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SO_(2)-Insertion induced enantioselective oxysulfonylation to access β-chiral sulfones with quaternary carbon stereocenters

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Science China Chemistry 2024年第3期67卷 908-913页

作者： Jun Zhang Xuefeng Wang Peiqi Wang Jiayuan Fang Shaoyu Li Jie Wu School of pharmaceutical and chemical Engineering&Institute for Advanced Studies Taizhou UniversityShanghai 200438China Department of Chemistry Fudan UniversityShanghai 200438China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of Chemistry and chemical Engineering Henan Normal UniversityXinxiang 453007China

β-Chiral sulfones are structural motifs widely found in natural products and bioactive molecules, while also serving as important intermediates for the synthesis of valuable chiral scaffolds. In contrast to the rapid growth of sulfur dioxide insertion chemistry over the last decade, enantioselective catalytic variants for accessing β-chiral sulfones, especially those bearing a quaternary carbon stereocenter, remain rare. Herein, we report an enantioselective copper/bisoxazoline catalyzed oxysulfonylation of alkenes to yield isoxazolinyl-containing β-chiral sulfones bearing quaternary carbon stereocenters with moderate to excellent yields and up to 96:4 er. The advantage and irreplaceability of this sulfur dioxide insertion catalytic system have been demonstrated by achieving transformations clearly unavailable with the previously reported sulfonyl chloride system. Additionally,the recoverability of the new-developed bisoxazoline ligand L9 and its reusability without any erosion of the catalytic activity and enantioselectivity further demonstrate the usefulness of the protocol.

关键词： β-chiral sulfones sulfur dioxide insertion oxysulfonylation copper catalysis enantioselectivity

Regulation of aqueous electrolyte interface via electrolyte strategies for uniform zinc deposition

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Nano Research 2024年第10期17卷 8678-8693页

作者： Wei Zhong Chaoqiang Tan Laixi Li Shichao Zhang Xinyang Wang Hao Cheng Yingying Lu Institute of Wenzhou Zhejiang UniversityWenzhou 325006China State Key Laboratory of chemical Engineering Institute of Pharmaceutical EngineeringCollege of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang UniversityHangzhou 311215China Zhejiang Huayou Cobalt Company Limited Tongxiang 314500China

Aqueous zinc ion batteries(AZIBs),renowned for their high theoretical energy density,safety,cost-effectiveness and ecofriendliness,offer immense potential in the realm of energy storage and conversion,finding applications in renewable energy and portable ***,the development of AZIBs still faces several challenges related to the electrochemical behavior of zinc anodes in aqueous electrolytes,primarily zinc dendrite formation,which emphasize the critical need for a fundamental understanding of the interfacial phenomena between the electrode and *** review focuses on the three models:the electric double layer(EDL)model,the solvation structure model,and the Zn/electrolyte interface *** guide the design of the electrolyte system in *** models provide a comprehensive understanding of the interactions between the electrode,electrolyte,and the solvated ions in the *** optimizing the salt types,salt concentrations,solvents and additives based on these models,it is possible to enhance the performance of AZIBs,including their energy density,cycle life,and *** review also highlights recent research progress in electrolyte modification of AZIBs for understanding battery behavior,along with perspectives for the direction of further investigations.

关键词： aqueous zinc ion batteries electric double layer solvation structure electrolyte optimization

Residual levels and health risk assessment of trace metals in Chinese resident diet

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Journal of Environmental Sciences 2024年第2期136卷 451-459页

作者： Yubing Dai Shuai Sun Rong Cao Haijun Zhang Jiping Chen Ningbo Geng CAS Key Laboratory of Separation Science for Analytical Chemistry Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Shenyang pharmaceutical University Shenyang 110016China University of Chinese Academy of Sciences Beijing 100049China

Large-scale metal contamination across the food web is an intractable problem due to increasing pollutant emissions,atmospheric transport,and dry and wet deposition of *** present study focus on several trace metals that are rarely studied but have special toxicity,including tin(Sn),antimony(Sb),gold(Au),hafnium(Hf),palladium(Pd),platinum(Pt),ruthenium(Ru),tellurium(Te)and iridium(Ir).We investigated trace metals residues and distribution characteristics,and further evaluated the potential health risks from major daily food intakes in 33 cities in ***,Sb,Ir,Hf,and Au were frequently detected in food samples with the concentrations ranged from ND(not detected)to 24.78μg/kg ww(wet weight).Eggs exhibited the highest residual level of all detected metals(13.70±14.70μg/kg ww in sum),while the lowest concentrations were observed in vegetables(0.53±0.17μg/kg ww in sum).Sn accounting for more than 50%of the total trace metals concentration in both terrestrial and aquatic animal origin *** terrestrial plant origin foods,Sn and Ir were the most abundant *** and Au were the most abundant elements in egg *** addition,Sb and Ir showed a clear trophic dilution effect in terrestrial environments,while in aquatic ecosystems,Sn,Hf,and Au exhibited obvious trophic amplification *** calculated average estimated daily intake(EDI)via food consumption in five regions of China was 0.09μg/(kg·day),implying the health risk of aforementioned elements was acceptable.

关键词： Trace metals Accumulation characteristics Dietary exposure Estimated daily intake(EDI)

Effects of small molecules on neurogenesis:Neuronal proliferation and differentiation

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Acta Pharmaceutica Sinica B 2024年第1期14卷 20-37页

作者： MichałK Jastrze˛bski Piotr Wo´jcik Piotr Ste˛pnicki Agnieszka A.Kaczor Department of Synthesis and chemical Technology of pharmaceutical Substances with Computer Modeling Laboratory Medical University of LublinFaculty of PharmacyLublin PL-20093Poland School of Pharmacy University of Eastern FinlandKuopio FI-70211Finland

Neurons are believed to be non-proliferating ***,neuronal stem cells are still present in certain areas of the adult brain,although their proliferation diminishes with *** as with other cells,their proliferation and differentiation are modulated by various *** mechanisms are foundational to the strategies developed to induce neuronal proliferation and differentiation,with potential therapeutic applications for neurodegenerative *** most common among these diseases are Parkinson's disease and Alzheimer's disease,associated with the formation ofβ-amyloid(Aβ)aggregates which cause a reduction in the number of *** such as LiCl,4-aminothiazoles,Pregnenolone,ACEA,harmine,D2AAK1,methyl 3,4-dihydroxybenzoate,and shikonin may induce neuronal proliferation/differentiation through the activation of pathways:MAPK ERK,PI3K/AKT,NFκB,Wnt,BDNF,and ***,combinations of these compounds can potentially transform somatic cells into *** transformation process involves the activation of neuron-specific transcription factors such as NEUROD1,NGN2,ASCL1,and SOX2,which subsequently leads to the transcription of downstream genes,culminating in the transformation of somatic cells into *** diseases are not the only conditions where inducing neuronal proliferation could be ***,the impact of pro-proliferative compounds on neurons has also been researched in mouse models of Alzheimer's disease.

关键词： Neurogenesis Proliferation Differentiation Maturation Small-molecules Drug coctail Alzheimer’s disease Parkinson’s disease

Removal and fluorescence detection of antibiotics from wastewater by layered double oxides/metal-organic frameworks with different topological configurations

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Chinese chemical Letters 2024年第8期35卷 401-405页

作者： Zhiqiang Liu Qiang Gao Wei Shen Meifeng Xu Yunxin Li Weilin Hou Hai-Wei Shi Yaozuo Yuan Erwin Adams Hian Kee Lee Sheng Tang School of Environmental and chemical Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China National Medical Products Administration Key Laboratory for Impurity Profile of chemical Drugs Nanjing 210019China chemical Drug Inspection Laboratory 2 Jiangsu Institute for Food and Drug ControlNanjing 210019China Department of pharmaceutical and Pharmacological Sciences Pharmaceutical AnalysisKU LeuvenHerestraat 49O&N2PB 923Leuven B-3000Belgium Department of Chemistry National University of Singapore3 Science Drive 3Singapore 117543Singapore

Owing to the serious potential side-effects on the environment and human health,the rapid detection and removal of antibiotics have become an important research *** this work,four zinc-based metal-organic frameworks(MOFs)with different functional groups,i.e.,Zn-MOF,Zn-MOF-CH_(3),Zn-MOF-NO_(2),Zn-MOF-COOH,were utilized for the construction of LDO/MOF composite materials with a nickel-iron-cobalt-based layered double oxide,*** results showed that the LDO/MOF composites not only had high sensitivity in detecting sulfonamide and quinolone antibiotics,but also had an appreciable ability to adsorb them from *** maximum adsorption capacities of all the four types of LDO@Zn-MOFs to all antibiotics can at least reach 150 mg/g,and the limits of detection in relation to all four antibiotics were at least as low as 100μg/*** work suggested the dual-function extraction performance can be attributed to the synergistic effects between the LDO and the ***,the strong ferromagnetism derived from the LDO provided great convenience for the separation and regeneration of the LDO/MOF composites.

关键词： Light-emitting metal-organic frameworks Layered double oxides Antibiotics Topological configurations Fluorescence detection

Recent advances in enzyme-free and enzyme-mediated single-nucleotide variation assay in vitro

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National Science Review 2024年第05期 365-384页

作者： Erhu Xiong Pengfei Liu Ruijie Deng Kaixiang Zhang Ronghua Yang Jinghong Li Key Laboratory of chemical biology &Traditional Chinese Medicine Research Ministry of EducationCollege of Chemistry and Chemical Engineering Hunan Normal University College of Biomass Science and Engineering Healthy Food Evaluation Research CenterSichuan University School of pharmaceutical Sciences Key Laboratory of Targeting Therapy and Diagnosis for Critical Diseases Zhengzhou University Department of Chemistry Center for Bioanalytical Chemistry Key Laboratory of Bioorganic Phosphorus Chemistry& Chemical BiologyTsinghua University Beijing Institute of Life Science and Technology

Single-nucleotide variants(SNVs) are the most common type variation of sequence alterations at a specific location in the genome, thus involving significant clinical and biological information. The assay of SNVs has engaged great awareness, because many genome-wide association studies demonstrated that SNVs are highly associated with serious human diseases. Moreover, the investigation of SNV expression levels in single cells are capable of visualizing genetic information and revealing the complexity and heterogeneity of single-nucleotide mutation-related diseases. Thus, developing SNV assay approaches in vitro, particularly in single cells, is becoming increasingly in demand. In this review, we summarized recent progress in the enzyme-free and enzyme-mediated strategies enabling SNV assay transition from sensing interface to the test tube and single cells, which will potentially delve deeper into the knowledge of SNV functions and disease associations, as well as discovering new pathways to diagnose and treat diseases based on individual genetic profiles. The leap of SNV assay achievements will motivate observation and measurement genetic variations in single cells, even within living organisms, delve into the knowledge of SNV functions and disease associations, as well as open up entirely new avenues in the diagnosis and treatment of diseases based on individual genetic profiles.

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High-performance localized high-concentration electrolytes by diluent design for long-cycling lithium metal batteries

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Chinese chemical Letters 2024年第4期35卷 244-247页

作者： Zhe Wang Li-Peng Hou Qian-Kui Zhang Nan Yao Aibing Chen Jia-Qi Huang Xue-Qiang Zhang College of chemical and pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018China Beijing Key Laboratory of Green chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China

Electrolyte design is essential for stabilizing lithium metal anodes and localized high-concentration electrolyte(LHCE) is a promising one. However, the state-of-the-art LHCE remains insufficient to ensure long-cycling lithium metal anodes. Herein, regulating the solvation structure of lithium ions in LHCE by weakening the solvating power of diluents is proposed for improving LHCE performance. A diluent,1,1,2,2,3,3,4,4-octafluoro-5-(1,1,2,2-tetrafluoroethoxy) pentane(OFE), with weaker solvating power is introduced to increase the proportion of aggregates(an anion interacts with more than two lithium ions,AGG-n) in electrolyte compared with the commonly used 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether(TTE). The decomposition of AGG-n in OFE-based LHCE intensifies the formation of anion-derived solid electrolyte interphase and improves the uniformity of lithium deposition. Lithium metal batteries with OFE-based LHCE deliver a superior lifespan of 190 cycles compared with 90 cycles of TTE-based LHCE under demanding conditions. Furthermore, a pouch cell with OFE-based LHCE delivers a specific energy of 417 Wh/kg and undergoes 49 cycles. This work provides guidance for designing high-performance electrolytes for lithium metal batteries.

关键词： Lithium metal anodes Electrolyte Diluents Solid electrolyte interphase Pouch cells

Low-melting mixture solvents: extension of deep eutectic solvents and ionic liquids for broadening green solvents and green chemistry

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Green chemical Engineering 2024年第04期 409-417页

作者： Yu Chen Zhiwu Yu MOE Key Laboratory of Bioorganic Phosphorous Chemistry and chemical biology Department of ChemistryTsinghua University

Green solvents such as water and ionic liquids(ILs) are pillars of the great mansion of green chemistry and green processing. Initially proposed as a new family of ILs,deep eutectic solvents(DESs) have received fast development in the past two decades. In this contribution,DESs are reviewed critically and the concept is extended to lowmelting mixture solvents(Lo MMSs),which cover all kinds of materials including ionic compounds,molecular compounds,and metals. Six classes of Lo MMSs are proposed as the new classification system and examples are given. Finally,several thermodynamic issues concerning Lo MMSs are discussed. Two new concepts,robustness of Lo MMSs and high-entropy Lo MMSs,are proposed.

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Identification of 3-ketocapnine reductase activity within the human microbiota

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mLife 2024年第2期3卷 307-316页

作者： Xiaotong Wu Lukuan Hou Haili Zhang Yi Ma Jufang Wang Mingwei Cai Xiaoyu Tang School of biology and Biological Engineering South China University of TechnologyGuangzhouChina Institute of chemical biology Shenzhen Bay LaboratoryShenzhenChina College of Chemistry and Pharmacy Northwest A&F UniversityYanglingChina

The microbial synthesis of sulfonolipids within the human body is likely involved in maintaining human health or causing ***,the enzymes responsible for their biosynthesis remain largely *** this study,we identified and verified the role of 3-ketocapnine reductase,the third-step enzyme,in the four-step conversion of L-phosphoserine into sulfobacin B both in vivo and in *** finding builds upon our previous research into sulfonolipid biosynthesis,which focused on the vaginal bacterium Chryseobacterium gleum DSM 16776 and the gut bacterium Alistipes finegoldii DSM *** comprehensive gene mapping,we demonstrate the widespread presence of potential sulfonolipid biosynthetic genes across diverse bacterial species inhabiting various regions of the human *** findings shed light on the prevalence of sulfonolipid-like metabolites within the human microbiota,suggesting a potential role for these lipid molecules in influencing the intricate biointeractions within the complex microbial ecosystem of the human body.

关键词： 3-ketocapnine reductase capnines human microbiota sulfonolipids