Calcium-ion batteries have been considered attractive candidates for large-scale energy storage applications due to their natural abundance and low redox potential of Ca^(2+)/Ca.However,current calcium ion technology ...Calcium-ion batteries have been considered attractive candidates for large-scale energy storage applications due to their natural abundance and low redox potential of Ca^(2+)/Ca.However,current calcium ion technology is still hampered by the lack of high-capacity and long-life electrode materials to accommodate the large Ca^(2+)(1.00Å).Herein,an amorphous vanadium structure induced by Mo doping and in-situ electrochemical activation is reported as a high-rate anode material for calcium ion batteries.The doping of Mo could destroy the lattice stability of VS4 material,enhancing the flexibility of the structure.The following electrochemical activation further converted the material into sulfide and oxides co-dominated composite(defined as MoVSO),which serves as an active material for the storage of Ca^(2+)during cycling.Consequently,this amorphous vanadium structure exhibits excellent rate capability,achieving discharge capacities of 306.7 and 149.2 mAh g^(-1)at 5 and 50 A g^(-1)and an ultra-long cycle life of 2000 cycles with 91.2%capacity retention.These values represent the highest level to date reported for calcium ion batteries.The mechanism studies show that the material undergoes a partial phase transition process to derive MoVSO.This work unveiled the calcium storage mechanism of vanadium sulfide in aqueous electrolytes and accelerated the development of high-performance aqueous calcium ion batteries.展开更多
Zeolite-encapsulated metal nanoclusters are at the heart of bifunctional catalysts,which hold great potential for petrochemical conversion and the emerging sustainable biorefineries.Nevertheless,efficient encapsulatio...Zeolite-encapsulated metal nanoclusters are at the heart of bifunctional catalysts,which hold great potential for petrochemical conversion and the emerging sustainable biorefineries.Nevertheless,efficient encapsulation of metal nanoclusters into a high-silica zeolite Y in particular with good structural integrity still remains a significant challenge.Herein,we have constructed Ru nanoclusters(~1 nm)encapsulated inside a high-silica zeolite Y(SY)with a SiO_(2)/Al_(2)O_(3) ratio(SAR)of 10 via a cooperative strategy for direct zeolite synthesis and a consecutive impregnation for metal encapsulation.Compared with the benchmark Ru/H-USY and other analogues,the as-prepared Ru/H-SY markedly boosts the yields of pentanoic biofuels and stability in the direct hydrodeoxygenation of biomass-derived levulinate even at a mild temperature of 180℃,which are attributed to the notable stabilization of transition states by the enhanced acid accessibility and properly sized constraints of zeolite cavities owing to the good structural integrity.展开更多
The electronic structure of Eu-doped NaTaO3 in Na-rich environment is investigated by the first-principles theory. By simulating the two different models of Eu3+ ions selectively located in Ta and Na sites, respectiv...The electronic structure of Eu-doped NaTaO3 in Na-rich environment is investigated by the first-principles theory. By simulating the two different models of Eu3+ ions selectively located in Ta and Na sites, respectively, the band gaps of two Eu-doped NaTaO3 models were all narrowed, which were assigned to lattice defects and impurity band of the Eu dopent. For the model of Eu3+ ions located in the Na+ sites of NaTaO3, the new impurity band mainly composited of Eu 4f orbital appeared at the top over the valence band, indicating the enhanced oxidative ability. For the model of Eu3+ ions located in the Ta5+ sites of NaTaO3, a midgap state generated was located at the bottom of conduct band and the band potential shifted up, confirming the strong reductive ability in the Na-rich enviornment. The densities of electron states were significantly increased in both the conduction and valence bands in Na-rich model, which resulted in the increased carrier migration rate and thus photocatalytic activity enhancement. It is proposed that Eu3+ ions doping at the Ta sites could enhance the reduced photocatalytic performance via controlling the nonstoichiometric Na/Ta molar ratio in the Eu-doped NaTaO3 system.展开更多
Crystal structure of a novel hydrated tridecameric polyaluminium chloride, [Al13(μ3-OH)6(μ2-OH)6(μ2-OH)12(H2O)24] Cl15·13H2O, has been determined by X-ray structure analysis, obtaining the detailed str...Crystal structure of a novel hydrated tridecameric polyaluminium chloride, [Al13(μ3-OH)6(μ2-OH)6(μ2-OH)12(H2O)24] Cl15·13H2O, has been determined by X-ray structure analysis, obtaining the detailed structural parameters and structure features. Moreover, the formation course was also discussed. The crystal belongs to monoclinic system, space group P21/c, with a = 1.3912(2), b = 2.3529(3), c = 2.2395(2) nm, β= 90.407(2)°, V = 7.3307(14) nm^3, Z = 4, Dc = 1.773 g/cm^3, F(000) = 4040, GOOF = 1.050,μ(MoKα)= 0.829 mm^-1, the final R = 0.0506 and wR = 0.1453 for 10553 observed reflections with I〉 2σ(I). The structure of polycation of the title compound is different from either Keggin-type Al13 consisting of a central tetrahedral AlO4 core surrounded by twelve octahedral AlO6 units through corner-sharing or the "three hexameric rings juxtaposed" side by side predicted by "Core-Links" model linked by thirteen octahedral AlO6 units through edge-sharing. It has a "tortoise-like" structure with turnup "forefeet" and "tail", that is, an octahedral AlO6 core is surrounded by a "hexameric ring" through edge-sharing, then six octahedral AlO6 units are suspended onto the periphery of the ring upper and lower alternately by sharing two neighboring corners with an average turn angle of 21° entad. This kind of hydrated tridecameric polyaluminium chloride with such form is very important to further understand the existing forms and transformation rules of aluminium ion in hydrolysis system of its salts, speculate the process and mechanism of various hydrolysis and polymerization forms from Al(H2O)6^3+ to Al(OH)3, and establish the relationship between structure and properties.展开更多
One complex with a zwitterionic dicarboxylate ligand, [Mn(L)(N3)]n 1 (L = 1-car- boxymethylpyridinium-3-carboxylate), was synthesized and structurally characterized. Complex 1 crystallizes in triclinic, space gr...One complex with a zwitterionic dicarboxylate ligand, [Mn(L)(N3)]n 1 (L = 1-car- boxymethylpyridinium-3-carboxylate), was synthesized and structurally characterized. Complex 1 crystallizes in triclinic, space group P1 with a = 7.570(2), b = 7.808(2), c = 9.232(3) A, β= 94.450(19)°, V= 489.0(3) A3, Z = 2, Mr = 277.11, Dc = 1.882 g/cm3, F(000) = 278,μ = 1.359 mm-1, S = 1.021, the final R = 0.0509 and wR = 0.1149 for 2236 observed reflections with 1 〉 2σ(I). Complex 1 consists of two-dimensional coordination layers in which the anionic uniform chains with mixed triple bridges (one end-on (EO) azide and two syn-syn carboxylates) are cross-linked by the flexible cationic N-methylpyridinium spacers. Magnetic studies demonstrated that the triple bridge in 1 transmits antiferromagnetic coupling between the Mn(Ⅱ) ions.展开更多
An Au/ceria(0.44%, mass fraction) catalyst containing gold ions was prepared by a modified deposition precipitation method, and the evolution of gold ions in the catalyst and its influence on the catalysis of CO oxi...An Au/ceria(0.44%, mass fraction) catalyst containing gold ions was prepared by a modified deposition precipitation method, and the evolution of gold ions in the catalyst and its influence on the catalysis of CO oxidation were investigated. It was found that the as-prepared catalyst containing gold ions with high valence could fully oxidize CO at -10 ℃ initially but was deactivated gradually at low temperatures during the reaction with CO or treatment by unpurified air. The deactivation of the catalyst during CO oxidation or treatment of it by unpurified air was independent and progressive at low temperatures while the activity of the catalyst at relatively high temperatures was maintained well. During the reaction with CO or treatment by unpurified air, the XPS results indicate that gold species evolved from high valence to low valence and the diffuse reflectance UV-Vis spectra show that high valence gold was reduced to charged gold clusters, gold clusters grew to small gold crystals and small gold crystals grew to large gold particles. Accordingly, the high valence gold corresponded to the activity at low temperatures and the metallic gold was active and relatively stable at high temperatures. The turnover frequencies(TOF) of the catalysts treated by different methods at 273 K decreased with the evolution of gold species from high valence to low valence, no maximum of TOF was observed although gold particles in the catalyst attained to about 2-3 nm during the treatment. An Au/ceria catalyst with a gold load of 0.87% (mass fraction) maintained a good activity for CO oxidation within 18 h at room temperature. The catalysts were characterized via transmitted electronic microscopy(TEM), inductively coupled plasma optical emission spectrometry(ICP-OES), X-ray diffraction(XRD) and BET specific surface area and UV-Vis DRS as well.展开更多
Europium and terbium complexes with strong fluorescence intensity and long fluorescence lifetime were prepared. By replacing half of the europium or terbium ion with M (M = Zn^2+, Cd^2+, and Cr^3+) using the dope...Europium and terbium complexes with strong fluorescence intensity and long fluorescence lifetime were prepared. By replacing half of the europium or terbium ion with M (M = Zn^2+, Cd^2+, and Cr^3+) using the doped method, and then incorporating it with 18-crown-6 ether and terephthalic acid, six heteronuclear samples EuZnLL'Cl3·3H2O(1), EuCdLL2'Cl3·5H2O(2), EuCrLL'Cl4· 4H2O(3), TbZnLL'Cl3·4H2O(4), TbCdLL'2Cl3·4H2O(5), and TbCrLL'2Cl4 ·4H2O(6) (L = terephthalic acid, L'= 18-Crown-6 ether) were obtained. The elemental analysis, molar conductivities, rare earth complexometry, Fourier Transform Infrared Spectroscopy (FT-IR), ultraviolet (UV), TGA, fluorescence intensity, and fluorescence lifetime of the samples were measured. The results showed that there were good luminescence properties for heteronuclear complexes (1), (2), (4), and (5), which were even stronger than those of the homonuclear complexes Eu2LL'2Cl4·4H2O and Tb2LL'2Cl4 ·4H2O, but the luminescence properties of EuCrLL'Cl4·4H2O, TbCrLL'Cl4·4H2O were very weak. A possible luminescence mechanism was suggested by the organic-inorganic doped mechanism and the law of intramolecular energy transfer.展开更多
Iron polymeric hydroxygroups pillared clays(Fe-PILC) were prepared by Na+-montmorillonite with iron pillaring agent. 2.01Au/Fe-PILC catalyst was obtained by deposited-precipitation(DP) method. 2.52Au/Fe-oxide catalyst...Iron polymeric hydroxygroups pillared clays(Fe-PILC) were prepared by Na+-montmorillonite with iron pillaring agent. 2.01Au/Fe-PILC catalyst was obtained by deposited-precipitation(DP) method. 2.52Au/Fe-oxide catalyst was prepared by co-precipitation method. The catalytic activity of these catalysts was measured by catalytic combustion of formaldehyde. The catalyst of 2.01Au/Fe-PILC exhibits the high catalytic activity. The catalytic combustion reaction of formaldehyde proceeds at considerable rates at 20 ℃ and complete burn-off of formaldehyde is achieved at 120 ℃. The structure of catalysts,the valence state of gold and the size of gold particles were investigated by means of X-ray powder diffractometry,X-ray photoelectron spectroscopy and transmission electron microscopy. The results show that gold atoms with partially positive charge exist in the catalyst and play an important role in the catalytic activity. In addition,nano-sized,well-dispersed gold particles and good adsorption properties of support are necessary to obtain high activity Au catalysts for catalytic combustion of formaldehyde.展开更多
A series of catalysts were prepared by using complex sol-gel methods.Experimental results confirm the effect of different agents on structure and activity of Fe-substituted rare earth hexaaluminate catalyst (LaFeAl11 ...A series of catalysts were prepared by using complex sol-gel methods.Experimental results confirm the effect of different agents on structure and activity of Fe-substituted rare earth hexaaluminate catalyst (LaFeAl11 O19 ) for methane combustion.The catalyst is yielded by complex sol-gel, respectively using three different complex agents (maltose, glucose and citric acid).XRD demonstrated that haxaaluminate is the major phase of catalyst prepared by maltose,while LaAlO3 is the major one of the catalyst by glucose and citric acid.At the same time, there is a little LaFeO3 and surface areas as well as 29.5 nm particle diameter when the complex agent is maltose.However, T10 ( temperature for 10% conversion of methane) and T100 ( temperature for 100% conversion of methane) for catalyst by glucose is 543 and 758 ℃, which is the best among the three complex agents for methane combustion.展开更多
Ternary complex of Eu (Ⅲ) with 8-hydroxyquinoline (8HOQ) and thenoyhrifluoro-acetone (TTA), Eu (TTA) (8HOQ)2·H2O was synthesized. The properties and structure of the complex were studied using elementa...Ternary complex of Eu (Ⅲ) with 8-hydroxyquinoline (8HOQ) and thenoyhrifluoro-acetone (TTA), Eu (TTA) (8HOQ)2·H2O was synthesized. The properties and structure of the complex were studied using elemental analysis, infrared spectra and ultraviolet absorption spectra. The fluorescence characteristics and emission mechanism of the complex were also discussed based on the fluorescence spectra.展开更多
A silicon-based tetracarboxylate connector has been prepared and employed in the construction of new metal-organic framework(MOF) material. A novel Cd(Ⅱ) coordination compound, namely, [Cd_4(H_2O)(L)(DMA)_2...A silicon-based tetracarboxylate connector has been prepared and employed in the construction of new metal-organic framework(MOF) material. A novel Cd(Ⅱ) coordination compound, namely, [Cd_4(H_2O)(L)(DMA)_2]_n(1, H_4L = 5,5?-(diphenylsilanediyl) diisophthalic acid, DMA = N,N-dimethylacetamide) has been successfully synthesized based on the ligand. X-ray single-crystal structure analysis reveals that polymer 1 crystallizes in monoclinic, space group P1 with a = 10.3335(11), b = 14.1557(15), c = 22.004(2) ?, α = 72.308(2), β = 88.105(2), γ = 88.363(3)o, V = 3064.2(6) ?~3, Cd_4Si_2C_(64)N_2O_(19)H_(52), Mr = 1659, Dc = 1.790 g/cm^3, μ(Mo Kα) = 1.486 mm^(-1), F(000) = 1630, Z = 2, the final R = 0.0660 and w R = 0.1302 for 12069 observed reflections(I 〉 2σ(I)). Its structure has been further characterized by elemental analysis, thermogravimetric analyses and IR spectroscopy. Additionally, luminescent property of the title compound has been explored, and shows intense photoluminescent property in the solid state at room temperature.展开更多
Generating sufficient strains on metal surfaces are highly challenging owing to that most metals can deform plastically to relax the strains on the surfaces.In this work,we developed a facile but highly efficient stac...Generating sufficient strains on metal surfaces are highly challenging owing to that most metals can deform plastically to relax the strains on the surfaces.In this work,we developed a facile but highly efficient stacked deposition strategy to in situ activation and reconstruction of NiO/NiOOH on Ni matrix,following with the migration of Fe ions to NiOOH.The Fe sites on the Ni/NiO/NiOOH facilitate the formation of the stable*OH oxygenated intermediates,and the Ni matrix in the catalyst provides the catalyst excellent stability.The oxygen evolution reaction(OER)performance of the stacked NiFe-5 with compressive strain displays the strengthened binding to oxygenated intermediates and superior OER activity,the ultralow overpotentials of 162 versus reversible hydrogen electrode at 10 mA cm^(-2).On the other hand,the Ni-5 without the incorporation of Fe has shown an outstanding hydrogen evolution reaction(HER)activity,affording an overpotential of 47 mV at 10 mA cm^(-2).The NiFe-5‖Ni-5 enables the overall water splitting at a voltage of 1.508 V to achieve 20 mA cm^(-2) with remarkable durability.The stacked deposition strategy improves binding strength of Ni-based catalysts to oxygenated intermediates via generating compressive strain,causing high catalytic activities on OER and HER.展开更多
The ever-growing pursuit of high energy density batteries has triggered extensive efforts toward developing alkali metal(Li,Na,and K)battery(AMB)technologies owing to high theoretical capacities and low redox potentia...The ever-growing pursuit of high energy density batteries has triggered extensive efforts toward developing alkali metal(Li,Na,and K)battery(AMB)technologies owing to high theoretical capacities and low redox potentials of metallic anodes.Typically,for new battery systems,the electrolyte design is critical for realizing the battery electrochemistry of AMBs.Conventional electrolytes in alkali ion batteries are generally unsuitable for sustaining the stability owing to the hyper-reactivity and dendritic growth of alkali metals.In this review,we begin with the fundamentals of AMB electrolytes.Recent advancements in concentrated and fluorinated electrolytes,as well as functional electrolyte additives for boosting the stability of Li metal batteries,are summarized and discussed with a special focus on structure-composition-performance relationships.We then delve into the electrolyte formulations for Na-and K metal batteries,including those in which Na/K do not adhere to the Li-inherited paradigms.Finally,the challenges and the future research needs in advanced electrolytes for AMB are highlighted.This comprehensive review sheds light on the principles for the rational design of promising electrolytes and offers new inspirations for developing stable AMBs with high performance.展开更多
Background:This study aimed to select compounds with unique inhibitory effects on muscle-invasive bladder cancer(MIBC)from coumarone derivatives with similar parent nuclear structures and to reveal their tumor-suppres...Background:This study aimed to select compounds with unique inhibitory effects on muscle-invasive bladder cancer(MIBC)from coumarone derivatives with similar parent nuclear structures and to reveal their tumor-suppressive effects using various approaches.Methods:Bladder cancer cell lines SW780 and T24,as well as human normal bladder epithelial cell line SV-HUC-1 were selected as the study model,and these urinary system cells were co-incubated with various concentrations of(S,E)-4-(4-methylbenzylidene)-3-phenylchroman-3-ol,(S,E)-4-(4-isocyanobenzylidene)-3-phenylchroman-3-ol,(S,E)-4-(4-fluorobenzylidene)-3-phenylchroman-3-ol(FPO),and(S,E)-3-phenyl-4-(4-(trifluoromethoxy)benzylidene)chroman-3-ol.Cell activity was detected using cell counting kit-8.FPO showed the strongest inhibitory effect on MIBC cells;therefore,it was selected for further experiments.We monitored the FPO-induced T24 cell morphological changes with an inverted microscope.The FPO-inhibited migration of T24 cells was examined using a cell scratch assay.We detected the clonogenic ability of T24 cells through a clone formation test and evaluated their proliferative ability using a 5-ethynyl-2’-deoxyuridine fluorescence staining kit.The inhibitory effect of FPO against the cell cycle was monitored using flow cytometry,and its suppressive effect on the DNA replication ability of T24 cells was detected using double fluorescence staining(Ki67 and phalloidin).Results:Among the four candidate coumarone derivatives,FPO showed the most significant inhibitory effect on MIBC cells and was less toxic to normal urothelial cells.FPO inhibited T24 cell growth in time and dose-dependent manners(the half-inhibitory concentration is 8μM).FPO significantly repressed the proliferation,migration,and clonogenic ability of bladder cancer T24 cells.Cell mobility was significantly inhibited by FPO:30μM FPO almost completely repressed migration occurred at after 24 h treatment.Moreover,FPO significantly suppressed the clonogenicity of bladder cancer cells in a dose-dependent manner.Mechanistically,FPO targeted the cell cycle,arresting the S and G2 phases on bladder cancer T24 cells.Conclusion:We discovered a novel anticancer chemical,FPO,and proposed a potential mechanism,through which it suppresses MIBC T24 cells by repressing the cell cycle in the S and G2 phases.This study contributes to the development of novel anticancer drugs for MIBC.展开更多
Vacancy engineering and Mott-Schottky heterostructure can accelerate charge transfer,regulate adsorption energy of reaction intermediates,and provide additional active sites,which are regarded as valid means for impro...Vacancy engineering and Mott-Schottky heterostructure can accelerate charge transfer,regulate adsorption energy of reaction intermediates,and provide additional active sites,which are regarded as valid means for improving catalytic activity.However,the underlying mechanism of synergistic regulation of interfacial charge transfer and optimization of electrocatalytic activity by combining vacancy and Mott-Schottky junction remains unclear.Herein,the growth of a bifunctional NiCo/NiCoP Mott-Schottky electrode with abundant phosphorus vacancies on foam nickel(NF)has been synthesized through continuous phosphating and reduction processes.The obtained NiCo/NiCoP heterojunctions show remarkable OER and HER activities,and the overpotentials for OER and HER are as low as 117 and 60 mV at 10 mA/cm^(2) in 1 mol/L KOH,respectively.Moreover,as both the cathode and anode of overall water splitting,the voltage of the bifunctional NiCo/NiCoP electrocatalyst is 1.44 V at 10 mA/cm^(2),which are far exceeding the benchmark commercial electrodes.DFT theoretical calculation results confirm that the phosphorus vacancies and build-in electric field can effectively accelerate ion and electron transfer between NiCo alloy and NiCoP semiconductor,tailor the electronic structure of the metal centers and lower the Gibbs free energy of the intermediates.Furthermore,the unique self-supported integrated structure is beneficial to facilitate the exposure of the active site,avoid catalyst shedding,thus improving the activity and structural stability of NiCo/NiCoP.This study provides an avenue for the controllable synthesis and performance optimization of Mott-Schottky electrocatalysts.展开更多
The mechanical properties of engineering plastics can be enhanced through effective surface mechanical treatment(SMT),which can be applied to various types of engineering plastics,eliminating the limitations of conven...The mechanical properties of engineering plastics can be enhanced through effective surface mechanical treatment(SMT),which can be applied to various types of engineering plastics,eliminating the limitations of conventional polymer processing and could potentially extend their applications and improve their performance and reliability as structural-functional materials.Inspired by metal forging,this work proposes a simple and effective SMT strategy to enhance the mechanical properties of polyamide 66(PA66).Tensile tests have shown that SMTed PA66 samples exhibit significant improvements in both Young’s modulus and ultimate tensile strength(UTS),with a 2104 MPa Young’s modulus,almost double that of the pristine samples,and a 35.56%increase in UTS,reaching 183 MPa.Additionally,the modulus within the localized SMTed surface layer could reach up to 14 GPa,which is approximately 14 times higher than that of the pristine sample.The Vickers hardness within the localized SMTed surface layer can be doubled,reaching 10.72 Hv,and the crystallinity can increase by approximately 20%compared to the untreated region.Furthermore,force field molecular dynamics(FFMD)simulations were conducted to investigate the ternary relationship between the SMT method,PA66’s molecular structure,and its properties.The combination of MD simulations and versatile structural characterizations provides evidence that the SMT method’s mechanism,under heat induction,results in a chain-combing procedure that changes the polymer’s molecular morphology microscopically and enhances its mechanical properties macroscopically.展开更多
Reasonably designing highly active,environmentally friendly,and cost-effective catalysts for efficient elimination of pollutants from water is desirable but challenging.Herein,an efficient heterogeneous photo-Fenton c...Reasonably designing highly active,environmentally friendly,and cost-effective catalysts for efficient elimination of pollutants from water is desirable but challenging.Herein,an efficient heterogeneous photo-Fenton catalyst tourmaline(TM)/tungsten oxide(WO_(3-x))(named TW10)containing tungsten/boron/iron(W/B/Fe)synergistic active centers and 90%of cheap natural tourmaline(TM)mineral rich in Fe and B elements.The TW10 catalyst can quickly activate peroxymonosulfate(PMS)to generate massive active free radicals,which may induce the rapid and efficient degradation of tetracycline(TC).The TW10/PMS/Visible light system can effectively degrade up to 98.7%of tetracycline(TC)in actual waters(i.e.seawater,Yellow River,and Yangtze River water),and the catalytic degradation rates reach 1.65,5.569,and 2.38 times higher than those of TM,WO_(3-x),and commercial P25(Degussa,Germany),respectively.In addition,the catalyst can be recycled and reused multiple times.Electron spin resonance spectroscopy(EPR),X-ray photoelectron spectroscopy(XPS),and liquid chromatograph-mass spectrometer(LC-MS)analyses confirm that the synergistic catalytic effect of W/B/Fe sites on the TW10 catalyst accelerates the electron transfer between Fe(Ⅱ)and Fe(Ⅲ),as well as between W(Ⅴ)and W(Ⅵ),and thus promotes the rapid degradation of TC.The catalytic reaction mechanism and degradation pathway of TC were explored.This work provides a feasible route for the design and development of new eco-friendly and efficient catalyst.展开更多
Based on the in-situ self-reduction and chemical stability,graphdiyne(GDY)and graphdiyne oxide(GDYO)are used as trapping agents to investigate the ability for recovering Au^(3+),Ag^+,and Pd^(2+)under different pH valu...Based on the in-situ self-reduction and chemical stability,graphdiyne(GDY)and graphdiyne oxide(GDYO)are used as trapping agents to investigate the ability for recovering Au^(3+),Ag^+,and Pd^(2+)under different pH values and interfering ions.Under strong acidity at pH=1,these two agents demonstrate high select recovery towards the three precious metal ions,which could be insitu reduced to nanoparticles(NPs).In addition,superparamagnetic Fe_(3)O_(4)NPs are deposited on the surfaces of GDY and GDYO.The magnetic responses enable GDYFe_(3)O_(4)to recover precious metals conveniently and efficiently by the aid of an external magnetic field.This study also confirms the antibacterial activity of the as-recovered NPs deposited on GDY and GDYO against Escherichia coli and Staphylococcus aureus(1×10^(5)colony-forming unit(CFU)·mL^(-1)),and the antibacterial rates are 100%.This strategy of recovering precious metals and subsequently reusing to combat pathogens will be of great significance for environmental remediation and biomedical applications.展开更多
Organosulfur materials containing sulfur-sulfur bonds are an emerging class of high-capacity cathodes for lithium storage.However,it remains a great challenge to achieve rapid conversion reaction kinetics at practical...Organosulfur materials containing sulfur-sulfur bonds are an emerging class of high-capacity cathodes for lithium storage.However,it remains a great challenge to achieve rapid conversion reaction kinetics at practical testing conditions of high cathode mass loading and low electrolyte utilization.In this study,a Li-rich pyrolyzed polyacrylonitrile/selenium disulfide(pPAN/Se_(2)S_(3))composite cathode is synthesized by deep lithiation to address the above challenges.The Li-rich molecular structure significantly boosts the lithium storage kinetics by accelerating lithium diffusivity and improving electronic conductivity.Even under practical test conditions requiring a lean electrolyte(Electrolyte/sulfur ratio of 4.1μL mg^(-1))and high loading(7 mg cm^(-2)of pPAN/Se_(2)S_(3)),DL-pPAN/Se_(2)S_(3)exhibits a specific capacity of 558 mAh g^(-1),maintaining 484 mAh g^(-1)at the 100th cycle with an average Coulombic efficiency of near 100%.Moreover,it provides(electro)chemically stable Li resources to offset Li consumption over charge-discharge cycles.As a result the as-fabricated anode-free cell shows a superior cycling stability with 90%retention of the initial capacity over 45 cycles.This study provides a novel approach for fabricating high-energy and stable Li-SPAN cells.展开更多
The photocatalytic degradation of dye Rhodamine B (RhB) in the presence of TiO2 nanostdpe or P25 under visible light irradiation was investigated. The degradation intermediates were identified using Infrared spectra...The photocatalytic degradation of dye Rhodamine B (RhB) in the presence of TiO2 nanostdpe or P25 under visible light irradiation was investigated. The degradation intermediates were identified using Infrared spectra (IR spectra), ^1H nuclear magnetic resonance (^1HNMR) spectra, and gas chromatography-mass spectroscopy (GC-MS). The IR and the ^1HNMR results showed that the large conjugated chromophore structure of RhB was efficiently destroyed under visible light irradiation in both the photocatalytic systems (TiO2 nanostfipe or P25 and Rhodamine B systems). GC-MS results showed that the main identified intermediates were ethanediotic acid, 1,2-benzenedicarboxylic acid, 4-hydroxy benzoic acid and benzoic acid, which were almost the same in the TiO2 nanostdpes and P25 systems. This work provides a good insight into the reaction pathway(s) for the TiO2-assisted photocatalytic degradation of dye pollutants under visible light irradiation.展开更多
基金supported by the Open Research Found of Songshan Lake Materials Laboratory(2021SLABFN04)Guangdong Basic and Applied Basic Research Foundation(2022A1515010920)+2 种基金Inner Mongolia Major Science and Technology Project(2020ZD0024)the Alashan League’s Project of Applied Technology Research and Development Fund(AMYY2020-01)the Local Science and Technology Development Project of the Central Government(2022ZY0011)
文摘Calcium-ion batteries have been considered attractive candidates for large-scale energy storage applications due to their natural abundance and low redox potential of Ca^(2+)/Ca.However,current calcium ion technology is still hampered by the lack of high-capacity and long-life electrode materials to accommodate the large Ca^(2+)(1.00Å).Herein,an amorphous vanadium structure induced by Mo doping and in-situ electrochemical activation is reported as a high-rate anode material for calcium ion batteries.The doping of Mo could destroy the lattice stability of VS4 material,enhancing the flexibility of the structure.The following electrochemical activation further converted the material into sulfide and oxides co-dominated composite(defined as MoVSO),which serves as an active material for the storage of Ca^(2+)during cycling.Consequently,this amorphous vanadium structure exhibits excellent rate capability,achieving discharge capacities of 306.7 and 149.2 mAh g^(-1)at 5 and 50 A g^(-1)and an ultra-long cycle life of 2000 cycles with 91.2%capacity retention.These values represent the highest level to date reported for calcium ion batteries.The mechanism studies show that the material undergoes a partial phase transition process to derive MoVSO.This work unveiled the calcium storage mechanism of vanadium sulfide in aqueous electrolytes and accelerated the development of high-performance aqueous calcium ion batteries.
基金supported by the National Natural Science Foundation of China (22288101,21991090,21991091,22078316,22272171 and 22109167)the Sino-French International Research Network (Zeolites)+2 种基金the BL01B1 beamline of SPring-8 and the 1W1B station of Beijing Synchrotron Radiation Facility (BSRF)for the support of XAS measurementsthe Division of Energy Research Resources of Dalian Institute of Chemical Physics for the support of iDPC-STEM measurementsthe support of the Alexander von Humboldt Foundation (CHN 1220532 HFST-P)。
文摘Zeolite-encapsulated metal nanoclusters are at the heart of bifunctional catalysts,which hold great potential for petrochemical conversion and the emerging sustainable biorefineries.Nevertheless,efficient encapsulation of metal nanoclusters into a high-silica zeolite Y in particular with good structural integrity still remains a significant challenge.Herein,we have constructed Ru nanoclusters(~1 nm)encapsulated inside a high-silica zeolite Y(SY)with a SiO_(2)/Al_(2)O_(3) ratio(SAR)of 10 via a cooperative strategy for direct zeolite synthesis and a consecutive impregnation for metal encapsulation.Compared with the benchmark Ru/H-USY and other analogues,the as-prepared Ru/H-SY markedly boosts the yields of pentanoic biofuels and stability in the direct hydrodeoxygenation of biomass-derived levulinate even at a mild temperature of 180℃,which are attributed to the notable stabilization of transition states by the enhanced acid accessibility and properly sized constraints of zeolite cavities owing to the good structural integrity.
基金Financially supported by the National Natural Science Foundation of China(No.21267014 and 21567017)
文摘The electronic structure of Eu-doped NaTaO3 in Na-rich environment is investigated by the first-principles theory. By simulating the two different models of Eu3+ ions selectively located in Ta and Na sites, respectively, the band gaps of two Eu-doped NaTaO3 models were all narrowed, which were assigned to lattice defects and impurity band of the Eu dopent. For the model of Eu3+ ions located in the Na+ sites of NaTaO3, the new impurity band mainly composited of Eu 4f orbital appeared at the top over the valence band, indicating the enhanced oxidative ability. For the model of Eu3+ ions located in the Ta5+ sites of NaTaO3, a midgap state generated was located at the bottom of conduct band and the band potential shifted up, confirming the strong reductive ability in the Na-rich enviornment. The densities of electron states were significantly increased in both the conduction and valence bands in Na-rich model, which resulted in the increased carrier migration rate and thus photocatalytic activity enhancement. It is proposed that Eu3+ ions doping at the Ta sites could enhance the reduced photocatalytic performance via controlling the nonstoichiometric Na/Ta molar ratio in the Eu-doped NaTaO3 system.
基金Project supported by NNSFC (No. 20563002), NSF of Inner Mongolia Autonomous Region (200508010204) and Key Item Foundation of Education Committee of Inner Mongolia Autonomous Region (ZD01070)
文摘Crystal structure of a novel hydrated tridecameric polyaluminium chloride, [Al13(μ3-OH)6(μ2-OH)6(μ2-OH)12(H2O)24] Cl15·13H2O, has been determined by X-ray structure analysis, obtaining the detailed structural parameters and structure features. Moreover, the formation course was also discussed. The crystal belongs to monoclinic system, space group P21/c, with a = 1.3912(2), b = 2.3529(3), c = 2.2395(2) nm, β= 90.407(2)°, V = 7.3307(14) nm^3, Z = 4, Dc = 1.773 g/cm^3, F(000) = 4040, GOOF = 1.050,μ(MoKα)= 0.829 mm^-1, the final R = 0.0506 and wR = 0.1453 for 10553 observed reflections with I〉 2σ(I). The structure of polycation of the title compound is different from either Keggin-type Al13 consisting of a central tetrahedral AlO4 core surrounded by twelve octahedral AlO6 units through corner-sharing or the "three hexameric rings juxtaposed" side by side predicted by "Core-Links" model linked by thirteen octahedral AlO6 units through edge-sharing. It has a "tortoise-like" structure with turnup "forefeet" and "tail", that is, an octahedral AlO6 core is surrounded by a "hexameric ring" through edge-sharing, then six octahedral AlO6 units are suspended onto the periphery of the ring upper and lower alternately by sharing two neighboring corners with an average turn angle of 21° entad. This kind of hydrated tridecameric polyaluminium chloride with such form is very important to further understand the existing forms and transformation rules of aluminium ion in hydrolysis system of its salts, speculate the process and mechanism of various hydrolysis and polymerization forms from Al(H2O)6^3+ to Al(OH)3, and establish the relationship between structure and properties.
基金Supported by the NNSFC(21301087)Programs of Higher-level talents of Inner Mongolia University(SPH-IMU-30105-125135)Inner Mongolia autonomous region natural science fund project(2013MS0206)
文摘One complex with a zwitterionic dicarboxylate ligand, [Mn(L)(N3)]n 1 (L = 1-car- boxymethylpyridinium-3-carboxylate), was synthesized and structurally characterized. Complex 1 crystallizes in triclinic, space group P1 with a = 7.570(2), b = 7.808(2), c = 9.232(3) A, β= 94.450(19)°, V= 489.0(3) A3, Z = 2, Mr = 277.11, Dc = 1.882 g/cm3, F(000) = 278,μ = 1.359 mm-1, S = 1.021, the final R = 0.0509 and wR = 0.1149 for 2236 observed reflections with 1 〉 2σ(I). Complex 1 consists of two-dimensional coordination layers in which the anionic uniform chains with mixed triple bridges (one end-on (EO) azide and two syn-syn carboxylates) are cross-linked by the flexible cationic N-methylpyridinium spacers. Magnetic studies demonstrated that the triple bridge in 1 transmits antiferromagnetic coupling between the Mn(Ⅱ) ions.
基金Supported by the National Natural Science Foundation of China(No.20563003)the Inner Mongolia Education Depart-ment Fund(No.NJZY07013)
文摘An Au/ceria(0.44%, mass fraction) catalyst containing gold ions was prepared by a modified deposition precipitation method, and the evolution of gold ions in the catalyst and its influence on the catalysis of CO oxidation were investigated. It was found that the as-prepared catalyst containing gold ions with high valence could fully oxidize CO at -10 ℃ initially but was deactivated gradually at low temperatures during the reaction with CO or treatment by unpurified air. The deactivation of the catalyst during CO oxidation or treatment of it by unpurified air was independent and progressive at low temperatures while the activity of the catalyst at relatively high temperatures was maintained well. During the reaction with CO or treatment by unpurified air, the XPS results indicate that gold species evolved from high valence to low valence and the diffuse reflectance UV-Vis spectra show that high valence gold was reduced to charged gold clusters, gold clusters grew to small gold crystals and small gold crystals grew to large gold particles. Accordingly, the high valence gold corresponded to the activity at low temperatures and the metallic gold was active and relatively stable at high temperatures. The turnover frequencies(TOF) of the catalysts treated by different methods at 273 K decreased with the evolution of gold species from high valence to low valence, no maximum of TOF was observed although gold particles in the catalyst attained to about 2-3 nm during the treatment. An Au/ceria catalyst with a gold load of 0.87% (mass fraction) maintained a good activity for CO oxidation within 18 h at room temperature. The catalysts were characterized via transmitted electronic microscopy(TEM), inductively coupled plasma optical emission spectrometry(ICP-OES), X-ray diffraction(XRD) and BET specific surface area and UV-Vis DRS as well.
基金Project supported by the National Natural Science Foundation of China (20461002) Chun Hui Plan Foundation of MOE(Z2004-2-15029)
文摘Europium and terbium complexes with strong fluorescence intensity and long fluorescence lifetime were prepared. By replacing half of the europium or terbium ion with M (M = Zn^2+, Cd^2+, and Cr^3+) using the doped method, and then incorporating it with 18-crown-6 ether and terephthalic acid, six heteronuclear samples EuZnLL'Cl3·3H2O(1), EuCdLL2'Cl3·5H2O(2), EuCrLL'Cl4· 4H2O(3), TbZnLL'Cl3·4H2O(4), TbCdLL'2Cl3·4H2O(5), and TbCrLL'2Cl4 ·4H2O(6) (L = terephthalic acid, L'= 18-Crown-6 ether) were obtained. The elemental analysis, molar conductivities, rare earth complexometry, Fourier Transform Infrared Spectroscopy (FT-IR), ultraviolet (UV), TGA, fluorescence intensity, and fluorescence lifetime of the samples were measured. The results showed that there were good luminescence properties for heteronuclear complexes (1), (2), (4), and (5), which were even stronger than those of the homonuclear complexes Eu2LL'2Cl4·4H2O and Tb2LL'2Cl4 ·4H2O, but the luminescence properties of EuCrLL'Cl4·4H2O, TbCrLL'Cl4·4H2O were very weak. A possible luminescence mechanism was suggested by the organic-inorganic doped mechanism and the law of intramolecular energy transfer.
基金Projects (20263001, 20601012) supported by the National Natural Science Foundation of ChinaProject (ND412) supported by Inner Mongolia University Youth Foundation, China
文摘Iron polymeric hydroxygroups pillared clays(Fe-PILC) were prepared by Na+-montmorillonite with iron pillaring agent. 2.01Au/Fe-PILC catalyst was obtained by deposited-precipitation(DP) method. 2.52Au/Fe-oxide catalyst was prepared by co-precipitation method. The catalytic activity of these catalysts was measured by catalytic combustion of formaldehyde. The catalyst of 2.01Au/Fe-PILC exhibits the high catalytic activity. The catalytic combustion reaction of formaldehyde proceeds at considerable rates at 20 ℃ and complete burn-off of formaldehyde is achieved at 120 ℃. The structure of catalysts,the valence state of gold and the size of gold particles were investigated by means of X-ray powder diffractometry,X-ray photoelectron spectroscopy and transmission electron microscopy. The results show that gold atoms with partially positive charge exist in the catalyst and play an important role in the catalytic activity. In addition,nano-sized,well-dispersed gold particles and good adsorption properties of support are necessary to obtain high activity Au catalysts for catalytic combustion of formaldehyde.
基金Project supported by the Natural Science Foundation of China and Inner Mongolia (20163001,20010901 - 12 )
文摘A series of catalysts were prepared by using complex sol-gel methods.Experimental results confirm the effect of different agents on structure and activity of Fe-substituted rare earth hexaaluminate catalyst (LaFeAl11 O19 ) for methane combustion.The catalyst is yielded by complex sol-gel, respectively using three different complex agents (maltose, glucose and citric acid).XRD demonstrated that haxaaluminate is the major phase of catalyst prepared by maltose,while LaAlO3 is the major one of the catalyst by glucose and citric acid.At the same time, there is a little LaFeO3 and surface areas as well as 29.5 nm particle diameter when the complex agent is maltose.However, T10 ( temperature for 10% conversion of methane) and T100 ( temperature for 100% conversion of methane) for catalyst by glucose is 543 and 758 ℃, which is the best among the three complex agents for methane combustion.
文摘Ternary complex of Eu (Ⅲ) with 8-hydroxyquinoline (8HOQ) and thenoyhrifluoro-acetone (TTA), Eu (TTA) (8HOQ)2·H2O was synthesized. The properties and structure of the complex were studied using elemental analysis, infrared spectra and ultraviolet absorption spectra. The fluorescence characteristics and emission mechanism of the complex were also discussed based on the fluorescence spectra.
基金supported by the Jilin province development and reform commission(NDRC) project:2014Y115
文摘A silicon-based tetracarboxylate connector has been prepared and employed in the construction of new metal-organic framework(MOF) material. A novel Cd(Ⅱ) coordination compound, namely, [Cd_4(H_2O)(L)(DMA)_2]_n(1, H_4L = 5,5?-(diphenylsilanediyl) diisophthalic acid, DMA = N,N-dimethylacetamide) has been successfully synthesized based on the ligand. X-ray single-crystal structure analysis reveals that polymer 1 crystallizes in monoclinic, space group P1 with a = 10.3335(11), b = 14.1557(15), c = 22.004(2) ?, α = 72.308(2), β = 88.105(2), γ = 88.363(3)o, V = 3064.2(6) ?~3, Cd_4Si_2C_(64)N_2O_(19)H_(52), Mr = 1659, Dc = 1.790 g/cm^3, μ(Mo Kα) = 1.486 mm^(-1), F(000) = 1630, Z = 2, the final R = 0.0660 and w R = 0.1302 for 12069 observed reflections(I 〉 2σ(I)). Its structure has been further characterized by elemental analysis, thermogravimetric analyses and IR spectroscopy. Additionally, luminescent property of the title compound has been explored, and shows intense photoluminescent property in the solid state at room temperature.
基金supported by the National Natural Science Foundations of China(21965024,22269016,51721002)the Inner Mongolia funding(2020JQ01,21300-5223601)the funding of Inner Mongolia University(10000-21311201/137,213005223601/003,21300-5223707)。
文摘Generating sufficient strains on metal surfaces are highly challenging owing to that most metals can deform plastically to relax the strains on the surfaces.In this work,we developed a facile but highly efficient stacked deposition strategy to in situ activation and reconstruction of NiO/NiOOH on Ni matrix,following with the migration of Fe ions to NiOOH.The Fe sites on the Ni/NiO/NiOOH facilitate the formation of the stable*OH oxygenated intermediates,and the Ni matrix in the catalyst provides the catalyst excellent stability.The oxygen evolution reaction(OER)performance of the stacked NiFe-5 with compressive strain displays the strengthened binding to oxygenated intermediates and superior OER activity,the ultralow overpotentials of 162 versus reversible hydrogen electrode at 10 mA cm^(-2).On the other hand,the Ni-5 without the incorporation of Fe has shown an outstanding hydrogen evolution reaction(HER)activity,affording an overpotential of 47 mV at 10 mA cm^(-2).The NiFe-5‖Ni-5 enables the overall water splitting at a voltage of 1.508 V to achieve 20 mA cm^(-2) with remarkable durability.The stacked deposition strategy improves binding strength of Ni-based catalysts to oxygenated intermediates via generating compressive strain,causing high catalytic activities on OER and HER.
基金financial support from Natural Science Foundation of Inner Mongolia(No.2019MS05068)Inner Mongolia scientific and technological achievements transformation project(CGZH2018132)+3 种基金Inner Mongolia major science and technology project(2020ZD0024)the research project of Inner Mongolia Electric Power(Group)Co.,Ltd for post-doctoral studies,the Hong Kong Polytechnic University start-up funding,National Nature Science Foundation of China(No.51872157)Shenzhen Key Laboratory on Power Battery Safety Research(No.ZDSYS201707271615073)financial support from the Australian Research Council(DE190100445).
文摘The ever-growing pursuit of high energy density batteries has triggered extensive efforts toward developing alkali metal(Li,Na,and K)battery(AMB)technologies owing to high theoretical capacities and low redox potentials of metallic anodes.Typically,for new battery systems,the electrolyte design is critical for realizing the battery electrochemistry of AMBs.Conventional electrolytes in alkali ion batteries are generally unsuitable for sustaining the stability owing to the hyper-reactivity and dendritic growth of alkali metals.In this review,we begin with the fundamentals of AMB electrolytes.Recent advancements in concentrated and fluorinated electrolytes,as well as functional electrolyte additives for boosting the stability of Li metal batteries,are summarized and discussed with a special focus on structure-composition-performance relationships.We then delve into the electrolyte formulations for Na-and K metal batteries,including those in which Na/K do not adhere to the Li-inherited paradigms.Finally,the challenges and the future research needs in advanced electrolytes for AMB are highlighted.This comprehensive review sheds light on the principles for the rational design of promising electrolytes and offers new inspirations for developing stable AMBs with high performance.
基金supported by National Nature Science Foundation of China(82172978)Taishan Scholars Program of Shandong Province(Grant No.tsqn201909147)+1 种基金the Key Project at Central Government Level:the ability establishment of sustainable use for valuable Chinese medicine resources(2060302)the Student Innovation Training Program in Jining Medical University(cx2021116).
文摘Background:This study aimed to select compounds with unique inhibitory effects on muscle-invasive bladder cancer(MIBC)from coumarone derivatives with similar parent nuclear structures and to reveal their tumor-suppressive effects using various approaches.Methods:Bladder cancer cell lines SW780 and T24,as well as human normal bladder epithelial cell line SV-HUC-1 were selected as the study model,and these urinary system cells were co-incubated with various concentrations of(S,E)-4-(4-methylbenzylidene)-3-phenylchroman-3-ol,(S,E)-4-(4-isocyanobenzylidene)-3-phenylchroman-3-ol,(S,E)-4-(4-fluorobenzylidene)-3-phenylchroman-3-ol(FPO),and(S,E)-3-phenyl-4-(4-(trifluoromethoxy)benzylidene)chroman-3-ol.Cell activity was detected using cell counting kit-8.FPO showed the strongest inhibitory effect on MIBC cells;therefore,it was selected for further experiments.We monitored the FPO-induced T24 cell morphological changes with an inverted microscope.The FPO-inhibited migration of T24 cells was examined using a cell scratch assay.We detected the clonogenic ability of T24 cells through a clone formation test and evaluated their proliferative ability using a 5-ethynyl-2’-deoxyuridine fluorescence staining kit.The inhibitory effect of FPO against the cell cycle was monitored using flow cytometry,and its suppressive effect on the DNA replication ability of T24 cells was detected using double fluorescence staining(Ki67 and phalloidin).Results:Among the four candidate coumarone derivatives,FPO showed the most significant inhibitory effect on MIBC cells and was less toxic to normal urothelial cells.FPO inhibited T24 cell growth in time and dose-dependent manners(the half-inhibitory concentration is 8μM).FPO significantly repressed the proliferation,migration,and clonogenic ability of bladder cancer T24 cells.Cell mobility was significantly inhibited by FPO:30μM FPO almost completely repressed migration occurred at after 24 h treatment.Moreover,FPO significantly suppressed the clonogenicity of bladder cancer cells in a dose-dependent manner.Mechanistically,FPO targeted the cell cycle,arresting the S and G2 phases on bladder cancer T24 cells.Conclusion:We discovered a novel anticancer chemical,FPO,and proposed a potential mechanism,through which it suppresses MIBC T24 cells by repressing the cell cycle in the S and G2 phases.This study contributes to the development of novel anticancer drugs for MIBC.
基金financially supported by the National Natural Science Foundation of China(NSFC,Nos.22269015,22205119)Natural Science Foundation of Inner Mongolia Autonomous Region of China(Nos.2021ZD11,2019BS02015).
文摘Vacancy engineering and Mott-Schottky heterostructure can accelerate charge transfer,regulate adsorption energy of reaction intermediates,and provide additional active sites,which are regarded as valid means for improving catalytic activity.However,the underlying mechanism of synergistic regulation of interfacial charge transfer and optimization of electrocatalytic activity by combining vacancy and Mott-Schottky junction remains unclear.Herein,the growth of a bifunctional NiCo/NiCoP Mott-Schottky electrode with abundant phosphorus vacancies on foam nickel(NF)has been synthesized through continuous phosphating and reduction processes.The obtained NiCo/NiCoP heterojunctions show remarkable OER and HER activities,and the overpotentials for OER and HER are as low as 117 and 60 mV at 10 mA/cm^(2) in 1 mol/L KOH,respectively.Moreover,as both the cathode and anode of overall water splitting,the voltage of the bifunctional NiCo/NiCoP electrocatalyst is 1.44 V at 10 mA/cm^(2),which are far exceeding the benchmark commercial electrodes.DFT theoretical calculation results confirm that the phosphorus vacancies and build-in electric field can effectively accelerate ion and electron transfer between NiCo alloy and NiCoP semiconductor,tailor the electronic structure of the metal centers and lower the Gibbs free energy of the intermediates.Furthermore,the unique self-supported integrated structure is beneficial to facilitate the exposure of the active site,avoid catalyst shedding,thus improving the activity and structural stability of NiCo/NiCoP.This study provides an avenue for the controllable synthesis and performance optimization of Mott-Schottky electrocatalysts.
基金The authors express their gratitude for the financial assistance received from the Liao Ning Revitalization Talents Program,China(No.XLYC2008022).
文摘The mechanical properties of engineering plastics can be enhanced through effective surface mechanical treatment(SMT),which can be applied to various types of engineering plastics,eliminating the limitations of conventional polymer processing and could potentially extend their applications and improve their performance and reliability as structural-functional materials.Inspired by metal forging,this work proposes a simple and effective SMT strategy to enhance the mechanical properties of polyamide 66(PA66).Tensile tests have shown that SMTed PA66 samples exhibit significant improvements in both Young’s modulus and ultimate tensile strength(UTS),with a 2104 MPa Young’s modulus,almost double that of the pristine samples,and a 35.56%increase in UTS,reaching 183 MPa.Additionally,the modulus within the localized SMTed surface layer could reach up to 14 GPa,which is approximately 14 times higher than that of the pristine sample.The Vickers hardness within the localized SMTed surface layer can be doubled,reaching 10.72 Hv,and the crystallinity can increase by approximately 20%compared to the untreated region.Furthermore,force field molecular dynamics(FFMD)simulations were conducted to investigate the ternary relationship between the SMT method,PA66’s molecular structure,and its properties.The combination of MD simulations and versatile structural characterizations provides evidence that the SMT method’s mechanism,under heat induction,results in a chain-combing procedure that changes the polymer’s molecular morphology microscopically and enhances its mechanical properties macroscopically.
基金supported by the National Natural Science Foundation of China(No.22068027)the“Grassland Talents”Project of Inner Mongolia Autonomous Region(No.CCYCLJ202)the Inner Mongolia University Research Start-up Research Project(No.21300-5205122)。
文摘Reasonably designing highly active,environmentally friendly,and cost-effective catalysts for efficient elimination of pollutants from water is desirable but challenging.Herein,an efficient heterogeneous photo-Fenton catalyst tourmaline(TM)/tungsten oxide(WO_(3-x))(named TW10)containing tungsten/boron/iron(W/B/Fe)synergistic active centers and 90%of cheap natural tourmaline(TM)mineral rich in Fe and B elements.The TW10 catalyst can quickly activate peroxymonosulfate(PMS)to generate massive active free radicals,which may induce the rapid and efficient degradation of tetracycline(TC).The TW10/PMS/Visible light system can effectively degrade up to 98.7%of tetracycline(TC)in actual waters(i.e.seawater,Yellow River,and Yangtze River water),and the catalytic degradation rates reach 1.65,5.569,and 2.38 times higher than those of TM,WO_(3-x),and commercial P25(Degussa,Germany),respectively.In addition,the catalyst can be recycled and reused multiple times.Electron spin resonance spectroscopy(EPR),X-ray photoelectron spectroscopy(XPS),and liquid chromatograph-mass spectrometer(LC-MS)analyses confirm that the synergistic catalytic effect of W/B/Fe sites on the TW10 catalyst accelerates the electron transfer between Fe(Ⅱ)and Fe(Ⅲ),as well as between W(Ⅴ)and W(Ⅵ),and thus promotes the rapid degradation of TC.The catalytic reaction mechanism and degradation pathway of TC were explored.This work provides a feasible route for the design and development of new eco-friendly and efficient catalyst.
基金financially supported by the National Natural Science Foundation of China(Nos.22062017 and 22164015)Inner Mongolia Autonomous Region Program for Key Science and Technology(No.2020GG0161)+3 种基金Ordos City Program for Key Science and Technology(No.2022YY003)the Program of Higher-Level Talents of Inner Mongolia University(No.10000-22311201/035)the Research Program of science and technology at Universities of Inner Mongolia Autonomous Region(No.NJZZ23091)the Program for Innovative Research Team in Universities of Inner Mongolia Autonomous Region(No.NMGIRT2210)。
文摘Based on the in-situ self-reduction and chemical stability,graphdiyne(GDY)and graphdiyne oxide(GDYO)are used as trapping agents to investigate the ability for recovering Au^(3+),Ag^+,and Pd^(2+)under different pH values and interfering ions.Under strong acidity at pH=1,these two agents demonstrate high select recovery towards the three precious metal ions,which could be insitu reduced to nanoparticles(NPs).In addition,superparamagnetic Fe_(3)O_(4)NPs are deposited on the surfaces of GDY and GDYO.The magnetic responses enable GDYFe_(3)O_(4)to recover precious metals conveniently and efficiently by the aid of an external magnetic field.This study also confirms the antibacterial activity of the as-recovered NPs deposited on GDY and GDYO against Escherichia coli and Staphylococcus aureus(1×10^(5)colony-forming unit(CFU)·mL^(-1)),and the antibacterial rates are 100%.This strategy of recovering precious metals and subsequently reusing to combat pathogens will be of great significance for environmental remediation and biomedical applications.
基金financial support from The Hong Kong Polytechnic University(ZZLM,YY4V,YY5K)Inner Mongolia Scientific and Technological Achievements Transformation Project(no.CGZH2018132)+6 种基金Inner Mongolia Major Science and Technology Project(no.2020ZD0024)the Alashan League’s Project of Applied Technology Research and Development Fund(no.AMYY2020-01)Local Science and Technology Development Project of the Central Government(no.2021ZY0006,2022ZY0011)National Natural Science Foundation of China(no.52202245)Natural Science Fund for Colleges and Universities in Jiangsu Province(no.22KJB430004)Natural Science Foundation of Jiangsu Province(BE2020759)Jiangsu Outstanding Professors
文摘Organosulfur materials containing sulfur-sulfur bonds are an emerging class of high-capacity cathodes for lithium storage.However,it remains a great challenge to achieve rapid conversion reaction kinetics at practical testing conditions of high cathode mass loading and low electrolyte utilization.In this study,a Li-rich pyrolyzed polyacrylonitrile/selenium disulfide(pPAN/Se_(2)S_(3))composite cathode is synthesized by deep lithiation to address the above challenges.The Li-rich molecular structure significantly boosts the lithium storage kinetics by accelerating lithium diffusivity and improving electronic conductivity.Even under practical test conditions requiring a lean electrolyte(Electrolyte/sulfur ratio of 4.1μL mg^(-1))and high loading(7 mg cm^(-2)of pPAN/Se_(2)S_(3)),DL-pPAN/Se_(2)S_(3)exhibits a specific capacity of 558 mAh g^(-1),maintaining 484 mAh g^(-1)at the 100th cycle with an average Coulombic efficiency of near 100%.Moreover,it provides(electro)chemically stable Li resources to offset Li consumption over charge-discharge cycles.As a result the as-fabricated anode-free cell shows a superior cycling stability with 90%retention of the initial capacity over 45 cycles.This study provides a novel approach for fabricating high-energy and stable Li-SPAN cells.
基金Project supported by the National Natural Science Foundation of China(No. 20567002)the Scientific Research Startup Foundation of InnerMongolia University (No. 203044)+2 种基金the Education Department of InnerMongolia Autonomous Region (No. NJ04093, NJ03121)the ChunhuiPlan of the Education Ministry (No. Z2004-2-15030)the "513 TalentsPlan" of Inner Mongolia University.
文摘The photocatalytic degradation of dye Rhodamine B (RhB) in the presence of TiO2 nanostdpe or P25 under visible light irradiation was investigated. The degradation intermediates were identified using Infrared spectra (IR spectra), ^1H nuclear magnetic resonance (^1HNMR) spectra, and gas chromatography-mass spectroscopy (GC-MS). The IR and the ^1HNMR results showed that the large conjugated chromophore structure of RhB was efficiently destroyed under visible light irradiation in both the photocatalytic systems (TiO2 nanostfipe or P25 and Rhodamine B systems). GC-MS results showed that the main identified intermediates were ethanediotic acid, 1,2-benzenedicarboxylic acid, 4-hydroxy benzoic acid and benzoic acid, which were almost the same in the TiO2 nanostdpes and P25 systems. This work provides a good insight into the reaction pathway(s) for the TiO2-assisted photocatalytic degradation of dye pollutants under visible light irradiation.