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Self-separation ionic liquid catalyst for the highly effective conversion of H2S by α,β-unsaturated carboxylate esters under mild conditions

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Green Energy & Environment 2024年第9期9卷 1440-1448页

作者： Wenjie Xiong Xiaomin Zhang Xingbang Hu Youting Wu Key Laboratory of Mesoscopic chemistry of MOE School of Chemistry and Chemical Engineering Nanjing University The Institute of Green chemistry and Engineering School of Chemistry and Chemical Engineering Nanjing University

The deep-processing utility of pure hydrogen sulfide （H2S） is a significant direction in natural gas chemical ***,a brand-new strategy of H2S conversion by a,β-unsaturated carboxylate esters into thiols or thioethers using task-specific carboxylate ionic liquids （ILs） as catalyst has been developed,firstly accomplishing the phase separation of product and catalyst without introducing the third *** can be considered as a cascade reaction in which the product selectivity can be controlled by adjusting the molar ratio of H2S to a,β-unsaturated carboxylate ***,the effects of ILs with different anions and cations,intermittent feeding operations,as well as pressure-time kinetic behaviors on cascade reaction were ***,the proposed interaction mechanism of H2S conversion using butyl acrylate catalyzed by[Emim][Ac]was revealed by DFT-based theoretical *** approach enables the self-phase separation promotion of catalyst and product and achieves 99%quantitative conversion under mild conditions in the absence of solvent,making the entire process ecologically ***-efficiency reaction activity can still be maintained after ten cycles of the ***,the good results,combined with its simplicity of operation and the high recyclability of the catalyst,make this green method environmentally friendly and *** is anticipated that this self-separation method mediated by task-specific ILs will provide a feasible strategy for H2S utilization,which will guide its application on an industrial scale.

关键词： Ionic liquid Cascade reaction Self-separation H 2 S conversion Catalysis

Understanding the cooperative effects in the catalysis of homodimeric fluoroacetate dehalogenase

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Science China chemistry 2024年第7期67卷 2382-2391页

作者： Ke-Wei Chen Jia-Nan Chen Jun Zhang Chao Wang Tian-Yu Sun Yun-Dong Wu Key Laboratory of Computational chemistry and Drug Design State Key Laboratory of Chemical OncogenomicSchool of Chemical Biology and BiotechnologyPeking University Shenzhen Graduate SchoolShenzhen 518055China Institute of Chemical biology Shenzhen Bay LaboratoryShenzhen 518132China College of chemistry and Molecular Engineering Peking UniversityBeijing 100871China Changping Laboratory Beijing 102200China

Fluoroacetate dehalogenases(FAcD),a homodimeric enzyme,catalyzes the conversion of fluoroacetic acid to glycolic acid(GoA).It has been proved that the enzyme has a half-of-the-site ***,its catalytic(C)subunit converts the first substrate to a covalent intermediate;then,the non-catalytic(NC)subunit binds a second substrate and promotes the conversion of the intermediate in the C subunit into the final *** the release of the product,the C subunit becomes the NC subunit,and the previous NC subunit becomes the C *** elucidate the detailed mechanism behind this cooperative catalysis,we have conducted microsecond-scale MD simulations along the reaction *** simulations indicate that the substrate in the NC subunit induces W185 and Y141 adopting an open conformation in the C *** opening of W185(C)facilitates the entry of catalytic water,enhancing the catalytic activity for product formation,while the opening of Y141(C)creates an unfavorable environment for product binding,promoting its *** interaction network analysis reveals that the substrate in the NC subunit can induce conformational changes through a conserved water chain at the interface.

关键词： enzyme catalysis molecular dynamics cooperative effect pre-reaction state

Molecules for COVID-19 treatment

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Chinese Chemical Letters 2024年第7期35卷 59-65页

作者： Zhigang Zeng Changzhou Liao Lei Yu Hubei Key Laboratory of Radiation chemistry and Functional Materials School of Nuclear Technology and Chemistry&BiologyHubei University of Science and TechnologyXianning 437100China Hubei Industry Technology Research Institute of Intelligent Health Xianning 437100China school of chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China

COVID-19 is a major event with worldwide *** the beginning of the epidemic,pharmaceutical chemists have paid attention to the therapeutic effect of a variety of small molecule medicines on COVID-19 infection.A series of organic molecules are designed and found to be effective in the treatment of COVID-19 *** fact,no matter how effective they are,with the development of the COVID-19 epidemic,various small molecule medicines are gradually recognized by *** is equivalent to a good science popularization of pharmaceutical *** review aims to introduce the molecules for COVID-19 treatment on the basis of their chemical structures,synthetic methods as well as their effects.

关键词： COVID-19 Small molecule medicines "Star"drugs Chemical structure Synthetic method

Heterostructure of 2D MoSe_(2) nanosheets vertically grown on bowllike carbon for high-performance sodium storage

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Nano Research 2024年第5期17卷 4023-4030页

作者： Nianxiang Shi Guangzeng Liu Baojuan Xi Xuguang An Changhui Sun Shenglin Xiong school of chemistry and chemistry Engineering Qilu Normal UniversityJinan 250200China school of chemistry and Chemical Engineering Shandong UniversityJinan 250100China school of Mechanical Engineering Chengdu UniversityChengdu 610106China

Transition metal dichalcogenides are attractive anode materials for sodium ion batteries(SIBs)due to their high theoretical capacity and large interlayer ***,its practical application is hampered by the sluggish kinetics of Na^(+)insertion and structure collapse caused by Na^(+)insertion/***,the heterostructures of MoSe_(2) nanosheets vertically growing on bowl-like carbon(MoSe_(2)@C)are designed and prepared by a template method coupled with selenization treatment to boost storage sodium *** hollow and collapse could provide enough storage space for Na^(+)and alleviate the volume expansion during the charge/discharge ***_(2) nanosheets vertically grown on carbon could expose more active sites for adsorbing Na^(+)to enhance the utilization rate of electrode ***,building heterostructures by combining different phase components could facilitate Na^(+)diffusion and advance reaction *** from these merits,the bowl-like MoSe_(2)@C shows outstanding reversible capacity(356.8 mAh·g^(-1) after 1500 cycles at 1 A·g^(-1))and remarkable rate performance(249.9 mAh·g^(-1)10 A·g^(-1)).

关键词： MoSe_(2)nanosheets bowl-like carbon heterostructure sodium ion batteries

Biocatalytic enhancement of laccase immobilized on ZnFe_(2)O_(4) nanoparticles and its application for degradation of textile dyes

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Chinese Journal of Chemical Engineering 2024年第4期68卷 216-223页

作者： Yuhang Wei Qingpeng Zhu Weiwei Xie Xinyue Wang Song Li Zhiming Chen school of Chemical and Environmental Engineering Anhui Laboratory of Functional Coordinated Complexes for Materials Chemistry and ApplicationAnhui Polytechnic UniversityWuhu 241000China school of biology and Food Engineering Anhui Polytechnic UniversityWuhu 241000China

Efficient and convenient treatment of industrial dyeing wastewater is of great significance to guarantee human and animal *** work presented the enhanced catalytic activity at pH 3.0 of laccase immobilized on amino-functionalized ZnFe_(2)O_(4) nanoparticles(ZnFe_(2)O_(4)-laccase)and its application for the degradation of textile *** to the existence of a large number of oxygen vacancies on the surface of the ZnFe_(2)O_(4) nanoparticles,negative ions accumulated on the magnetic carriers,which resulted in a harsh optimal pH value of the ZnFe_(2)O_(4)-*** activity assays revealed that the ZnFe_(2)O_(4)-laccase possessed superior pH and thermal stabilities,excellent reusability,and noticeable organic solvent ***,the ZnFe_(2)O_(4) laccase presented efficient and sustainable degradation of high concentrations of textile *** initial decoloration efficiencies of malachite green(MG),brilliant green(BG),azophloxine,crystal violet(CV),reactive blue 19(RB19),and procion red MX-5B were approximately 99.1%,95.0%,93.3%,87.4%,86.1%,and 85.3%,*** 10 consecutive reuses,the degradation rates of the textile dyes still maintained about 98.2%,92.5%,83.2%,81.5%,79.8%and 65.9%,*** excellent dye degradation properties indicate that the ZnFe_(2)O_(4)-laccase has a technical application in high concentrations of dyestuff treatment.

关键词： ZnFe_(2)O_(4)-laccase Catalytic activity Stability and reusability Degradation of textile dye

Silvery fullerene in Ag102 nanosaucer

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National Science Review 2024年第7期11卷 158-167页

作者： Zhi Wang Yuchen Wang Chengkai Zhang Yan-Jie Zhu Ke-Peng Song Christine M.Aikens Chen-Ho Tung Di Sun school of chemistry and Chemical Engineering Shandong University Department of chemistry Kansas State University

Despite the discovery of a series of fullerenes and a handful of noncarbon clusters with the typical topology of Ih-C60, the smallest fullerene with a large degree of curvature, C20, and its other-element counterparts are difficult to isolate experimentally. In coinage metal nanoclusters（NCs）, the first all-gold fullerene, Au32, was discovered after a long-lasting pursuit, but the isolation of similar silvery fullerene structures is still challenging. Herein, we report a flying saucer-shaped 102-nuclei silver NC（Ag102） with a silvery fullerene kernel of Ag32, which is embraced by a robust cyclic anionic passivation layer of（KPO4）10. This Ag32kernel can be viewed as a non-centered icosahedron Ag12encaged into a dodecahedron Ag20, forming the silvery fullerene of Ag12@Ag20. The anionic layer（KPO4）10is located at the interlayer between the Ag32kernel and Ag70shell, passivating the Ag32silvery fullerene and templating the Ag70shell. The ~tBuPhS-and CF3COO-ligands on the silver shell show a regioselective arrangement with the 60 ~tBuPhS-ligands as expanders covering the upper and lower of the flying saucer and 10 CF3COO-as terminators neatly encircling the edges of the structure. In addition, Ag102 shows excellent photothermal conversion efficiency（η） from the visible to near-infrared region（η = 67.1% ± 0.9% at 450 nm, 60.9% ± 0.9% at 660 nm and 50.2% ± 0.5% at 808 nm）, rendering it a promising material for photothermal converters and potential application in remote laser ignition. This work not only captures silver kernels with the topology of the smallest fullerene C20, but also provides a pathway for incorporating alkali metal（M） into coinage metal NCs via M-oxoanions.

关键词： silvery fullerene >Ag102 nanosaucer cyclic anionic passivation layer photothermal conversion DFT calculation

Activatable photoacoustic bioprobe for visual detection of aging in vivo

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Chinese Chemical Letters 2024年第4期35卷 324-329页

作者： Zihong Li Jie Cheng Ping Huang Guoliang Wu Weiying Lin Institute of Optical Materials and Chemical biology Guangxi Key Laboratory of Electrochemical Energy MaterialsSchool of Chemistry and Chemical EngineeringGuangxi UniversityNanning 530004China

Aging is a natural physiological process with various challenges, related to the loss of homeostasis within the organism, which is not a disease, but a significantly strong risk factor for multiple diseases, including myocardial infarction, stroke, some age-related cancers, macular degeneration, osteoarthritis, neurodegeneration, and many others. In the body, the main manifestation of aging is cellular aging, which exists within tissues and has a local or global impact on tissue function. However, the lack of effective aging detection tools has always been an issue that cannot be ignored in the field of aging research. Therefore,it is necessary to construct a non-invasive tool for in vivo detection of aging. Here, we show that the photoacoustic probe(LGAL), which has peak excitation and emission wavelengths in the near-infrared optical window, binds in vivo and at high contrast to the hallmark of aging, and allows for the microscopic imaging of aging through the intact mice. Firstly, this tool LGAL has been successfully applied to detect senescence in cells, displaying stronger photoacoustic signals than normal cells. Then, by using the photoacoustic probe, the blood vessels and tissues inside the mice can be visualized. Young and elderly mice exhibit varying intensities of photoacoustic signals, marking the first time a probe has been used to explore the aging of blood vessels and tissues inside the mice. Finally, we monitored the changes in the degree of aging during tumor treatment under photoacoustic(PA) imaging for the first time. As the treatment time increased, the degree of aging of the tumor gradually deepened. We expect the powerful tool could be a noninvasive and powerful tool for the study of aging biology.

关键词： Near-infrared Photoacoustic Aging Senescence Tumor Sa-β-gal

Discovery of GluN2A subtype-selective N-methyl-d-aspartate(NMDA)receptor ligands

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Acta Pharmaceutica Sinica B 2024年第5期14卷 1987-2005页

作者： Liyang Jiang Na Liu Fabao Zhao Boshi Huang Dongwei Kang Peng Zhan Xinyong Liu Department of Medicinal chemistry Key Laboratory of Chemical Biology(Ministry of Education)School of Pharmaceutical SciencesCheeloo College of MedicineShandong UniversityJinan 250012China

The N-methyl-d-aspartate(NMDA)receptors,which belong to the ionotropic Glutamate receptors,constitute a family of ligand-gated ion *** the various subtypes of NMDA receptors,the GluN1/2A subtype plays a significant role in central nervous system(CNS)*** present article aims to provide a comprehensive review of ligands targeting GluN2A-containing NMDA receptors,encompassing negative allosteric modulators(NAMs),positive allosteric modulators(PAMs)and competitive ***,the ligands’structure–activity relationships(SARs)and the binding models of representative ligands are also discussed,providing valuable insights for the clinical rational design of effective drugs targeting CNS diseases.

关键词： NMDA receptors GluN2A subtype Subtype-selective ligands SARs Protein ligand interactions

Evaluating the tumor stratification with a lysosomal pH sensitive-probe by fluorescence lifetime imaging

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Chinese Chemical Letters 2024年第3期35卷 262-267页

作者： Jun Yan Xing Liang Qian Zhang Luolin Wang Weiying Lin Guangxi Key Laboratory of Electrochemical Energy Materials Institute of Optical Materials and Chemical BiologySchool of Chemistry and Chemical EngineeringGuangxi UniversityNanning 530004China

Owing to the anaerobic metabolism in the tumor,abundant acidic metabolites are produced and accumulated in the ***,the cells in different tumor layers are directly linked to the pH ***,due to the lack of robust tools,the high-efficient evaluation of the acidic micro-environment of tumor stratification faces the challenge of accurate *** designed a new pH sensitive fluorescent lifetime probe target to *** we expected,the fluorescence lifetime of PLN possesses a good linear fit to the pH value,which could detect the pH change at a single lysosome level in real time,and then evaluate the different acidity of tumor *** probe PLN is successfully used to evaluate the tumor stratification by fluorescence lifetime imaging microscopy(FLIM)for the first time,which is of great significance in the preoperative diagnosis of clinical tumor treatment or evaluation of drug delivery effect.

关键词： FLIM pH Fluorescence imaging Lysosome Tumor imaging