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Mediated electron transfer process in α-MnO_(2)catalyzed Fenton-like reaction for oxytetracycline degradation

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Chinese chemical Letters 2024年第8期35卷 367-372页

作者： Yiqian Jiang Zihan Yang Xiuru Bi Nan Yao Peiqing Zhao Xu Meng State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China University of Chinese Academy of Sciences Beijing 100049China

In Fenton-like oxidation,the catalyst directly influences the reaction mechanism for the degradation of pollutants from ***,a α-MnO_(2)catalyst(OAm-1)was synthesized via a self-assembly method with the assistance of a ***-1 possessed a large specific surface area of_(2)21 m2/g,abundant mesoporous structures and a large proportion of Mn(III).Further characterization exhibited that OAm-1 had abundant oxygen vacancies and excellent reducibility and *** adsorption and catalytic ability of OAm-1 were studied in the degradation of oxytetracycline(OTC)via the activation of hydrogen peroxide(H_(2)O_(2)).Through the radical quenching experiments,electron resonance spectroscopy(EPR),X-ray photoelectron spectroscopy(XPS)and Fourier-transform infrared spectroscopy(FT-IR)analysis,Mn(III)of OAm-1 was proved to be the active sites for the chemisorption of *** electrochemical ex-periments and analysis have shown that a process of electron transfer mediated by OAm-1 occurred be-tween the pollutant and H_(2)O_(2)during a Fenton-like *** work experimentally verifies the elec-tron transfer process dominated nonradical mechanism overα-MnO_(2),which is helpful for understanding the catalytic mechanism of the Fenton-like oxidation.

关键词： Mediated electron transfer Hydrogen peroxide Oxidative degradation Manganese oxide Fenton oxidation

Iridium-Catalyzed Site-and Enantioselective C(sp^(2))-H Borylation of Benzhydryl Ethers:Enantioselectivity Amplification by Kinetic Resolution Relay

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Chinese Journal of Chemistry 2023年第17期41卷 2119-2124页

作者： Ke Jing Lili Chen Panke Zhang Senmiao Xu State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhouGansu 730000China Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhouHenan 450001China

Comprehensive Summary,We herein report a simple ether-directed iridium-catalyzed site-and enantioselective C(sp^(2))-H borylation of benzhydryl ethers for the first *** chiral benzhydryl ethers were obtained with high enantioselectivities in the presence of a tailor-made chiral bidentate boryl *** found that the kinetic resolution relay significantly amplified the *** synthetic utility of the current method was demonstrated by gram-scale C—H borylation and C—B bond transformations.

关键词： Asymmetric catalysis Benzhydryl ethers C-H activation Enantioselectivity Kinetic resolution

Tribological behavior of shape memory cyanate ester materials and their tunable friction mechanism

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Friction 2023年第10期11卷 1794-1803页

作者： Zhangzhang TANG Lihe GUO Mingkun XU Hongwei RUAN Jing YANG Tingmei WANG Jianqiang ZHANG Qihua WANG Yaoming ZHANG Key Laboratory of Science and Technology on Wear and Protection of Materials Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China College of Petrochemical Technology Lanzhou University of TechnologyLanzhou 730050China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

High-performance polymer friction materials with tunable tribological behavior to fit varied work conditions remain a challenge of widespread interest for a variety of *** memory polymer exhibits morphing and modulus changing over temperature changing provides a promising material to adjust the friction ***,we investigated the tribological properties of shape memory cyanate ester(SMCE)under different *** SMCE exhibits the tribological behavior of good friction material with stable high coefficient of friction(COF)and a low wear ***,the COF increases and wear rate decreases with the temperature increasing show the tunable friction property of the *** propose a new model of wear-compensation through shape recovery to explain the adjustable friction behavior of thermal-responsive polymer from the aspect of shape recovery and energy *** study provides a high-performance friction material and paves the route for the application of shape memory polymer(SMP)in tribology field with tunable property.

关键词： tribological behavior shape memory polymer cyanate ester tunable friction wear rate

A confined growth strategy to construct 3DOM SiO_(2) nanoreactor insitu embedded Co_(3)O_(4) nanoparticles catalyst for the catalytic combustion of VOCs:Superior H_(2)O and SO_(2) resistance

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Nano Research 2024年第1期17卷 207-220页

作者： Weigao Han Shilin Wu Fang Dong Weiliang Han Yinghao Chu Linghui Su Zhicheng Tang State Key Laboratory for Oxo Synthesis and Selective Oxidation National Engineering Research Center for Fine Petrochemical IntermediatesLanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China University of Chinese Academy of Sciences Beijing 100049China Dalian National Laboratory for Clean Energy Dalian 116023China College of Architecture and Environment Sichuan UniversityChengdu 610000China

SO_(2)poisoning is a common problem in the catalytic combustion of volatile organic compounds(VOCs).In this work,we took three-dimensionally ordered macroporous and mesoporous(3DOM)SiO_(2)as the nanoreactor to protect active sites from SO_(2)erosion in the catalytic combustion of ***,the confined growth of metal active nanoparticles in the multi-stage pore is also full of *** we successfully confined Co_(3)O_(4)nanoparticles(NPs)in macroporous and mesoporous ***,the precursors’growth in the pore was controlled and nanoreactors with different pore sizes were prepared by adjusting the loading amount and preparation *** is discovered that the Co_(3)O_(4)NPs confined in 3DOM SiO_(2)nanoreactor showed superior sulfur and water *** functional theory(DFT)calculations verified that the Co-Si catalyst had high SO_(2)adsorption energy(-0.48 eV),which illustrated that SO_(2)was hard to attach to the surface of the Co-Si *** SiO_(2)nanoreactor had low SO_(2)adsorption energy(-5.15 eV),which indicated that SO_(2)was easily absorbed on SiO_(2)*** illustrated that the SiO_(2)nanoreactor could protect effectively active sites from SO_(2)erosion.

关键词： zeolitic imidazolate frameworks(ZIFs) Co_(3)O_(4) benzene catalytic combustion nanoreactor sulfur and water resistance

Recent progress in nanomaterial-enhanced fluorescence polarization/anisotropy sensors

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Chinese chemical Letters 2019年第9期30卷 1575-1580页

作者： Jia Chen Juewen Liu Xingguo Chen Hongdeng Qiu cas Key Laboratory of Chemistry of Northwestern Plant Resources and Key Laboratory for Natural Medicine of Gansu Province Lanzhou Institute of Chemical Physics Chinese Academy of Sciences Lanzhou 730000 China University of Chinese Academy of Sciences Chinese Academy of Sciences Beijing 10039 China Department of Chemistry Waterloo Institute for Nanotechnology University of Waterloo Waterloo Ontario N2L 3G1 Canada State Key Laboratory of Applied Organic Chemistry Lanzhou University Lanzhou 730000 China

As a promising signaling transduction approach, fluorescence polarization(FP)/fluorescence anisotropy(FA), provides a powerful quantitative tool for the rotational motion of fluorescently labeled molecules in chemical or biological homogeneous systems. Unlike fluorescence intensity, FP/FA is almost independent the concentration or quantum of fluorophores, but they are highly dependent on the size or molecular weight of the molecules or materials attached to fluorophores. Recently, significant progress in FP/FA was made, due to the introduction of some nanomaterials as FP/FA enhancers. The detection sensitivity is thus greatly improved by using nanomaterials as FP/FA enhancers, and nanomaterial-based FP/FA is currently used successfully in immunoassay, and analysis of protein, nucleic acid, small molecule and metal ***-based FP/FA provides a new kind of strategy to design fluorescent sensors and establishes innovative analytical methods. In this review, we summarize the scientific publications in the field of FP/FA sensor in recent five years, and first introduce the recent progress of FP/FA sensor based on nanomaterial. Subsequently, the various analytical applications of FP/FA based on nanomaterial are discussed. Finally, we provide perspectives on the current challenges and future prospects in this promising field.

关键词： Fluorescence polarization/anisotropy Nanomaterials Sensor Recent progress Application

Screening, structural characterization and anti-adipogenesis effect of a water-soluble polysaccharide from Lycium barbarum L. by an activity-oriented approach

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FOOD BIOSCIENCE 2023年第3期53卷 409-420页

作者： Wang, Han Li, Yunchun Dai, Yunyun Ma, Ling Di, Duolong Liu, Jianfei Chinese Acad Sci Lanzhou Inst Chem Phys CAS Key Lab Chem Northwestern Plant Resources Key Lab Nat Med Gansu Prov Lanzhou 730000 Peoples R China Ningxia Inst Drug Control Intersect Ningan Santa Yinchuan 750001 Peoples R China Chinese Acad Sci Lanzhou Inst Chem Phys Key Lab Chem Northwestern Plant Resources 18 Tianshui Middle Rd Lanzhou 730000 Peoples R China Chinese Acad Sci Lanzhou Inst Chem Phys Key Lab Nat Med Gansu Prov 18 Tianshui Middle Rd Lanzhou 730000 Peoples R China

This study aimed to describe the structural features and anti-adipogenesis effect of polysaccharides obtained from Lycium barbarum L. by a bioactivity-oriented purification method. First, crude polysaccharide LICP009 was identified as the main bioactive compound with potential inhibition of intracellular lipid accumulation. Bioac-tivity guided fractionation was further performed using ion-exchange chromatography and Sephadex G-50 to obtain the purified component LICP009-2-1. This component was mainly composed of arabinose (Ara), galactose (Gal), glucose (Glc), galacturonic acid (GalA), and glucuronic acid (GlcA) in a molar ratio of 40.2:31.5:4.2:5.8:5.7 with a molecular weight of 1.35 x 104 g/mol. Linkage and NMR data indicated that the backbone of LICP009-2-1 was consisted of a repeated unit of -> 3,6)-beta-D-Galp-(1 -> residues, with three branches composed of alpha-L-Araf-(1 ->, alpha-L-Araf-(1 -> 5)-alpha-L-Araf-(1 -> 5)-alpha-L-Araf-(1 -> 3)-beta-D-Galp-(1 ->, and alpha-L-Araf-(1 -> 2)-alpha-L-Araf-(1 ->[4)-beta-D-Galp-(1]3 -> . In differentiated 3T3-L1 adipocyte model, LICP009-2-1 exhibited an antiadipogenic effect by decreasing lipid accumulation, as well as downregulating the expression of key tran-scription factors and proteins in the adipogenesis pathway in a dose-dependent manner. In high-fat-diet-induced obese mice, oral administration of LICP009-2-1 counteracted the progression of obesity and hyperlipidemia. These results indicated that LICP009-2-1 plays anti-adipogenic and anti-obesity roles both in vitro and in vivo, and could be an anti-obesity agent utilized as medicinal, pharmacological and functional food ingredient.

关键词： Lycium barbarum L Heteropolysaccharide Anti-adipogenesis Structural characterization

Biomimetic asymmetric catalysis

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Science China Chemistry 2023年第6期66卷 1553-1633页

作者： Xiao Xiao Kaini Xu Zhong-Hua Gao Zhou-Hao Zhu Changqing Ye Baoguo Zhao Sanzhong Luo Song Ye Yong-Gui Zhou Senmiao Xu Shou-Fei Zhu Hongli Bao Wei Sun Xiaoming Wang Kuiling Ding State Key Laboratory of Organometallic Chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China The Education Ministry Key Laboratory of Resource Chemistry Shanghai Key Laboratory of Rare Earth Functional Materialsand Shanghai Frontiers Science Center of Biomimetic CatalysisShanghai Normal UniversityShanghai 200234China Center of Basic Molecular Science Department of ChemistryTsinghua UniversityBeijing 100084China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Molecular Recognition and FunctionInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China State Key Laboratory and institute of Elemento-Organic Chemistry College of ChemistryNankai UniversityTianjin 300071China Key Laboratory of Coal to Ethylene Glycol and Its Related Technology State Key Laboratory of Structural ChemistryCenter for Excellence in Molecular SynthesisFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Enzymes are the core for biological transformations in *** structures and functions have drawn enormous attention from biologists as well as chemists since last *** large demand of bioactive molecules and the pursuit of efficiency and greenness of synthesis have spurred the rapid development of biomimetic chemistry in the past several *** asymmetric catalysis,mimicking the structures and functions of enzymes,has been recognized as one of the most promising synthetic strategies for the synthesis of valuable chiral *** review summarizes the evolution of asymmetric catalysis inspired by aldolases,vitamin B_(1)/B_(6)-dependent enzymes,NAD(P)H,flavin,hydrogenases,heme oxygenases,nonheme oxygenases,and dinuclear/multinuclear metalloenzymes in aspects of biomimetic design,catalyst development and related catalytic *** well-established synthetic approaches originating from biological reactions have demonstrated the unique prowess of biomimetic asymmetric catalysis in bridging the gap between bio-catalysis and chemical synthesis.

关键词： biomimetic catalysis amine catalysis carbene catalysis vitamin Br carbonyl catalysis vitamin Bo NAD(P)H flavin biomimetic oxidation dinuclear/multinuclear metal catalysis asymmetric hydrogenation

Synthesis of biochar/clay mineral nanocomposites using oil shale semi-coke waste for removal of organic pollutants

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Biochar 2023年第1期5卷 123-143页

作者： Feng Zhao Bin Mu Tenghe Zhang Chunjuan Dong Yongfeng Zhu Li Zong Aiqin Wang Key Laboratory of Clay Mineral Applied Research of Gansu Province Center of Eco-Materials and Green ChemistryLanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhouPeople’s Republic of China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China.

Due to the poor surface/interfacial interaction and the large gaps in the size and microstructure between biomass and clay mineral,it was difficult to adjust the structure and performance of biochar/clay mineral composites at the molecular ***,oil shale semi-coke composed of multi-minerals and organic matters was used as a promising precursor to prepare biochar/clay mineral nanocomposites via phosphoric acid-assisted hydrothermal treatment followed by KOH activation for removal of organic pollutants from aqueous *** results revealed that the nanocomposites presented well-defined sheet-like morphology,and the carbon species uniformly anchored on the surface of clay *** the changes in the pore structure,surface charge and functional groups after two-step modification,the nanocomposites exhibited much better adsorption property toward organic pollutants than the raw oil shale semi-coke,and the maximum adsorption capacities of methylene blue,methyl violet,tetracycline,and malachite green were 165.30 mg g^(−1),159.02 mg g^(−1),145.89 mg g^(−1),and 2137.36 mg g^(−1),*** adsorption mechanisms involved electrostatic attraction,π-πstacking and hydrogen *** five consecutive adsorption-desorption,there was no obvious decrease in the adsorption capacity of malachite green,exhibiting good cyclic regeneration *** is expected to provide a feasible strategy for the preparation of biochar/clay mineral nanocomposites with the excellent adsorption performances for removal of organic pollutants based on full-component resource utilization of oil shale semi-coke.

关键词： Oil shale semi-coke Clay mineral Biochar nanocomposites Adsorption mechanism Solid waste resource utilization

Facile synthesis of enzyme functional metal-organic framework for colorimetric detecting H_2O_2 and ascorbic acid

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Chinese chemical Letters 2017年第5期28卷 1006-1012页

作者： Cunji Gao Hongmei Zhu Jia Chen Hongdeng Qiu Key Laboratory of Chemistry of Northwestern Plant Resources Key Laboratory for Natural Medicine of Gansu ProvinceLanzhou Institute of Chemical PhysicsChinese Academy of Sciences institute of Microbiology and Biochemical Pharmacy School of PharmacyLanzhou University

In this work,a metal-organic frameworks material MIL-88 was prepared easily using solvent-thermal method,and was first found to have catalytic activities similar to those of biological enzymes such as catalase and *** material was characterized by XRD,SEM,TEM,EDX,FT-IR techniques and an N2 adsorption *** exhibited peroxidase-like activity through catalytic oxidation of the peroxidase substrate 3,3＇,5,5＇-tetramethylbenzidine（TMB） in the presence of H2O2,producing a blue-colored *** optimal conditions,the absorbance at 652 nm is linearly correlated with the concentration of H2O2 from 2.0×10^-6 mol/L to 2.03×10^-5 mol/L（R-2=0.981） with a detection limit of 5.62×10^-7 mol/L（S/N=3）.More importantly,a sensitive and selective method for ascorbic acid detection was developed using this material as a *** analytical method for ascorbic acid detection was observed to have a linear range from 2.57×10^-6 mol/L to 1.01×10^-5 mol/L（R-2=0.989） with a detection limit of 1.03×10^-6 mol/L（S/N=3）.This work suggests MOFs have advantages of preparing biomimetic catalysts and extends applications of the functional MOFs in the field of biosensor.

关键词： Metal-organic frameworks Horseradish peroxidase H2O2 Ascorbic acid Colorimetric detection Biomimetic catalyst