Exploring carbon emission effects based on the evolution of residents’ dietary structure to achieve the carbon neutrality goal and mitigate climate change is an important task.This study took China as the research ob...Exploring carbon emission effects based on the evolution of residents’ dietary structure to achieve the carbon neutrality goal and mitigate climate change is an important task.This study took China as the research object(data excluding Hong Kong,Macao and Taiwan) and used the carbon emission coefficient method to quantitatively measure the food carbon emissions from 1987–2020,then analyzed the carbon emission effects under the evolution of dietary structure.The results showed that during the study period,the Chinese dietary structure gradually changed to a high-carbon consumption pattern.The dietary structure of urban residents developed to a balanced one,while that of rural residents developed to a high-quality one.During the study period,the per capita food carbon emissions and total food consumption of Chinese showed an increasing trend.The per capita food carbon emissions of residents in urban and rural showed an overall upward trend.The total food carbon emissions in urban increased significantly,while that in rural increased first and then decreased.The influence of beef and mutton on carbon emissions is the highest in dietary structure.Compared with the balanced dietary pattern,the food carbon emissions of Chinese residents had not yet reached the peak,but were evolving to a high-carbon consumption pattern.展开更多
The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct ...The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but challenging.Herein,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation.Simultaneously,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction barrier.As a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.展开更多
Rock-encased-backfill(RB)structures are common in underground mining,for example in the cut-andfill and stoping methods.To understand the effects of cyclic excavation and blasting activities on the damage of these RB ...Rock-encased-backfill(RB)structures are common in underground mining,for example in the cut-andfill and stoping methods.To understand the effects of cyclic excavation and blasting activities on the damage of these RB structures,a series of triaxial stepwise-increasing-amplitude cyclic loading experiments was conducted with cylindrical RB specimens(rock on outside,backfill on inside)with different volume fractions of rock(VF=0.48,0.61,0.73,and 0.84),confining pressures(0,6,9,and 12 MPa),and cyclic loading rates(200,300,400,and 500 N/s).The damage evolution and meso-crack formation during the cyclic tests were analyzed with results from stress-strain hysteresis loops,acoustic emission events,and post-failure X-ray 3D fracture morphology.The results showed significant differences between cyclic and monotonic loadings of RB specimens,particularly with regard to the generation of shear microcracks,the development of stress memory and strain hardening,and the contact forces and associated friction that develops along the rock-backfill interface.One important finding is that as a function of the number of cycles,the elastic strain increases linearly and the dissipated energy increases exponentially.Also,compared with monotonic loading,the cyclic strain hardening characteristics are more sensitive to rising confining pressures during the initial compaction stage.Another finding is that compared with monotonic loading,more shear microcracks are generated during every reloading stage,but these microcracks tend to be dispersed and lessen the likelihood of large shear fracture formation.The transition from elastic to plastic behavior varies depending on the parameters of each test(confinement,volume fraction,and cyclic rate),and an interesting finding was that the transformation to plastic behavior is significantly lower under the conditions of 0.73 rock volume fraction,400 N/s cyclic loading rate,and 9 MPa confinement.All the findings have important practical implications on the ability of backfill to support underground excavations.展开更多
We present a study of low surface brightness galaxies(LSBGs) selected by fitting the images for all the galaxies inα.40 SDSS DR7 sample with two kinds of single-component models and two kinds of two-component models(...We present a study of low surface brightness galaxies(LSBGs) selected by fitting the images for all the galaxies inα.40 SDSS DR7 sample with two kinds of single-component models and two kinds of two-component models(disk+bulge):single exponential,single sersic,exponential+deVaucular(exp+deV),and exponential+sérsic(exp+ser).Under the criteria of the B band disk central surface brightness μ_(0,disk)(B)≥22.5 mag arcsec^(-2) and the axis ratio b/a> 0.3,we selected four none-edge-on LSBG samples from each of the models which contain 1105,1038,207,and 75 galaxies,respectively.There are 756 galaxies in common between LSBGs selected by exponential and sersic models,corresponding to 68.42% of LSBGs selected by the exponential model and 72.83% of LSBGs selected by the sersic model,the rest of the discrepancy is due to the difference in obtaining μ_(0) between the exponential and sersic models.Based on the fitting,in the range of 0.5≤n≤1.5,the relation of μ_(0) from two models can be written as μ_(0,sérsic)-μ_(0,exp)=-1.34(n-1).The LSBGs selected by disk+bulge models(LSBG_(2)comps) are more massive than LSBGs selected by single-component models(LSBG_1comp),and also show a larger disk component.Though the bulges in the majority of our LSBG_(2)comps are not prominent,more than 60% of our LSBG_(2)comps will not be selected if we adopt a single-component model only.We also identified 31 giant low surface brightness galaxies(gLSBGs) from LSBG_(2)comps.They are located at the same region in the color-magnitude diagram as other gLSBGs.After we compared different criteria of gLSBGs selection,we find that for gas-rich LSBGs,M_(*)> 10^(10)M_⊙ is the best to distinguish between gLSBGs and normal LSBGs with bulge.展开更多
The star-forming clumps in star-bursting dwarf galaxies provide valuable insights into understanding the evolution of dwarf galaxies.In this paper,we focus on five star-bursting dwarf galaxies featuring off-centered c...The star-forming clumps in star-bursting dwarf galaxies provide valuable insights into understanding the evolution of dwarf galaxies.In this paper,we focus on five star-bursting dwarf galaxies featuring off-centered clumps in the Mapping Nearby Galaxies at Apache Point Observatory survey.Using the stellar population synthesis software Fitting Analysis using Differential evolution Optimization,we obtain the spatially resolved distribution of the star formation history,which allows us to construct the g-band images of the five galaxies at different ages.These images can help us to probe the evolution of the morphological structures of these galaxies.While images of a stellar population older than 1 Gyr are typically smooth,images of a stellar population younger than 1 Gyr reveal significant clumps,including multiple clumps which appear at different locations and even different ages.To study the evolutionary connections of these five galaxies to other dwarf galaxies before their star-forming clumps appear,we construct the images of the stellar populations older than three age nodes,and define them to be the images of the"host"galaxies.We find that the properties such as the central surface brightness and the effective radii of the hosts of the five galaxies are in between those of dwarf ellipticals(dEs)and dwarf irregulars(dIrrs),with two clearly more similar to dEs and one more similar to dIrrs.Among the five galaxies,8257-3704 is particularly interesting,as it shows a previous starburst event that is not quite visible from its gri image,but only visible from images of the stellar population at a few hundred million years.The star-forming clump associated with this event may have appeared at around 600 Myr ago and disappeared at around 40 Myr ago.展开更多
The structural parameters of a galaxy can be used to gain insight into its formation and evolution history.In this paper,we strive to compare the Milky Way’s structural parameters to other,primarily edge-on,spiral ga...The structural parameters of a galaxy can be used to gain insight into its formation and evolution history.In this paper,we strive to compare the Milky Way’s structural parameters to other,primarily edge-on,spiral galaxies in order to determine how our Galaxy measures up to the Local Universe.For our comparison,we use the galaxy structural parameters gathered from a variety of literature sources in the optical and near-infrared wave bands.We compare the scale length,scale height,and disk flatness for both the thin and thick disks,the thick-to-thin disk mass ratio,the bulge-to-total luminosity ratio,and the mean pitch angle of the Milky Way’s spiral arms to those in other galaxies.We conclude that many of the Milky Way’s structural parameters are largely ordinary and typical of spiral galaxies in the Local Universe,though the Galaxy’s thick disk appears to be appreciably thinner and less extended than expected from zoom-in cosmological simulations of Milky Way-mass galaxies with a significant contribution of galaxy mergers involving satellite galaxies.展开更多
How galaxies assemble masses through their own star formation or interaction with the external environment is still an important topic in the field of galaxy formation and evolution.We use Value Added Catalogs with ga...How galaxies assemble masses through their own star formation or interaction with the external environment is still an important topic in the field of galaxy formation and evolution.We use Value Added Catalogs with galaxy features that are spatially and temporally resolved from Sloan Digital Sky Survey Data Release 17 to investigate the mass growth histories of early-type galaxies(ETGs)and late-type galaxies(LTGs).We find that the mass growth of ETGs is earlier than that of LTGs for massive galaxies(M_(*)>10^(10)M_⊙),while low-mass(M_(*)≤10^(10)M_⊙)ETGs have statistically similar mass assembly histories as low-mass LTGs.The stellar metallicity of all massive galaxies shows a negative gradient and basically does not change with time.However,in low-mass galaxies,the stellar metallicity gradient of elliptical galaxies is negative,and the stellar metallicity gradient of lenticular and spiral galaxies evolves from positive to negative.ETGs are not all in a high-density environment,but exhibit mass dependence.As the tidal strength increases,the star formation rate of low-mass ETGs rapidly decreases.These results support a picture where massive galaxies exhibit inside-out quenching mode,while low-mass galaxies show outside-in quenching mode.Environmental effects play an important role in regulating the mass assembly histories of low-mass ETGs.展开更多
Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent year...Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent years,deformable catalysts for HER have made great progress and would become a research hotspot.The catalytic activities of deformable catalysts could be adjustable by the strain engineering and surface reconfiguration.The surface curvature of flexible catalytic materials is closely related to the electrocatalytic HER properties.Here,firstly,we systematically summarized self-adaptive catalytic performance of deformable catalysts and various micro–nanostructures evolution in catalytic HER process.Secondly,a series of strategies to design highly active catalysts based on the mechanical flexibility of lowdimensional nanomaterials were summarized.Last but not least,we presented the challenges and prospects of the study of flexible and deformable micro–nanostructures of electrocatalysts,which would further deepen the understanding of catalytic mechanisms of deformable HER catalyst.展开更多
Using archival Fermi-LAT data with a time span of~12 yr,we study the population of Millisecond Pulsars(MSPs)in Globular Clusters(GlCs)and investigate their dependence on cluster dynamical evolution in the Milky Way.We...Using archival Fermi-LAT data with a time span of~12 yr,we study the population of Millisecond Pulsars(MSPs)in Globular Clusters(GlCs)and investigate their dependence on cluster dynamical evolution in the Milky Way.We show that theγ-ray luminosity(L_(γ))and emissivity(i.e.,ε_(γ)=L_(γ)/M,with M the cluster mass)are good indicators of the population and abundance of MSPs in GlCs,and they are highly dependent on the dynamical evolution history of the host clusters.Specifically speaking,the dynamically older GlCs with more compact structures are more likely to have larger L_(γ)andε_(γ),and these trends can be summarized as strong correlations with cluster stellar encounter rateΓand the specific encounter rate(Λ=Γ/M),with L_(γ)∝Γ^(0.7±0.11)andε_(γ)∝Λ^(0.73±0.13)for dynamically normal GlCs.However,as GlCs evolve into deep core collapse,these trends are found to be reversed,implying that strong encounters may have lead to the disruption of Low-Mass X-ray Binaries and ejection of MSPs from core-collapsed systems.Besides,the GlCs are found to exhibit largerε_(γ)with increasing stellar mass function slope(ε_(γ)∝10^((0.52±0.1)α)),decreasing tidal radius(ε_(γ)∝R_(t)^(-10±0.22))and distances from the Galactic Center(GC,ε_(γ)∝R_(gc)^(-1.13±0.21)).These correlations indicate that,as GlCs losing kinetic energy and spiral in toward the GC,tidal stripping and mass segregation have a preference in leading to the loss of normal stars from GlCs,while MSPs are more likely to concentrate to cluster center and be deposited into the GC.Moreover,we gaugeε_(γ)of GlCs is~10-1000 times larger than the Galactic bulge,the latter is thought to reside thousands of unresolved MSPs and may be responsible for the GC 7-ray excess,which supports that GlCs are generous contributors to the population of MSPs in the GC.展开更多
The far-field microdynamic disturbance caused by the excavation of deep mineral resources and underground engineering can induce surrounding rock damage in high-stress conditions and even lead to disasters.However,the...The far-field microdynamic disturbance caused by the excavation of deep mineral resources and underground engineering can induce surrounding rock damage in high-stress conditions and even lead to disasters.However,the mechanical properties and damage/fracture evolution mechanisms of deep rock induced by microdynamic disturbance under three-dimensional stress states are unclear.Therefore,a true triaxial multilevel disturbance test method is proposed,which can completely simulate natural geostress,excavation stress redistribution(such as stress unloading,concentration and rotation),and subsequently the microdynamic disturbance triggering damaged rock failure.Based on a dynamic true triaxial test platform,true triaxial microdynamic disturbance tests under different frequency and amplitudes were carried out on monzogabbro.The results show that increasing amplitude or decreasing frequency diminishes the failure strength of monzogabbro.Deformation modulus gradually decreases during disturbance failure.As frequency and amplitude increase,the degradation rate of deformation modulus decreases slightly,disturbance dissipated energy increases significantly,and disturbance deformation anisotropy strengthens obviously.A damage model has been proposed to quantitatively characterize the disturbance-induced damage evolution at different frequency and amplitude under true triaxial stress.Before disturbance failure,the micro-tensile crack mechanism is dominant,and the micro-shear crack mechanism increases significantly at failure.With the increase of amplitude and frequency,the micro-shear crack mechanism increases.When approaching disturbance failure,the acoustic emission fractal dimension changes from a stable value to local large oscillation,and finally increases sharply to a high value at failure.Finally,the disturbance-induced failure mechanism of surrounding rock in deep engineering is clearly elucidated.展开更多
Three mechanisms for an alternative to the Doppler effect as an explanation for the redshift are reviewed. A fourth mechanism is the attenuation of the light as given by the Beer-Lambert law. The average value of the ...Three mechanisms for an alternative to the Doppler effect as an explanation for the redshift are reviewed. A fourth mechanism is the attenuation of the light as given by the Beer-Lambert law. The average value of the Hubble constant is therefore derived by processing the galaxies of the NED-D catalog in which the distances are independent of the redshift. The observed anisotropy of the Hubble constant is reproduced by adopting a rim model, a chord model, and both 2D and 3D Voronoi diagrams.展开更多
Identification of the S genotype of Malus plants will greatly promote the discovery of new genes,the cultivation and production of apple,the breeding of new varieties,and the origin and evolution of self-incompatibili...Identification of the S genotype of Malus plants will greatly promote the discovery of new genes,the cultivation and production of apple,the breeding of new varieties,and the origin and evolution of self-incompatibility in Malus plants.In this experiment,88 Malus germplasm resources,such as Aihuahong,Xishuhaitang,and Reguanzi,were used as materials.Seven gene-specific primer combinations were used in the genotype identification.PCR amplification using leaf DNA produced a single S-RNase gene fragment in all materials.The results revealed that 70 of the identified materials obtained a complete S-RNase genotype,while only one S-RNase gene was found in 18 of them.Through homology comparison and analysis,13 S-RNase genotypes were obtained:S_(1)S_(2)(Aihuahong,etc.),S_(1)S_(28)(Xixian Haitang,etc.),S_(1)S_(51)(Hebei Pingdinghaitang),S_(1)S_(3)(Xiangyangcun Daguo,etc.),S_(2)S_(3)(Zhaiyehaitang,etc.),S_(3)S_(51)(Xishan 1),S_(3)S_(28)(Huangselihaerde,etc.),S_(2)S_(28)(Honghaitang,etc.),S_(4)S_(28)(Bo 11),S_(7)S_(28)(Jiuquan Shaguo),S_(10)S_e(Dongchengguan 13),S_(10)S_(21)(Dongxiangjiao)and S_(3)S_(51)(Xiongyue Haitang).Simultaneously,the frequency of the S gene in the tested materials was analyzed.The findings revealed that different S genes had varying frequencies in Malus resources,as well as varying frequencies between intraspecific and interspecific.S_(3) had the highest frequency of 68.18%,followed by S_(1)(42.04%).In addition,the phylogenetic tree and origin evolution analysis revealed that the S gene differentiation was completed prior to the formation of various apple species,that cultivated species also evolved new S genes,and that the S_(50) gene is the oldest S allele in Malus plants.The S_(1),S_(29),and S_(33) genes in apple-cultivated species,on the other hand,may have originated in M.sieversii,M.hupehensis,and M.kansuensis,respectively.In addition to M.sieversii,M.kansuensis and M.sikkimensis may have also played a role in the origin and evolution of some Chinese apples.展开更多
The corrosion rates of additive-manufactured Mg alloys are higher than their as-cast counterparts,possibly due to increased kinetics for the hydrogen evolution reaction on secondary phases,which may include oxide incl...The corrosion rates of additive-manufactured Mg alloys are higher than their as-cast counterparts,possibly due to increased kinetics for the hydrogen evolution reaction on secondary phases,which may include oxide inclusions.Scanning Kelvin Probe Force Microscopy demonstrated that MgO inclusions could act as cathodes for Mg corrosion,but their low conductivity likely precludes this.However,the density of state calculations through density functional theory using hybrid HSE06 functional revealed overlapping electronic states at the Mg/MgO interface,which facilitates electron transfers and participates in redox reactions.Subsequent determination of the hydrogen absorption energy at the Mg/MgO interface reveals it to be an excellent catalytic site,with HER being found to be a factor of 23x more efficient at the interface than on metallic Mg.The results not only support the plausibility of the Mg/MgO interface being an effective cathode to the adjacent anodic Mg matrix during corrosion but also contribute to the understanding of the enhanced cathodic activities observed during the anodic dissolution of magnesium.展开更多
The complex and volatile international landscape has significantly impacted global grain supply security. This study uses a complex network analysis model to examine the evolution and trends of the global major grain ...The complex and volatile international landscape has significantly impacted global grain supply security. This study uses a complex network analysis model to examine the evolution and trends of the global major grain trade from 1990 to 2020, focusing on network topology, centrality ranking, and community structure. There are three major findings. First, the global major grain trade network has expanded in scale, with a growing emphasis on diversification and balance. During the study period, the United States, Canada, China, and Brazil were the core nodes of the network. Grain-exporting countries were mainly situated in Asia, the Americas, and Europe, and importing countries in Asia, Africa, and Europe. Second, a significant increase in the number of high centrality countries with high export capacity occurred, benefiting from natural advantages such as fertile land and favorable climates. Third, the main global grain trade network is divided into four communities, with the Americas-Europe community being the largest and most widespread. The formation of the community pattern was influenced by geographic proximity, driven by the core exporting countries. Therefore, the world needs to enhance the existing trade model, promote the multi-polarization of the grain trade network, and establish a global vision for the future community. Countries and regions should participate actively in global grain trade security governance and institutional reform, expand trade links with other countries, and optimize import and export policies to reduce trade risks.展开更多
Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performan...Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performance for hydrogen evolution reaction(HER). With the VS concentration change from 2.4% to 8.5%, the H* adsorption strength on S sites changed and NiS_(2)-VS 5.9% shows the most optimized H* adsorption for HER with an ultralow onset potential(68 m V) and has long-term stability for 100 h in 1 M KOH media. In situ attenuated-total-reflection Fourier transform infrared spectroscopy(ATR-FTIRS) measurements are usually used to monitor the adsorption of intermediates. The S-H* peak of the Ni S_(2)-VS 5.9% appears at a very low voltage, which is favorable for the HER in alkaline media. Density functional theory calculations also demonstrate the Ni S_(2)-VS 5.9% has the optimal |ΔG^(H*)| of 0.17 e V. This work offers a simple and promising pathway to enhance catalytic activity via precise vacancies strategy.展开更多
By combination of the transient Raman spectroscopic measurement and the density functional theoretical calculations,the structural evolution and stability of TATB under shock compression was investigated.Due to the im...By combination of the transient Raman spectroscopic measurement and the density functional theoretical calculations,the structural evolution and stability of TATB under shock compression was investigated.Due to the improvement in synchronization control between two-stage light gas gun and the transient Raman spectra acquisition,as well as the sample preparation,the Raman peak of the N-O mode of TATB was firstly observed under shock pressure up to 13.6 GPa,noticeably higher than the upper limit of 8.5 GPa reported in available literatures.By taking into account of the continuous shift of the main peak and other observed Raman peaks,we did not distinguish any structural transition or any new species.Moreover,both the present Raman spectra and the time-resolved radiation of TATB during shock loading showed that TATB exhibits higher chemical stability than previous declaration.To reveal the detailed structural response and evolution of TATB under compression,the density functional theoretical calculations were conducted,and it was found that the pressure make N-O bond lengths shorter,nitro bond angles larger,and intermolecular and intra-molecular hydrogen bond interactions enhanced.The observed red shift of Raman peak was ascribed to the abnormal enhancement of H-bound effect on the scissor vibration mode of the nitro group.展开更多
A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high lumines...A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high luminescent quantum efficiency.What is more attractive is that the luminescent properties such as wavelength and intensity can be regulated by controlling the structure at the molecular level.Hence,it is time to summarize the related research on CN structural evolution and make a prospect on future developments.In this review,we first summarize the research history and multiple structural evolution of CN.Then,the progress of improving the luminescence performance of CN through structural evolution was discussed.Significantly,the relationship between CN structure evolution and energy conversion in the forms of photoluminescence,chemiluminescence,and electrochemiluminescence was reviewed.Finally,key challenges and opportunities such as nanoscale dispersion strategy,luminous efficiency improving methods,standardization evaluation,and macroscopic preparation of CN are highlighted.展开更多
Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy ...Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.展开更多
With the rapid urbanization process,the space of traditional villages in China is undergoing significant changes.Studying the spatial evolution of traditional villages is significant in promoting rural spatial transfo...With the rapid urbanization process,the space of traditional villages in China is undergoing significant changes.Studying the spatial evolution of traditional villages is significant in promoting rural spatial transformation and realizing rural revitalization and sustainable rural development.Based on the traceability analysis of spatial production theory,this paper constructed an analytical framework for the spatial production evolution of traditional villages,analyzed the spatial evolution process and characteristics of traditional villages by using buffer analysis,spatial syntax,and other research methods,and revealed the characteristics of the spatial production evolution of traditional villages and the driving mechanism.The results show that:(1)The village spatial formation and development follow the village life cycle theory and usually develop from embryonic villages to diversified and integrated villages;(2)The evolution of village spatial production is characterized by the diversity of material space,the sublimation of daily life space,and the integration of social system space and generalization of emotional space;(3)The evolution of village spatial production from backward and poor village to ecologically well-off village is influenced by a combination of factors;(4)The village has formed a spatial structure of"people-land-scape-culture-industry",realized comprehensive reconstruction and spatial reproduction.The study results reflect the spatial evolution characteristics of traditional villages in mountainous areas in a more comprehensive way,which helps to promote the protection and development of traditional villages in mountainous areas and,to a certain extent,provides a reference for the development of rural revitalization.展开更多
Constructing heterostructured nanohybrid is considered as a prominent route to fabricate alternative electrocatalysts to commercial Pt/C for hydrogen evolution reaction(HER).In this work,(NH_(4))_(4)[NiH_(6)Mo_(6)O_(4...Constructing heterostructured nanohybrid is considered as a prominent route to fabricate alternative electrocatalysts to commercial Pt/C for hydrogen evolution reaction(HER).In this work,(NH_(4))_(4)[NiH_(6)Mo_(6)O_(4)]·5H_(2)O polyoxometalates(NiMo_(6))are adopted as the cluster precursors for simple fabrication of heterostructured Pt-Ni_(3)Mo_(3)N nanohybrids supported by carbon black(Pt-Ni_(3)Mo_(3)N/C)without using additional N sources.The improved porosity and enhanced electronic interaction of Pt-Ni_(3)Mo_(3)N/C should be attributed to the integration of Pt with NiMo_(6),which favors the mass transport,promotes the formation of exposed catalytic sites,and benefits the regulation of intrinsic activity.Thus,the as-obtained Pt-Ni_(3)Mo_(3)N/C exhibits impressive and durable HER performance as indicated by the low overpotential of 13.7 mV at the current density of 10 mA cm^(-2) and the stable overpotential during continuous working at 100 mA cm^(-2) for 100 h.This work provides significant insights for the synthesis of new highly active heterostructured electrocatalysts for renewable energy devices.展开更多
基金Under the auspices of National Natural Science Foundation of China(No.42171230)。
文摘Exploring carbon emission effects based on the evolution of residents’ dietary structure to achieve the carbon neutrality goal and mitigate climate change is an important task.This study took China as the research object(data excluding Hong Kong,Macao and Taiwan) and used the carbon emission coefficient method to quantitatively measure the food carbon emissions from 1987–2020,then analyzed the carbon emission effects under the evolution of dietary structure.The results showed that during the study period,the Chinese dietary structure gradually changed to a high-carbon consumption pattern.The dietary structure of urban residents developed to a balanced one,while that of rural residents developed to a high-quality one.During the study period,the per capita food carbon emissions and total food consumption of Chinese showed an increasing trend.The per capita food carbon emissions of residents in urban and rural showed an overall upward trend.The total food carbon emissions in urban increased significantly,while that in rural increased first and then decreased.The influence of beef and mutton on carbon emissions is the highest in dietary structure.Compared with the balanced dietary pattern,the food carbon emissions of Chinese residents had not yet reached the peak,but were evolving to a high-carbon consumption pattern.
基金supported by the Taishan Scholar Program of Shandong Province,China (tsqn202211162)the National Natural Science Foundation of China (22102079)the Natural Science Foundation of Shandong Province of China (ZR2021YQ10,ZR2022QB163)。
文摘The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but challenging.Herein,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation.Simultaneously,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction barrier.As a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.
基金We acknowledge the funding support from the National Natural Science Foundation of China Youth Fund(Grant No.52004019)the National Natural Science Foundation of China(Grant No.41825018)China Postdoctoral Science Foundation(Grant No.2023M733481).
文摘Rock-encased-backfill(RB)structures are common in underground mining,for example in the cut-andfill and stoping methods.To understand the effects of cyclic excavation and blasting activities on the damage of these RB structures,a series of triaxial stepwise-increasing-amplitude cyclic loading experiments was conducted with cylindrical RB specimens(rock on outside,backfill on inside)with different volume fractions of rock(VF=0.48,0.61,0.73,and 0.84),confining pressures(0,6,9,and 12 MPa),and cyclic loading rates(200,300,400,and 500 N/s).The damage evolution and meso-crack formation during the cyclic tests were analyzed with results from stress-strain hysteresis loops,acoustic emission events,and post-failure X-ray 3D fracture morphology.The results showed significant differences between cyclic and monotonic loadings of RB specimens,particularly with regard to the generation of shear microcracks,the development of stress memory and strain hardening,and the contact forces and associated friction that develops along the rock-backfill interface.One important finding is that as a function of the number of cycles,the elastic strain increases linearly and the dissipated energy increases exponentially.Also,compared with monotonic loading,the cyclic strain hardening characteristics are more sensitive to rising confining pressures during the initial compaction stage.Another finding is that compared with monotonic loading,more shear microcracks are generated during every reloading stage,but these microcracks tend to be dispersed and lessen the likelihood of large shear fracture formation.The transition from elastic to plastic behavior varies depending on the parameters of each test(confinement,volume fraction,and cyclic rate),and an interesting finding was that the transformation to plastic behavior is significantly lower under the conditions of 0.73 rock volume fraction,400 N/s cyclic loading rate,and 9 MPa confinement.All the findings have important practical implications on the ability of backfill to support underground excavations.
基金supported by the National Key R&D Program of China (grant No.2022YFA1602901)support of the National Natural Science Foundation of China(NSFC) grant Nos. 12090040, 12090041, and 12003043+5 种基金supported by the Youth Innovation Promotion AssociationCAS (No. 2020057)the science research grants of CSST from the China Manned Space Projectsupport of the NSFC grant Nos.11733006 and U1931109supported by the Strategic Priority Research Program of the Chinese Academy of Sciences,Grant No. XDB0550100partially supported by the Open Project Program of the Key Laboratory of Optical Astronomy,National Astronomical Observatories,Chinese Academy of Sciences。
文摘We present a study of low surface brightness galaxies(LSBGs) selected by fitting the images for all the galaxies inα.40 SDSS DR7 sample with two kinds of single-component models and two kinds of two-component models(disk+bulge):single exponential,single sersic,exponential+deVaucular(exp+deV),and exponential+sérsic(exp+ser).Under the criteria of the B band disk central surface brightness μ_(0,disk)(B)≥22.5 mag arcsec^(-2) and the axis ratio b/a> 0.3,we selected four none-edge-on LSBG samples from each of the models which contain 1105,1038,207,and 75 galaxies,respectively.There are 756 galaxies in common between LSBGs selected by exponential and sersic models,corresponding to 68.42% of LSBGs selected by the exponential model and 72.83% of LSBGs selected by the sersic model,the rest of the discrepancy is due to the difference in obtaining μ_(0) between the exponential and sersic models.Based on the fitting,in the range of 0.5≤n≤1.5,the relation of μ_(0) from two models can be written as μ_(0,sérsic)-μ_(0,exp)=-1.34(n-1).The LSBGs selected by disk+bulge models(LSBG_(2)comps) are more massive than LSBGs selected by single-component models(LSBG_1comp),and also show a larger disk component.Though the bulges in the majority of our LSBG_(2)comps are not prominent,more than 60% of our LSBG_(2)comps will not be selected if we adopt a single-component model only.We also identified 31 giant low surface brightness galaxies(gLSBGs) from LSBG_(2)comps.They are located at the same region in the color-magnitude diagram as other gLSBGs.After we compared different criteria of gLSBGs selection,we find that for gas-rich LSBGs,M_(*)> 10^(10)M_⊙ is the best to distinguish between gLSBGs and normal LSBGs with bulge.
基金supported by National Key R&D Program of China(Nos.2019YFA0405501 and 2022YFF0503402)the National Natural Science Foundation of China(NSFC,Nos.12233005 and 12041302)+6 种基金support from the Natural Science Foundation of Shanghai(Project Number:22ZR1473000)the Program of Shanghai Academic Research Leader(No.22XD1404200)supports from the CAS Pioneer Hundred Talents ProgramUSTC Research Funds of the Double First-Class Initiativethe NSFC grant 12273037the NSFC grants 12033004,12333003support from the NSFC through grants 12273091 and U2031139。
文摘The star-forming clumps in star-bursting dwarf galaxies provide valuable insights into understanding the evolution of dwarf galaxies.In this paper,we focus on five star-bursting dwarf galaxies featuring off-centered clumps in the Mapping Nearby Galaxies at Apache Point Observatory survey.Using the stellar population synthesis software Fitting Analysis using Differential evolution Optimization,we obtain the spatially resolved distribution of the star formation history,which allows us to construct the g-band images of the five galaxies at different ages.These images can help us to probe the evolution of the morphological structures of these galaxies.While images of a stellar population older than 1 Gyr are typically smooth,images of a stellar population younger than 1 Gyr reveal significant clumps,including multiple clumps which appear at different locations and even different ages.To study the evolutionary connections of these five galaxies to other dwarf galaxies before their star-forming clumps appear,we construct the images of the stellar populations older than three age nodes,and define them to be the images of the"host"galaxies.We find that the properties such as the central surface brightness and the effective radii of the hosts of the five galaxies are in between those of dwarf ellipticals(dEs)and dwarf irregulars(dIrrs),with two clearly more similar to dEs and one more similar to dIrrs.Among the five galaxies,8257-3704 is particularly interesting,as it shows a previous starburst event that is not quite visible from its gri image,but only visible from images of the stellar population at a few hundred million years.The star-forming clump associated with this event may have appeared at around 600 Myr ago and disappeared at around 40 Myr ago.
文摘The structural parameters of a galaxy can be used to gain insight into its formation and evolution history.In this paper,we strive to compare the Milky Way’s structural parameters to other,primarily edge-on,spiral galaxies in order to determine how our Galaxy measures up to the Local Universe.For our comparison,we use the galaxy structural parameters gathered from a variety of literature sources in the optical and near-infrared wave bands.We compare the scale length,scale height,and disk flatness for both the thin and thick disks,the thick-to-thin disk mass ratio,the bulge-to-total luminosity ratio,and the mean pitch angle of the Milky Way’s spiral arms to those in other galaxies.We conclude that many of the Milky Way’s structural parameters are largely ordinary and typical of spiral galaxies in the Local Universe,though the Galaxy’s thick disk appears to be appreciably thinner and less extended than expected from zoom-in cosmological simulations of Milky Way-mass galaxies with a significant contribution of galaxy mergers involving satellite galaxies.
基金supported by the Natural Science Research Programs of Jiangsu Province University(23KJB160001 and 23KJB140004)by the support of the scientific research fund of Jiangsu Second Normal University(927801/032)+1 种基金supported by the Hebei Natural Science Foundation(grant No.A2022408002)the Fundamental Research Funds for the Universities in Hebei Province(grant No.JYQ202003)。
文摘How galaxies assemble masses through their own star formation or interaction with the external environment is still an important topic in the field of galaxy formation and evolution.We use Value Added Catalogs with galaxy features that are spatially and temporally resolved from Sloan Digital Sky Survey Data Release 17 to investigate the mass growth histories of early-type galaxies(ETGs)and late-type galaxies(LTGs).We find that the mass growth of ETGs is earlier than that of LTGs for massive galaxies(M_(*)>10^(10)M_⊙),while low-mass(M_(*)≤10^(10)M_⊙)ETGs have statistically similar mass assembly histories as low-mass LTGs.The stellar metallicity of all massive galaxies shows a negative gradient and basically does not change with time.However,in low-mass galaxies,the stellar metallicity gradient of elliptical galaxies is negative,and the stellar metallicity gradient of lenticular and spiral galaxies evolves from positive to negative.ETGs are not all in a high-density environment,but exhibit mass dependence.As the tidal strength increases,the star formation rate of low-mass ETGs rapidly decreases.These results support a picture where massive galaxies exhibit inside-out quenching mode,while low-mass galaxies show outside-in quenching mode.Environmental effects play an important role in regulating the mass assembly histories of low-mass ETGs.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.51902101 and 21875203)the Natural Science Foundation of Hunan Province(Nos.2021JJ40044 and 2023JJ50287)Natural Science Foundation of Jiangsu Province(No.BK20201381).
文摘Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent years,deformable catalysts for HER have made great progress and would become a research hotspot.The catalytic activities of deformable catalysts could be adjustable by the strain engineering and surface reconfiguration.The surface curvature of flexible catalytic materials is closely related to the electrocatalytic HER properties.Here,firstly,we systematically summarized self-adaptive catalytic performance of deformable catalysts and various micro–nanostructures evolution in catalytic HER process.Secondly,a series of strategies to design highly active catalysts based on the mechanical flexibility of lowdimensional nanomaterials were summarized.Last but not least,we presented the challenges and prospects of the study of flexible and deformable micro–nanostructures of electrocatalysts,which would further deepen the understanding of catalytic mechanisms of deformable HER catalyst.
基金supported by the Youth Program of the National Natural Science Foundation of China No.12003017。
文摘Using archival Fermi-LAT data with a time span of~12 yr,we study the population of Millisecond Pulsars(MSPs)in Globular Clusters(GlCs)and investigate their dependence on cluster dynamical evolution in the Milky Way.We show that theγ-ray luminosity(L_(γ))and emissivity(i.e.,ε_(γ)=L_(γ)/M,with M the cluster mass)are good indicators of the population and abundance of MSPs in GlCs,and they are highly dependent on the dynamical evolution history of the host clusters.Specifically speaking,the dynamically older GlCs with more compact structures are more likely to have larger L_(γ)andε_(γ),and these trends can be summarized as strong correlations with cluster stellar encounter rateΓand the specific encounter rate(Λ=Γ/M),with L_(γ)∝Γ^(0.7±0.11)andε_(γ)∝Λ^(0.73±0.13)for dynamically normal GlCs.However,as GlCs evolve into deep core collapse,these trends are found to be reversed,implying that strong encounters may have lead to the disruption of Low-Mass X-ray Binaries and ejection of MSPs from core-collapsed systems.Besides,the GlCs are found to exhibit largerε_(γ)with increasing stellar mass function slope(ε_(γ)∝10^((0.52±0.1)α)),decreasing tidal radius(ε_(γ)∝R_(t)^(-10±0.22))and distances from the Galactic Center(GC,ε_(γ)∝R_(gc)^(-1.13±0.21)).These correlations indicate that,as GlCs losing kinetic energy and spiral in toward the GC,tidal stripping and mass segregation have a preference in leading to the loss of normal stars from GlCs,while MSPs are more likely to concentrate to cluster center and be deposited into the GC.Moreover,we gaugeε_(γ)of GlCs is~10-1000 times larger than the Galactic bulge,the latter is thought to reside thousands of unresolved MSPs and may be responsible for the GC 7-ray excess,which supports that GlCs are generous contributors to the population of MSPs in the GC.
基金the financial support from the National Natural Science Foundation of China(No.52109119)the Guangxi Natural Science Foundation(No.2021GXNSFBA075030)+2 种基金the Guangxi Science and Technology Project(No.Guike AD20325002)the Chinese Postdoctoral Science Fund Project(No.2022M723408)the Open Research Fund of State Key Laboratory of Simulation and Regulation of Water Cycle in River Basin(China Institute of Water Resources and Hydropower Research)(No.IWHR-SKL-202202)。
文摘The far-field microdynamic disturbance caused by the excavation of deep mineral resources and underground engineering can induce surrounding rock damage in high-stress conditions and even lead to disasters.However,the mechanical properties and damage/fracture evolution mechanisms of deep rock induced by microdynamic disturbance under three-dimensional stress states are unclear.Therefore,a true triaxial multilevel disturbance test method is proposed,which can completely simulate natural geostress,excavation stress redistribution(such as stress unloading,concentration and rotation),and subsequently the microdynamic disturbance triggering damaged rock failure.Based on a dynamic true triaxial test platform,true triaxial microdynamic disturbance tests under different frequency and amplitudes were carried out on monzogabbro.The results show that increasing amplitude or decreasing frequency diminishes the failure strength of monzogabbro.Deformation modulus gradually decreases during disturbance failure.As frequency and amplitude increase,the degradation rate of deformation modulus decreases slightly,disturbance dissipated energy increases significantly,and disturbance deformation anisotropy strengthens obviously.A damage model has been proposed to quantitatively characterize the disturbance-induced damage evolution at different frequency and amplitude under true triaxial stress.Before disturbance failure,the micro-tensile crack mechanism is dominant,and the micro-shear crack mechanism increases significantly at failure.With the increase of amplitude and frequency,the micro-shear crack mechanism increases.When approaching disturbance failure,the acoustic emission fractal dimension changes from a stable value to local large oscillation,and finally increases sharply to a high value at failure.Finally,the disturbance-induced failure mechanism of surrounding rock in deep engineering is clearly elucidated.
文摘Three mechanisms for an alternative to the Doppler effect as an explanation for the redshift are reviewed. A fourth mechanism is the attenuation of the light as given by the Beer-Lambert law. The average value of the Hubble constant is therefore derived by processing the galaxies of the NED-D catalog in which the distances are independent of the redshift. The observed anisotropy of the Hubble constant is reproduced by adopting a rim model, a chord model, and both 2D and 3D Voronoi diagrams.
基金financially supported by the Agricultural Science and Technology Innovation Program(CAASASTIP-2021-RIP-02)。
文摘Identification of the S genotype of Malus plants will greatly promote the discovery of new genes,the cultivation and production of apple,the breeding of new varieties,and the origin and evolution of self-incompatibility in Malus plants.In this experiment,88 Malus germplasm resources,such as Aihuahong,Xishuhaitang,and Reguanzi,were used as materials.Seven gene-specific primer combinations were used in the genotype identification.PCR amplification using leaf DNA produced a single S-RNase gene fragment in all materials.The results revealed that 70 of the identified materials obtained a complete S-RNase genotype,while only one S-RNase gene was found in 18 of them.Through homology comparison and analysis,13 S-RNase genotypes were obtained:S_(1)S_(2)(Aihuahong,etc.),S_(1)S_(28)(Xixian Haitang,etc.),S_(1)S_(51)(Hebei Pingdinghaitang),S_(1)S_(3)(Xiangyangcun Daguo,etc.),S_(2)S_(3)(Zhaiyehaitang,etc.),S_(3)S_(51)(Xishan 1),S_(3)S_(28)(Huangselihaerde,etc.),S_(2)S_(28)(Honghaitang,etc.),S_(4)S_(28)(Bo 11),S_(7)S_(28)(Jiuquan Shaguo),S_(10)S_e(Dongchengguan 13),S_(10)S_(21)(Dongxiangjiao)and S_(3)S_(51)(Xiongyue Haitang).Simultaneously,the frequency of the S gene in the tested materials was analyzed.The findings revealed that different S genes had varying frequencies in Malus resources,as well as varying frequencies between intraspecific and interspecific.S_(3) had the highest frequency of 68.18%,followed by S_(1)(42.04%).In addition,the phylogenetic tree and origin evolution analysis revealed that the S gene differentiation was completed prior to the formation of various apple species,that cultivated species also evolved new S genes,and that the S_(50) gene is the oldest S allele in Malus plants.The S_(1),S_(29),and S_(33) genes in apple-cultivated species,on the other hand,may have originated in M.sieversii,M.hupehensis,and M.kansuensis,respectively.In addition to M.sieversii,M.kansuensis and M.sikkimensis may have also played a role in the origin and evolution of some Chinese apples.
基金Agency for Science,Technology and Research(A*STAR),under the RIE2020 Advanced Manufacturing and Engineering(AME)Programmatic Grant(Grant no.A18B1b0061)。
文摘The corrosion rates of additive-manufactured Mg alloys are higher than their as-cast counterparts,possibly due to increased kinetics for the hydrogen evolution reaction on secondary phases,which may include oxide inclusions.Scanning Kelvin Probe Force Microscopy demonstrated that MgO inclusions could act as cathodes for Mg corrosion,but their low conductivity likely precludes this.However,the density of state calculations through density functional theory using hybrid HSE06 functional revealed overlapping electronic states at the Mg/MgO interface,which facilitates electron transfers and participates in redox reactions.Subsequent determination of the hydrogen absorption energy at the Mg/MgO interface reveals it to be an excellent catalytic site,with HER being found to be a factor of 23x more efficient at the interface than on metallic Mg.The results not only support the plausibility of the Mg/MgO interface being an effective cathode to the adjacent anodic Mg matrix during corrosion but also contribute to the understanding of the enhanced cathodic activities observed during the anodic dissolution of magnesium.
基金funded by the National Natural Science Foundation of China(42271313)the Chinese Academy of Agricultural Sciences Innovation Project(CAAS-ASTIP2021-AII)the Central Public-interest Scientific Institution Basal Research Fund,China(JBYW-AII-2022-06,JBYWAII-2022-40)。
文摘The complex and volatile international landscape has significantly impacted global grain supply security. This study uses a complex network analysis model to examine the evolution and trends of the global major grain trade from 1990 to 2020, focusing on network topology, centrality ranking, and community structure. There are three major findings. First, the global major grain trade network has expanded in scale, with a growing emphasis on diversification and balance. During the study period, the United States, Canada, China, and Brazil were the core nodes of the network. Grain-exporting countries were mainly situated in Asia, the Americas, and Europe, and importing countries in Asia, Africa, and Europe. Second, a significant increase in the number of high centrality countries with high export capacity occurred, benefiting from natural advantages such as fertile land and favorable climates. Third, the main global grain trade network is divided into four communities, with the Americas-Europe community being the largest and most widespread. The formation of the community pattern was influenced by geographic proximity, driven by the core exporting countries. Therefore, the world needs to enhance the existing trade model, promote the multi-polarization of the grain trade network, and establish a global vision for the future community. Countries and regions should participate actively in global grain trade security governance and institutional reform, expand trade links with other countries, and optimize import and export policies to reduce trade risks.
基金funded by the National Natural Science Foundation of China (NSFC) (Nos. 22221001, 22201115, 21931001, and 21922105)the Special Fund Project of Guiding Scientific and Technological Innovation Development of Gansu Province (2019ZX–04)+3 种基金the 111 Project (B20027)by the Fundamental Research Funds for the Central Universities (lzujbky-2023-eyt03)support Natural Science Foundation of Gansu Providence (22JR5RA540)Gansu Province Youth Science and Technology Talent Promotion Project (GXH202220530-02)。
文摘Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performance for hydrogen evolution reaction(HER). With the VS concentration change from 2.4% to 8.5%, the H* adsorption strength on S sites changed and NiS_(2)-VS 5.9% shows the most optimized H* adsorption for HER with an ultralow onset potential(68 m V) and has long-term stability for 100 h in 1 M KOH media. In situ attenuated-total-reflection Fourier transform infrared spectroscopy(ATR-FTIRS) measurements are usually used to monitor the adsorption of intermediates. The S-H* peak of the Ni S_(2)-VS 5.9% appears at a very low voltage, which is favorable for the HER in alkaline media. Density functional theory calculations also demonstrate the Ni S_(2)-VS 5.9% has the optimal |ΔG^(H*)| of 0.17 e V. This work offers a simple and promising pathway to enhance catalytic activity via precise vacancies strategy.
基金supported by the National Natural Science Foundation of China(Grant Nos.12072299,11902276)the Natural Science Foundation of Sichuan Province(Grant No.2022NSFSC1802)+1 种基金the Basic Research Project of Southwest Jiaotong University(Grant No.2682023ZTPY009)the National Key Laboratory for Shock Wave and Detonation Physics of China(Grant No.JCKYS2019212007)。
文摘By combination of the transient Raman spectroscopic measurement and the density functional theoretical calculations,the structural evolution and stability of TATB under shock compression was investigated.Due to the improvement in synchronization control between two-stage light gas gun and the transient Raman spectra acquisition,as well as the sample preparation,the Raman peak of the N-O mode of TATB was firstly observed under shock pressure up to 13.6 GPa,noticeably higher than the upper limit of 8.5 GPa reported in available literatures.By taking into account of the continuous shift of the main peak and other observed Raman peaks,we did not distinguish any structural transition or any new species.Moreover,both the present Raman spectra and the time-resolved radiation of TATB during shock loading showed that TATB exhibits higher chemical stability than previous declaration.To reveal the detailed structural response and evolution of TATB under compression,the density functional theoretical calculations were conducted,and it was found that the pressure make N-O bond lengths shorter,nitro bond angles larger,and intermolecular and intra-molecular hydrogen bond interactions enhanced.The observed red shift of Raman peak was ascribed to the abnormal enhancement of H-bound effect on the scissor vibration mode of the nitro group.
基金supported by the Natural Science Foundation of Hebei Province(Grant No.E2022209039)Key Research Project of North China University of Science and Technology(Grant No.ZD-YG-202301)Tangshan Talent Funding Project(Grant No.A202202007).
文摘A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high luminescent quantum efficiency.What is more attractive is that the luminescent properties such as wavelength and intensity can be regulated by controlling the structure at the molecular level.Hence,it is time to summarize the related research on CN structural evolution and make a prospect on future developments.In this review,we first summarize the research history and multiple structural evolution of CN.Then,the progress of improving the luminescence performance of CN through structural evolution was discussed.Significantly,the relationship between CN structure evolution and energy conversion in the forms of photoluminescence,chemiluminescence,and electrochemiluminescence was reviewed.Finally,key challenges and opportunities such as nanoscale dispersion strategy,luminous efficiency improving methods,standardization evaluation,and macroscopic preparation of CN are highlighted.
基金supported by the National Natural Science Foundation of China(52363028,21965005)the Natural Science Foundation of Guangxi Province(2021GXNSFAA076001)the Guangxi Technology Base and Talent Subject(GUIKE AD18126001,GUIKE AD20297039)。
文摘Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.
基金supported by the National Natural Science Foundation of China(Grant No.42061035)the Guizhou Provincial Program on Commercialization of Scientific and Technological Achievements([2022]010).
文摘With the rapid urbanization process,the space of traditional villages in China is undergoing significant changes.Studying the spatial evolution of traditional villages is significant in promoting rural spatial transformation and realizing rural revitalization and sustainable rural development.Based on the traceability analysis of spatial production theory,this paper constructed an analytical framework for the spatial production evolution of traditional villages,analyzed the spatial evolution process and characteristics of traditional villages by using buffer analysis,spatial syntax,and other research methods,and revealed the characteristics of the spatial production evolution of traditional villages and the driving mechanism.The results show that:(1)The village spatial formation and development follow the village life cycle theory and usually develop from embryonic villages to diversified and integrated villages;(2)The evolution of village spatial production is characterized by the diversity of material space,the sublimation of daily life space,and the integration of social system space and generalization of emotional space;(3)The evolution of village spatial production from backward and poor village to ecologically well-off village is influenced by a combination of factors;(4)The village has formed a spatial structure of"people-land-scape-culture-industry",realized comprehensive reconstruction and spatial reproduction.The study results reflect the spatial evolution characteristics of traditional villages in mountainous areas in a more comprehensive way,which helps to promote the protection and development of traditional villages in mountainous areas and,to a certain extent,provides a reference for the development of rural revitalization.
基金the financial support from the Key Research and Development Program sponsored by the Ministry of Science and Technology(MOST)(2022YFB4002000,2022YFA1203400)the National Natural Science Foundation of China(22102172,22072145,22372155,22005294,21925205,21721003)。
文摘Constructing heterostructured nanohybrid is considered as a prominent route to fabricate alternative electrocatalysts to commercial Pt/C for hydrogen evolution reaction(HER).In this work,(NH_(4))_(4)[NiH_(6)Mo_(6)O_(4)]·5H_(2)O polyoxometalates(NiMo_(6))are adopted as the cluster precursors for simple fabrication of heterostructured Pt-Ni_(3)Mo_(3)N nanohybrids supported by carbon black(Pt-Ni_(3)Mo_(3)N/C)without using additional N sources.The improved porosity and enhanced electronic interaction of Pt-Ni_(3)Mo_(3)N/C should be attributed to the integration of Pt with NiMo_(6),which favors the mass transport,promotes the formation of exposed catalytic sites,and benefits the regulation of intrinsic activity.Thus,the as-obtained Pt-Ni_(3)Mo_(3)N/C exhibits impressive and durable HER performance as indicated by the low overpotential of 13.7 mV at the current density of 10 mA cm^(-2) and the stable overpotential during continuous working at 100 mA cm^(-2) for 100 h.This work provides significant insights for the synthesis of new highly active heterostructured electrocatalysts for renewable energy devices.