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Structural insight into palladium-nickel clusters over mordenite zeolite for carbene-insertion reaction

FRONTIERS OF CHEMICAL SCIENCE AND EngINEERIng 2024年第9期18卷 104-0页

作者： Li, Guangchao Ho, Ping-Luen Baron ng, bryan kit yue Wu, Tai-Sing Rymarz, Pawel Tsang, Shik Chi Edman Hong Kong Polytech Univ Dept Appl Biol & Chem Technol Hong Kong 999077 Peoples R China Univ Oxford Dept Chem Oxford OX1 3QR England Synchrotron Radiat Res Ctr Hsinchu 30076 Taiwan

The advancement of heterogeneous catalysts incorporating metal clusters in the nanometric size range has garnered significant attention due to their extraordinary catalytic activity and selectivity. The detailed characterization and understanding of the atomic structure of these metal clusters within catalysts is crucial for elucidating the underlying reaction mechanisms. In the present study, a distinctive three-atom PdNi cluster, characterized by two Pd atoms at terminal positions and a central Ni atom, was synthesized over mordenite zeolite. The presence of atomic PdNi clusters within the eight-membered ring side pocket area was confirmed by multiple advanced analytical techniques, including magic-angle spinning nuclear magnetic resonance spectroscopy, synchrotron X-ray powder diffraction, extended X-ray absorption fine structure spectroscopy, and high-angle annular dark-field scanning transmission electron microscopy. The catalytic activity of the confined active species was examined by the carbene-mediated reactions of ethyl-2-diazoacetate to ethyl-2-methoxyacetate as a model reaction. Compared to the Pd-mordenite and Ni-mordenite, the PdNi-mordenite catalyst incorporates a PdNi cluster, which demonstrates a superior performance, achieving 100% conversion and high selectivity under the same reaction conditions. Our study elucidates the potential of constructing bimetallic clusters in zeolites, providing valuable insights for developing new heterogeneous catalysts applicable to a wide range of catalytic processes.

关键词： zeolite metal cluster synchrotron X-ray diffraction carbene-mediated reaction CARBONYLATION ADSORPTION CATALYSTS

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Modulation doping of p-type Cu_(12)Sb_(4)S_(13)toward improving thermoelectric performance

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Journal of Materials Science & Technology 2024年第4期171卷 71-79页

作者： Khak Ho Lim Mingquan Li Yu Zhang yue Wu Qimin Zhou Qingyue Wang Xuan Yang Pingwei Liu Wen-Jun Wang Ka Wai Wong Ka Ming ng Yu Liu Andreu Cabot Institute of Zhejiang University-Quzhou Quzhou 324000China College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310007China School of Chemistry and Chemical Engineering Hefei University of TechnologyHefei 230009China Materials Research Institute The Pennsylvania State UniversityUniversity ParkPA 16802USA Ostia Technologies Limited United Kingdom Department of Chemical and Biological Engineering The Hong Kong University of Science and TechnologyClear Water BayHong KongChina ICREA Pg.Lluis Companys 23Barcelona 08010Spain Catalonia Energy Research Institute-IREC Sant Adria del BesosBarcelona 08930Spain

The commercial viability of thermoelectric(TE)devices relies heavily on two factors:cost reduction and efficiency *** this study,we first produce p-type Cu_(12)Sb_(4)S_(16-x)(x=0,3,4)using a low-temperature bottom-up approach and demonstrate Cu_(12)Sb_(4)S_(13)to show the best TE performance among the three tested ***,the TE energy conversion efficiency of Cu_(12)Sb_(4)S_(13)is further enhanced by optimizing its electronic band structure through the incorporation of small amounts of *** an optimal Te content of 5 mol%,more than a twofold increase in the TE figure of merit(zT)is *** gain insight into the mechanism of improvement on the transport properties of the mate-rial,we compare the interphase transport mechanism by incorporating nanodomains of different metals(Ag and Cu)into the Cu_(12)Sb_(4)S_(13)*** improved electrical conductivity obtained with Cu_(12)Sb_(4)S_(13)-Te nanocomposites is attributed to a charge flooding of the Cu_(12)Sb_(4)S_(13)*** contrast,excessive down-ward band-bending at the interphases of Ag/Cu metal-semiconductor drastically reduces the electrical ***,a weighted mobility(μw)analysis shows a dominant thermal activation of carri-ers in Cu_(12)Sb_(4)S_(13)-Te *** this material,a strong decrease in lattice thermal conductivity is also found,which is associated with a phonon-carrier scattering *** work shows the impor-tance of proper band-engineering in TE nanocomposites to decouple electrical and thermal transport to enhance TE performance,and the efficacy ofμw for electrical and thermal transport analysis.

关键词： Modulation doping Thermoelectric Interphase transport Charge flooding Phonon-carrier scattering

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An unusual cause of myocardial infarction in an elderly man

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Journal of geriatric cardiology : JGC 2024年第8期21卷 826-827页

作者： Shing Ching Chiu Sun yue Division of Cardiology Department of Medicine and Geriatrics United Christian Hospital Hong Kong China.

Cardiac involvement in eosinophilic granulomatosis with polyangiitis (EPGA) is increasingly recognized,but it is unusual to be the initial *** report a case of vasculitic myocardial infarction (MI) and cardiogenic shock in an elderly man caused by EPGA.A 73-year-old man presented with acute chest pain radiating to back for two *** has a history of asthma and allergic rhinitis for more than ten years well controlled by inhaled *** electrocardiogram showed sinus rhythm,right bundle-branch block and anterolateral ST-segment *** had elevated troponin T of 548 ng/L (reference:ng/L),creatine kinase of 454 IU/L (reference:39–308 IU/L)。

关键词： infarction involvement elevated

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An unusual cause of myocardial infarction in an elderly man

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Journal of Geriatric Cardiology 2024年第08期 826-827页

作者： Shing Ching Chiu Sun yue Division of Cardiology Department of Medicine and Geriatrics United Christian Hospital

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Impact of inorganic and organic pollutants from a Belgian wastewater treatment plant on adjacent surface and groundwaters

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Frontiers of Environmental Science & Engineering 2024年第4期18卷 75-90页

作者： Mingyue Luo Yiqi Su Delphine Jenny Vandeputte Yuwei Jia Guanlei Li Willy Baeyens Marijke Huysmans Marc Elskens yue Gao Analytical Environmental and Geo-Chemistry Department(AMGC)Vrije Universiteit Brussel(VUB)Pleinlaan 21050 BrusselsBelgium Hydrology and Hydraulic Engineering(HYDR) Vrije Universiteit Brussel(VUB)Pleinlaan 21050 BrusselsBelgium

Under the pressure of global droughts and water shortage,it is essential to evolve toward a sustainable and robust water *** possible avenue is the maximum reuse of treated wastewater,but the quality of which determines its ***,inorganic(Cd,Pb,Cr,Ni,Cu,and As)and organic(xenoestrogens and polycyclic aromatic contaminants,PACs)contaminants were monthly monitored in an effluent of the wastewater treatment plant(WWTP),the surrounding surface waters and the local groundwater in *** and particulate concentrations of inorganic contaminants in these water bodies were *** addition,Diffusive Gradients in Thin-films(DGT)was used in situ to obtain bioavailable metal *** the WWTP effluent and surface waters,only Ni exceeds the Annual Average-Environmental Quality Standard(AA-EQS),while in the groundwater,dissolved As was the predominant ***,in the surface and effluent waters the highest lability degrees were observed for Cd and *** concentrations of these metal species in the effluent water were lower than in the other water ***-organic pollutants,xenoestrogens and PACs were analyzed by dual Estrogen and Aryl hydrocarbon Receptor-Chemical Activated LUciferase gene eXpression(ER&AhR-CALUX)*** the annual averaged(AA)bioequivalent concentration of E2(0.18 ng/L)is below the AA-EQS standard(0.4 ng/L),and the bioequivalent concentration of benzo[a]pyrene never exceeded the maximum admissible concentration(MAC),the reclamation and reuse of treated wastewater for groundwater replenishment and agricultural irrigation should pose no environmental problems,at least in a short-term.

关键词： Metal contaminants DGT Labile metal fractions ERE/AhR-CALUX BEQ Xenoestrogens and polycyclic aromatic contaminants

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Chemical profiling of principle active and toxic constituents in herbs containing aristolochic acids

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Chinese Herbal Medicines 2024年第2期16卷 293-300页

作者： Lijun yue Kaijun Yang Feng Jiang Shuai Dong Kang Yang Dan Zhu School of Pharmacy Minzu University of ChinaBeijing 100081China Key Laboratory of Ethnomedicine Ministry of Education Minzu University of ChinaBeijing 100081China Hospital of Minzu University of China Beijing 100081China

Objective:To clear the amounts of the principal active/toxic components in herbs containing aristolochic acids(HCAAs),which are still used as medicine and/or seasoning in many ethnic minority areas of ***:In this study,six major active and toxic components in HCAAs were extracted with ultrasonic *** 6-O-methyl guanosine as internal standard,the target compounds were analyzed qualitatively and quantitatively by using ultrahigh performance liquid chromatography-electrospray ionization-tandem mass spectrometry(UPLC-ESI-MS/MS)with multiple reaction monitoringinformation dependent acquisition-enhanced production ion scanning mode(MRM-IDA-EPI)combined with dynamic background subtraction(DBS)***:The method showed good linearity in the linear range of the six *** limit range of detection was from 0.01 ng/mL to 0.27 ng/*** of the detection repeatability,extraction repeatability and accuracy of the method were *** extraction,the samples remained stable at 15℃ within 24 *** analytes were all found in samples except aristolactam(AL)in sample 2,and the contents varied *** contents of these compounds decreased in fruits,leaves and stems of Aristolochia delavayi ***:This method has the advantages of less sample dosage,simple operation,short analysis cycle,high sensitivity,specificity and *** laid a good foundation for guiding the safety of HCAAs,the indepth study of pharmacological and toxicological effects and the scientific and standardized processing and compatibility of HCAAs.

关键词： aristolactam aristolochic acids chemical profiling herbs containing aristolochic acids ultrahigh performance liquid chromatography-electrospray ionizationtandem mass spectrometry(UPLC-ESI-MS/MS)

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Molecular Characteristics of Cephalosporin-Resistant Neisseria gonorrhoeae Strains in China:A Retrospective Study

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International Journal of Dermatology and Venereology 2024年第2期7卷 78-83页

作者： Jin Zhang Xiao-Yu Zhu Jing-Wei Liu yue-Ping Yin Shao-Chun Chen Reference Laboratory for STD Control Hospital for Skin Diseases(Institute of Dermatology)Chinese Academy of Medical Sciences&Peking Union Medical CollegeNanjingJiangsu 210042China National Center for STD Control Chinese Center for Disease Control and PreventionNanjingJiangsu 210042China

Objective:An increasing level of antimicrobial resistance to extended-spectrum cephalosporins has been reported,so we conducted this study to investigate the molecular characteristics of cephalosporin resistant Neisseria gonorrhoeae(ng)strains isolated from China Gonococcal Antimicrobial Resistance Surveillance Programme(China-GRSP).Methods:In total,2,038 ng isolates were collected from the China-GRSP between 2015 and *** multiantigen sequence typing(ng-MAST),multilocus sequence typing(MLST),and ng sequence typing for antimicrobial resistance(ng-STAR)were used to determine characteristics and resistant determinants of cephalosporin-resistant *** results are described as ***:Seventy-four(3.6%)cephalosporin-resistant isolates were ***_(ST7363)was the most prevalent MLST among cefixime-resistant(CFX-R)isolates,whereas MLST_(ST7365)(n=8)in was the most prevalent sequence type among ceftriaxone-resistant(CRO-R)***-R strains were mainly associated with penA-X(n=27,44.3%),penA-XIII(n=6,9.8%),penA-XVIII(n=5,8.2%),and CRO-R strains were mainly related to penA-XVIII(n=10,25.6%),penA-43(n=9,23.1%),penA-XIII(n=7,17.9%).Conclusion:The main conclusion of this study is that the predominant cephalosporin-resistant clones in China include locally emerged and imported *** CFX-R and CRO-R strains are primarily related to penA mutations,and their predominant genotypes are *** the increase in international travel,tracking high-risk-resistant clones and identifying outbreaks and their associations with epidemiological characteristics are critical to improve public health.

关键词： gonorrhea resistance cephalosporin cefixime ceftriaxone

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N-doped hollow carbon nanospheres embedded in N-doped graphene forming a three-dimensional interconnected layered porous support loaded with palladium nanoparticles as an efficient electrocatalyst for formic acid oxidation

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新型炭材料(中英文) 2024年

作者： FAng yue YAng Fu-kai QU Wei-li DEng Chao WAng Zhen-bo Key Laboratory of Photochemical Biomaterials and Energy Storage Materials Shenzhen Key Laboratory of Special Functional Materials Shenzhen Engineering Laboratory for Advance Technology of Ceramics Guangdong Research Center for Interfacial Engineering of Functional Materials College of Materials Science and Engineering Shenzhen University MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering State Key Lab of Urban Water Resource and Environment Harbin Institute of Technology College of Chemistry and Chemical Engineering Harbin Normal University No.1 Normal University South Road

The efficient electrocatalysts with low cost, high activity and good durability plays a crucial role in the application of direct formic acid fuel cells. Herein, Pd nanoparticles supported on N-doped hollow carbon nanospheres (NHCN) embedded in Ndoped graphene (ng) with three-dimensional (3D) layered porous configuration by a simple and economical method were investigated as direct formic acid fuel cell catalysts. Owing to the unique 3D interconnected layered porous configuration doped with nitrogen atoms, Pd/NHCN@ng catalyst with smaller Pd nanoparticle size shows large catalytic active surface area, superior electrocatalyticactivity,highsteady-statecurrentdensity,strongabilitytoresistCOpoisoning,farsurpassingthoseofconventionalPd/C,Pd/ng,andPd/***/GOratio,itisfoundthatwhenthe HCN/GO mass ratio is 1∶1, Pd/NHCN@ng catalyst has the most outstanding performance in catalytic oxidation of formic acid,with an activity 4.21 times that of Pd/C. This work has developed a superior carbon-based support material for electrocatalysts, which brings broad application prospects for the development of fuel cells.

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Molecular compositions and sources of organic aerosols at a rural site on the Guanzhong Plain,Northwest China:The importance of biomass burning

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Particuology 2024年第6期89卷 44-56页

作者： Yali Liu Minxia Shen Haijiao Liu Wenting Dai Weining Qi Yifan Zhang Lu Li yue Cao Xin Wang Xiao Guo Yingkun Jiang Jianjun Li State Key Laboratory of Loess and Quaternary Geology Key Lab of Aerosol Chemistry and PhysicsInstitute of Earth EnvironmentChinese Academy of SciencesXi'an 710061China Xi'an Institute for Innovative Earth Environment Research Xi'an 710061China National Observation and Research Station of Regional Ecological Environment Change and Comprehensive Management in the Guanzhong Plain ShaanxiChina

The concentration of PM_(2.5)has considerably reduced in recent years,but remains relatively high in *** particular,the increasing contribution of organic compounds to PM_(2.5)generates popular pressure for further reductions,resulting in an urgent need to study organic aerosol(OA).To investigate the molecular composition and source contribution of OA in the rural area of the Guanzhong Plain,Northwest China,PM_(2.5)samples were collected during 3–23 August 2016 and 5–20 January 2017 and studied for more than 100 organic tracer *** mean concentration of total measured organic compounds is 662±296 ng/m^(3)in summer and 3258±1925 ng/m^(3)in *** is the most abundant single compound found throughout the sampling period,which is a crucial tracer for biomass burning emissions,preliminary suggesting that biomass burning is an essential source of *** summer,organic compounds such as lipid compounds,sugar compounds,and polycyclic aromatic hydrocarbons(PAHs),more come from higher plants,wood burning,vehicle exhausts,plastic waste,and other direct emission *** PAHs(OPAHs),nitrophenols,and phthalic acids more come from the atmosphere through the oxidation reaction of aromatic precursors,especially photochemical ***,in winter,most of the increases in concentrations of organic compounds are attributed to biomass *** analysis of a haze event(14–19 January 2017)during the winter sampling period shows that the increases in the concentration of organic compounds are unaccompanied by strong secondary formation under lower relative humidity(49.1%±13.5%).The main reason for the growth of OA in this haze event is the accumulation of primary OA(POA).The source apportionment by the positive matrix factorization(PMF)model shows that biomass burning(37.1%)is the primary source of OA in the rural regions of the Guanzhong Plain,especially in winter(40.6%).The contribution of secondary formation decreases from 26.0%in summer t

关键词： Organic aerosol Molecular composition Seasonal variation Source apportionment Guanzhong Plain

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Impacts of angiotensin II on retinal artery changes in apolipoprotein E deficient mice

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International Journal of Ophthalmology(English edition) 2024年第1期17卷 16-24页

作者： Li-Hui Meng Shi-Yu Cheng He Chen yue-Lin Wang Wen-Fei Zhang Huan Chen Xin-Yu Zhao You-Xin Chen Department of Ophthalmology Peking Union Medical College HospitalChinese Academy of Medical SciencesBeijing 100730China Key Lab of Ocular Fundus Diseases Chinese Academy of Medical SciencesBeijing 100730China

AIM:To investigate the impacts of angiotensin II(Ang II)on retinal artery changes in apolipoprotein E deficient(apoE^(-/-))***:ApoE^(-/-)male mice were infused by minipumps with Ang II at 1000 ng/kg·min(Ang II group)or saline(control group)for *** were underwent ophthalmic fundus examination on day 0,14,and 28 of *** examination,ribonucleic acid(RNA)sequencing and local Ang II measurement of retinas were ***:Ophthalmic fundus examination showed Ang II infusion promoted the formation of retinal arterial aneurysm-like lesions on day *** coherence tomography revealed the ganglion cell and inner plexiform layer(GCIPL)thickness in the control group was significantly thinner than that in Ang II group(Png demonstrated diffused swelling of GCIPL layer and its disordered structure in Ang II *** electron microscopy showed Ang II infusion caused aggravation of atherosclerotic lesions,including increased swelling,roughness,disorganization of the retinal vasculature,and vacuoles ***-sequencing and gene ontology enrichment analysis demonstrated that the structure and function of cellular membrane might be disturbed and visual function might be compromised by Ang *** local level of Ang II was higher in Ang II infusion group but did not show significant differences compared to the control group(P=0.086).CONCLUSION:Ang II infusion promotes the formation of retinal arterial aneurysm-like lesions in apoE^(-/-)mice,causing aggravation of atherosclerotic lesions,more severe disorganization of the retinal vasculature and disturbance of the cellular membrane.

关键词： angiotensin II retinal artery aneurysm apoE^(-/-)mice

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