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Two sandwich-type uranyl-containing polytungstates catalyze aerobic synthesis of benzimidazoles

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Rare Metals 2024年第3期43卷 1316-1322页

作者： Yu-Feng Liu Qi-Long Hu Xue-Jiao Chen Ke Li Pei Luo Guo-Ping Yang School of Chemistry and Material Science Jiangxi Province Key Laboratory of Synthetic ChemistryJiangxi Key Laboratory for Mass Spectrometry and InstrumentationEast China University of TechnologyNanchang330013China School of Environmental Science and Engineering Southern University of Science and TechnologyShenzhen518055China

Diversified synthetic strategies are extremely important for the structural diversity of uranium-containing polyoxometalates(U-POMs)and their functional ***,two sandwich-type U-POMs were reported,which are Na_(5.6)K_(6.4)[(UO_(2))(H_(2)O)(TeW_(9)O_(33))]_(2)·21H_(2)O(UTeW_(9))and Na_(8.9)K_(2.7)H_(1.19)[K_(0.79)(UO_(2))_(2.21)(PW_(9)O_(34))_(2)]·12H_(2)O(UPW_9)using in-situ strategy and lacunary precursor strategy,***_9 shows a typical Keggin-typeopen or half-sandwich configuration.

关键词： configuration expansion sandwich

Microstructure Regulation and Combustion Performance Optimization of PVDF/Al Composite Powder by Non-covalent Functionalized Graphenes

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Journal of Wuhan University of Technology(Materials Science) 2024年第4期39卷 904-911页

作者：易卓然 DENG Haoyuan QIN Mei 孙一 LUO Guoqiang State Key laboratory of Advanced Technology for Materials synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Graphene prepared by non-covalent modification of sulfonated poly(ether-ether-ketone)(SPG)was combined with polyvinylidene fluoride(PVDF)/Al to improve the PVDF/Al thermal conductivity while reducing the effect of the thermal resistance at the graphene-polymer *** regulation rule of SPG with different contents on the energy release of fluorine-containing system was *** the content of SPG is 4%,the peak pressure and rise rate of SPG/PVDF/Al composite powder during ignition reach the maximum of 4845.28 kPa and 8683.58 kPa/*** the content of SPG is 5%,the PVDF/Al composite powder is completely coated by SPG,and the calorific value of the material reachs the maximum of 29.094 kJ/*** the design and micro-control of the composite powder,the calorific value of the material can be effectively improved,but the improvement of the mass release rate still depends on the graphene content and surface modification state.

关键词： energetic materials PVDF/Al composites graphene modification energy release combustion

4-Nitrocatechol as a novel matrix for low-molecular-weight compounds in situ detection and imaging in biological tissues by MALDI-MSI

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Chinese Chemical Letters 2024年第6期35卷 486-490页

作者： Hualei Xu Manman Han Haiqiang Liu Liang Qin Lulu Chen Hao Hu Ran Wu Chenyu Yang Hua Guo Jinrong Li Jinxiang Fu Qichen Hao Yijun Zhou Jinchao Feng Xiaodong Wang Key laboratory of mass spectrometry Imaging and Metabolomics(Minzu University of China) State Ethnic Affairs CommissionBeijing 100081China College of Life and Environmental Sciences Centre for Imaging&Systems BiologyMinzu University of ChinaBeijing 100081China

Low-molecular-weight(LMW)compounds are ubiquitous in living organisms and play essential roles in biological *** direct analysis of LMW compounds in biological tissues by matrix-assisted laser desorption/ionization mass spectrometry imaging(MALDI-MSI)could provide a more comprehensive understanding of their essential ***,we evaluated 4-nitrocatechol(4-NC)as a novel positive-ion matrix for enhancing in situ detection and imaging of LMW compounds from the rat liver,brain,and germinating Chinese-yew seed by *** results showed that the 4-NC possessed remarkable features,including strong ultraviolet absorption,uniform matrix crystal,excellent chemical stability,and fewer matrix-related background *** use of 4-NC led to the successful detection of 232,218,and193 LMW compounds from the three abovementioned tissue sections,***,the use of 4-NC improved the imaging quality of LMW compounds in tissue sections through MALDI-MSI and has the potential as a matrix for MALDI tissue imaging of LMW compounds.

关键词： MALDI-MSI 4-Nitrocatechol LMW compounds In situ detection Tissue imaging

Single-cell mass spectrometry studies of drug metabolism heterogeneity and primary resistance to gefitinib in non-small cell lung cancer cells

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Chinese Chemical Letters 2024年第2期35卷 436-440页

作者： Guizhen Zhu Yaoyao Zhao Wenmei Zhang Yuanyuan Wu Yuanxing Liu Guangsheng Guo Xiayan Wang Zhihong Liu Center of Excellence for Environmental Safety and Biological Effects Beijing Key Laboratory for Green Catalysis and SeparationDepartment of ChemistryBeijing University of TechnologyBeijing 100124China Minzu University of China Beijing 100081China Key laboratory for the synthesis and Application of organic Functional Molecules College of Health Science and EngineeringHubei UniversityWuhan 430062China

Patients with epidermal growth factor receptor(EGFR)wild-type non-small cell lung cancer(NSCLC)often show primary resistance to gefitinib *** is thus necessary to study the metabolism of gefitinib in NSCLC cells to comprehensively reveal the reasons for the primary resistance of ***,we develop a platform for studying drug metabolism heterogeneity based on single-cell mass spectrometry(sDMH-scMS)by integrating living-cell electrolaunching ionization MS(ILCEI-MS)and high-performance liquid chromatography-MS(HPLC-MS)analysis,and the primary resistance of NSCLC cells to gefitinib was studied using this *** ILCEI-MS analysis showed that approximately 11.9%of NSCLC single cells contained the gefitinib metabolite M11;HPLC-MS detection diluted the intensity of M11 in subpopulations and concealed the heterogeneity of drug metabolism in tumor single *** intensity of gefitinib in EGFR wild-type A549 cells was markedly lower than in mutant PC9 cells,and the intensity of gefitinib metabolites was significantly higher than in PC9 cells,suggesting that the primary resistance of NSCLC cells is related to gefitinib ***,the combination of gefitinib and the drug-metabolizing enzyme inhibitorα-naphthoflavone was shown to overcome the primary resistance of the NSCLC ***,the results of this study are expected to be applicable for clinical drug resistance diagnosis and treatment at the single-cell level.

关键词： Single-cell mass spectrometry Drug metabolism Non-small cell lung cancer Gefitinib Primary resistance

Selective nickel-electrocatalyzed benzylic C-H oxygenation of functionalized alkyl arenes

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Chinese Chemical Letters 2024年第2期35卷 396-401页

作者： Shunyao Tang Siyi Wang Dongmei Zhang Xinxing Zhang Guang Yang Yanwei Wang Youai Qiu State Key laboratory of Elemento-organic Chemistry Frontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin 300071China College of Chemistry Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)Renewable Energy Conversion and Storage Center (RECAST)Frontiers Science Center for New Organic MatterNankai UniversityTianjin 300071China

Herein, a site-selective paired electrochemical C–H oxidation of functionalized alkyl arenes promoted by nickel catalyst is disclosed. A Ni(Ⅱ)-dioxygen species formed in situ efficiently enable the oxidation process under mild conditions with a broad substrate scope with excellent functional group compatibilities,such as free carboxylic acid, aldehyde, halogen(including aryl iodide), amide and amino acid. The use of the nickel catalyst in combination with water provides a safe, green and economical method for oxidation of a range of molecules varying in complexity and drug derivatives, demonstrating its potential application in organic synthesis and the pharmaceutical industry. Reaction outcomes and mechanistic studies revealed the key role of the in situ Ni(Ⅱ)-dioxygen species for the subsequent oxidation of C(sp^(3))–H bonds,and short-lived reactive intermediates(aryl radical cation) was rapidly captured by the combination of a bipolar ultramicroelectrode(BUME) with nano-electrospray ionization mass spectrometry.

关键词： Electrochemical C-H oxidation Functionalized alkyl arenes Paired nickel-electrocatalysis H_(2)O oxidation Ketones

mass spectrometry analysis of intact protein N-glycosylation signatures of cells and sera in pancreatic adenocarcinomas

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Journal of Zhejiang University-Science B(Biomedicine & Biotechnology) 2024年第1期25卷 51-64页

作者： Mingming XU Zhaoliang LIU Wenhua HU Ying HAN Zhen WU Sufeng CHEN Peng XIA Jing DU Xumin ZHANG Piliang HAO Jun XIA Shuang YANG Center for Clinical mass spectrometry College of Pharmaceutical SciencesSoochow UniversitySuzhou215123China School of Life Science and Technology ShanghaiTech UniversityShanghai201210China State Key laboratory of Genetic Engineering Department of BiochemistrySchool of Life SciencesFudan UniversityShanghai200438China Department of Clinical laboratory Center Zhejiang Provincial People’s HospitalPeople’s Hospital of Hangzhou Medical CollegeHangzhou310014China

Pancreatic cancer is among the most malignant cancers,and thus early intervention is the key to better survival ***,no methods have been derived that can reliably identify early precursors of development into ***,it is urgent to discover early molecular changes during pancreatic *** aberrant glycosylation is closely associated with cancer progression,numerous efforts have been made to mine glycosylation changes as biomarkers for diagnosis;however,detailed glycoproteomic information,especially site-specific N-glycosylation changes in pancreatic cancer with and without drug treatment,needs to be further ***,we used comprehensive solid-phase chemoenzymatic glycoproteomics to analyze glycans,glycosites,and intact glycopeptides in pancreatic cancer cells and patient *** profiling of N-glycans in cancer cells revealed an increase in the secreted glycoproteins from the primary tumor of MIA PaCa-2 cells,whereas human sera,which contain many secreted glycoproteins,had significant changes of glycans at their specific *** results indicated the potential role for tumor-specific glycosylation as disease *** also found that AMG-510,a small molecule inhibitor against Kirsten rat sarcoma viral oncogene homolog(KRAS)G12C mutation,profoundly reduced the glycosylation level in MIA PaCa-2 cells,suggesting that KRAS plays a role in the cellular glycosylation process,and thus glycosylation inhibition contributes to the anti-tumor effect of AMG-510.

关键词： Pancreatic cancer Glycosylation Biomarker Glycoproteomics mass spectrometry

Catalytic behavior of Mo-Bi-Fe-Co-K-M-O(M=Ce,Gd,CeGd)catalysts for selective oxidation of isobutene

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Journal of Rare Earths 2024年第1期42卷 84-93,I0003页

作者： Qinghui Li Huahua Zhao Jian Yang Jun Zhao Liang Yan Huanling Song Lingjun Chou State Key laboratory for Oxo synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou730000China University of Chinese Academy of Sciences Beijing100049China

The further improvement of methacrolein(MAL)selectivity from isobutene(IB)oxidation is crucial and *** this study,based on the typical Mo-Bi-Fe-Co-K-O mixed metal oxide,the rare earth element Gd-doped,Ce-doped and CeGd co-doped catalysts were prepared by co-precipitation strategy to increase the selectivity of MAL from 47.9%to 49.8%,64.2% and 68.6%,*** order to elucidate in-depth the promoting effect of Ce and/or Gd,various characterizations were utilized including X-ray diffraction patterns(XRD),Raman,X-ray fluorescence spectrometry(XRF),X-ray photoelectron spectroscopy(XPS),O_(2)-temperature programmed desorption(O_(2)-TPD),H2-temperature programmed reduction(H2-TPR),CO_(2)-temperature programmed desorption(CO_(2)-TPD),IB-temperature programmed desorption(i-C4-TPD)and in-situ IB-Fourier transform infrared spectroscopy(IB-FTIR).Both Ce and Gd finely regulate the bulk and surface structure of the catalyst,thus altering the redox ability,oxygen mobility and storage ability and *** with Ce,Gd addition slightly regulates the variation of Co^(2+)/Co^(3+)redox couples,greatly enhances the interaction among the components on the catalyst,thus only increases the content of surface oxygen species and has little effect on their *** Cecontaining catalyst performs stronger oxygen storage and migration ability,thus leading to the overproduction of surface Odefectspecies,which are proposed to be the active sites for the production of MAL and *** CeGd co-doped catalyst possesses the proper content of surface Odefectspecies,thus exhibits much higher MAL ***,the promoting mechanism of Ce and/or Gd over IB oxidation is ***,this work is helpful for understanding the influence of rare earth elements on the structure of mixed metal oxides and the olefin selective oxidation reaction.

关键词： Mixed metal oxide catalyst Rare earth element Isobutene Selective oxidation Methacrolein

A Novel Gymnosperm Wood from the Lopingian(Late Permian)in Zhangzi,Shanxi,North China and Its Paleoecological and Paleogeographic Implications

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Journal of Earth Science 2024年第1期35卷 167-176页

作者： Xiao Shi Jianxin Yu Yuewu Sun Zhen Xu Hui Li College of Earth Sciences Jilin UniversityChangchun 130061China International Center of Future Science Dinosaur Evolution Research CenterJilin UniversityChangchun 130012China State Key laboratory of Biogeology and Environmental Geology School of Earth SciencesChina University of GeosciencesWuhan 430074China Research Center of Palaeontology and Stratigraphy Jilin UniversityChangchun 130026China Jiangxi Key laboratory for mass spectrometry and Instrumentation East China University of TechnologyNanchang 330013China

The Permian-Triassic transition saw extreme climatic changes that severely impacted the terrestrial *** plants,particularly fossil woods,are sensitive to climatic changes,and they,therefore,are unique materials revealing extreme environmental and climatic changes on land at that *** conifer woods were discovered in the Lopingian(Late Permian)strata of the Sunjiagou Formation in Shanxi Province,North *** newly finding permineralized woods record the unique landscape of Lopingian North *** represent a new conifer genus and species:Shanxiopitys zhangziensis *** *** of growth pattern and anatomical characteristics of the fossil woods indicate these trees grew under optimal growing conditions,and without seasonal growth ***,climate signals from leaf fossils,vertebrate fossils and sedimentary evidences indicate a strongly seasonal climate in North China during the ***,it is speculated that these trees likely lived in the gallery forests,which were distributed along the paleo-rivers within a seasonal landscape in the central North China block during the Lopingian.

关键词： Shanxiopitys zhangziensis gen.et sp.nov. wood ecology geography gallery forest Lopingian North China

Single-atom Zn confined in hierarchical hollow microstructure as an acid/base-resistant microwave absorption materials

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Nano Research 2024年第8期17卷 6785-6794页

作者： Yue Lou Jiao Li Xiaokun Li Zhenyu Zhu Zhan Shi Biao Xu School of Chemistry and Chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China State Key laboratory of Inorganic synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China

Developing acid/base-resistant and low-price microwave-absorbing materials with lighter weight is highly desired for practical applications in extreme ***,we demonstrate the successful synthesis of the N-doped porous carbon(NC)material with hierarchical pore structure by the spray pyrolysis *** large specific surface area(SBET=707.53 m^(2)·g^(−1))of materials enables multiple scattering of incident electromagnetic waves,and N doping greatly enhances the electrical conductivity of the ***,single-atom Zn can adjust the local electronic structure of adjacent sites such as carbon and nitrogen atoms,induce the center of polarization,and thus change the dielectric and electronic properties of the host *** porous carbon coating of single-atom Zn avoids the deterioration of electromagnetic parameters caused by the accumulation of magnetic particles under high-temperature *** the same time,they can also be used in various complex environments,such as acidic and basic ***,NC-1000,with high surface area,low density,and good chemical stability,obtained a minimum reflection loss(RLmin)of−50.5 dB and an effective absorption bandwidth(EAB)exceeding 5.1 GHz at the thickness of 1.9 *** soaking in the strong acid and base solution,the electromagnetic wave absorption performance of the material decreased bymass production for this novel type of materials.

关键词： hierarchical hollow microstructure microwave absorption metal-organic framework(MOF) impedance matching singleatom Zn acid/base-resistant