Complex oxides are an important class of materials with enormous potential for electrochemical appli-cations.Depending on their composition and structure,such complex oxides can exhibit either a single conductivity(ox...Complex oxides are an important class of materials with enormous potential for electrochemical appli-cations.Depending on their composition and structure,such complex oxides can exhibit either a single conductivity(oxygen-ionic or protonic,or n-type,or p-type electronic)or a combination thereof gener-ating distinct dual-conducting or even triple-conducting materials.These properties enable their use as diverse functional materials for solid oxide fuel cells,solid oxide electrolysis cells,permeable membranes,and gas sensors.The literature review shows that the field of solid oxide materials and related electro-chemical cells has a significant level of research engagement,with over 8,000 publications published since 2020.The manual analysis of such a large volume of material is challenging.However,by examining the review articles,it is possible to identify key patterns,recent achievements,prospects,and remaining obstacles.To perform such an analysis,the present article provides,for the first time,a comprehensive summary of previous review publications that have been published since 2020,with a special focus on solid oxide materials and electrochemical systems.Thus,this study provides an important reference for researchers specializing in the fields of solid state ionics,high-temperature electrochemistry,and energyconversiontechnologies.展开更多
The electrocatalytic oxidation of biomass-derived furfural(FF)feedstocks into 2-furoic acid(FA)holds immense industrial potential in optics,cosmetics,polymers,and food.Herein,we fabricated Co O/Ni O/nickel foam(NF)and...The electrocatalytic oxidation of biomass-derived furfural(FF)feedstocks into 2-furoic acid(FA)holds immense industrial potential in optics,cosmetics,polymers,and food.Herein,we fabricated Co O/Ni O/nickel foam(NF)and Cu_(2)O/Ni O/NF electrodes via in situ pulsed laser irradiation in liquids(PLIL)for the bifunctional electrocatalysis of oxygen evolution reaction(OER)and furfural oxidation reaction(FOR),respectively.Simultaneous oxidation of NF surface to NiO and deposition of CoO and/or Cu_(2)O on NF during PLIL offer distinct advantages for enhancing both the OER and FOR.CoO/NiO/NF electrocatalyst provides a consistently low overpotential of~359 m V(OER)at 10 m A/cm^(2),achieving the maximum FA yield(~16.37 m M)with 61.5%selectivity,79.5%carbon balance,and a remarkable Faradaic efficiency of~90.1%during 2 h of FOR at 1.43 V(vs.reversible hydrogen electrode).Mechanistic pathway via in situ electrochemical-Raman spectroscopy on CoO/NiO/NF reveals the involvement of phase transition intermediates(NiOOH and CoOOH)as surface-active centers during electrochemical oxidation.The carbonyl carbon in FF is attacked by hydroxyl groups to form unstable hydrates that subsequently undergo further oxidation to yield FA products.This method holds promise for large-scale applications,enabling simultaneous production of renewable building materials and fuel.展开更多
Opencast coal mining has a large impact on the land surface,both at the mining pits themselves and at waste sites.After artifcial management is stopped,a reclaimed opencast coal mine dump is afected by wind and water ...Opencast coal mining has a large impact on the land surface,both at the mining pits themselves and at waste sites.After artifcial management is stopped,a reclaimed opencast coal mine dump is afected by wind and water erosion from natural processes,resulting in land degradation and even safety incidents.In this paper,the soil erosion and land degradation after 5 years of such natural processes,at the Xilinhot opencast coal mine dump in Inner Mongolia,were investigated.A multisource data acquisition method was applied:the vegetation fraction coverage(VFC)was extracted from GF-1 satellite imagery,high-precision terrain characteristics and the location and degree of soil erosion were obtained using a drone,and the physical properties of the topsoil were obtained by feld sampling.On this basis,the degree and spatial distribution of erosion cracks were identifed,and the causes of soil erosion and land degradation were analyzed using the geographical detector.The results show that(1)multi-source data acquisition method can provide efective basic data for the quantitative evaluation of the ecological environment at dumps,and(2)slope aspect and VFC are the main factors afecting the degree of degradation and soil erosion.Based on above analysis,several countermeasures are proposed to mitigate land degradation:(1)The windward slope be designed to imitate the natural landform.(2)Reasonable engineering measures should be applied at the slope to restrain soil erosion.(3)The Pioneer plants should be widely planted on the platform at the early stage of reclamation.展开更多
We investigated the role of metal atomization and solvent decomposition into reductive species and carbon clusters in the phase formation of transition-metal carbides(TMCs;namely,Co_(3)C,Fe_(3)C,TiC,and MoC)by pulsed ...We investigated the role of metal atomization and solvent decomposition into reductive species and carbon clusters in the phase formation of transition-metal carbides(TMCs;namely,Co_(3)C,Fe_(3)C,TiC,and MoC)by pulsed laser ablation of Co,Fe,Ti,and Mo metals in acetone.The interaction between carbon s-p-orbitals and metal d-orbitals causes a redistribution of valence structure through charge transfer,leading to the formation of surface defects as observed by X-ray photoelectron spectroscopy.These defects influence the evolved TMCs,making them effective for hydrogen and oxygen evolution reactions(HER and OER)in an alkaline medium.Co_(3)C with more oxygen affinity promoted CoO(OH)intermediates,and the electrochemical surface oxidation to Co_(3)O_(4)was captured via in situ/operando electrochemical Raman probes,increasing the number of active sites for OER activity.MoC with more d-vacancies exhibits strong hydrogen binding,promoting HER kinetics,whereas Fe_(3)C and TiC with more defect states to trap charge carriers may hinder both OER and HER activities.The results show that the assembled membrane-less electrolyzer with Co_(3)C∥Co_(3)C and MoC∥MoC electrodes requires~2.01 and 1.99 V,respectively,to deliver a 10 mA cm−2 with excellent electrochemical and structural stability.In addition,the ascertained pulsed laser synthesis mechanism and unit-cell packing relations will open up sustainable pathways for obtaining highly stable electrocatalysts for electrolyzers.展开更多
Herein,we propose a simple and rapid approach for synthesizing a CuS/Ru composite that serves as a bifunctional electrocatalyst to promote hydrogen production and concurrently convert sulfion into a value-added sulfur...Herein,we propose a simple and rapid approach for synthesizing a CuS/Ru composite that serves as a bifunctional electrocatalyst to promote hydrogen production and concurrently convert sulfion into a value-added sulfur product.This composite comprises Ru nanoclusters supported on the CuS nanostructure,achieved through simple pulsed laser irradiation in liquid approach.The optimized CuS/Ru-30 electrocatalyst demonstrates remarkable bifunctional electrocatalytic activity,exhibiting a negligible working potential of 0.28 V(vs.RHE)for the anodic sulfion oxidation reaction(SOR)and a minimal overpotential of 182 m V for cathodic hydrogen evolution reaction(HER)to achieve 10 mA cm^(-2)of current density.Moreover,the Cu S/Ru-30 electrocatalyst shows exceptional selectivity for converting sulfion into valuable sulfur during anodic oxidation reactions.Remarkably,in a two-electrode electrolyzer system utilizing Cu S/Ru-30 as both the anode and cathode,the SOR+HER coupled water electrolysis system demands only 0.52 V to reach 10 mA cm^(-2),which is considerably lesser compared to the OER+HER coupled water electrolysis(1.85 V).The experimental results and density function theory(DFT)calculations reveal that the strong electron interaction between CuS and Ru nanoclusters generates a built-in electric field,greatly enhancing electron transfer efficiency.This significantly boosts the HER performance and facilitates the adsorption and production of sulfur intermediates.This study presents a rapid and simple strategy for synthesizing a dual-functional catalyst suitable for low-voltage hydrogen generation while facilitating the recovery of valuable sulfur sources.展开更多
In semiconductor photocatalysts,the easy recombination of photogenerated carriers seriously affects the application of photocatalytic materials in water treatment.To solve the serious problem of electron−hole pair rec...In semiconductor photocatalysts,the easy recombination of photogenerated carriers seriously affects the application of photocatalytic materials in water treatment.To solve the serious problem of electron−hole pair recombination in perylene diimide(PDI)organic semiconductors,we loaded ferric hydroxyl oxide(FeOOH)on PDI materials,successfully prepared novel FeOOH@PDI photocatalytic materials,and constructed a photo-Fenton system.The system was able to achieve highly efficient degradation of BPA under visible light,with a degradation rate of 0.112 min^(−1)that was 20 times higher than the PDI system,and it also showed universal degradation performances for a variety of emerging organic pollutants and anti-interference ability.The mechanism research revealed that the FeOOH has the electron trapping property,which can capture the photogenerated electrons on the surface of PDI,effectively reducing the compounding rate of photogenerated carriers of PDI and accelerating the iron cycling and H2O2 activation on the surface of FeOOH at the same time.This work provides new insights and methods for solving the problem of easy recombination of carriers in semiconductor photocatalysts and degrading emerging organic pollutants.展开更多
Recently,high temperature(T_(c)≈80 K)superconductivity(SC)has been discovered in La_(3)Ni_(2)O_(7)(LNO)under pressure.This raises the question of whether the superconducting transition temperature T_(c) could be furt...Recently,high temperature(T_(c)≈80 K)superconductivity(SC)has been discovered in La_(3)Ni_(2)O_(7)(LNO)under pressure.This raises the question of whether the superconducting transition temperature T_(c) could be further enhanced under suitable conditions.One possible route for achieving higher T_(c) is element substitution.Similar SC could appear in the Fmmm phase of rare-earth(RE)R_(3)Ni_(2)O_(7)(RNO,R=RE element)material series under suitable pressure.The electronic properties in the RNO materials are dominated by the Ni 3d orbitals in the bilayer NiO_(2) plane.In the strong coupling limit,the SC could be fully characterized by a bilayer single 3d_(x^(2)−y^(2))-orbital t–J‖–J⊥ model.With RE element substitution from La to other RE element,the lattice constant of the Fmmm RNO material decreases,and the resultant electronic hopping integral increases,leading to stronger superexchanges between the 3d_(x^(2)−y^(2)) orbitals.Based on the slave-boson mean-field theory,we explore the pairing nature and the evolution of T_(c) in RNO materials under pressure.Consequently,it is found that the element substitution does not alter the pairing nature,i.e.,the inter-layer s-wave pairing is always favored in the superconducting RNO under pressure.However,the T_(c) increases from La to Sm,and a nearly doubled T_(c) could be realized in SmNO under pressure.This work provides evidence for possible higher T_(c) R_(3)Ni_(2)O_(7) materials,which may be realized in further experiments.展开更多
The hysteresis of magnetoresistance observed in superconductors is of great interest due to its potential connectionwith unconventional superconductivity.In this study,we perform electrical transport measurements on k...The hysteresis of magnetoresistance observed in superconductors is of great interest due to its potential connectionwith unconventional superconductivity.In this study,we perform electrical transport measurements on kagome superconductorCsV_(3)Sb_(5)nanoflakes and uncover unusual hysteretic behavior of magnetoresistance in the superconducting state.This hysteresis can be induced by applying either a large DC or AC current at temperatures(T)well below the superconductingtransition temperature(T_(c)).As T approaches T_(c),similar weak hysteresis is also detected by applying a smallcurrent.Various scenarios are discussed,with particular focus on the effects of vortex pinning and the presence of timereversal-symmtery-breaking superconducting domains.Our findings support the latter,hinting at chiral superconductivityin kagome superconductors.展开更多
The article presents the composition and current state of poisonous plants distributed on the Ustyurt plateau. Ustyurt is one of the largest deserts in Central Asia, differing from other deserts of the world in geogra...The article presents the composition and current state of poisonous plants distributed on the Ustyurt plateau. Ustyurt is one of the largest deserts in Central Asia, differing from other deserts of the world in geographical location, relief, flora and fauna and other features. The territory of Ustyurt occupies 21.3 million hectares, of which the Karakalpak part accounts for 7.2 million hectares. Poisonous alkaloid-bearing plants of the Karakalpak part of the Ustyurt plateau Anabasis aphylla, Atriplex flabellum, Kalidium capsicum, Salsola arbusculaeformis, Salsola foliosa, Aellenia subaphylla, Anabasis brachiata, Rheum tataricum, Capparis spinosa, Glycyrrhiza aspera. Alkaloid-bearing plants that are not eaten or poorly eaten by cattle Ephedra distachya, Delphinium songaricum, Anabasis salsa, alkaloid-bearing plants eaten by animals without harm Carex physodes, Eremopyrum orientale, Agrophyllum repens, Astragalus amodendron, Astragalus villosissimus, species of the genera Calligonum, Salsola. Poisonous plants of the Karakalpak part of the Ustyurt plateau. An analysis of the pasture flora of the Karakalpak part of the Ustyurt plateau shows that 62 species of wild poisonous plants belonging to 49 genera and 19 families grow here. Although these plants are considered poisonous, but in modern pharmaceutics and medicine, they are used as medicinal.展开更多
Leveraging the high resolution,sensitivity,and wide frequency coverage of the Atacama Large Millimeter/submillimeter Array(ALMA),the QUARKS survey,standing for“Querying Underlying mechanisms of massive star formation...Leveraging the high resolution,sensitivity,and wide frequency coverage of the Atacama Large Millimeter/submillimeter Array(ALMA),the QUARKS survey,standing for“Querying Underlying mechanisms of massive star formation with ALMA-Resolved gas Kinematics and Structures”,is observing 139 massive starforming clumps at ALMA Band 6(λ~1.3 mm).This paper introduces the Atacama Compact Array(ACA)7 m data of the QUARKS survey,describing the ACA observations and data reduction.Combining multiwavelength data,we provide the first edition of QUARKS atlas,offering insights into the multiscale and multiphase interstellar medium in high-mass star formation.The ACA 1.3 mm catalog includes 207 continuum sources that are called ACA sources.Their gas kinetic temperatures are estimated using three formaldehyde transitions with a non-LTE radiation transfer model,and the mass and density are derived from a dust emission model.The ACA sources are massive(16–84 percentile values of 6–160 M_(⊙)),gravity-dominated(M∝R^(1.1))fragments within massive clumps,with supersonic turbulence(M>1)and embedded star-forming protoclusters.We find a linear correlation between the masses of the fragments and the massive clumps,with a ratio of 6%between the two.When considering fragments as representative of dense gas,the ratio indicates a dense gas fraction(DGF)of 6%,although with a wide scatter ranging from 1%to 10%.If we consider the QUARKS massive clumps to be what is observed at various scales,then the size-independent DGF indicates a self-similar fragmentation or collapsing mode in protocluster formation.With the ACA data over four orders of magnitude of luminosity-to-mass ratio(L/M),we find that the DGF increases significantly with L/M,which indicates clump evolutionary stage.We observed a limited fragmentation at the subclump scale,which can be explained by a dynamic global collapse process.展开更多
After the mass closures of entire coal mine districts in Europe at the end of the last century, a new phenomenon of surface movement was observed—an upward movement.Although most surface movement(i.e., subsidence) oc...After the mass closures of entire coal mine districts in Europe at the end of the last century, a new phenomenon of surface movement was observed—an upward movement.Although most surface movement(i.e., subsidence) occurs in the months and years after mining by the longwall method, surface movement still occurs many decades after mining is terminated.After the closure and flooding of underground excavations and surrounding rock, this movement was reversed.This paper focuses on quantifying the upward movement in two neighboring coal mines(Winterslag and Zwartberg, Belgium).The study is based on data from a remote sensing technique: interferometry with synthetic aperture radar(INSAR).The results of the study show that the rate of upward movement in the decade after closure is about 10 mm/year on average.The upward movements are not linked directly to the past exploitation directly underneath a location.The amounts of subsidence at specific locations are linked mainly to their positions relative to an inverse trough shape situated over the entire mined-out areas and their immediate surroundings.Local features, such as geological faults, can have a secondary effect on the local variation of the uplift.The processes of subsidence and uplift are based on completely different mechanisms.Subsidence is initiated by a caving process, while the process of uplift is clearly linked to flooding.展开更多
A new basal neoceratopsian dinosaur, Helioceratops brachygnathus gen. et sp. nov., is described from the Quantou Formation (late Early Cretaceous or early Late Cretaceous) in the Liufangzi locality (Jilin province,...A new basal neoceratopsian dinosaur, Helioceratops brachygnathus gen. et sp. nov., is described from the Quantou Formation (late Early Cretaceous or early Late Cretaceous) in the Liufangzi locality (Jilin province, China). Helioceratops differs from other basal neoceratopsians with its deep dentary ramus, its steeply-inclined ventral predentary facet, its heterogeneous dentary crowns, and by the denticles and secondary ridges asymmetrically distributed on either side of the primary ridge on its dentary teeth. Along with Auroraceratops and Yamaceratops, Helioceratops represents one of the most derived non-coronosaurian neoceratopsians. The palaeogeographical distribution of basal neoceratopsians appears limited to northern China and southern Mongolia in the current state of our knowledge. It is therefore probable that this region constituted the birthplace for more advanced, Late Cretaceous Coronosanria.展开更多
The Cretaceous/Paleogene (K/Pg) Working Group, after many years of studies, voted to define the Global Stratotype Section and Point (GSSP) for the base of the Danian Stage at the base of the boundary clay at a sec...The Cretaceous/Paleogene (K/Pg) Working Group, after many years of studies, voted to define the Global Stratotype Section and Point (GSSP) for the base of the Danian Stage at the base of the boundary clay at a section near El Kef Tunisia. The GSSP was approved by the International Commission on Stratigraphy (ICS) and ratified by the International Union of Geological Sciences (IUGS) in 1991. Nevertheless, the GSSP was not officially published, although some papers dealing with geological aspects of the K/Pg boundary at El Kef have been published and this is quite well known. In April 2006, the GSSP was revisited, a marker was put in place and protection of the site was requested. Many correlation criteria are present at the GSSP of which the most useful are the meteorite impact evidence (iridium anomaly, Ni-rich spinel, etc.) and the mass extinction of planktic micro- and nannofossils. This event coincides with the GSSP, allowing us to propose that the K/Pg boundary is marked exactly by the moment of the meteorite impact, which implies that all the sediments generated by the impact belong to the Danian. This definition solves problems of correlation in the Yucatan peninsula (Mexico) and its surroundings.展开更多
AIM: To investigate whether nicotinamide overload plays a role in type 2 diabetes. METHODS: Nicotinamide metabolic patterns of 14 diabetic and 14 non-diabetic subjects were compared using HPLC. Cumulative effects of...AIM: To investigate whether nicotinamide overload plays a role in type 2 diabetes. METHODS: Nicotinamide metabolic patterns of 14 diabetic and 14 non-diabetic subjects were compared using HPLC. Cumulative effects of nicotinamide and N^1-methylnicotinamide on glucose metabolism, plasma HzO2 levels and tissue nicotinamide adenine dinucleotide (NAD) contents of adult Sprague-Dawley rats were observed. The role of human sweat glands and rat skin in nicotinamide metabolism was investigated using sauna and burn injury, respectively. RESULTS: Diabetic subjects had significantly higher plasma N^1-methylnicotinamide levels 5 h after a 100-mg nicotinamide load than the non-diabetic subjects (0.89 ± 0.13 μmol/L vs 0.6 ± 0.13 μmol/L, P 〈 0.001). Cumulative doses of nicotinamide (2 g/kg) significantly increased rat plasma Nl-methylnicotinamide concentrations associated with severe insulin resistance, which was mimicked by Nl-methy-Inicotinamide. Moreover, cumulative exposure to N^1- methylnicotinamide (2 g/kg) markedly reduced rat muscle and liver NAD contents and erythrocyte NAD/ NADH ratio, and increased plasma H2O2 levels. Decrease in NAD/NADH ratio and increase in H2O2 generation were also observed in human erythrocytes after exposure to N^1-methylnicotinamide in vitro. Sweating eliminated excessive nicotinamide (5.3-fold increase in sweat nicotinamide concentration 1 h after a 100-mg nicotinamide load). Skin damage or aldehyde oxidase inhibition with tamoxifen or olanzapine, both being notorious for impairing glucose tolerance, delayed N^1- methylnicotinamide clearance. CONCLUSION: These findings suggest that nicotinamide overload, which induced an increase in plasma N^1- methylnicotinamide, associated with oxidative stress and insulin resistance, plays a role in type 2 diabetes.展开更多
AIM To investigate the temporal sequence of pathological changes in the cellular structures of retina and choroidea in the early stages of diabetes in laboratory animals.METHODS Experimental type 1 diabetes was modele...AIM To investigate the temporal sequence of pathological changes in the cellular structures of retina and choroidea in the early stages of diabetes in laboratory animals.METHODS Experimental type 1 diabetes was modeled by three intraperitoneal injections of an alloxan solution into 30 male nonlinear rats at 16 wk of age. The 30 th and 60 th days from the final alloxan injection were chosen as the endpoints. Light and electron microscopy and morphometric and immunohistochemical studies were performed on histological slices of eyeballs from experimental animals.RESULTS Diabetic disturbances progressed to 60 d of the experiment. Thus, in the retina, a partial destruction of photoreceptors accompanied by interstitial edema was observed. The morphometric analysis revealed a reduction in the thickness of the retina. A reduction in the number of blood vessels of the choroid with disturbances of the endothelial cells and the vascular walls and a persistent reduction in the number of melanocytes were observed. The number of proliferating Ki-67 positive cells decreased, and the number of macrophages increased with diabetes development.CONCLUSION The starting point in the development of destructive changes involves early reduction in the number of melanocytes of the choroidea and alterations in the retinal pigment epithelium.展开更多
The timing of reproduction can significantly affect an offspring's fitness, thereby also influencing the fitness of the parents, especially in species inhabiting extreme environments, such as deserts. Female reproduc...The timing of reproduction can significantly affect an offspring's fitness, thereby also influencing the fitness of the parents, especially in species inhabiting extreme environments, such as deserts. Female reproductive cycles in Phrynocephalus przewalskii were studied from April to September 2008. Significant cycles of gonadal volume were found in all studied populations and the cycles were similar among the various populations. Females began vitellogenesis in April and contained oviductal eggs form May to June. Gonad volume decreased significantly in July and reached minimum volume from August to September. The follicular growth was negatively correlated with increasing precipitation and temperature in all populations. Hatching occurs during summer and early fall, when most of the annual rainfall occurs. Mean clutch size based on all populations was 2.7 ± 0.9 SE (n = 71).展开更多
Why heavily parameterized neural networks(NNs) do not overfit the data is an important long standing open question. We propose a phenomenological model of the NN training to explain this non-overfitting puzzle. Our li...Why heavily parameterized neural networks(NNs) do not overfit the data is an important long standing open question. We propose a phenomenological model of the NN training to explain this non-overfitting puzzle. Our linear frequency principle(LFP) model accounts for a key dynamical feature of NNs: they learn low frequencies first, irrespective of microscopic details. Theory based on our LFP model shows that low frequency dominance of target functions is the key condition for the non-overfitting of NNs and is verified by experiments. Furthermore,through an ideal two-layer NN, we unravel how detailed microscopic NN training dynamics statistically gives rise to an LFP model with quantitative prediction power.展开更多
We investigate rotational dynamics of an actively driven rotor through experiments and numerical simulations. While probability density distributions of rotor angular velocity are strongly non-Gaussian, relative proba...We investigate rotational dynamics of an actively driven rotor through experiments and numerical simulations. While probability density distributions of rotor angular velocity are strongly non-Gaussian, relative probabilities of observing rotation in opposite directions are shown to be linearly related to the angular velocity magnitude. We construct a stochastic model to describe transitions between different states from rotor angular velocity data and use the stochastic model to show that symmetry properties in probability density distributions are related to the detailed fluctuation relation(FR) of entropy productions.展开更多
Detection of local strain at the nanometer scale with high sensitivity remains challenging.Here we report near-field infrared nano-imaging of local strains in bilayer graphene by probing strain-induced shifts of phono...Detection of local strain at the nanometer scale with high sensitivity remains challenging.Here we report near-field infrared nano-imaging of local strains in bilayer graphene by probing strain-induced shifts of phonon frequency.As a non-polar crystal,intrinsic bilayer graphene possesses little infrared response at its transverse optical phonon frequency.The reported optical detection of local strain is enabled by applying a vertical electrical field that breaks the symmetry of the two graphene layers and introduces finite electrical dipole moment to graphene phonon.The activated phonon further interacts with continuum electronic transitions,and generates a strong Fano resonance.The resulted Fano resonance features a very sharp near-field infrared scattering peak,which leads to an extraordinary sensitivity of-0.002%for the strain detection.Our results demonstrate the first nano-scale near-field Fano resonance,provide a new way to probe local strains with high sensitivity in non-polar crystals,and open exciting possibilities for studying strain-induced rich phenomena.展开更多
The catalytic conversion of ethane to high value-added chemicals is significantly important for utilization of hydrocarbon resources.However, it is a great challenge due to the typically required high temperature(>...The catalytic conversion of ethane to high value-added chemicals is significantly important for utilization of hydrocarbon resources.However, it is a great challenge due to the typically required high temperature(> 400 ℃) conditions.Herein, a highly active catalytic conversion process of ethane at room temperature(25 ℃) is reported on single iron atoms confined in graphene via the porphyrin-like N4-coordination structures.Combining with the operando time of flight mass spectrometer and density functional theory calculations, the reaction is identified as a radical mechanism, in which the C–H bonds of the same C atom are preferentially and sequentially activated, generating the value-added C2 chemicals, simultaneously avoiding the over-oxidation of the products to CO2.The in-situ formed O–FeN4–O structure at the single iron atom serves as the active center for the reaction and facilitates the formation of ethyl radicals.This work deepens the understanding of alkane C–H activation on the FeN4 center and provides the reference in development of efficient catalyst for selective oxidation of light alkane.展开更多
文摘Complex oxides are an important class of materials with enormous potential for electrochemical appli-cations.Depending on their composition and structure,such complex oxides can exhibit either a single conductivity(oxygen-ionic or protonic,or n-type,or p-type electronic)or a combination thereof gener-ating distinct dual-conducting or even triple-conducting materials.These properties enable their use as diverse functional materials for solid oxide fuel cells,solid oxide electrolysis cells,permeable membranes,and gas sensors.The literature review shows that the field of solid oxide materials and related electro-chemical cells has a significant level of research engagement,with over 8,000 publications published since 2020.The manual analysis of such a large volume of material is challenging.However,by examining the review articles,it is possible to identify key patterns,recent achievements,prospects,and remaining obstacles.To perform such an analysis,the present article provides,for the first time,a comprehensive summary of previous review publications that have been published since 2020,with a special focus on solid oxide materials and electrochemical systems.Thus,this study provides an important reference for researchers specializing in the fields of solid state ionics,high-temperature electrochemistry,and energyconversiontechnologies.
基金supported by the Korea Basic Science Institute(National research Facilities and Equipment Center)grant funded by the Ministry of Education(2019R1A6C1010042,2021R1A6C103A427)the financial support from the National Research Foundation of Korea(NRF)(2022R1A2C2010686,2022R1A4A3033528,2021R1I1A1A01060380,2021R1C1C2010726,2019H1D3A1A01071209)。
文摘The electrocatalytic oxidation of biomass-derived furfural(FF)feedstocks into 2-furoic acid(FA)holds immense industrial potential in optics,cosmetics,polymers,and food.Herein,we fabricated Co O/Ni O/nickel foam(NF)and Cu_(2)O/Ni O/NF electrodes via in situ pulsed laser irradiation in liquids(PLIL)for the bifunctional electrocatalysis of oxygen evolution reaction(OER)and furfural oxidation reaction(FOR),respectively.Simultaneous oxidation of NF surface to NiO and deposition of CoO and/or Cu_(2)O on NF during PLIL offer distinct advantages for enhancing both the OER and FOR.CoO/NiO/NF electrocatalyst provides a consistently low overpotential of~359 m V(OER)at 10 m A/cm^(2),achieving the maximum FA yield(~16.37 m M)with 61.5%selectivity,79.5%carbon balance,and a remarkable Faradaic efficiency of~90.1%during 2 h of FOR at 1.43 V(vs.reversible hydrogen electrode).Mechanistic pathway via in situ electrochemical-Raman spectroscopy on CoO/NiO/NF reveals the involvement of phase transition intermediates(NiOOH and CoOOH)as surface-active centers during electrochemical oxidation.The carbonyl carbon in FF is attacked by hydroxyl groups to form unstable hydrates that subsequently undergo further oxidation to yield FA products.This method holds promise for large-scale applications,enabling simultaneous production of renewable building materials and fuel.
基金supported by the National Key R&D Program of China(Grant No.2016YFC0501103)the National Natural Science Foundation of China[Grant No.420701250].
文摘Opencast coal mining has a large impact on the land surface,both at the mining pits themselves and at waste sites.After artifcial management is stopped,a reclaimed opencast coal mine dump is afected by wind and water erosion from natural processes,resulting in land degradation and even safety incidents.In this paper,the soil erosion and land degradation after 5 years of such natural processes,at the Xilinhot opencast coal mine dump in Inner Mongolia,were investigated.A multisource data acquisition method was applied:the vegetation fraction coverage(VFC)was extracted from GF-1 satellite imagery,high-precision terrain characteristics and the location and degree of soil erosion were obtained using a drone,and the physical properties of the topsoil were obtained by feld sampling.On this basis,the degree and spatial distribution of erosion cracks were identifed,and the causes of soil erosion and land degradation were analyzed using the geographical detector.The results show that(1)multi-source data acquisition method can provide efective basic data for the quantitative evaluation of the ecological environment at dumps,and(2)slope aspect and VFC are the main factors afecting the degree of degradation and soil erosion.Based on above analysis,several countermeasures are proposed to mitigate land degradation:(1)The windward slope be designed to imitate the natural landform.(2)Reasonable engineering measures should be applied at the slope to restrain soil erosion.(3)The Pioneer plants should be widely planted on the platform at the early stage of reclamation.
基金National Research Foundation of Korea,Grant/Award Numbers:2019H1D3A1A01071209,2021R1I1A1A01060380,2022R1A2C2010686,2022R1A4A3033528Korea Basic Science Institute,Grant/Award Numbers:2019R1A6C1010042,2021R1A6C103A427。
文摘We investigated the role of metal atomization and solvent decomposition into reductive species and carbon clusters in the phase formation of transition-metal carbides(TMCs;namely,Co_(3)C,Fe_(3)C,TiC,and MoC)by pulsed laser ablation of Co,Fe,Ti,and Mo metals in acetone.The interaction between carbon s-p-orbitals and metal d-orbitals causes a redistribution of valence structure through charge transfer,leading to the formation of surface defects as observed by X-ray photoelectron spectroscopy.These defects influence the evolved TMCs,making them effective for hydrogen and oxygen evolution reactions(HER and OER)in an alkaline medium.Co_(3)C with more oxygen affinity promoted CoO(OH)intermediates,and the electrochemical surface oxidation to Co_(3)O_(4)was captured via in situ/operando electrochemical Raman probes,increasing the number of active sites for OER activity.MoC with more d-vacancies exhibits strong hydrogen binding,promoting HER kinetics,whereas Fe_(3)C and TiC with more defect states to trap charge carriers may hinder both OER and HER activities.The results show that the assembled membrane-less electrolyzer with Co_(3)C∥Co_(3)C and MoC∥MoC electrodes requires~2.01 and 1.99 V,respectively,to deliver a 10 mA cm−2 with excellent electrochemical and structural stability.In addition,the ascertained pulsed laser synthesis mechanism and unit-cell packing relations will open up sustainable pathways for obtaining highly stable electrocatalysts for electrolyzers.
基金supported by the Korea Basic Science Institute(National research Facilities and Equipment Center)grant funded by the Ministry of Education(No.2019R1A6C1010042)the financial support from the National Research Foundation of Korea(NRF)(2022R1A2C2010686,2022R1A4A3033528,2021R1C1C2010726)。
文摘Herein,we propose a simple and rapid approach for synthesizing a CuS/Ru composite that serves as a bifunctional electrocatalyst to promote hydrogen production and concurrently convert sulfion into a value-added sulfur product.This composite comprises Ru nanoclusters supported on the CuS nanostructure,achieved through simple pulsed laser irradiation in liquid approach.The optimized CuS/Ru-30 electrocatalyst demonstrates remarkable bifunctional electrocatalytic activity,exhibiting a negligible working potential of 0.28 V(vs.RHE)for the anodic sulfion oxidation reaction(SOR)and a minimal overpotential of 182 m V for cathodic hydrogen evolution reaction(HER)to achieve 10 mA cm^(-2)of current density.Moreover,the Cu S/Ru-30 electrocatalyst shows exceptional selectivity for converting sulfion into valuable sulfur during anodic oxidation reactions.Remarkably,in a two-electrode electrolyzer system utilizing Cu S/Ru-30 as both the anode and cathode,the SOR+HER coupled water electrolysis system demands only 0.52 V to reach 10 mA cm^(-2),which is considerably lesser compared to the OER+HER coupled water electrolysis(1.85 V).The experimental results and density function theory(DFT)calculations reveal that the strong electron interaction between CuS and Ru nanoclusters generates a built-in electric field,greatly enhancing electron transfer efficiency.This significantly boosts the HER performance and facilitates the adsorption and production of sulfur intermediates.This study presents a rapid and simple strategy for synthesizing a dual-functional catalyst suitable for low-voltage hydrogen generation while facilitating the recovery of valuable sulfur sources.
基金supported by the National Natural Science Foundation of China(No.22306178 and 22176155)Outstanding Youth Talents of Sichuan Science and Technology Program(No.22JCQN0061)+1 种基金National Natural Science Foundation of China(No.22306012)Guangdong Basic and Applied Basic Research Foundation(No.2022A1515110578).
文摘In semiconductor photocatalysts,the easy recombination of photogenerated carriers seriously affects the application of photocatalytic materials in water treatment.To solve the serious problem of electron−hole pair recombination in perylene diimide(PDI)organic semiconductors,we loaded ferric hydroxyl oxide(FeOOH)on PDI materials,successfully prepared novel FeOOH@PDI photocatalytic materials,and constructed a photo-Fenton system.The system was able to achieve highly efficient degradation of BPA under visible light,with a degradation rate of 0.112 min^(−1)that was 20 times higher than the PDI system,and it also showed universal degradation performances for a variety of emerging organic pollutants and anti-interference ability.The mechanism research revealed that the FeOOH has the electron trapping property,which can capture the photogenerated electrons on the surface of PDI,effectively reducing the compounding rate of photogenerated carriers of PDI and accelerating the iron cycling and H2O2 activation on the surface of FeOOH at the same time.This work provides new insights and methods for solving the problem of easy recombination of carriers in semiconductor photocatalysts and degrading emerging organic pollutants.
基金supported by the National Natural Science Foundation of China(Grant Nos.12234016,12174317,and 12074031)the New Cornerstone Science Foundation.
文摘Recently,high temperature(T_(c)≈80 K)superconductivity(SC)has been discovered in La_(3)Ni_(2)O_(7)(LNO)under pressure.This raises the question of whether the superconducting transition temperature T_(c) could be further enhanced under suitable conditions.One possible route for achieving higher T_(c) is element substitution.Similar SC could appear in the Fmmm phase of rare-earth(RE)R_(3)Ni_(2)O_(7)(RNO,R=RE element)material series under suitable pressure.The electronic properties in the RNO materials are dominated by the Ni 3d orbitals in the bilayer NiO_(2) plane.In the strong coupling limit,the SC could be fully characterized by a bilayer single 3d_(x^(2)−y^(2))-orbital t–J‖–J⊥ model.With RE element substitution from La to other RE element,the lattice constant of the Fmmm RNO material decreases,and the resultant electronic hopping integral increases,leading to stronger superexchanges between the 3d_(x^(2)−y^(2)) orbitals.Based on the slave-boson mean-field theory,we explore the pairing nature and the evolution of T_(c) in RNO materials under pressure.Consequently,it is found that the element substitution does not alter the pairing nature,i.e.,the inter-layer s-wave pairing is always favored in the superconducting RNO under pressure.However,the T_(c) increases from La to Sm,and a nearly doubled T_(c) could be realized in SmNO under pressure.This work provides evidence for possible higher T_(c) R_(3)Ni_(2)O_(7) materials,which may be realized in further experiments.
基金supported by the“Pioneer”and“Leading Goose”R&D Program of Zhejiang(Grant No.2024SDXHDX0007)the National Natural Science Foundation of China(Grant No.12474131)+4 种基金the China Postdoctoral Science Foundation(Grant Nos.2022M722845 and 2023T160586)the Zhejiang Provincial Natural Science Foundation of China for Distinguished Young Scholars(Grant No.LR23A040001)the Research Center for Industries of the Future(RCIF)at Westlake University(Grant No.WU2023C009)the National Key R&D Program of China(Grant Nos.2020YFA0308800 and 2022YFA1403400)the Beijing Natural Science Foundation(Grant No.Z210006).The authors thank the support provided by Dr.Chao Zhang from Instrumentation and Service Center for Physical Sciences at Westlake University.
文摘The hysteresis of magnetoresistance observed in superconductors is of great interest due to its potential connectionwith unconventional superconductivity.In this study,we perform electrical transport measurements on kagome superconductorCsV_(3)Sb_(5)nanoflakes and uncover unusual hysteretic behavior of magnetoresistance in the superconducting state.This hysteresis can be induced by applying either a large DC or AC current at temperatures(T)well below the superconductingtransition temperature(T_(c)).As T approaches T_(c),similar weak hysteresis is also detected by applying a smallcurrent.Various scenarios are discussed,with particular focus on the effects of vortex pinning and the presence of timereversal-symmtery-breaking superconducting domains.Our findings support the latter,hinting at chiral superconductivityin kagome superconductors.
文摘The article presents the composition and current state of poisonous plants distributed on the Ustyurt plateau. Ustyurt is one of the largest deserts in Central Asia, differing from other deserts of the world in geographical location, relief, flora and fauna and other features. The territory of Ustyurt occupies 21.3 million hectares, of which the Karakalpak part accounts for 7.2 million hectares. Poisonous alkaloid-bearing plants of the Karakalpak part of the Ustyurt plateau Anabasis aphylla, Atriplex flabellum, Kalidium capsicum, Salsola arbusculaeformis, Salsola foliosa, Aellenia subaphylla, Anabasis brachiata, Rheum tataricum, Capparis spinosa, Glycyrrhiza aspera. Alkaloid-bearing plants that are not eaten or poorly eaten by cattle Ephedra distachya, Delphinium songaricum, Anabasis salsa, alkaloid-bearing plants eaten by animals without harm Carex physodes, Eremopyrum orientale, Agrophyllum repens, Astragalus amodendron, Astragalus villosissimus, species of the genera Calligonum, Salsola. Poisonous plants of the Karakalpak part of the Ustyurt plateau. An analysis of the pasture flora of the Karakalpak part of the Ustyurt plateau shows that 62 species of wild poisonous plants belonging to 49 genera and 19 families grow here. Although these plants are considered poisonous, but in modern pharmaceutics and medicine, they are used as medicinal.
基金upported by the National Natural Science Foundation of China(NSFC,Grant No.12033005)the National Key R&D Program of China(No.2022YFA1603102)+2 种基金the China Manned Space Project(CMS-CSST-2021-A09,CMS-CSST-2021-B06)the China-Chile Joint Research Fund(CCJRF No.2211)support from the Tianchi Talent Program of Xinjiang Uygur Autonomous Region。
文摘Leveraging the high resolution,sensitivity,and wide frequency coverage of the Atacama Large Millimeter/submillimeter Array(ALMA),the QUARKS survey,standing for“Querying Underlying mechanisms of massive star formation with ALMA-Resolved gas Kinematics and Structures”,is observing 139 massive starforming clumps at ALMA Band 6(λ~1.3 mm).This paper introduces the Atacama Compact Array(ACA)7 m data of the QUARKS survey,describing the ACA observations and data reduction.Combining multiwavelength data,we provide the first edition of QUARKS atlas,offering insights into the multiscale and multiphase interstellar medium in high-mass star formation.The ACA 1.3 mm catalog includes 207 continuum sources that are called ACA sources.Their gas kinetic temperatures are estimated using three formaldehyde transitions with a non-LTE radiation transfer model,and the mass and density are derived from a dust emission model.The ACA sources are massive(16–84 percentile values of 6–160 M_(⊙)),gravity-dominated(M∝R^(1.1))fragments within massive clumps,with supersonic turbulence(M>1)and embedded star-forming protoclusters.We find a linear correlation between the masses of the fragments and the massive clumps,with a ratio of 6%between the two.When considering fragments as representative of dense gas,the ratio indicates a dense gas fraction(DGF)of 6%,although with a wide scatter ranging from 1%to 10%.If we consider the QUARKS massive clumps to be what is observed at various scales,then the size-independent DGF indicates a self-similar fragmentation or collapsing mode in protocluster formation.With the ACA data over four orders of magnitude of luminosity-to-mass ratio(L/M),we find that the DGF increases significantly with L/M,which indicates clump evolutionary stage.We observed a limited fragmentation at the subclump scale,which can be explained by a dynamic global collapse process.
文摘After the mass closures of entire coal mine districts in Europe at the end of the last century, a new phenomenon of surface movement was observed—an upward movement.Although most surface movement(i.e., subsidence) occurs in the months and years after mining by the longwall method, surface movement still occurs many decades after mining is terminated.After the closure and flooding of underground excavations and surrounding rock, this movement was reversed.This paper focuses on quantifying the upward movement in two neighboring coal mines(Winterslag and Zwartberg, Belgium).The study is based on data from a remote sensing technique: interferometry with synthetic aperture radar(INSAR).The results of the study show that the rate of upward movement in the decade after closure is about 10 mm/year on average.The upward movements are not linked directly to the past exploitation directly underneath a location.The amounts of subsidence at specific locations are linked mainly to their positions relative to an inverse trough shape situated over the entire mined-out areas and their immediate surroundings.Local features, such as geological faults, can have a secondary effect on the local variation of the uplift.The processes of subsidence and uplift are based on completely different mechanisms.Subsidence is initiated by a caving process, while the process of uplift is clearly linked to flooding.
基金the National Infrastructure of Mineral Rock and Fossil Resources for Sciences and Technology Program(2005DKA21405-7)the Science and Technology Research and Development Program of Changchun City(04-07SF092)supported by an FNRS grant.
文摘A new basal neoceratopsian dinosaur, Helioceratops brachygnathus gen. et sp. nov., is described from the Quantou Formation (late Early Cretaceous or early Late Cretaceous) in the Liufangzi locality (Jilin province, China). Helioceratops differs from other basal neoceratopsians with its deep dentary ramus, its steeply-inclined ventral predentary facet, its heterogeneous dentary crowns, and by the denticles and secondary ridges asymmetrically distributed on either side of the primary ridge on its dentary teeth. Along with Auroraceratops and Yamaceratops, Helioceratops represents one of the most derived non-coronosaurian neoceratopsians. The palaeogeographical distribution of basal neoceratopsians appears limited to northern China and southern Mongolia in the current state of our knowledge. It is therefore probable that this region constituted the birthplace for more advanced, Late Cretaceous Coronosanria.
文摘The Cretaceous/Paleogene (K/Pg) Working Group, after many years of studies, voted to define the Global Stratotype Section and Point (GSSP) for the base of the Danian Stage at the base of the boundary clay at a section near El Kef Tunisia. The GSSP was approved by the International Commission on Stratigraphy (ICS) and ratified by the International Union of Geological Sciences (IUGS) in 1991. Nevertheless, the GSSP was not officially published, although some papers dealing with geological aspects of the K/Pg boundary at El Kef have been published and this is quite well known. In April 2006, the GSSP was revisited, a marker was put in place and protection of the site was requested. Many correlation criteria are present at the GSSP of which the most useful are the meteorite impact evidence (iridium anomaly, Ni-rich spinel, etc.) and the mass extinction of planktic micro- and nannofossils. This event coincides with the GSSP, allowing us to propose that the K/Pg boundary is marked exactly by the moment of the meteorite impact, which implies that all the sediments generated by the impact belong to the Danian. This definition solves problems of correlation in the Yucatan peninsula (Mexico) and its surroundings.
基金Supported by National Natural Science Foundation of China, No. 30570665the Foundation of Dalian Technology Bureau, No. 2008E13SF182the Foundation of Key Laboratory of Education Department of Liaoning Province,No. 2009S005
文摘AIM: To investigate whether nicotinamide overload plays a role in type 2 diabetes. METHODS: Nicotinamide metabolic patterns of 14 diabetic and 14 non-diabetic subjects were compared using HPLC. Cumulative effects of nicotinamide and N^1-methylnicotinamide on glucose metabolism, plasma HzO2 levels and tissue nicotinamide adenine dinucleotide (NAD) contents of adult Sprague-Dawley rats were observed. The role of human sweat glands and rat skin in nicotinamide metabolism was investigated using sauna and burn injury, respectively. RESULTS: Diabetic subjects had significantly higher plasma N^1-methylnicotinamide levels 5 h after a 100-mg nicotinamide load than the non-diabetic subjects (0.89 ± 0.13 μmol/L vs 0.6 ± 0.13 μmol/L, P 〈 0.001). Cumulative doses of nicotinamide (2 g/kg) significantly increased rat plasma Nl-methylnicotinamide concentrations associated with severe insulin resistance, which was mimicked by Nl-methy-Inicotinamide. Moreover, cumulative exposure to N^1- methylnicotinamide (2 g/kg) markedly reduced rat muscle and liver NAD contents and erythrocyte NAD/ NADH ratio, and increased plasma H2O2 levels. Decrease in NAD/NADH ratio and increase in H2O2 generation were also observed in human erythrocytes after exposure to N^1-methylnicotinamide in vitro. Sweating eliminated excessive nicotinamide (5.3-fold increase in sweat nicotinamide concentration 1 h after a 100-mg nicotinamide load). Skin damage or aldehyde oxidase inhibition with tamoxifen or olanzapine, both being notorious for impairing glucose tolerance, delayed N^1- methylnicotinamide clearance. CONCLUSION: These findings suggest that nicotinamide overload, which induced an increase in plasma N^1- methylnicotinamide, associated with oxidative stress and insulin resistance, plays a role in type 2 diabetes.
基金Supported by the Russian Science Foundation,No.16-15-00039
文摘AIM To investigate the temporal sequence of pathological changes in the cellular structures of retina and choroidea in the early stages of diabetes in laboratory animals.METHODS Experimental type 1 diabetes was modeled by three intraperitoneal injections of an alloxan solution into 30 male nonlinear rats at 16 wk of age. The 30 th and 60 th days from the final alloxan injection were chosen as the endpoints. Light and electron microscopy and morphometric and immunohistochemical studies were performed on histological slices of eyeballs from experimental animals.RESULTS Diabetic disturbances progressed to 60 d of the experiment. Thus, in the retina, a partial destruction of photoreceptors accompanied by interstitial edema was observed. The morphometric analysis revealed a reduction in the thickness of the retina. A reduction in the number of blood vessels of the choroid with disturbances of the endothelial cells and the vascular walls and a persistent reduction in the number of melanocytes were observed. The number of proliferating Ki-67 positive cells decreased, and the number of macrophages increased with diabetes development.CONCLUSION The starting point in the development of destructive changes involves early reduction in the number of melanocytes of the choroidea and alterations in the retinal pigment epithelium.
文摘The timing of reproduction can significantly affect an offspring's fitness, thereby also influencing the fitness of the parents, especially in species inhabiting extreme environments, such as deserts. Female reproductive cycles in Phrynocephalus przewalskii were studied from April to September 2008. Significant cycles of gonadal volume were found in all studied populations and the cycles were similar among the various populations. Females began vitellogenesis in April and contained oviductal eggs form May to June. Gonad volume decreased significantly in July and reached minimum volume from August to September. The follicular growth was negatively correlated with increasing precipitation and temperature in all populations. Hatching occurs during summer and early fall, when most of the annual rainfall occurs. Mean clutch size based on all populations was 2.7 ± 0.9 SE (n = 71).
基金Supported by the National Key R&D Program of China(Grant No.2019YFA0709503)the Shanghai Sailing Program+3 种基金the Natural Science Foundation of Shanghai(Grant No.20ZR1429000)the National Natural Science Foundation of China(Grant No.62002221)Shanghai Municipal of Science and Technology Project(Grant No.20JC1419500)the HPC of School of Mathematical Sciences at Shanghai Jiao Tong University。
文摘Why heavily parameterized neural networks(NNs) do not overfit the data is an important long standing open question. We propose a phenomenological model of the NN training to explain this non-overfitting puzzle. Our linear frequency principle(LFP) model accounts for a key dynamical feature of NNs: they learn low frequencies first, irrespective of microscopic details. Theory based on our LFP model shows that low frequency dominance of target functions is the key condition for the non-overfitting of NNs and is verified by experiments. Furthermore,through an ideal two-layer NN, we unravel how detailed microscopic NN training dynamics statistically gives rise to an LFP model with quantitative prediction power.
基金National Natural Science Foundation of China(Grant Nos.11422427 and 11402069)the Program for Professor of Special Appointment at Shanghai Institutions of Higher Learning,China(Grant No.GZ2016004).
文摘We investigate rotational dynamics of an actively driven rotor through experiments and numerical simulations. While probability density distributions of rotor angular velocity are strongly non-Gaussian, relative probabilities of observing rotation in opposite directions are shown to be linearly related to the angular velocity magnitude. We construct a stochastic model to describe transitions between different states from rotor angular velocity data and use the stochastic model to show that symmetry properties in probability density distributions are related to the detailed fluctuation relation(FR) of entropy productions.
基金Supported by the National Key Research and Development Program of China (Grant No.2016YFA0302001)the National Natural Science Foundation of China (Grant Nos.11774224,12074244,11521404,and 61701394)+1 种基金support from the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learningadditional support from a Shanghai talent program。
文摘Detection of local strain at the nanometer scale with high sensitivity remains challenging.Here we report near-field infrared nano-imaging of local strains in bilayer graphene by probing strain-induced shifts of phonon frequency.As a non-polar crystal,intrinsic bilayer graphene possesses little infrared response at its transverse optical phonon frequency.The reported optical detection of local strain is enabled by applying a vertical electrical field that breaks the symmetry of the two graphene layers and introduces finite electrical dipole moment to graphene phonon.The activated phonon further interacts with continuum electronic transitions,and generates a strong Fano resonance.The resulted Fano resonance features a very sharp near-field infrared scattering peak,which leads to an extraordinary sensitivity of-0.002%for the strain detection.Our results demonstrate the first nano-scale near-field Fano resonance,provide a new way to probe local strains with high sensitivity in non-polar crystals,and open exciting possibilities for studying strain-induced rich phenomena.
基金the financial support from the Ministry of Science and Technology of China (Nos.2016YFA0204100 and 2016YFA0200200)the National Natural Science Foundation of China (Nos.21890753, 21573220 and 21802124)+2 种基金the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences (No.QYZDB-SSW-JSC020)the DNL Cooperation Fund, CAS (No.DNL180201)the financial and technique supports from the Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University
文摘The catalytic conversion of ethane to high value-added chemicals is significantly important for utilization of hydrocarbon resources.However, it is a great challenge due to the typically required high temperature(> 400 ℃) conditions.Herein, a highly active catalytic conversion process of ethane at room temperature(25 ℃) is reported on single iron atoms confined in graphene via the porphyrin-like N4-coordination structures.Combining with the operando time of flight mass spectrometer and density functional theory calculations, the reaction is identified as a radical mechanism, in which the C–H bonds of the same C atom are preferentially and sequentially activated, generating the value-added C2 chemicals, simultaneously avoiding the over-oxidation of the products to CO2.The in-situ formed O–FeN4–O structure at the single iron atom serves as the active center for the reaction and facilitates the formation of ethyl radicals.This work deepens the understanding of alkane C–H activation on the FeN4 center and provides the reference in development of efficient catalyst for selective oxidation of light alkane.