通讯机构：
[Cuiju Zhu; Mingqiang Qiu] A;Authors to whom correspondence should be addressed.<&wdkj&>Key Laboratory of Pesticides & Chemical Biology Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan 430079, China
摘要：
Organic electrochemistry has attracted tremendous interest within the novel sustainable methodologies that have not only reduced the undesired byproducts, but also utilized cleaner and renewable energy sources. Particularly, oxidative electrochemistry has gained major attention. On the contrary, reductive electrolysis remains an underexplored research direction. In this context, we discuss advances in transition-metal-free cathodically generated radicals for selective organic transformations since 2016. We highlight the electroreductive reaction of alkyl radicals, aryl radicals, acyl radicals, silyl radicals, fluorosulfonyl radicals and trifluoromethoxyl radicals.
期刊：
Drug Discovery Today,2023年:103546 ISSN：1359-6446
通讯作者：
Li, Qing X;Yang, Guang-Fu
作者机构：
[Yang, Jing-Fang; Yang, Guang-Fu; Wang, Meng-Yao; Wang, Di; Wang, Fan; Hao, Ge-Fei] Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, PR China;[Yang, Jing-Fang; Yang, Guang-Fu; Wang, Meng-Yao; Wang, Di; Wang, Fan; Hao, Ge-Fei] International Joint Research Center for Intelligent Biosensor Technology and Health, Central China Normal University, Wuhan, 430079, PR China;[Yang, Jing-Fang] State Key Laboratory for Biology of Plant Diseases and Insect Pests, Institute of Plant Protection, Chinese Academy of Agricultural Sciences, Beijing 100193, PR China;[Zhou, Zhong-Shi] State Key Laboratory for Biology of Plant Diseases and Insect Pests, Institute of Plant Protection, Chinese Academy of Agricultural Sciences, Beijing 100193, PR 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 550025, PR China
通讯机构：
[Li, Qing X] D;[Yang, Guang-Fu] C;Department of Molecular Biosciences and Bioengineering, University of Hawaii at Manoa, Honolulu, HI 96822, USA. Electronic address:;Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300072, PR China. Electronic address:
摘要：
As major forces for modulating protein folding and molecular recognition, cation-π interactions are extensively identified in protein structures. They are even more competitive than hydrogen bonds in molecular recognition and, thus, are vital in numerous biological processes. In this review, we introduce the methods for the identification and quantification of cation-π interactions, provide insights into the characteristics of cation-π interactions in the natural state, and reveal their biological function together with our developed database (Cation-π Interaction in Protein Data Bank; CIPDB; http://chemyang.ccnu.edu.cn/ccb/database/CIPDB). This review lays the foundation for the in-depth study of cation-π interactions and will guide the use of molecular design for drug discovery. Teaser: We provide an overview of the cation-π interaction from its emergence to measurement and collection, along with a data set developed by us, which guides further research in biology and drug design.
期刊：
JOURNAL OF ORGANIC CHEMISTRY,2023年88(11):7463-7468 ISSN：0022-3263
通讯作者：
Ke Gao
作者机构：
[Gao, Ke; Sun, Yulin] Cent China Normal Univ, CCNU uOttawa Joint Res Ctr, Key Lab Pesticide & Chem Biol, Minist Educ,Coll Chem, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Ke Gao] C;CCNU-uOttawa Joint Research Centre, Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan, Hubei 430079, P. R. China
摘要：
An inexpensive and efficient aminoguanidine-catalyzed reductive cyclization of o-phenylenediamines with CO2 in the presence of triethoxysilane is described. Various functionalized benzimidazoles, benzoxazole, and benzothiazole were synthesized in high yields. Mechanistic studies indicate that formic acid as a cocatalyst promotes the cyclization reaction.
作者机构：
[Zhang Bingwen; Yang Wenchao] Cent China Normal Univ, Natl Key Lab Green Pesticide, Key Lab Pesticide Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[Wang Xiaofeng] Univ Chinese Acad Sci, Hangzhou Inst Adv Study, Sch Chem & Mat Sci, Hangzhou 310024, Peoples R China.;[Wang Xiaofeng; Xue Yanqing; Lin Yuqi; Liu Wen; Wang Jing] Chinese Acad Sci, Shanghai Inst Organ Chem, State Key Lab Bioorgan & Nat Prod Chem, Shanghai 200032, Peoples R China.
通讯机构：
[Wang, XF; Liu, W ] C;[Wang, XF ] U;Univ Chinese Acad Sci, Hangzhou Inst Adv Study, Sch Chem & Mat Sci, Hangzhou 310024, Peoples R China.;Chinese Acad Sci, Shanghai Inst Organ Chem, State Key Lab Bioorgan & Nat Prod Chem, Shanghai 200032, Peoples R China.
作者机构：
[Zhang, Zhi-Han; Lu, Liang-Qiu; Yu, Xu-Hui; Xiao, Wen-Jing; Shi, De-Qing] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, 152 Luoyu Rd, Wuhan 430079, Hubei, Peoples R China.;[Xiao, Wen-Jing] Shanghai Inst Organ Chem, State Key Lab Organometall Chem, 345 Lingling Rd, Shanghai 200032, Peoples R China.
通讯机构：
[De-Qing Shi] K;Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan, Hubei 430079, China
摘要：
The asymmetric Michael addition of phosphorus nucleophiles to electron-deficient alkenes is one of the most direct and atom-economical methods to provide chiral organophosphorus compounds with high efficiency in recent years. Herein, we report a cobalt-catalyzed imidazolyl-directed asymmetric phospha-Michael-type reaction of diarylphosphine oxides with electron-deficient alkenes for synthesizing chiral organophosphorus compounds in moderate to good yields and good to excellent enantioselectivities (25 examples, up to 99% yield, and 99% ee). This protocol features broad substrate scope, good functional group tolerance, and mild conditions as well as avoids the release of massive metal wastes and the use of noble transition metal catalysts. The excellent enantioselectivity of the phospha-Michael reaction can be due to the adoption of a novel chiral N4-ligand. Furthermore, the DFT calculation indicates that the bulky 2,4,6-(i-Pr)3C6H2 group of the ligand induces large steric hindrance which blocks the nucleophilic attack from the Si-face.
摘要：
Alcoholic liver disease (ALD) has attracted widespread attention because of the ever-increasing alcohol consumption and high morbidity. However, there is still no effective detection method to prevent the deterioration of the disease. Cholesterol, as the main component of the cell membrane (CM), often transported to lipid droplets (LDs) for storage in hepatocytes. Meanwhile, abnormal changes of cholesterol could cause liver diseases, such as Tangier disease. Based on cholesterol could serve as a hub that affects the cell membrane fluidity (CMF) and the number of LDs, we planned to study the microscopic changes of CMF and LDs in ALD. As viscous media could limit the intramolecular motion of fluorescent probes, aggregation induced emission luminogens (AIEgens), which typically have rotators and vibrators in their structures and emit strongly in the aggregate state, may be promising candidates for CMF and LD study. So two AIE probes (TPCN and NDPB) were designed and synthesized based on the typical AIE skeleton, tetraphenylethylene (TPE), which could selectively target CMs and LDs, respectively. These probes exhibited high chemical stability, controllable emission, and excellent subcellular specificity. They successfully sensed the correlated changes of CMs and LDs in ALD model, which would contribute to understanding the microscopic process of ALD pathogenesis and further development of ALD therapeutic drugs.
期刊：
ACS CHEMICAL BIOLOGY,2023年18(4):915-923 ISSN：1554-8929
通讯作者：
Jun Guo
作者机构：
[Zhang, Zhi-Ming; Zhang, Ru-Yan; Feng, Ran-Ran; Ding, Dong; Wen, Yu; Guo, Jun; Zhou, Shi-Hao] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Hubei Int Sci & Technol Cooperat Base Pesticide &, Wuhan 430079, Peoples R China.;[Wei, Hua-Wei] Jiangsu East Mab Biomed Technol Co Ltd, Nantong 226499, Peoples R China.
通讯机构：
[Jun Guo] K;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, International Joint Research Center for Intelligent Biosensing Technology and Health, Hubei International Scientific and Technological Cooperation Base of Pesticide and Green Synthesis, College of Chemistry, Central China Normal University, Wuhan 430079, China
摘要：
Modification of antigens to improve their immunogenicity represents a promising direction for the development of protein vaccine. Here, we designed facilely prepared adjuvant-free vaccines in which the N-glycan of SARS-CoV-2 receptor-binding domain (RBD) glycoprotein was oxidized by sodium periodate. This strategy only minimally modifies the glycans and does not interfere with the epitope peptides. The RBD glycoprotein oxidized by high concentrations of periodate (RBD(HO)) significantly enhanced antigen uptake mediated by scavenger receptors and promoted the activation of antigen-presenting cells. Without any external adjuvant, two doses of RBD(HO) elicited 324- and 27-fold increases in IgG antibody titers and neutralizing antibody titers, respectively, compared to the unmodified RBD antigen. Meanwhile, the RBD(HO) vaccine could cross-neutralize all of the SARS-CoV-2 variants of concern. In addition, RBD(HO) effectively enhanced cellular immune responses. This study provides a new insight for the development of adjuvant-free protein vaccines.
摘要：
Removing microcystins (MCs) safely and effectively has become an urgent global problem because of their extremely hazardous to the environment and public health. Microcystinases derived from indigenous microorganisms have received widespread attention due to their specific MC biodegradation function. However, linearized MCs are also very toxic and need to be removed from the water environment. How MlrC binds to linearized MCs and how it catalyzes the degradation process based on the actual three-dimensional structure have not been determined. In this study, the binding mode of MlrC with linearized MCs was explored using a combination of molecular docking and site-directed mutagenesis methods. A series of key substrate binding residues, including E70, W59, F67, F96, S392 and so on, were identified. Sodium dodecane sulfate-polyacrylamide gel electrophoresis (SDS-PAGE) was used to analyze samples of these variants. The activity of MlrC variants were measured using high performance liquid chromatography (HPLC). We used fluorescence spectroscopy experiments to research the relationship between MlrC enzyme (E), zinc ion (M), and substrate (S). The results showed that MlrC enzyme, zinc ion and substrate formed E-M-S intermediates during the catalytic process. The substrate-binding cavity was made up of N and C-terminal domains and the substrate-binding site mainly included N41, E70, D341, S392, Q468, S485, R492, W59, F67, and F96. The E70 residue involved in both substrate catalysis and substrate binding. In conclusion, a possible catalytic mechanism of the MlrC enzyme was further proposed based on the experimental results and a literature survey. These findings provided new insights into the molecular mechanisms of the MlrC enzyme to degrade linearized MCs, and laid a theoretical foundation for further biodegradation studies of MCs.
作者机构：
[Qin, Ying; Zhu, Chengzhou; Liu, Mingwang; Li, Jinli; Tan, Rong; Gu, Wenling; Wang, Hengjia] 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.;[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.;[Li, Jinli] Jingchu Univ Technol, Sch Elect & Informat Engn, Jingmen 448000, Peoples R China.
通讯机构：
[Liuyong Hu] H;[Wenling Gu; Chengzhou Zhu] K;Hubei Key Laboratory of Plasma Chemistry and Advanced Materials, Hubei Engineering Technology Research Center of Optoelectronic and New Energy Materials, Wuhan Institute of Technology, Wuhan 430205, PR China<&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, PR China
作者机构：
[Lu, Liang-Qiu; Rao, Li; Wang, Bao-Cheng; Qu, Bao-Le; Xiao, Wen-Jing; Xiong, Fen-Ya] Cent China Normal Univ, Minist Educ, CCNU Ottawa Joint Res Ctr, Coll Chem,Key Lab Pesticide & Chem Biol, 152 Luoyu Rd, Wuhan 430079, Hubei, Peoples R China.;[Tan, Ying; Fang, Kai-Xin; Feng, Ying] Tsinghua Univ, Tsinghua Shenzhen Int Grad Sch, State Key Lab Chem Oncogen, Key Lab Chem Biol, Shenzhen, Peoples R China.;[Lu, Liang-Qiu] Chinese Acad Sci, Lanzhou Inst Chem Phys LICP, State Key Lab Oxo Synth & Select Oxidat, Lanzhou 730000, Peoples R China.;[Lu, Liang-Qiu] Henan Normal Univ, Sch Chem & Chem Engn, Xinxiang 453007, Henan, Peoples R China.
通讯机构：
[Prof. Ying Tan] S;[Prof. Liang-Qiu Lu] C;CCNU-uOttawa Joint Research Centre, Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, 430079 Wuhan, Hubei, P. R. China<&wdkj&>State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics (LICP), Chinese Academy of Sciences, 730000 Lanzhou, P. R. China<&wdkj&>School of Chemistry and Chemical Engineering, Henan Normal University, 453007 Xinxiang, Henan, China<&wdkj&>State Key Laboratory of Chemical Oncogenomics, Key Laboratory of Chemical Biology, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, P. R. China
关键词：
Antitumor Activity;Aza-Ortho-Quinone Methide;Aza-Sulfur Ylide;Azaheterocycle;Transition Metal Catalysis
摘要：
Metal-polarized aza-ortho-quinone methides (aza-o-QMs) are a unique and efficient handle for azaheterocycle synthesis. Despite great achievements, the potential of these reactive intermediates has not yet been fully exploited, especially the new reaction modes. Herein, we disclosed an unprecedented dearomatization process of metal-polarized aza-o-QMs, affording transient dearomatized spiroaziridine intermediates. Based on this serendipity, we accomplished three sequential dearomatization-rearomatization reactions of benzimidazolines with aza-sulfur ylides, enabling the divergent synthesis of bis-nitrogen heterocycles with high efficiency and flexibility. Moreover, experimental and theoretical studies were performed to explain the proposed mechanisms and observed selectivity. Further cellular evaluation of the dibenzodiazepine products identified a hit compound for new antitumor drugs.
摘要：
Accelerating the migration of interfacial carriers ina heterojunctionis of paramount importance for driving high-performance photoelectricresponses. However, the inferior contact area and large resistanceat the interface limit the eventual photoelectric performance. Herein,we fabricated an S-scheme heterojunction involving a 2D/2D dual-metalloporphyrinmetal-organic framework with metal-center-regulated CuTCPP-(Cu)/CuTCPP-(Fe)through electrostatic self-assembly. The ultrathin nanosheet-likearchitectures reduce the carrier migration distance, while the similarporphyrin backbones promote reasonable interface matching through pi-pi conjugation, thereby inhibiting the recombinationof photogenerated carriers. Furthermore, the metal-center-regulatedS-scheme band alignments create a giant built-in electric field, whichprovides a huge driving force for efficient carrier separation andmigration. Coupling with the biomimetic catalytic activity of CuTCPP-(Fe),the resultant heterojunction was utilized to construct photoelectrochemicaluric acid biosensors. This work provides a general strategy to enhancephotoelectric responses by engineering the interfacial structure ofheterojunctions.
作者机构：
Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, China;Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, China;School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, Singapore, Singapore;[Tierui Zhang; Tierui Zhang Tierui Zhang Tierui Zhang] Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, China;[Jinyu Yan; Yuan Li; Shuxin Ouyang; Jinyu Yan Jinyu Yan Jinyu Yan; Yuan Li Yuan Li Yuan Li; Shuxin Ouyang Shuxin Ouyang Shuxin Ouyang] Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, China<&wdkj&>Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, China
通讯机构：
[Shuxin Ouyang; Shuxin Ouyang Shuxin Ouyang Shuxin Ouyang] E;[Tierui Zhang; Tierui Zhang Tierui Zhang Tierui Zhang] K;Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, China<&wdkj&>Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, China<&wdkj&>Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, China
摘要：
We classify the representative photocatalytic materials for photosynthesis of hydrogen peroxide (H2O2) in recent years and discuss the related modification methods in detail, providing inspiration and insights for the future design of photocatalysts for H2O2 production. Abstract Hydrogen peroxide (H2O2), an environmental‐friendly oxidant and renewable liquid fuel, has received wide attention in various research and industrial fields. Current industrial production of H2O2 relies on the anthraquinone method, which is hardly viewed as a sustainable and green process. Photocatalysis, harnessing solar energy as the driving force for redox reactions, provides a green and promising approach for H2O2 production. However, due to the poor ability of light absorption, fast recombination of carriers, and poor intrinsic activity of active sites of pristine photocatalysts, photocatalytic H2O2 production cannot provide great yield. Thus, great efforts have been dedicated to design efficient photocatalysts for photosynthesis of H2O2 in the past decades. In this review, we summarize significant progress in the development of advanced photocatalytic materials for light‐driven H2O2 production. Starting with a brief introduction on basic principles and advantages of photosynthesis of H2O2, the representative materials are classified and discussed in detail; finally, a brief outlook on addressing future challenges and opportunities of photocatalytic H2O2 production is proposed. This review aims to confirm current challenges and research developments in the photosynthesis of H2O2 and provide inspiration for the development of high‐efficiency photocatalysts for photocatalytic H2O2 production in the future.
通讯机构：
[Lingling Feng] K;Key Laboratory of Pesticide & Chemical Biology (CCNU), Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China
摘要：
The frequency and intensity of harmful cyanobacterial blooms (HCBs) are increasing all over the world, their prevention and control have become a great challenge. In this paper, a series of 1,3,4-thiadiazole thioacetamides (T series) were designed and synthesized as potential algaecides. Among them, the compound T3 showed its best algacidal activity against Synechocystis sp. PCC 6803 (PCC 6803, EC50 = 1.51 mu M) and Microcystis aeruginosa FACHB 905 (FACHB905, EC50 = 4.88 mu M), which was more effective than the lead compound L1 (PCC6803, EC50 = 7.7 mu M; FACHB905, EC50 = 8.8 mu M) and the commercially available herbicide prometryn (PCC6803, EC50 = 4.64 mu M;FACHB905, EC50 = 6.52 mu M). Meanwhile, T3 showed a lower inhibitory activity (EC50 = 12.76 mu M) than prometryn (EC50 = 7.98 mu M) to Chlorella FACHB1227, indicating that T3 had selective inhibition to prokaryotic algae (PCC6803, FACHB905) and eukaryotic algae (FACHB1227). Furthermore, the algacidal and anti-algae activities of T3 were significantly better than those of prometryn, while the toxicity of zebrafish and human cells was less than prometryn. Electron microscope, physiological, biochemical and metabonomic anal-ysis showed that T3 interfered with light absorption and light conversion during photosynthesis by significantly reducing chlorophyll content, thus inhibited metabolic pathways such as the Calvin cycle and TCA cycle, and eventually led to the cell rupture of cyanobacteria. These results afforded further development of effective and safe algaecides.
作者：
Gao, Yang-Yang;Yang, Wei-Cheng;Ashby Jr, Charles R.;Hao, Ge-Fei
期刊：
Drug Resistance Updates,2023年67:100934 ISSN：1368-7646
通讯作者：
Charles R. Ashby
作者机构：
[Yang, Wei-Cheng; Gao, Yang-Yang; Hao, Ge-Fei] Guizhou Univ, Ctr Res & Dev Fine Chem, Natl Key Lab Green Pesticide, Key Lab Green Pesticide & Agr Bioengn,Minist Educ, Guiyang 550025, Peoples R China.;[Hao, Ge-Fei] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[Ashby Jr, Charles R.] St Johns Univ, Dept Pharmaceut Sci, New York, NY 10003 USA.
通讯机构：
[Charles R. Ashby] D;Department of Pharmaceutical Sciences, St. John’s University, New York, NY, USA
关键词：
Drug resistance;Cryptic binding sites;Resistance management
摘要：
The emergence of drug resistance is a primary obstacle for successful chemotherapy. Drugs that target cryptic binding sites (CBSs) represent a novel strategy for overcoming drug resistance. In this short communication, we explain and discuss how the discovery of CBSs and their inhibitors can overcome drug resistance.
摘要：
Copper, an essential micronutrient, controls multiple fundamental processes throughout all forms of life, such as respiration, cell proliferation and neurotransmitter biosynthesis. High redox activity makes copper a double-edged sword for cell survival, and abnormal copper metabolism is commonly associated with cancer and other diseases. Recently, advances in copper biology have forged new links between researchers from different disciplines to dissect the use of copper targets in cancer treatment. Copper is crucial for maintaining the rapid growth and proliferation of cancer cells, a process known as ‘cuproplasia’. However, excess mitochondrial copper accumulation also triggers ‘cuproptosis’, a new form of programmed cell death, involving the destabilization of Fe-S cluster proteins and the aggregation of DLAT. Accordingly, both activating cuproptosis by copper ionophores and suppressing cuproplasia through copper depletion are noteworthy anticancer options, but this field currently lacks systematic reviews from both biological and chemical perspectives. This review provides a comprehensive overview of the leading known copper biology and copper-targeted cancer therapy, focusing on copper homeostasis, signal transduction, and copper overload/depletion, which should be beneficial for the development of the next-generation of inorganic anticancer drugs. We expect that our review will provide a balanced perspective to the development and comprehension of copper-based cancer therapy.
作者机构：
[Wang, Huai-Yu; Ma, Jin-Tian; Wu, An-Xin; Wu, Chun-Yan; Zhuang, Shi-Yi; Yu, Zhi-Cheng; Wu, Yan-Dong; Chen, Xiang-Long; Yang, Dong-Sheng] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[Tang, Bo-Cheng] Hong Kong Polytech, Dept Appl Biol & Chem Technol, State Key Lab Chem Biol & Drug Discovery, Kowloon, Hong Kong 999077, Peoples R China.
通讯机构：
[Yan-Dong Wu; An-Xin Wu] K;Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China
摘要：
A concise and efficient hydrodefluorination process was developed for the synthesis of gem-difluoroalkenes. This reaction employs rongalite as a masked proton source and does not require any additional catalysts or reductants. Notably, trifluoromethyl alkenes having both terminal and internal double bonds are compatible with this process, allowing for a wider range of substrates. The successful late-stage functionalizations of pharmaceuticals and gram-scale syntheses were used to demonstrate the viability of this method.
作者机构：
[Lu, Liang-Qiu; Rao, Li; Zhou, Zheng-Xin; Xiao, Wen-Jing; Li, Yu-Jie; Liu, Xiao-Peng; Xiao, Yu-Qing] Cent China Normal Univ, CCNU uOttawa Joint Res Ctr, Key Lab Pesticide & Chem Biol, Minist Educ,Coll Chem, 152 Luoyu Rd, Wuhan 430079, Hubei, Peoples R China.;[Li, Miao-Miao] Zhengzhou Univ, Henan Inst Adv Technol, Div Mol Catalysis & Synth, Zhengzhou 45000, Peoples R China.;[Cao, Meng-Yue; Liu, Xiao-Peng] Westlake Univ, Sch Sci, Hangzhou 310024, Peoples R China.;[Lu, Liang-Qiu] Chinese Acad Sci, Lanzhou Inst Chem Phys LICP, State Key Lab Oxo Synth & Select Oxidat, Lanzhou 730000, Peoples R China.;[Lu, Liang-Qiu] Henan Normal Univ, Sch Chem & Chem Engn, Xinxiang 453007, Henan, Peoples R China.
通讯机构：
[Dr. Li Rao; Prof. Liang-Qiu Lu] C;CCNU-uOttawa Joint Research Centre, Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan, Hubei, 430079 China<&wdkj&>State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics (LICP), Chinese Academy of Sciences, Lanzhou, 730000 P. R. China<&wdkj&>School of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang, Henan, 453007 China<&wdkj&>CCNU-uOttawa Joint Research Centre, Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan, Hubei, 430079 China
摘要：
Ring-opening transformations of donor-acceptor (D-A) cyclopropanes enable the rapid assembly of complex molecules. However, the enantioselective formation of chiral quaternary stereocenters using substrates bearing two different acceptors remains a challenge. Herein, we describe the first palladium-catalyzed highly diastereo- and enantioselective (3+2) cycloaddition of vinyl cyclopropanes bearing two different electron-withdrawing groups, a subset of D-A cyclopropanes. The key to the success of this reaction is the remote stereoinduction through hydrogen bond from chiral ligands, which thereby addressed the aforementioned challenge. A variety of chiral five-membered heterocycles were produced in good yields and with high stereoselectivity (up to 99 % yields, 99 : 1 er and >19 : 1 dr). In-depth mechanistic investigations, including control experiments and theoretical calculations, revealed the origin of the stereoselectivity and the importance of H-bonding in stereocontrol.
摘要：
Journal of Thermoplastic Composite Materials, Volume 37, Issue 1, Page 387-401, January 2024. <br/>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：
Immune checkpoint inhibitors (ICIs) therapy targeting programmed cell death ligand 1 (PD-L1) and programmed death protein 1 (PD-1) had exhibited significant clinical benefits for cancer treatment such as triple negative breast cancer (TNBC). However, the relatively low anti-tumor immune response rate and ICIs drug resistance highlight the necessity of developing ICIs combination therapy strategies to improve the anti-tumor effect of immunotherapy. Herein, the immunomodulator epigallocatechin gallate palmitate (PEGCG) and the immunoadjuvant metformin (MET) self-assembled into tumor-targeted micelles via hydrogen bond and electrostatic interaction, which encapsulated the therapeutic agents doxorubicin (DOX)loaded PEGCG-MET micelles (PMD) and combined with ICIs (anti-PD-1 antibody) as therapeutic strategy to reduce the endogenous expression of PD-L1 and improve the tumor immunosuppressive microenvironment. The results presented that PMD integrated chemotherapy and immunotherapy to enhance antitumor efficacy in vitro and in vivo , compared with DOX or anti-PD-1 antibody for the therapy of TNBC. PMD micelles might be a potential candidate, which could remedy the shortcomings of antibody-based ICIs and provide synergistic effect to enhance the antitumor effects of ICIs in tumor therapy.(c) 2023 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
摘要：
An amphiphilic AIE photosensitizer has been successfully developed, which allows for easily inserting into the bacterial membranes. Binding experiments with phospholipid preliminary demonstrates its membrane specificity. As expected, it is proved to possess a broad-spectrum bacterial staining performance and photodynamic antibacterial activity toward S. aureus and E. coli.
