0022-2623
通讯作者：
Guo, J
作者机构：
[Bian, Miao-Miao; Zhang, Ru-Yan; Cui, Hong-Ying; Ding, Dong; Guo, J; Wen, Yu; Guo, Jun; Zhou, Shi-Hao; Zou, Yong-Ke] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构：
[Guo, J ] 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：
Weak antigens represented by MUC1 are poorly immunogenic, which greatly constrains the development of relevant vaccines. Herein, we developed a multifunctional lipidated protein as a carrier, in which the TLR1/2 agonist Pam(3)CSK(4) was conjugated to the N-terminus of MUC1-loaded carrier protein BSA through pyridoxal 5'-phosphate-mediated transamination reaction. The resulting Pam(3)CSK(4)-BSA-MUC1 conjugate was subsequently incorporated into liposomes, which biomimics the membrane structure of tumor cells. The results indicated that this lipidated protein carrier significantly enhanced antigen uptake by APCs and obviously augmented the retention of the vaccine at the injection site. Compared with the BSA-MUC1 and BSA-MUC1 + Pam(3)CSK(4) groups, Pam(3)CSK(4)-BSA-MUC1 evoked 22- and 11-fold increases in MUC1-specific IgG titers. Importantly, Pam(3)CSK(4)-BSA-MUC1 elicited robust cellular immunity and significantly inhibited tumor growth. This is the first time that lipidated protein was constructed to enhance antigen immunogenicity, and this universal carrier platform exhibits promise for utilization in various vaccines, holding the potential for further clinical application.
作者机构：
[Kong, Sheng; Yi, Beibei; Guo, R; Ma, Yujiao; Guo, Rui; Zhang, Guozhu; Du, Qianqian; Zhang, He; Zhang, GZ; Zheng, Jialian] Cent China Normal Univ CCNU, Int Joint Res Ctr Intelligent Biosensing Technol &, CCNU uOttawa Joint Res Ctr, Key Lab Pesticides & Chem Biol,Minist Educ,Coll Ch, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Guo, R ; Zhang, GZ] C;Cent China Normal Univ CCNU, Int Joint Res Ctr Intelligent Biosensing Technol &, CCNU uOttawa Joint Res Ctr, Key Lab Pesticides & Chem Biol,Minist Educ,Coll Ch, Wuhan 430079, Hubei, Peoples R China.
关键词：
Amines;Silylation;Copper catalysis;Hydrogen atom transfer;C−H activation
摘要：
The development of a general and selective method for alpha-C-(sp(3))-H silylation of feedstock amines has been a long-standing challenge. In this paper, we disclose a mild, general, practical, and highly regio- and diastereoselective alpha-C-(sp(3))-H silylation of various readily available acyclic, cyclic, and aromatic amines with silylboranes through a copper-catalyzed intramolecular 1,5-hydrogen atom transfer (HAT) strategy. The mild activation of 2-iodobenzamide to generate an aryl radical enabled by a ligand-coordinated silyl copper complex without additional heating or photoinduced conditions, as well as the intramolecular selective 1,5-HAT process to produce the crucial alpha-aminoalkyl radical species, is the key to the success of this chemistry. This silylation protocol has demonstrated its potential utility in the late-stage modification of structurally complex drugs and bioactive molecules. Therefore, it is expected that this method will find applications in synthetic chemistry and drug discovery.
作者机构：
[Qiu, Xiaofeng; Zheng, Juan; Zhu, Xiaoxiao; Zhang, Qian; Guo, Yanbing; Zhu, Yuhua; Chen, Wei; Zhang, Baojian; Guo, YB; Luo, Zhu; Li, Weihao; Pan, Chuanqi; Fang, Yarong; Wang, Jinlong] Cent China Normal Univ, Inst Environm & Appl Chem, Engn Res Ctr Photoenergy Utilizat Pollut Control &, Minist Educ,Coll Chem,Key Lab Pesticide & Chem Bio, Wuhan 430079, Peoples R China.;[Guo, Yanbing; Guo, YB; Luo, Zhu; Wang, Jinlong] Wuhan Inst Photochem & Technol, Wuhan 430082, Peoples R China.;[Wu, Jinsong; Wang, Yutao] Wuhan Univ Technol, Nanostruct Res Ctr, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China.;[Hu, Jinpeng; Wang, Sibo] Fujian Longxin 3D Array Technol Co Ltd, Longyan 364000, Peoples R China.;[Cui, Shuang] SINOPEC Beijing Res Inst Chem Ind Co Ltd, Div Anal, Beijing 100013, Peoples R China.
通讯机构：
[Guo, YB ; Luo, Z] C;Cent China Normal Univ, Inst Environm & Appl Chem, Engn Res Ctr Photoenergy Utilizat Pollut Control &, Minist Educ,Coll Chem,Key Lab Pesticide & Chem Bio, Wuhan 430079, Peoples R China.;Wuhan Inst Photochem & Technol, Wuhan 430082, Peoples R China.
关键词：
(Pt−S−O)-Ti active structure;C3H8 catalytic oxidation;C−H bond activation;Pt-based catalysts;SO2 promotion
摘要：
Typically, SO(2) unavoidably deactivates catalysts in most heterogeneous catalytic oxidations. However, for Pt-based catalysts, SO(2) exhibits an extraordinary boosting effect in propane catalytic oxidation, but the promotive mechanism remains contentious. In this study, an in situ-formed tactful (Pt-S-O)-Ti structure was concluded to be a key factor for Pt/TiO(2) catalysts with a substantial SO(2) tolerance ability. The experiments and theoretical calculations confirm that the high degree of hybridization and orbital coupling between Pt 5d and S 3p orbitals enable more charge transfer from Pt to S species, thus forming the (Pt-S-O)-Ti structure with the oxygen atom dissociated from the chemisorbed O(2) adsorbed on oxygen vacancies. The active oxygen atom in the (Pt-S-O)-Ti active structure is a robust site for C(3)H(8) adsorption, leading to a better C(3)H(8) combustion performance. This work can provide insights into the rational design of chemical bonds for high SO(2) tolerance catalysts, thereby improving economic and environmental benefits.
期刊：
Journal of Colloid and Interface Science,2024年653(Pt A):540-550 ISSN：0021-9797
通讯作者：
Yang, Guohai;Qu, Lu-Lu
作者机构：
[Luo, Siyu; Chen, Yu; Guo, Yuxin; Rong, Chengyu; Gu, Yingqiu] School of Chemistry & Materials Science, Jiangsu Normal University, Xuzhou 221116, PR China;[Gao, Wenhui] School of Life Science, Jiangsu Normal University, Xuzhou, 221116, PR China;[Yang, Guohai] School of Chemistry & Materials Science, Jiangsu Normal University, Xuzhou 221116, PR China. Electronic address: yangguohai@jsnu.edu.cn;[Xu, Weiqing; Zhu, Chengzhou] National Key Laboratory of Green Pesticide, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan, Hubei 430079, PR China;[Qu, Lu-Lu] School of Chemistry & Materials Science, Jiangsu Normal University, Xuzhou 221116, PR China. Electronic address: luluqu@jsnu.edu.cn
通讯机构：
[Qu, Lu-Lu; Yang, Guohai] S;School of Chemistry & Materials Science, Jiangsu Normal University, Xuzhou 221116, PR China. Electronic address:
摘要：
Reactive oxygen species (ROS) are ideal alternative antibacterial reagents for rapid and effective sterilization. Although a variety of ROS-based antimicrobial strategies have been developed, many are still limited by their inefficiency. Herein, we report the synthesis of the Ag-MXene nanozyme, which have superior peroxidase-like activity for antibacterial applications. As a result, Ag-MXene nanozyme can efficiently increase the level of intracellular ROS, converting H(2)O(2) into hydroxyl radicals that effectively kill both Gram-negative and Gram-positive bacteria and disrupting the bacterial biofilm formation. Moreover, a sensitive and selective colorimetric biosensor was constructed for assaying cholesterol based on the Ag-MXene's prominent peroxidase-mimicking activity and the cholesterol oxidase cascade reaction. The biosensor exhibits high performance with a linear cholesterol detection range of 2-800μM, and a detection limit of 0.6μM. Ag-MXene nanozyme can be used for the rapid detection of cholesterol in serum without complicated sample pretreatment. Collectively, it is conceivable that the proposed Ag-MXene nanozyme could be used as a biocide and as a cholesterol sensor. This study provides a broad prospect for the rapid detection and sterilization of MXene nanozymes in the biomedical field.
作者机构：
[Feng, Guoqiang; Gong, Shengyi; Gui, Zhisheng] Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan 430079, China
摘要：
Dual-state emissive (DSE) materials exhibit fluorescence in both solid and solution states and have become an emerging material in the fields of materials science and sensing in recent years. However, due to the lack of effective and universal preparation methods, DSE materials, especially those with long emission wavelengths, are still scarce. Developing an effective method for constructing such DSE molecules is urgently needed. In this study, we constructed three DSE molecules (NRP-Boc, DCIP-Boc, and DCMP-Boc) with far-red to near-infrared fluorescence by simply modifying three traditional aggregation-caused quenching (ACQ) fluorophores with tert-butyloxycarbonyl (Boc) groups. Density functional theory (DFT) calculations and crystal data revealed the reasons for the bright fluorescence of these three molecules in solution and solid, demonstrating that this Boc protection method is a simple and effective strategy for constructing DSE molecules. We also found that these three DSE molecules have the potential to target and visualize lipid droplets (LDs). Among them, DCIP-Boc shows advantages of a large Stokes shift, long emission wavelength, low fluorescence background, and good photostability in cells, providing a powerful new molecular tool with DSE property for high-fidelity imaging of LDs.
作者机构：
[Liu, Lijuan; Zhang, Lizhi; Gong, JM; Meng, Mingxia; Gong, Jingming; Yao, Qingfeng; Cai, Zheng; Sun, Hongwei; Jiang, Fang] Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensing Technol &, Key Lab Pesticide & Chem Biol, Coll Chem,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Gong, JM ] C;Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensing Technol &, Key Lab Pesticide & Chem Biol, Coll Chem,Minist Educ, Wuhan 430079, Peoples R China.
摘要：
As emerging contaminants in the environment, antibiotic resistance genes (ARGs) have aroused a global health crisis and posed a serious threat to ecological safety and human health. Thus, efficient and accurate onsite detection of ARGs is crucial for environmental surveillance. Here, we presented a colorimetric-photoelectrochemical (PEC) dual-mode bioassay for simultaneous detection of multiple ARGs by smartly incorporating rolling circle amplification (RCA) into a stimuli-responsive DNA nanoassembly, using the tetracycline resistance genes tetA and tetC as models. The tailored DNA nanoassembly containing RCA amplicons hybridized with specific signal probes: CuO nanoflowers-anchored signal DNA1 and HgO nanoparticles-anchored signal DNA2, respectively. Upon exposure to an acidic stimulus, numerous Cu(2+) and Hg(2+) were released, serving as the reporting agent of colorimetric/PEC dual-mode assay. The released Cu(2+) and Hg(2+) induced localized surface plasmon resonance shifts in Au nanorods and triangular Ag nanoplates through an etching process, respectively, enabling visual analysis of ARGs with distinguishing color changes. Meanwhile, numerous Cu(2+) and Hg(2+) triggered the amplified PEC variations via reacting with the photoactive layers of CuS/CdS and ZnS, respectively. Thus, a rapid and ultrasensitive colorimetric/PEC dual-mode detection of multiple ARGs was achieved with the detection limit down to 17.2 aM. Furthermore, such dual-mode bioassay could discriminate single-base mismatch and successfully determine ARGs in E. coli plasmids and sludge samples, holding great promise for point-of-care genetic diagnostics.
期刊：
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY,2024年311:123979 ISSN：1386-1425
通讯作者：
Liu, SH;Zhang, J
作者机构：
[Peng, Zhen; Liu, Sheng Hua; Liu, SH] Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Zhang, Jing; Feng, Na; Zhang, J] Southern Med Univ, Nanfang Hosp, Dept Lab Med, Guangzhou 510515, Peoples R China.;[Zhang, Jianyu] Hong Kong Univ Sci & Technol, Hong Kong Branch, Chinese Natl Engn Res Ctr Tissue Restorat & Recons, Dept Chem,Kowloon, Clear Water Bay, Hong Kong 999077, Peoples R China.;[Zhang, Jianyu] Hong Kong Univ Sci & Technol, Inst Adv Study, Kowloon, Clear Water Bay, Hong Kong 999077, Peoples R China.
通讯机构：
[Liu, SH ] C;[Zhang, J ] S;Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;Southern Med Univ, Nanfang Hosp, Dept Lab Med, Guangzhou 510515, Peoples R China.
摘要：
High-performance luminescent gold(I) complexes have attracted considerable attention due to their potential applications in various fields, but their construction is a significantly challenging task. Herein, we designed and synthesized a series of novel dinuclear gold(I) complexes 1-4 based on 1,2-bis(diphenylphosphino)benzene and 1,4-bis(diphenylphosphino)benzene frameworks, where para-substitutions of benzene ring were employed for comparison and bulky t-butyl groups were introduced into carbazole ligands to assist flexibly regulating the aurophilicity. Among them, the structure of complex 1 was confirmed by single-crystal X-ray diffraction, and all the complexes exhibited typical aggregation-induced emission characteristics. Due to the construction of intramolecular aurophilicity and the formation of molecular clusters, noticeable enhancement of the luminescent efficiency was achieved for the core complex 1. Together with the introduction of flexible t-butyl groups, good responsiveness towards external mechanical force and solvent vapors were also realized. Moreover, the specific bioimaging ability of complex 1 towards cancer cells was demonstrated. Thus, this work presents the crucial capability of aurophilic manipulation in tuning the luminescence and smart behaviors of gold complexes, and it will open a new route to developing high-performance luminescent materials.
摘要：
An electrochemcial synthesis of indoline‐fused polycycles by constructing both the five‐ and six‐membered heterocyclic rings in a single step from arylamide‐tethered ynones has been developed, which provides facile access to various indoline‐based tetracyclic 6/5/6/6 skeletons with highly regioselective control in a sustainable, metal‐ and oxidant‐free condition. Abstract Indoline‐fused polycyclic scaffolds are virtually universal in biological and pharmaceutical. Here we demonstrate a facile electrooxidative cascade cyclization for indoline‐based derivatives, employing amidyl radicals with ynones under mild conditions. The efficient method enables the formation of two new C−N and C−C bonds in a single step with high regioselectivity. Various indoline‐based tetracyclic 6/5/6/6 skeletons can be achieved through a biscyclization/dehydrogenation cascade process. Additionally, this electrochemical strategy proceeds in a sustainable metal‐ and oxidant‐free condition, with H2 being the solely byproduct.
作者机构：
[Ling, Cancan; Zhang, Lizhi; Zhan, Guangming] School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China;[Ling, Cancan; Zhan, Guangming] Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, Central China Normal University, Wuhan 430079, China;[Liang, Chuan; Liu, Xiufan; Sun, Hongwei; Zhao, Jincai; Zhou, Bing; Li, Yaling; Li, Meiqi] Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, Central China Normal University, Wuhan 430079, China;[Li, Hao] School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China. Electronic address: hao_li@sjtu.edu.cn;[Zhang, Lizhi] Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, Central China Normal University, Wuhan 430079, China. Electronic address: zhanglizhi@sjtu.edu.cn
通讯机构：
[Hao Li; Lizhi Zhang] S;School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China<&wdkj&>Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, Central China Normal University, Wuhan 430079, China<&wdkj&>School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
摘要：
Regioselective 1,2-dichalcogenation of alkenes has attracted significant attention in modern organic synthetic chemistry. While there are a plethora of methods to access alkene dichalcogenated architectures, sulfonylsulfination of alkenes is extremely challenging due to the inherent characteristics of the sulfur atom. Herein, a multicomponent fragment coupling of alkenes, sulfinates, and DABSO was developed to construct densely functionalized sulfonylsulfinated products, which are otherwise challenging to access, with broad substrate scope and group tolerance under mild and operationally simple conditions, using an inexpensive 100-1000 ppm organic photocatalyst. In addition, the protocol was applied to the late-stage functionalization of complex molecules, and the obtained products were converted into diverse downstream transformations to demonstrate their synthetic potential. Experimental and theoretical mechanistic investigations suggest that these reactions proceed through sequential sulfonyl and sulfinyl oxygen radical mutual transformations and radical-polar crossover coupling. This strategy provides access to previously inaccessible alkene sulfonylsulfinated products in good-to-high regio- and stereoselectivity, along with opening up previously unexplored synthetic directions.
摘要：
Fe-SSZ-13 (Fe -13) is an effectual catalyst for NOx abatement with extensive application potential in the selective reduction of NOx by NH3 (NH3-SCR). It is necessary to further research and expand the fundamental knowledge of Fe -13 catalysts. In this research, Fe -13 zeolites possessing Si/Al ratios of 6.9, 12.0, and 17.5 were prepared. Fe13(6.9) showed excellent catalytic activity because it had a larger number of isolated Fe3+ ions and welldispersed Fe species. Upon hydrothermal aging, the Fe -13(6.9) catalyst diminished significantly in catalytic activity. Among the three, Fe -13(17.5) exhibited the best hydrothermal stability. It is because Fe -13, possessing a higher Si/Al ratio, had fewer Si-OH-Al bonds but more Si(0Al) structures. Thus, Fe -13(17.5) suffered less structural collapse during hydrothermal aging, leading to a smaller decrease in active isolated Fe3+ ions and acid sites, as well as a lower aggregation of Fe species. Moreover, above 200 degrees C, Fe -13(6.9) exhibited a higher reaction rate compared to Fe -13(12.0) and Fe -13(17.5), and the SCR reaction route of Fe -13(6.9) was distinctly different from that of the other two catalysts.
作者机构：
[Xu, Yuling; Luo, Lishi; Sun, Yao; Pang, Yida; Yang, Jingfang; Li, Chonglu] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Luo, Lishi] Hunan Univ, State Key Lab Chemo Biosensing & Chemometr, Changsha 410082, Peoples R China.;[Sharma, Amit] Amity Univ Punjab, Amity Sch Chem Sci, Dept Phys, Mohali 140306, India.;[Liu, Shuang] Wuhan Univ Technol, Sch Mat Sci & Engn, Wuhan 430070, Peoples R China.;[Zhan, Jianbo] Hubei Prov Ctr Dis Control & Prevent, Inst Hlth Inspect & Testing, Wuhan, Hubei, 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.
摘要：
Albeit sonodynamic therapy (SDT) has achieved encouraging progress in microbial sterilization, the scarcity of guidelines for designing highly effective sonosensitizers and the intricate biofilm microenvironment (BME), substantially hamper the therapeutic efficacy against biofilm infections. To address the bottlenecks, we innovatively design a Ru(II) metallacycle-based sonosensitizer/sonocatalyst (named Ru-A3-TTD) to enhance the potency of sonotherapy by employing molecular engineering strategies tailored to BME. Our approach involves augmenting Ru-A3-TTD’s production of ultrasonic-triggered reactive oxygen species (ROS), surpassing the performance of commercial sonosensitizers, through a straightforward but potent π-expansion approach. Within the BME, Ru-A3-TTD synergistically amplifies sonotherapeutic efficacy via triple-modulated approaches: (i) effective alleviation of hypoxia, leading to increased ROS generation, (ii) disruption of the antioxidant defense system, which shields ROS from glutathione consumption, and (iii) enhanced biofilm penetration, enabling ROS production in deep sites. Notably, Ru-A3-TTD sono-catalytically oxidizes NADPH, a critical coenzyme involved in antioxidant defenses. Consequently, Ru-A3-TTD demonstrates superior biofilm eradication potency against multidrug-resistant Escherichia coli compared to conventional clinical antibiotics, both in vitro and in vivo. To our knowledge, this study represents the pioneering instance of a supramolecular sonosensitizer/sonocatalyst. It provides valuable insights into the structure-activity relationship of sonosensitizers and paves a promising pathway for the treatment of biofilm infections.
