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Expanded Porphyrin Exhibiting Off-Centered Out-of-Plane Coordination to Dysprosium

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CCS Chemistry 2024年第7期6卷 1731-1738页

作者： Dmitry I.Nazarov Jorge Labella Alexey V.kuzmin Maxim A.Faraonov evgenii N.Ivanov Salavat S.khasanov Tomas Torres Mikhail k.Islyaikin Dmitri V.konarev Federal Research Center of Problems of Chemical Physics and Medicinal Chemistry RAS 142432 Chernogolovka Department of Organic Chemistry Universidad Autonoma de Madrid28049 Madrid Institute of Solid-State Physics RAS 142432 Chernogolovka Research Institute of Macroheterocycles Ivanovo State University of Chemistry and Technology15300 Ivanovo G.A.krestov Institute of Solution Chemistry of the Russian Academy of Sciences 153045 Ivanovo Institute for Advanced Research in Chemical Sciences Universidad Autonoma de Madrid28049 Madrid IMDEA-Nanociencia 28049 Madrid

The complexation of high-spin lanthanides to porphyrinoids is a powerful strategy for the development of advanced molecular *** this context,the use of expanded porphyrinoids remains elusive since their coordination chemistry is challenging to ***,taking inspiration from on-surface chemistry,we explored the coordination of Dy^(3+)to a six-membered porphyrinoid,namely,the hemihexaphyrazine ***,we observed the selective formation of a mono-nuclear off-centered,out-of-plane H_(2)Hhp-Dy^(3+)complex when performing the complexation under reductive *** this reaction,the oxidation state of the macrocycle did not *** X-ray diffraction analysis,we found that the coordination number of Dy in this complex was *** macrocycle cocrystallized with decamethylcobaltocene(Cp_(2)^(*)Co)molecules,giving rise to a wellordered solid-state packing,governed byπ-π*** a result of this organization,a small magnetic coupling between the neighboring molecules was *** in all,this work provides key insights into the coordination of magnetically active metals with expanded porphyrinoids,thus motivating the development of advanced spintronic devices.

关键词： porphyrins dysprosium macrocycle coordination chemistry magnetism

Design of Biologically Active Macromolecular Ligands and Their Luminescent Complexes with Terbium Ions

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Chinese Journal of Polymer Science 2024年第5期42卷 604-611,I0007页

作者： Tatiana N.Nekrasova Andrei I.Fischer Natalia A.Nesterova Anatoliy V.Dobrodumov Anzhelika V.Garshinina Olga D.Shuvaeva Natalya V.Zakharova evgenii F.Panarin Institute of Macromolecular Compounds Russian Academy of Sciences31 Bolshoy pr.St Petersburg199004Russia Smorodintsev Research Institute of Influenza Russian Ministry of Health15/17 ul.prof.PopovaSt Petersburg197376Russia

Water-soluble copolymers of p-methacrylamidobenzoic acid(MABA)with neutral comonomers(N-vinylpyrrolidone(VP),N-methyl-N-vinylacetamide(MVAA),N-methacryloyl glucosamine(MAG))and anionic comononer sodium styrene sulfonate(NaSS)were synthesized by radical *** interactions between the prepared copolymers and Tb^(3+)ions in aqueous solutions were studied;the significant influence of chemical structure of a comonomer on luminescence intensity of Tb^(3+)complexes with the copolymers was *** luminescence intensity of Tb^(3+)complexes with the copolymers containing N-vinylamide units(VP,MVAA)is three times more intense than that observed for the complexes between Tb^(3+)and MAG-containing *** the case of NaSS-containing copolymers,the luminescence intensity is controlled by the values of binding constants between Tb^(3+)and MABA and the content of MABA units in a *** studied copolymers and their complexes with Tb^(3+)have low cytotoxicity and a pronounced antiviral activity against human respiratory syncytial virus.

关键词： Luminescence Water-soluble copolymers Lanthanide complexes Antiviral activity Cytotoxicity

In vivo real-time monitoring delayed administration of M2 macrophages to enhance healing of tendon by NIR-II fluorescence imaging

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Nano Research 2024年第5期17卷 4379-4390页

作者： Yuzhou Chen Mo Chen Chengxuan Yu Huizhu Li Liman Sai Nguyen T.k.Thanh Yueming Wang Yan Wo Jian Zhang Xing Yang evgenii L.Guryev Andrei V.Zvyagin Hao De Min Tang Shiyi Chen Yunxia Li Yuefeng Hao Sijia Feng Jun Chen Sports Medicine Institute of Fudan University Department of Sports MedicineHuashan HospitalFudan UniversityShanghai 200040China Department of Orthopedic Surgery Xinhua Hospital Affiliated to Shanghai Jiao Tong University School of MedicineShanghai 200092China Department of Bone and Joint Surgery Department of OrthopedicsRenji HospitalSchool of MedicineShanghai Jiao Tong UniversityShanghai 200001China Department of Physics Shanghai Normal UniversityShanghai 200234China Biophysics Group Department of Physics and AstronomyUniversity College LondonLondon WC1E 6BTUK UCL Healthcare Biomagnetic and Nanomaterials Laboratories London W1S 4BSUK Department of Anatomy and Physiology School of MedicineShanghai Jiao Tong UniversityShanghai 200025China Department of Orthopedics Affiliated Suzhou Hospital of Nanjing Medical UniversitySuzhou 215500China Institute of Biology and Biomedicine Lobachevsky State University of Nizhny NovgorodNizhny Novgorod 603950Russia Mathematical Institute University of OxfordOxford OX26GGUK Institute of Natural Sciences School of MathematicsShanghai Jiao Tong UniversityShanghai 200240China

The administration time is a critical but long-neglected point in cell therapy based on macrophages because the incorrect time of macrophage administration could result in diverse outcomes regarding the same macrophage *** this work,the second near-infrared(NIR-II)fluorescence imaging in vivo tracking of M2 macrophages during a pro-healing therapy in the mice model of rotator cuff injury revealed that the behavior of administrated macrophages was influenced by the timing of their *** delayed cell therapy(DCT)group had a longer retention time of injected M2 macrophages in the repairing tissue than that in the immediate cell therapy(ICT)*** keller-Segel model and histological analysis further demonstrated that DCT altered the chemotaxis of M2 macrophages and improved the healing outcome of the repaired structure in comparison with *** results offer a possible explanation of previous conflicting results on reparative cell therapy and provoke reconsideration of the timing of these therapies.

关键词： macrophage cell therapy NIR-II in vivo imaging delayed therapy tendon healing

Olefin Polymerization Behavior of Titanium(IV) Complexes with Fluorinated and Non-fluorinated Aliphatic Phenoxyimine Ligands

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Chinese Journal of Polymer Science 2024年第1期42卷 52-62,I0007页

作者： Vladislav A.Tuskaev kasim F.Magomedov Svetlana Ch.Gagieva Dmitry A.kurmaev Yulia V.Nelyubina evgenii k.gol.bev Maria D.Evseeva Viktor G.Vasil'ev Galina G.Nikiforova Mikhail I.Buzin Vyacheslav S.Bogdanov Boris M.Bulychev Department of Chemistry M.V.Lomonosov Moscow State UniversityMoscow 119992Russian Federation A.N.Nesmeyanov Institute of Organoelement Compounds Russian Academy of SciencesMoscow119991Russian Federation Enikolopov Institute of Synthetic Polymer Materials Russian Academy of SciencesMoscow 117393Russian Federation

A series of Ti(Ⅳ) dichloride and dialkoxide com plexes with phenoxyimine ligands containing fluorinated and nonfluorinated aliphatic imine fragments have been *** molecular structures of complexes 1 and 4 were established by single-crystal X-ray diffraction *** complexes adopt a distorted octahedral coordination structure around the titanium atom and two oxygen atoms are situated in trans position while two nitrogen atoms and two outgoing ligands(Cl or iPrO) are situated in cis *** of activators(MMAO-12 and combinations Et_nAICl_(3-n)+Bu_(2)Mg) and outgoing ligand(Cl or iPrO) nature on the catalytic activity and properties of the resulting polymers was *** Ti complexes,despite the nature of the outgoing ligands(Cl or iPrO) in the presence of Al/Mg activators,was found to display a high ethylene polymerization activity in the range 1600-3830 kg_(polymer)·mol_(Ti)^(-1)·h^(-1)·atm^(-1) with a viscosity average molecular weight(M_v) value in the range 1.1×10~6-7.1×10~6 Dalton(Da).The resulting UHMWPE can be processed by a solventless method into high-strength and high-modulus oriented *** rheological characteristics of a polymer melt have been *** absence of a cross-over point did not allow to compare the values of the molecular weight distribution of polymers obtained on fluorinated and non-fluorinated pre-catalysts,however,the estimation of the entanglement density is in good agreement with the mechanical characteristics of oriented film *** activation with methylalumoxane,the activity of the com plexes decreased very significantly;however,a polymer with a molecular weight of about 12 million Da was *** the process of ethylene/octene-1 copolymerization,fluorine-containing precatalysts showed a clear advantage over non-fluorinated analogues both in activity and in comonomer content.

关键词： FI catalysts Titanium(IV) (Co)polymerization Al/Mg co-catalyst Ultra-high molecular weight polyethylene

The effect of long-term application of nitrogen-rich fertilizers on soil resistome:A study of conventional and organic cropping systems

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Soil Ecology Letters 2024年第3期6卷 135-150页

作者： Alexey S.Vasilchenko evgenii O.Burlakov Darya V.Poshvina Denis S.Gruzdev Sergey V.kravchenko Aleksandr V.Iashnikov Ning Ling Anastasia V.Vasilchenko Laboratory of Antimicrobial Resistance Institute of Environmental and Agricultural Biology(X-BIO)Tyumen State UniversityTyumenRussia Research Institute of Mathematics Physics and Computer ScienceDerzhavin Tambov State UniversityTambovRussia International Integrated Research Laboratory for Climate Change Land Use and BiodiversityInstitute of Environmental and Agricultural Biology(X-BIO)Tyumen State UniversityTyumenRussia SciBear OU Tartu Mnt 67/1-13bKesklinna Linnaosa10115 TallinnEstonia Center for Grassland Microbiome State Key Laboratory of Grassland Agro-EcosystemsCollege of Pastoral Agriculture Science and TechnologyLanzhou UniversityLanzhou 730000China

Metagenomic studies of various soil environments have previously revealed the widespread distribution of antibiotic resistance genes(ARGs)around the *** this study,we applied shotgun metagenomics to investigate differences in microbial communities and resistomes in Chernozem soils that have been under long-term organic and conventional cropping *** organic cropping system was seeded with Triticum spelta without any *** conventional cropping system was seeded with Tríticum durum Desf and used mineral fertilizer(NPk),that resulted in an increased amount of total and available carbon and nitrogen in *** all samples,we identified a total of 21 ARG classes,among which the dominant were vancomycin,tetracycline and *** of soil microbial communities revealed differences between the studied fields in the relative abundances of 14 and 53 genera in topsoil and subsoil,*** analysis showed significant correlations(positive and negative)among 18 genera and 6 ARGs,as well as between these ARGs and some chemical properties of *** analysis of metagenome-assembled genomes revealed that Nitrospirota,Thermoproteota,Actinobacteriota and Binatota phyla of archaea and bacteria serve as hosts for glycopeptide and fluoroquinolone/tetracycline ***,the data obtained enrich knowledge about the consequences of human agricultural activities in terms of soil microbiome modification and highlight the role of nitrogen cycling taxa,including uncultivated genera,in the formation of soil resistome.

关键词： soil microbiome inorganic fertilizer nitrogen cycle uncultured bacteria chemolithotrophs Binatia

Aqueous-phase reforming of hydroxyacetone solution to bio-based H_(2)over supported Pt catalysts

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Green Energy & Environment 2024年第4期9卷 777-788页

作者： A.k.k.Vikla k.koichumanova Songbo He k.Seshan Joint International Research Laboratory of Circular Carbon Nanjing Tech UniversityNanjing211816China Faculty of Science and Technology University of Twente7500 AE EnschedeThe Netherlands CoRe Pro 9723 BL GroningenThe Netherlands

Aqueous-phase reforming(APR)is an attractive process to produce bio-based hydrogen from waste biomass streams,during which the catalyst stability is often challenged due to the harsh reaction *** this work,three Pt-based catalysts supported on C,AlO(OH),and ZrO_(2)were investigated for the APR of hydroxyacetone solution in afixed bed reactor at 225℃and 35 *** them,the Pt/C catalyst showed the highest turnover frequency for H_(2)production(TOF of 8.9 molH_(2)molPt^(-1)min^(-1))and the longest catalyst *** the AlO(OH)and ZrO_(2)supported Pt catalysts,the side reactions consuming H_(2),formation of coke,and Pt sintering result in a low H_(2)production and the fast catalyst *** proposed reaction pathways suggest that a promising APR catalyst should reform all oxygenates in the aqueous phase,minimize the hydrogenation of the oxygenates,maximize the WGS reaction,and inhibit the condensation and coking reactions for maximizing the hydrogen yield and a stable catalytic performance.

关键词： APR Hydroxyacetone TOF Bio-based H_(2) Support effect

Direct scaling of residual displacements for bilinear and pinching oscillators

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Earthquake Engineering and Engineering Vibration 2024年第1期23卷 129-149页

作者： Mohammad Saifullah Vinay k.Gupta Department of Civil Engineering Indian Institute of Technology KanpurKanpur 208016India

The estimation of residual displacements in a structure due to an anticipated earthquake event has increasingly become an important component of performance-based earthquake engineering because controlling these displacements plays an important role in ensuring cost-feasible or cost-effective repairs in a damaged structure after the *** attempt is made in this study to obtain statistical estimates of constant-ductility residual displacement spectra for bilinear and pinching oscillators with 5%initial damping,directly in terms of easily available seismological,site,and model *** of the available models for the bilinear and pinching oscillators are useful when design spectra for a seismic hazard at a site are not *** statistical estimates of a residual displacement spectrum are proposed in terms of earthquake magnitude,epicentral distance,site geology parameter,and three model parameters for a given set of ductility demand and a hysteretic energy capacity coefficient in the case of bilinear and pinching models,as well as for a given set of pinching parameters for displacement and strength at the breakpoint in the case of pinching model *** proposed scaling model is applicable to horizontal ground motions in the western *** earthquake magnitudes less than 7 or epicentral distances greater than 20 km.

关键词： residual displacement spectrum bilinear hysteresis model pinching hysteresis model nonlinear analysis scaling model

Analysis of the Oscillatory Flows of Multiple Shock Waves in a Constant Area Duct

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Journal of Thermal Science 2024年第3期33卷 794-806页

作者： k JAMES Jintu kIM Heuy Dong Department of Mechanical Engineering Andong National UniversityAndong36729Republic of Korea CAD-IT korea Co. Ltd.Seoul08591Republic of Korea

The oscillatory response of multiple shock waves to downstream perturbations in a supersonic flow is studied numerically in a rectangular *** shock waves are formed inside the duct at a shock Mach number of *** duct has an exit height of H,and the effect of duct resonance on multiple shock oscillations is investigated by attaching exit ducts of lengths 0H,50H,and *** downstream disturbance frequency varied from 10 Hz to 200 Hz to explore the oscillation characteristics of the multiple shock *** oscillatory response of shock waves under self-excited and forced oscillation conditions are analyzed in terms of wall static pressure,shock train leading-edge location,shock train length,and the size of the separation *** extent of the initial shock location increases with an increase in exit duct length for the self-excited oscillation *** analysis of the shock train leading edge and the spectral analysis of wall static pressure variations are *** variation in the shock train length is analyzed using the pressure ratio method for self-excited as well as forced *** RMS amplitude of the normalized shock train length(ζ_(ST))increases with an increase in the exit duct length for the self-excited oscillation *** the downstream perturbation frequency is increased,ζ_(ST)is decreased for exit duct *** all exit duct designs and downstream forcing frequencies,the size of the separation bubble grows and shrinks during the shock oscillations,demonstrating the dependence on duct resonance and forced oscillations.

关键词： shock train downstream disturbance supersonic flow shock wave boundary layer interaction duct resonance flow separation

Impact of Fin Arrangement on Heat Transfer and Melting Characteristics of Phase Change Material

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Journal of Thermal Science 2024年第2期33卷 435-456页

作者： Arun UNIYAL Yogesh k.PRAJAPATI Department of Mechanical Engineering National Institute of Technology UttarakhandSrinagar(Garhwal)246174India Department of Mechanical Engineering BIT SindriDhanbadJharkhand828123India

Present work investigates the heat transfer and melting behaviour of phase change material(PCM) in six enclosures(enclosure-1 to 6) filled with paraffin *** enclosures are equipped with distinct arrangements of the fins while keeping the fin's surface area equal in each *** analysis has been presented to recognize the suitable fin arrangements that facilitate improved heat transfer and melting rate of the *** wall of the enclosure is maintained isothermal for the temperature values 335 k,350 k and 365 *** length of the enclosure including fins is ranging between 0 and *** have been illustrated through the estimation of important performance parameters such as energy absorbing capacity,melting rate,enhancement ratio,and Nusselt *** has been found that melting time(to melt 100% of the PCM) is 60.5%less in enclosure-2(with two fins of equal length) as compared to the enclosure-1,having no *** the fin surface area equal,if the longer fin is placed below the shorter fin(enclosure-3),melting time is further decreased by 14.1% as compared to ***,among all the configurations,enclosure-6 with wire-mesh fin structure exhibits minimum melting time which is 68.4% less as compared to the *** on the findings,it may be concluded that fins are the main driving agent in the enclosure to transfer the heat from heated wall to the *** design and positioning of the fins improve the heat transfer rate followed by melting of the PCM in the entire area of the *** of the favourable vortices and natural convection current in the enclosure accelerate the melting phenomenon and help to reduce charging time.

关键词： phase change material enclosure fin melting fraction energy storage heat transfer