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.
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.
期刊：
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY,2024年 ISSN：0021-8561
作者机构：
[Zuo, Lingzi; Fan, Yuxuan; Feng, Lingling; He, Yanlin; Cheng, Cai; Zhang, Liexiong; Guo, Xiaoliang; Cheng, Guonian; Yu, Jie; Tang, Guangmei; Huang, Shi; Chen, Ruiqing] Key Laboratory of Pesticide & Chemical Biology (CCNU), Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China;[Liu, Yanyang; Feng, Lingling] Wuhan Institute of Photochemistry and Technology, 7 North Bingang Road, Wuhan, Hubei 430083, China;[Feng, Lingling] National Key Laboratory of Green Pesticide, Central China Normal University, Wuhan 430079, 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.
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.
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 pi-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. A facile pi-expansion strategy is proposed to boost the reactive oxygen species-generation capability, resulting in the development of the first example of a supramolecular sonosensitizer (Ru-A3-TTD). Ru-A3-TTD effectively overcame challenges posed by the complex biofilm microenvironment, including hypoxia, antioxidant defense mechanisms, and hypopermeability for amplifying sonotherapeutic efficacy in eradicating multidrug-resistant biofilms.+ image
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.
期刊：
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY,2024年311:123979 ISSN：1386-1425
通讯作者：
Zhang, Jing;Liu, Sheng Hua
作者机构：
[Peng, Zhen] National Key Laboratory of Green Pesticide, College of Chemistry, Central China Normal University, Wuhan 430079, China;[Zhang, Jianyu] Department of Chemistry, Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction and Institute for Advanced Study, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon 999077, Hong Kong, China;[Feng, Na] Department of Laboratory Medicine, Nanfang Hospital, Southern Medical University, Guangzhou 510515, China;[Zhang, Jing] Department of Laboratory Medicine, Nanfang Hospital, Southern Medical University, Guangzhou 510515, China. Electronic address: zhangjingzisefeng@163.com;[Liu, Sheng Hua] National Key Laboratory of Green Pesticide, College of Chemistry, Central China Normal University, Wuhan 430079, China. Electronic address: chshliu@mail.ccnu.edu.cn
通讯机构：
[Zhang, Jing] D;[Liu, Sheng Hua] N;Department of Laboratory Medicine, Nanfang Hospital, Southern Medical University, Guangzhou 510515, China. Electronic address:;National Key Laboratory of Green Pesticide, College of Chemistry, Central China Normal University, Wuhan 430079, China. Electronic address:
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.
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.
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. Two Pd-catalyzed asymmetric [3+2] annulations are disclosed, providing a modular platform for the enantioselective synthesis of chiral thio-oxazolidinones. Preliminary mechanistic studies are performed to rationalize the observed enantio- and diastereo-controls.+ image
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：
[Shujun Ming; Siqi Yu; Libao Wang; Jianjian Li; Chaktong Au] Hubei Key Laboratory for Processing and Application of Catalytic Materials, School of Chemistry and Chemical Engineering, Huanggang Normal University, Huanggang 438000, PR China;[Xinnan Li; Tao Li] Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, PR China;[Wei Chen; Yanbing Guo] Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, PR China;[Lei Pang; Fan Yang] DongFeng Trucks R&D Center, Wuhan 430056, PR China;[Shidong Tian; Kelun Li] Shaanxi Coal and Chemical Industry Technology Research Institute Co., Ltd., Xi'an 710100, PR China
通讯机构：
[Yanbing Guo; Tao Li] K;Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, PR China<&wdkj&>Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, PR China
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. Fe-13(6.9) showed excellent catalytic activity because it had a larger number of isolated Fe3+ ions and well-dispersed 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 SiOHAl 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 °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：
[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
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.
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.
作者机构：
[Yi, Yun-Ying; Liu, Yu-Ting; Song, Ying-Chun; Wang, Ming-Xuan; Zhang, Wen-Xin; Wang, Zi-Yue; Zhu, Yan-Ping; Sun, Yuan-Yuan] Yantai Univ, Minist Educ, Collaborat Innovat Ctr Adv Drug Delivery Syst & Bi, Sch Pharm,Key Lab Mol Pharmacol & Drug Evaluat, Yantai 264005, Shandong, Peoples R China.;[Wu, An-Xin] 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;[Zhu, YP ] Y;Yantai Univ, Minist Educ, Collaborat Innovat Ctr Adv Drug Delivery Syst & Bi, Sch Pharm,Key Lab Mol Pharmacol & Drug Evaluat, Yantai 264005, Shandong, 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.
关键词：
Total synthesis;Oxidative cyclization;Natural products;Switchable synthesis;Luotonin alkaloids
摘要：
Abstract A total synthesis strategy was developed for the synthesis of luotonin A, B and their analogues using synergistic FeCl3/KI‐catalyzed oxidative cyclization. This protocol utilizes cheap and widely available N‐propargyl 2‐methyl‐quinazolinones and arylamines under mild conditions, and it has a wide substrate scope and high atom economy. Different natural products (luotonin A, B and derivatives) can be synthesized via a unique switchable approach. Further transformations from luotonin B to luotonin E and structural modification of natural products demonstrate the potential applications of this method. Moreover, camptothecin can also be modified with the reported protocol to afford the hydroxyl‐substituted product.
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.
摘要：
An asymmetric cascade cyclization of enynamides and alpha-diazoketones to produce chiral bicyclic lactams bearing chiral all-carbon quaternary stereocenters is realized with up to 95% yield, 98% ee, and >19:1 dr. The combination of visible light photoactivation and the relay of gold and N-oxide catalysis in a cascade process enabled the facile generation and controlled assembly of two reactive intermediates, ketene and aza-o-quinone methide. Theoretical calculations revealed a stepwise [4 + 2] cycloaddition mechanism, with the stereochemistry controlled by the amide group of the catalyst. Remarkably, this study presents the first example of chiral N-oxides serving as catalysts for asymmetric ketene cycloaddition and illustrates how a cascade strategy could be a promising means to access significant chiral heterocyclic scaffolds.
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.
作者机构：
[Zhao, Xia; Gu, Wenxin; Sun, Tengteng; Qin, Jingwen] Tianjin Normal Univ, Tianjin Key Lab Struct & Performance Funct Mol, Key Lab Inorgan Organ Hybrid Funct Mat Chem, Minist Educ,Coll Chem, Tianjin 300387, Peoples R China.;[Ye, Fei] Cent China Normal Univ, CCNU uOttawa Joint Res Ctr, Key Lab Pesticides & Chem Biol, Minist Educ,Coll Chem, Wuhan 430079, Peoples R China.;[Lu, Kui] Tianjin Univ Sci & Technol, Coll Biotechnol, China Int Sci & Technol Cooperat Base Food Nutr Sa, Tianjin 300457, Peoples R China.
通讯机构：
[Zhao, X ] T;[Ye, F ] C;Tianjin Normal Univ, Tianjin Key Lab Struct & Performance Funct Mol, Key Lab Inorgan Organ Hybrid Funct Mat Chem, Minist Educ,Coll Chem, Tianjin 300387, Peoples R China.;Cent China Normal Univ, CCNU uOttawa Joint Res Ctr, Key Lab Pesticides & Chem Biol, Minist Educ,Coll Chem, Wuhan 430079, Peoples R China.
摘要：
A copper-catalyzed thiocyanation of cycloketone oxime esters with ammonium thiocyanate has been developed for the first time. This innovative approach allows access to cyano and thiocyano bifunctionally substituted alkanes, which can be further transformed into their respective trifluoromethylthiol-substituted or difluoromethylthiol-substituted alkylnitriles, alkynyl sulfides, and phosphorothioate esters. The readily available nature of ammonium thiocyanate and the cost-effectiveness of the copper catalyst make this method a promising strategy for the synthesis of sulfur-containing alkylnitriles. A copper-catalyzed thiocyanation of cyclobutanone oxime esters by potassium ammonium thiocyanate was achieved for the first time. Subsequent derivatization of thiocyano substituted alkylnitriles led to various sulfur-containing alkylnitriles.
