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Elucidating the structure-activity relationship of Cu-Ag bimetallic catalysts for electrochemical CO_(2) reduction

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Journal of Energy Chemistry 2024年第6期93卷 345-351,I0009页

作者： Qining Huang Lili Wan Qingxuan Ren Jingshan Luo Institute of Photoelectronic Thin Film Devices and Technology State Key Laboratory of Photovoltaic Materials and CellsKey Laboratory of Photoelectronic Thin Film Devices and Technology of TianjinMinistry of Education Engineering Research Center of Thin Film Photoelectronic TechnologyNankai UniversityTianjin 300350China Frontiers Science center for New organic Matter Nankai UniversityTianjin 300071China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Developing bimetallic catalysts is an effective strategy for enhancing the activity and selectivity of electrochemical CO_(2) reduction reactions,where understanding the structure-activity relationship is essential for catalyst ***,we prepared two Cu-Ag bimetallic catalysts with Ag nanoparticles attached to the top or the bottom of Cu *** tested in a flow cell,the Cu-Ag catalyst with Ag nanoparticles on the bottom achieved a faradaic efficiency of 54%for ethylene production,much higher than the catalyst with Ag nanoparticles on the *** catalysts were further studied in the H-cell and zero-gap MEA *** was found that placing the two metals in the intensified reaction zone is crucial to triggering the tandem reaction of bimetallic *** work elucidates the structure-activity relationship of bimetallic catalysts for CO_(2) reduction and demonstrates the importance of considering both catalyst structures and cell characteristics to achieve high activity and selectivity.

关键词： Electrochemical CO_(2)reduction Bimetallic catalyst Cu-Ag Structure-activity relationship

Visible-light-promoted tandem decarboxylation coupling/cyclization of N-aryl glycines with quinoxalinones: Easy access to tetrahydroimidazo [1,5-a]quinoxalin-4(5H)-ones

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Green Synthesis and Catalysis 2024年第1期5卷 31-34页

作者： Zhen Tang Chao Pi Yangjie Wu Xiuling Cui Henan Key Laboratory of Chemical Biology and organic Chemistry Key Laboratory of Applied Chemistry of Henan UniversitiesGreen Catalysis CenterCollege of ChemistryZhengzhou UniversityZhengzhou450052China

A visible-light-promoted formal[2+2+1]cyclization of N-aryl glycines with quinoxalin-2(1H)-ones to synthesize tetrahydroimidazo[1,5-a]quinoxalin-4(5H)-ones have been *** protocol features operational simplicity,mild reaction conditions with blue LED light employing Ru(bpy)3Cl2.6H2O as a photoredox catalyst,a combination of O2 from air and Cu(OAc)2 as the oxidant and broad substrate applicability.

关键词： Cyclization Decarboxylation Visible-light-promoted Quinoxalin-2(1H)-ones Mild conditions

Soybean maize strip intercropping:A solution for maintaining food security in China

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Journal of Integrative Agriculture 2024年第7期23卷 2503-2506页

作者： Jiang Liu Wenyu Yang Sichuan Engineering Research center for Crop Strip Intercropping System/Key Laboratory of Crop Ecophysiology and farming System in Southwest Ministry of Agriculture and Rural AffairsChengdu 611130China College of Life Science Sichuan Agricultural UniversityYa’an 625014China State Key Laboratory of Crop Gene Exploration and Utilization in Southwest China Chengdu 611130China

The practice of intercropping leguminous and gramineous crops is used for promoting sustainable agriculture,optimizing resource utilization,enhancing biodiversity,and reducing reliance on petroleum ***,promoting conventional intercropping strategies in modern agriculture can prove *** innovative technology of soybean maize strip intercropping(SMSI)has been proposed as a *** system has produced remarkable results in improving domestic soybean and maize production for both food security and sustainable *** this article,we provide an overview of SMSI and explain how it differs from traditional *** also discuss the core principles that foster higher yields and the prospects for its future development.

关键词： strip intercropping food security soybean maize spatial arrangement

Dynamically switchable porphyrin-based molecular tweezer for on-off fullerene recognition

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Chinese Chemical Letters 2024年第6期35卷 283-287页

作者： Zhimin Sun Xin-Hui Guo Yue Zhao Qing-Yu Meng Li-Juan Xing He-Lue Sun College of Chemistry and Materials Science Hebei Key Laboratory of Organic Functional MoleculesHebei Normal UniversityShijiazhuang 050024China

Herein,a novel molecular tweezer based on 2,2'-bipyridine-bridged porphyrin subunits was constructed for efficient fullerenes *** syn conformation of the molecule,which was obtained by Zn(Ⅱ)coordination,gives rise to a proper cavity to interact with fullerene guests to form a stable 1:1 complex in toluene *** exhibits distinct binding selectivity towards C_(60)over C_(70).Moreover,the fullerene recognition capacity can be adequately suppressed by importing H_(2)PO_(4)^(-)to competitively capture Zn(Ⅱ)along with syn-anti conformational ***,the molecular tweezer regenerated to bind the fullerene by introducing the Ca^(2+)into the ***,the association-disassociation process can be switched reversibly and repeatedly.

关键词： Molecular tweezer Fullerene recognition Supramolecular chemistry Conformation conversion Coordination

Isocyanide-Based One-Pot Cascade Synthesis of 3-Acyl Isoindolinones

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Chinese Journal of Chemistry 2024年第3期42卷 259-263页

作者： Jia Liu Yi-Ming Zhu Xiao-Ping Xu Shun-Jun Ji Key Laboratory of organic Synthesis of Jiangsu Province College of ChemistryChemical Engineering and Materials Science & Collaborative Innovation Center of Suzhou Nano Science and TechnologySoochow UniversitySuzhouJiangsu215123 China Suzhou Baolidi Functional Materials Research Institute SuzhouJiangsu215144 China

A series of 3-acyl-substituted isoindolinone derivatives were synthesized in a one-pot manner via the reaction of o-bromobenzaldehydes,isocyanides,and carboxylic acids in the presence of palladium catalyst and base. The reaction employing easily available starting materials features simple operation and high efficiency. The mechanistic study showed that the reaction might undergo 1) Pd-catalyzed [3+2] cyclization of o-bromobenzaldehyde with isocyanide and the re-insertion of another molecule of isocyanide,2) addition of carboxylic acid to in situ formed ketenimine followed by a rearrangement relay to give 3,3-diacyl-substituted isoindolinone derivative. Further transformations of the obtained products through decarbonylation could also be realized.

关键词： One-pot reaction Isocyanide Pd catalysis Rearrangement reaction Isoindolinone

A Transparent Photoresist Made of Titanium Dioxide Nanoparticle-Embedded Acrylic Resin with a Tunable Refractive Index for UV-Imprint Lithography

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Engineering 2024年第6期37卷 96-104页

作者： Yinglu Liu Dan Wang Changlin Liu Qianqian Hao Jian Li Jie-Xin Wang Xiuyun Chen Peng Zhong Xibin Shao Jian-Feng Chen State Key Laboratory of organic–Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Research center of the Ministry of Education for High Gravity Engineering and Technology Beijing University of Chemical TechnologyBeijing 100029China BOE Technology Group Co. Ltd.Beijing 100176China

Transparent photoresists with a high refractive index(RI)and high transmittance in visible wavelengths have promising functionalities in optical *** work reports a kind of tunable optical material composed of titanium dioxide nanoparticles embedded in acrylic resin with a high RI for ultraviolet(UV)-imprint *** hybrid film exhibits a tunable RI of up to 1.67(589 nm)after being cured by UV light,while maintaining both a high transparency of over 98%in the visible light range and a low haze of less than 0.05%.The precision machining of optical microstructures can be imprinted easily and efficiently using the hybrid resin,which acts as a light guide plate(LGP)to guide the light from the side to the top in order to conserve the energy of the display *** preliminary studies based on both laboratory and commercial experiments pave the way for exploiting the unparalleled optical properties of nanocomposite resins and promoting their industrial application.

关键词： Photoresist Tunable refractive index Hanson solubility Ultraviolet imprint organic-inorganic composites

Synergistic silver-mediated and palladium-catalyzed nondirected olefination of aryl C–H bond: quick access to multi-substituted aryl olefins

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Science China Chemistry 2024年第3期67卷 882-889页

作者： Jian Yao Lili Shao Xiaohong Huo Xiaoming Wang Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Frontiers Science Center for Transformative MoleculesSchool of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Organometallic Chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 20032China School of Chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China

Transition metal-catalyzed olefination of aryl C-H bond is a powerful tool for the synthesis of alkenes. While the Pd-catalyzed oxidative C-H olefination of arenes, also known as Fujiwara-Moritani reaction, has been established as one of the most efficient methods, the substrates are largely limited to terminal olefins with electron-withdrawing group(s). Herein, we report a synergistic silver-mediated and palladium-catalyzed non-directed C-H olefination of arenes with vinyl(pseudo)halides, which offers a complementary strategy to the typical Fujiwara-Moritani reaction. The reactions proceeded well for a variety of halogenated arenes, heteroarenes, and olefin substrates, providing an efficient access to various multi-substituted aryl olefins, including trisubstituted/tetrasubstituted olefins and several complex olefins derived from medicines or natural products. Mechanistic studies indicated a bimetallic Pd/Ag cooperation is operative in the catalysis, i.e., the reaction is initiated by aryl C-H bond cleavage via ligation with phosphine/Ag species, followed by transferring of the aryl moiety to a vinyl palladium intermediate,which is in turn formed by oxidative addition of vinyl(pseudo)halide to a Pd complex. This method enables the synthesis of a wide range of challenging multi-substituted vinyl products from simple arenes(directing-group free) in a streamlined and controllable fashion.

关键词： direct C–H olefination multi-substituted aryl alkenes bimetallic Pd/Ag cooperation C–H functionalization

5S-Heudelotinone alleviates experimental colitis by shaping the immune system and enhancing the intestinal barrier in a gut microbiota-dependent manner

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Acta Pharmaceutica Sinica B 2024年第5期14卷 2153-2176页

作者： Qing Meng Jianshuang Guo Ke Lv Yang Liu Jin Zhang Mingyue Li Xirui Cheng Shenghua Chen Xiaoguang Huo Quan Zhang Yue Chen Jing Li State Key Laboratory of Medicinal Chemical Biology College of PharmacyNankai UniversityTianjin 300353China College of Chemistry and Frontiers Science center for New organic Matter Haihe Laboratory of Sustainable Chemical TransformationsNankai UniversityTianjin 300071China Accendatech Company Ltd.Tianjin 300193China

Aberrant changes in the gut microbiota are implicated in many diseases,including inflammatory bowel disease(IBD).Gut microbes produce diverse metabolites that can shape the immune system and impact the intestinal barrier integrity,indicating that microbe-mediated modulation may be a promising strategy for preventing and treating *** fecal microbiota transplantation and probiotic supplementation are well-established IBD therapies,novel chemical agents that are safe and exert strong effects on the gut microbiota are urgently ***,we report the total synthesis of heudelotinone and the discovery of 5S-heudelotinone(an enantiomer)as a potent agent against experimental colitis that acts by modulating the gut microbiota.5S-Heudelotinone alters the diversity and composition of the gut microbiota and increases the concentration of short-chain fatty acids(SCFAs);thus,it regulates the intestinal immune system by reducing proinflammatory immune cell numbers,and maintains intestinal mucosal integrity by modulating tight junctions(TJs).Moreover,5S-heudelotinone(2)ameliorates colitis-associated colorectal cancer(CAC)in an azoxymethane(AOM)/dextran sulfate sodium(DSS)-induced in situ carcinoma ***,these findings reveal the potential of a novel natural product,namely,5S-heudelotinone,to control intestinal inflammation and highlight that this product is a safe and effective candidate for the treatment of IBD and CAC.

关键词： 5S-heudelotinone Total synthesis Inflammatory bowel disease Gut microbiota Short-chain fatty acids Immune system Intestinal barrier Drug discovery

All‑Covalent organic Framework Nanofilms Assembled Lithium‑Ion Capacitor to Solve the Imbalanced Charge Storage Kinetics

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Nano-Micro Letters 2024年第6期16卷 246-260页

作者： Xiaoyang Xu Jia Zhang Zihao Zhang Guandan Lu Wei Cao Ning Wang Yunmeng Xia Qingliang Feng Shanlin Qiao College of Chemistry and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018People’s Republic of China School of Chemistry and Chemical Engineering Northwestern Polytechnical UniversityXi’an 710072People’s Republic of China Hebei Engineering Research center of organic Solid Photoelectric Materials for Electronic Information Shijiazhuang 050018People’s Republic of China

Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in *** development of these nanofilms offers a promising solution to address the persistent challenge of imbalanced charge storage kinetics between battery-type anode and capacitor-type cathode in lithium-ion capacitors(LICs).Herein,for the first time,custom-made COFBTMB-TP and COFTAPB-BPY nanofilms are synthesized as the anode and cathode,respectively,for an all-COF nanofilm-structured *** COFBTMB-TP nanofilm with strong electronegative–CF3 groups enables tuning the partial electron cloud density for Li^(+) migration to ensure the rapid anode kinetic *** thickness-regulated cathodic COFTAPB-BPY nanofilm can fit the anodic COF nanofilm in the *** to the aligned 1D channel,2D aromatic skeleton and accessible active sites of COF nanofilms,the whole COFTAPB-BPY//COFBTMB-TP LIC demonstrates a high energy density of 318 mWh cm^(−3) at a high-power density of 6 W cm^(−3),excellent rate capability,good cycle stability with the capacity retention rate of 77%after *** COFTAPB-BPY//COFBTMB-TP LIC represents a new benchmark for currently reported film-type LICs and even film-type *** being comprehensively explored via ex situ XPS,7Li solid-state NMR analyses,and DFT calculation,it is found that the COFBTMB-TP nanofilm facilitates the reversible conversion of semi-ionic to ionic C–F bonds during lithium ***-TP exhibits a strong interaction with Li^(+) due to the C–F,C=O,and C–N bonds,facilitating Li^(+) desolation and absorption from the *** work addresses the challenge of imbalanced charge storage kinetics and capacity between the anode and cathode and also pave the way for future miniaturized and wearable LIC devices.

关键词： Covalent organic frameworks Lithium-ion capacitor Charge storage kinetic