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Rearranged 19-nor-7,8-seco-labdane diterpenoids and Diels-Alder cycloadducts from the Chinese liverwort Pallavicinia ambigua:Structural elucidation,photoinduced rearrangement,and cytotoxic activity

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Chinese chemical Letters 2024年第3期35卷 415-418页

作者： Chunyang Zhang Yuelan Li Zhaojun Chu Shuangzhi Yuan Yanan Qiao Jiaozhen Zhang Lin Li Yueqing Zhang Ruifeng Tian Yajie Tang Hongxiang Lou Department of natural products Chemistry Key Lab of Chemical Biology(MOE)School of Pharmaceutical SciencesShandong UniversityJi'nan 250012China State key laboratory of Microbial Technology Shandong UniversityQingdao 266237China

Two distinctive rearranged 19-nor-7,8-seco-labdane diterpenoids(1 and 2)with a novel tetracyclo[5.***.1.0^(2,5.)0^(4,10)]decane skeleton,a derivative of the open tetrahydrofuran ring(7),three dimeric compounds(8-10),and four revised homologs(3-6)were obtained from Chinese liverwort Pallavicinia *** structures were identified via combined analysis of their spectroscopic data,single-crystal X-ray diffraction patterns,and ECD *** light-driven conversion of compound 5 to compounds 1-4 demonstrated that photochemically induced postmodification involved in biosynthesis is an important way to diversify natural structures.A preliminary cytotoxicity assay revealed that compound 5 showed significant inhibition in the human prostate cancer(PC-3)cell line via an apoptotic pathway.

关键词： Liverwort Pallavicinia ambigua 19-nor-7 8-seco-Labdan diterpenoid Photoinduced rearrangement Cytotoxic activity

Revealing the Multifunctional Electrocatalysis of Indium-Modulated Phthalocyanine for High-Performance Lithium-Sulfur Batteries

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Energy & Environmental Materials 2024年第1期7卷 5-12页

作者： Yang Guo Zhaoqing Jin Jianhao Lu Zilong Wang Zihao Song Anbang Wang Weikun Wang Yaqin Huang Beijing key laboratory of Electrochemical Process and Technology for Materials Key Laboratory of Biomedical Materials of Natural Macromolecules Ministry of Education Beijing University of Chemical Technology Research Institute of chemical Defense Beijing Key Laboratory of Advanced Chemical Energy Storage Technology and Materials

The sluggish kinetics of complicated multiphase conversions and the severe shuttling effect of lithium polysulfides（LiPSs） significantly hinder the applications of Li-S battery,which is one of the most promising candidates for the next-generation energy storage ***,a bifunctional electrocatalyst,indium phthalocyanine self-assembled with carbon nanotubes（InPc@CNT） composite material,is proposed to promote the conversion kinetics of both reduction and oxidation processes,demonstrating a bidirectional catalytic effect on both nucleation and dissolution of Li2S species.

关键词： bidirectional catalyst indium phthalocyanine lithium−sulfur batteries pouch cells

One stone three birds:Ni-catalyzed asymmetric allenylic substitution of allenic ethers,hydroalkylation of 1,3-enynes and double alkylation of enynyl ethers

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Chinese chemical Letters 2024年第8期35卷 282-287页

作者： Zhirong Yang Shan Wang Ming Jiang Gengchen Li Long Li Fangzhi Peng Zhihui Shao key laboratory of Medicinal Chemistry for natural Resource Ministry of EducationSchool of Chemical Science and TechnologyYunnan Provincial Center for Research&Development of Natural Productsand State Key Laboratory for Conservation and Utilization of Bio-Resources in YunnanYunnan UniversityKunming 650091China

The development of low-cost,earth-abundant and environmentally benign transition metal catalysts,which can catalyze multiple different types of asymmetric reactions,is an important objective in mod-ern asymmetric *** we demonstrate that a chiral Ni/P-Phos catalyst achieves three types of asymmetric reactions:allenylic substitution of racemic allenic ethers,1,4-hydroalkylation of prochiral 1,3-enynes and double alkylation of newly designed enynyl ether *** methods complement each other and produce various axially chiral allene derivatives bearing a pyrazolidine-3,5-dione unit,which is widely present in drugs and biologically active molecules with versatile pharmacological activities.

关键词： Nickel Asymmetric catalysis Allenylic substitution Hydroalkylation Double alkylation Allene 1,3-Enyne Pyrazolidine-3,5-dione

A universal strategy for the refined frameworks and improved performance of distinct commercial polyacrylonitriles in sulfur cathodes

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Science China Materials 2024年第9期67卷 2915-2924页

作者： Yikun Yi Feng Hai Wenting Chen Xin Gao Jingyu Guo Weicheng Xue Mingtao Li shaanxi key laboratory of Energy chemical Process Intensification School of Chemical Engineering and TechnologyXi’an Jiaotong UniversityXi’an710049China

Sulfurized polyacrylonitrile(SPAN)with the exceptional stability,safety,low cost,and high capacity have been positioned as a highly promising cathode material for next-generation lithium-ion ***,in the market,polyacrylonitrile(PAN)sourced from different suppliers and available at varying prices exhibits significant variations in physical and chemical properties,resulting in diverse behaviors in Li-SPAN *** studying the mechanism,we found that the PAN copolymerization structure leads to the stacking of chain segments which obstructs the embedding of sulfur and lithium ***,we propose a universal strategy for the refined frameworks by an exogenous additive to modify various PAN raw materials,and the battery capacity and cycling performance are obviously *** a result,the copolymerized SPAN with a poor original capacity is nearly doubled to over 500 mAh g^(-1),almost comparable to high-quality yet expensively imported products;for the sample with a high initial capacity but fading in ether-based electrolytes,it can be modified to maintain stability over 400 *** strategy offers an alternative approach for SPAN modification that is characterized by its simplicity and low cost,thereby facilitating the large-scale development of Li-SPAN batteries.

关键词： copolymerization structure universal strategy exogenous additive SPAN modification

Chemoselective Transfer Hydrogenation of Nitroarenes with Ammonia Borane Catalyzed by Copper N-Heterocyclic Carbene Complexes

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Chinese Journal of Chemistry 2024年第15期42卷 1721-1726页

作者： Hui Zhou Hongmei Jiao Xing Lu Yuanyuan Gao Zhiqiang Ren Haojie Ma Yuqi Zhang Bo Han laboratory of New Energy&New Function Materials Shaanxi Key Laboratory of Chemical Reaction EngineeringCollege of Chemistry and Chemical EngineeringYan'an UniversityYan'anShaanxi 716000China

Herein,we present a method for the homogeneous hydrogenation of nitroarenes to produce anilines using low catalyst loading(1 mo%)of copper N-heterocyclic carbene complexes as the catalyst and ammonia borane as the source of hydrogen.A wide range of nitroarenes,featuring diverse functional groups,were selectively transformed into their corresponding primary aromatic amines with high *** process can be readily scaled up and exhibits compatibility with various sensitive functional groups,including halogen,trifluoromethyl,aminomethyl,alkenyl,cyano,ester,amide,and ***,this catalytic methodology finds application in the synthesis of essential drug *** investigations suggest that the in-situ-generated Cu-H species may serve as active intermediates,with reduction pathways involving species such as azobenzene,1,2-diphenylhydrazine,nitrosobenzene,and N-phenylhydroxylamine.

关键词： Homogeneous catalysis Hydrogenation N-Heterocyclic carbene complexes Nitroarenes Ammonia borane

Highly sensitive fluorescent sensing and photocatalytic degradation performance of two-dimensional Tb-organic network

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Journal of Rare Earths 2024年第2期42卷 303-313,I0003页

作者： Ting Gao Zhihu Ma Yixia Ren Zhixiang Wang Meili Zhang Xiaoli Chen Jijiang Wang laboratory of New Energy and New Function Materials Shaanxi Key Laboratory of Chemical Reaction EngineeringCollege of Chemistry and Chemical EngineeringYan'an UniversityYan'an716000China

A novel tetra-nuclear Tb-organic network,named as [Tb_(4)(2-pyia)_(6)(HAc)_(0.5)(2,2'-bipy)(H_(2)O)_(4.5)]·2,2'-bipy·H_(2)O(1),was synthesized hydrothermally based on 5-(pyridin-2-ylmethoxy) isophthalic acid(H_(2)pyia) and 2,2'-bipyridine(2,2'-bipy) ligands,and characterized by single crystal X-ray diffraction,thermogravimetric(TG) analyses,powder X-ray diffraction(PXRD) and infrared(IR) technology.1 possesses a two-dimensional network based on the tetra-nuclear inorganic building units,and the π-πstacking interactions between the pyia^(2-) ligands and the guest 2,2'-bipy molecules play an important role in the forming of 3D supramolecular structure.1 exhibits excellent fluorescent sensing performance for Fe^(3+)(1.26×10^(-8) mol/L),Cr_(2)O_(7)^(2-)(8.1×10^(-7) mol/L),2,4,6-trinitrophenol(TNP)(2.71×10^(-8) mol/L)and tetracycline(TCT)(2.76×10^(-7) mol/L) in aqueous solution with lower detection *** sensing mechanisms of 1 were investigated by density functional theory(DFT) calculations,ultraviolet-visible(UV-Vis) diffuse reflectance spectroscopy,PXRD and fluorescent lifetime *** activated product of 1 was prepared by heating at 255℃ under constant pressure and used to photo-catalytically degrade *** 1 and the activated one have good photocatalytic degradation performance for TCT with degradation rates of 84.29% and 96.07%,*** photocatalytic mechanisms were discovered by UV-Vis diffuse reflectance spectroscopy and radical trap *** Tb-organic framework might be an excellent multifunctional fluorescent sensor and a good photocatalytic agent for TCT degradation in the future.

关键词： Tb-organic network Fluorescent sensing Photocatalytic degradation Rare earths

Progress in research on metal-based materials in stabilized Zn anodes

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Rare Metals 2024年第1期43卷 20-40页

作者： Le Li Shao-Feng Jia Ming-Hui Cao Yong-Qiang Ji Heng-Wei Qiu Dan Zhang shaanxi key laboratory of Industrial Automation School of Mechanical EngineeringShaanxi University of TechnologyHanzhong 723001China School of Electronic and Information Engineering Qingdao UniversityQingdao 266071China State key laboratory for Artifcial Microstructure and Mesoscopic Physics School of PhysicsPeking UniversityBeijing 100871China Department of Chemistry Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical BiologyTsinghua UniversityBeijing 100084China shaanxi key laboratory of Catalysis School of Chemistry and Environment ScienceShaanxi University of TechnologyHanzhong 723001China

Aqueous zinc-ion batteries(ZIBs) combine the benefits of metallic Zn anodes with those of aqueous electrolytes and are well suited for large-scale energy storage because of their inherent high safety, cost-effectiveness, and eco-friendliness. Currently, the practical application of such batteries is hindered by the poor cycling performance of Zn anodes due to uncontrolled dendrite formation and severe side reactions, although recent reports suggest that these problems can be mitigated through the modification of Zn anodes with metal-based *** that the mechanisms of improving Zn deposition and the structural evolution of metal-based materials have not been systematically reviewed, we herein systematically overview the metal-based materials used to stabilize Zn anodes, starting with a brief summary of the anode working mechanism and the challenges faced by stabilized Zn anodes. Subsequently, the design principles of Zn anodes stabilized by metal-based materials and the related recent progress are reviewed, and the key challenges and perspectives for the future development of such Zn anodes are proposed.

关键词： Zinc-ion batteries(ZIBs) Zn anode Metalbased materials Alloying metal Stabilized Zn anodes

Cationic Conjugated Oligomers for Efficient and Rapid Antibacterial Photodynamic Therapy via Both Type Ⅰ and Type Ⅱ Pathways

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Chinese Journal of Chemistry 2024年第1期42卷 61-66页

作者： Huan Wang Shuwen Guo Qiong Yuan Meiqi Li Yanli Tang Country key laboratory of Analytical Chemistry for Life Science of shaanxi Province Key Laboratory of Applied Surface and Colloid ChemistryMinistry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi'anShaanxi 710119China

Recently,photodynamic therapy(PDT)has attracted wide attention due to its less susceptibility to drug resistance,broad-spectrum biocidal activity and biosafety in normal ***,the traditional photosensitizers(Ps)face the disadvantage of poor therapeutic efficacy due to the requirement of an aerobic environment to generate ^(1)O_(2) through Type Ⅱ ***,we designed and synthesized a novel cationic conjugated oligomer oligo(phenylene vinylene)(OPV)and studied its antibacterial photodynamic activity against both Gram-negative Escherichia coli(***)and Gram-positive bacteria methicillin-resistant Staphylococcus aureus(MRSA).Importantly,the OpV can rapidly produce reactive oxygen species(ROs)through double pathways,Type Ⅰ and Ⅱ mechanism under white light irradiation,and efficiently kill *** and MRSA at a nanomolar *** dual type photosensitizing capability makes OPV promising for enhanced PDT to treat pathogens and tumors in complex environments.

关键词： Conjugated oligomers Antibacterial photodynamic therapy Oligo(phenylene vinylene) Reactive oxygen species Typelandll pathways

The chemical structures,biosynthesis,and biological activities of secondary metabolites from the culinary-medicinal mushrooms of the genus Hericium:a review

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Chinese Journal of natural Medicines 2024年第8期22卷 676-698页

作者： QI Jianzhao WU Jing KANG Shijie GAO Jingming Hirokazu Kawagishi LIU Hongwei LIU Chengwei key laboratory for Enzyme and Enzyme-Like Material Engineering of Heilongjiang College of Life ScienceNortheast Forestry UniversityHarbin 150040China shaanxi key laboratory of natural products&chemical biology College of Chemistry&PharmacyNorthwest A&F UniversityYangling 712100China Faculty of Agriculture Shizuoka UniversityShizuoka 422-8529Japan State key laboratory of Mycology Institute of MicrobiologyChinese Academy of SciencesBeijing 100101China

Fungal phytochemicals derived from higher fungi,particularly those from the culinary-medicinal genus Hericium,have gained significant attention in drug discovery and *** review aims to provide a comprehensive analysis of the chemical structures,biosynthetic pathways,biological activities,and pharmacological properties of monomeric compounds isolated from Hericium *** the past 34 years,253 metabolites have been identified from various Hericium species,including cyathane diterpenes,alkaloids,benzofurans,chromenes,phenols,pyrones,steroids,and other miscellaneous *** investigations into the biosynthesis of erinacines,a type of cyathane diterpene,have led to the discovery of novel cyathane *** research has highlighted the biological activities and pharmacological properties of Hericium-derived compounds,with particular emphasis on their neuroprotective and neurotrophic effects,immunomodulatory capabilities,anti-cancer activity,antioxidant properties,and antimicrobial *** A,in particular,has been extensively ***,transcriptomic,and proteomic analyses of Hericium species have facilitated the discovery of new compounds and provided insights into enzymatic reactions through genome *** diverse chemical structures and biological activities of Hericium compounds underpin their potential applications in medicine and as dietary *** review not only advances our understanding of Hericium compounds but also encourages further research into Hericium species within the realms of medicine,health,functional foods,and agricultural *** broad spectrum of compound types and their diverse biological activities present promising opportunities for the development of new pharmaceuticals and edible products.

关键词： Hericium Secondary metabolites Biological activity Biosynthesis