Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au...Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au nanoparticles(NPs)(denoted as HP-Au@CoxSy@ZIF-67)hybrid is synthesized by low-temperature sulfuration treatment.The well-defined macroporous-mesoporous-microporous structure is obtained based on the combination of polystyrene spheres,as-formed CoxSy nanosheets,and ZIF-67 frameworks.This novel three-dimensional hierarchical structure significantly enlarges the three-phase interfaces,accelerating the mass transfer and exposing the active centers for oxygen evolution reaction.The electronic structure of Co is modulated by Au through charge transfer,and a series of experiments,together with theoretical analysis,is performed to ascertain the electronic modulation of Co by Au.Meanwhile,HP-Au@CoxSy@ZIF-67 catalysts with different amounts of Au were synthesized,wherein Au and NaBH4 reductant result in an interesting“competition effect”to regulate the relative ratio of Co^(2+)/Co^(3+),and moderate Au assists the electrochemical performance to reach the highest value.Consequently,the optimized HP-Au@CoxSy@ZIF-67 exhibits a low overpotential of 340 mV at 10 mA cm^(-2)and a Tafel slope of 42 mV dec-1 for OER in 0.1 M aqueous KOH,enabling efficient water splitting and Zn-air battery performance.The work here highlights the pivotal roles of both microstructural and electronic modulation in enhancing electrocatalytic activity and presents a feasible strategy for designing and optimizing advanced electrocatalysts.展开更多
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
The production of renewable fuels through water splitting via photocatalytic hydrogen production holds significant promise.Nonetheless,the sluggish kinetics of hydrogen evolution and the inadequate water adsorption on...The production of renewable fuels through water splitting via photocatalytic hydrogen production holds significant promise.Nonetheless,the sluggish kinetics of hydrogen evolution and the inadequate water adsorption on photocatalysts present notable challenges.In this study,we have devised a straightforward hydrothermal method to synthesize Bi_(2)O_(3)(BO)derived from metal‐organic frameworks(MOFs),loaded with flower-like ZnIn_(2)S_(4)(ZIS).This approach substantially enhances water adsorption and surface catalytic reactions,resulting in a remarkable enhancement of photocatalytic activity.By employing triethanolamine(TEOA)as a sacrificial agent,the hydrogen evolution rate achieved with 15%(mass fraction)ZIS loading on BO reached an impressive value of 1610μmol∙h^(−1)∙g^(−1),marking a 6.34-fold increase compared to that observed for bare BO.Furthermore,through density functional theory(DFT)and ab initio molecular dynamics(AIMD)calculations,we have identified the reactions occurring at the ZIS/BO S-scheme heterojunction interface,including the identification of active sites for water adsorption and catalytic reactions.This study provides valuable insights into the development of high-performance composite photocatalytic materials with tailored electronic properties and wettability.展开更多
A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C_(3)N_(4))have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high l...A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C_(3)N_(4))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
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
Transition metal phosphides with metallic properties are a promising candidate for electrocatalytic water oxidation,and developing highly active and stable metal phosphide-based oxygen evolution reaction catalysts is ...Transition metal phosphides with metallic properties are a promising candidate for electrocatalytic water oxidation,and developing highly active and stable metal phosphide-based oxygen evolution reaction catalysts is still challenging.Herein,we present a facile ion exchange and phosphating processes to transform intestine-like CoNiP_(x)@P,N-C into lotus pod-like CoNiFeP_(x)@P,N-C heterostructure in which numerous P,N-codoped carboncoated CoNiFeP_(x)nanoparticles tightly anchors on the 2D carbon matrix.Meanwhile,the as-prepared CoNiFeP_(x)@P,N-C enables a core-shell structure,high specific surface area,and hierarchical pore structure,which present abundant heterointerfaces and fully exposed active sites.Notably,the incorporation of Fe can also induce electron transfer in CoNiP_(x)@P,IM-C,thereby promoting the oxygen evolution reaction.Consequently,CoNiFeP_(x)@P,IM-C delivers a low overpotential of 278 mV(vs RHE)at a current density of10 mA cm^(-1)and inherits excellent long-term stability with no observable current density decay after 30 h of chronoamperometry test.This work not only highlights heteroatom induction to tune the electronic structure but also provides a facile approach for developing advanced and stable oxygen evolution reaction electrocatalysts with abundant heterointerfaces.展开更多
Optimizing the catalytic activity and stability of molybdenum disulfide (MoS_(2)) towards alkaline hydrogen evolution reaction (HER) is significant for sustaining green hydrogen. A moderate localized electronic struct...Optimizing the catalytic activity and stability of molybdenum disulfide (MoS_(2)) towards alkaline hydrogen evolution reaction (HER) is significant for sustaining green hydrogen. A moderate localized electronic structure of active sites plays a crucial role in determining the activity and stability of the catalysts, yet how to construct such localized electronic structure still remains indeterminacy. Enlightened by theoretical prediction, herein, the introduction of both single-atom Re and the adjacent S vacancy in MoS_(2) (denoted as Re-MoS_(2)-Vs) exhibits collaborative effect on regulating the localized electronic structure of active sites (viz. Re-(S, Vs)-Mo). Such regulated electronic structure helps to decrease the energy barrier of the water dissociation and optimize hydrogen adsorption energy for enhancing alkaline HER performance. Most importantly, Mo-S bonds in the above local Re-(S, Vs)-Mo configurations are also strengthened for preventing the leaching of Mo and S atoms and then ensuring the long-time stability. Consequently, the deliberately designed Re-MoS_(2)-Vs with a Re coordination number of ~ 5.0 is experimentally verified to exhibit a comparable electrocatalytic performance and robust operational stability over 120 h. This strategy provides a promising guidance for modulating the electronic structure of MoS_(2) based catalysts via double-tuning atomic-scale local configuration for HER applications.展开更多
With drilling and seismic data of Transtensional(strike-slip)Fault System in the Ziyang area of the central Sichuan Basin,SW China plane-section integrated structural interpretation,3-D fault framework model building,...With drilling and seismic data of Transtensional(strike-slip)Fault System in the Ziyang area of the central Sichuan Basin,SW China plane-section integrated structural interpretation,3-D fault framework model building,fault throw analyzing,and balanced profile restoration,it is pointed out that the transtensional fault system in the Ziyang 3-D seismic survey consists of the northeast-trending F_(I)19 and F_(I)20 fault zones dominated by extensional deformation,as well as 3 sets of northwest-trending en echelon normal faults experienced dextral shear deformation.Among them,the F_(I)19 and F_(I)20 fault zones cut through the Neoproterozoic to Lower Triassic Jialingjiang Formation,presenting a 3-D structure of an“S”-shaped ribbon.And before Permian and during the Early Triassic,the F_(I)19 and F_(I)20 fault zones underwent at least two periods of structural superimposition.Besides,the 3 sets of northwest-trending en echelon normal faults are composed of small normal faults arranged in pairs,with opposite dip directions and partially left-stepped arrangement.And before Permian,they had formed almost,restricting the eastward growth and propagation of the F_(I)19 fault zone.The F_(I)19 and F_(I)20 fault zones communicate multiple sets of source rocks and reservoirs from deep to shallow,and the timing of fault activity matches well with oil and gas generation peaks.If there were favorable Cambrian-Triassic sedimentary facies and reservoirs developing on the local anticlinal belts of both sides of the F_(I)19 and F_(I)20 fault zones,the major reservoirs in this area are expected to achieve breakthroughs in oil and gas exploration.展开更多
This study selected the Sino-US route data from the top 30 global container liner companies between December 1,2019,and December 29,2019,as the data source utilizing the complex network research methodology.It constru...This study selected the Sino-US route data from the top 30 global container liner companies between December 1,2019,and December 29,2019,as the data source utilizing the complex network research methodology.It constructs a Sino-US container shipping network through voyage weighting and analyzes the essential structural characteristics to explore the network’s complex structural fea-tures.The network’s evolution is examined from three perspectives,namely,time,space,and event influence,aiming to comprehens-ively explore the network’s evolution mechanism.The results revealed that:1)the weighted Sino-US container shipping network exhib-its small-world and scale-free properties.Key hub ports in the United States include NEW YORK NY,SAVANNAH GA,LOS ANGELES CA,and OAKLAND CA,whereas SHANGHAI serving as the hub port in China.The geographical distribution of these hub ports is uneven.2)Concerning the evolution of the weighted Sino-US container shipping network,from a temporal perspective,the evolution of the regional structure of the entire Sino-US region and the Inland United States is in a stage of radiative expansion and de-velopment,with a need for further enhancement in competitiveness and development speed.The evolution of the regional structure of southern China and Europe is transitioning from the stage of radiative expansion and development to an advanced equilibrium stage.The shipping development in Northern China,the Western and Eastern United States,and Asia is undergoing significant changes but faces challenges of fierce competition and imbalances.From a spatial perspective,the rationality and effectiveness of the improved weighted Barrat-Barthelemy-Vespignani(BBV)model are confirmed through theoretical derivation.The applicability of the improved evolution model is verified by simulating the evolution of the weighted Sino-US container shipping network.From an event impact per-spective,the Corona Virus Disease 2019(COVID-19)pandemic has not fundamentally affected the spatial pattern of the weighted Sino-US container shipping network but has significantly impacted the network’s connectivity.The network lacks sufficient resilience and stability in emergency situations.3)Based on the analysis of the structural characteristics and evolution of the weighted Sino-US con-tainer shipping network,recommendations for network development are proposed from three aspects:emphasizing the development of hub ports,focusing on the balanced development of the network,and optimizing the layout of Chinese ports.展开更多
The establishment of efficient oxygen evolution electrocatalysts is of great value but also challenging.Herein,a durable metal–organic framework(MOF)with minor atomically dispersed ruthenium and an optimized electron...The establishment of efficient oxygen evolution electrocatalysts is of great value but also challenging.Herein,a durable metal–organic framework(MOF)with minor atomically dispersed ruthenium and an optimized electronic structure is constructed as an efficient electrocatalyst.Significantly,the obtained NiRu_(0.08)-MOF with doping Ru only needs an overpotential of 187 mV at 10 mA cm^(-2) with a Tafel slop of 40 mV dec^(-1) in 0.1M KOH for the oxygen evolution reaction,and can work continuously for more than 300 h.Ultrahigh Ru mass activity is achieved,reaching 56.7 Ag^(-1)_(Ru) at an overpotential of 200 mV,which is 36 times higher than that of commercial RuO_(2).X-ray adsorption spectroscopy and density function theory calculations reveal that atomically dispersed ruthenium on metal sites in MOFs is expected to optimize the electronic structure of nickel sites,thus improving the conductivity of the catalyst and optimizing the adsorption energy of intermediates,resulting in significant optimization of electrocatalytic performance.This study could provide a new avenue for the design of efficient and stable MOF electrocatalysts.展开更多
A backfilling body-coal pillar-backfilling body(BPB)structure formed by pillar-side cemented paste backfilling can bear overburden stress and ensure safe mining.However,the failure response of BPB composite samples mu...A backfilling body-coal pillar-backfilling body(BPB)structure formed by pillar-side cemented paste backfilling can bear overburden stress and ensure safe mining.However,the failure response of BPB composite samples must be investigated.This paper examines the deformation characteristics and damage evolution of six types of BPB composite samples using a digital speckle correlation method under uniaxial compression conditions.A new damage evolution equation was established on the basis of the input strain energy and dissipated strain energy at the peak stress.The prevention and control mechanisms of the backfilling body on the coal pillar instability were discussed.The results show that the deformation localization and macroscopic cracks of the BPB composite samples first appeared at the coal-backfilling interface,and then expanded to the backfilling elements,ultimately appearing in the coal elements.The elastic strain energy in the BPB composite samples reached a maximum at the peak stress,whereas the dissipated energy continued to accumulate and increase.The damage evolution curve and equation agree well with the test results,providing further understanding of instability prevention and the control mechanisms of the BPB composite samples.The restraining effect on the coal pillar was gradually reduced with decreasing backfilling body element's volume ratio,and the BPB composite structure became more vulnerable to failure.This research is expected to guide the design,stability monitoring,instability prevention,and control of BPB structures in pillar-side cemented paste backfilling mining.展开更多
This study aimed to investigate the mechanism of nitrogen doping,migration,and conversion during ammonia torrefaction and also explore the evolution law of the chemical structure of cellulose.The results showed that t...This study aimed to investigate the mechanism of nitrogen doping,migration,and conversion during ammonia torrefaction and also explore the evolution law of the chemical structure of cellulose.The results showed that the ammonia torrefaction pretreatment could significantly optimize the distribution of nitrogen and oxygen elements in cellulose.The carbon skeleton first captured the active nitrogenous radicals to form-NHn-N,and pyridine-N and pyrrole-N originated from the conversion of-NHn-N.The existence of C=O played a major role in the immobilization of nitrogen.The nitrogen in bio-oil exists mainly in the form of five-and six-membered heterocycles.The correlation analysis showed that the main precursors for the formation of nitrogenous heterocyclic compounds were five-membered Oheterocyclic compounds.Finally,the product distribution characteristics in the torrefaction-pyrolysis systems were summarized,and the nitrogen doping and conversion mechanisms were proposed.This study expanded the boundaries of cellulose pretreatment and the production of high-value chemicals.展开更多
The Tongnan secondary negative structure in central Sichuan Basin has controls and influences on the structural framework and petroleum geological conditions in the Gaoshiti-Moxi area.To clarify the controls and influ...The Tongnan secondary negative structure in central Sichuan Basin has controls and influences on the structural framework and petroleum geological conditions in the Gaoshiti-Moxi area.To clarify the controls and influences,the deformation characteristics,structural attributes and evolution process of the Tongnan negative structure were investigated through a series of qualitative and quantitative methods such as balanced profile restoration,area-depth-strain(ADS)analysis,and structural geometric forward numerical simulation,after comprehensive structural interpretation of high-precision 3D seismic data.The results are obtained in three aspects.First,above and below the P/AnP(Permian/pre-Permian)unconformity,the Tongnan negative structure demonstrates vertical differential structural deformation.It experiences two stages of structural stacking and reworking:extensional depression(from the Sinian Dengying Formation to the Permian),and compressional syncline deformation(after the Jurassic).The multi-phase trishear deformation of the preexisting deep normal faults dominated the extensional depression.The primary depression episodes occurred in the periods from the end of Late Proterozoic to the deposition of the 1st–2nd members of the Dengying Formation,and from the deposition of Lower Cambrian Longwangmiao Formation–Middle–Upper Cambrian until the Ordovician.Second,the multi-stage evolution process of the Tongnan negative structure controlled the oil and gas migration and adjustment and present-day differential gas and water distribution between the Tongnan negative structure and the Gaoshiti and Moxi-Longnüsi structural highs.Third,the Ordovician,which is limitedly distributed in the Tongnan negative structure and is truncated by the P/AnP unconformity on the top,has basic geological conditions for the formation of weathering karst carbonate reservoirs.It is a new petroleum target deserving attention.展开更多
Efficient and durable oxygen evolution reaction(OER)requires the electrocatalyst to bear abundant active sites,optimized electronic structure as well as robust component and mechanical stability.Herein,a bimetallic la...Efficient and durable oxygen evolution reaction(OER)requires the electrocatalyst to bear abundant active sites,optimized electronic structure as well as robust component and mechanical stability.Herein,a bimetallic lanthanum-nickel oxysulfide with rich oxygen vacancies based on the La_(2)O_(2)S prototype is fabricated as a binder-free precatalyst for alkaline OER.The combination of advanced in situ and ex situ characterizations with theoretical calculation uncovers the synergistic effect among La,Ni,O,and S species during OER,which assures the adsorption and stabilization of the oxyanion SO_(4)^(2-)onto the surface of the deeply reconstructed porous heterostructure composed of confining Ni OOH nanodomains by La(OH)_3 barrier.Such coupling,confinement,porosity and immobilization enable notable improvement in active site accessibility,phase stability,mass diffusion capability and the intrinsic Gibbs free energy of oxygen-containing intermediates.The optimized electrocatalyst delivers exceptional alkaline OER activity and durability,outperforming most of the Ni-based benchmark OER electrocatalysts.展开更多
In order to study the sintering characteristics of Ca-rich iron ore,chemical analysis,laser diffraction,scanning electron microscopy,XRD-Rietveld method,and micro-sintering were used to analyze the mineralogical prope...In order to study the sintering characteristics of Ca-rich iron ore,chemical analysis,laser diffraction,scanning electron microscopy,XRD-Rietveld method,and micro-sintering were used to analyze the mineralogical properties and sintering pot tests were used to study the sintering behavior.In addition,a grey correlation mathematical model was used to calculate and compare the comprehensive sintering performance under different calcium-rich iron ore contents.The results demonstrate that the Ca-rich iron ore has coarse grain size and strong self-fusing characteristics with Ca element in the form of calcite(CaCO_(3)) and the liquid phase produced by the self-fusing of the calcium-rich iron ore is well crystallized.Its application with a 20wt%content in sintering improves sinter productivity,reduces fuel consumption,enhances reduction index,and improves gas permeability in blast furnace by 0.45 t/(m^(2)·h),6.11 kg/t,6.17%,and 65.39 kPa·℃,respectively.The Ca-rich iron ore sintering can improve the calorific value of sintering flue gas compared with magnetite sintering,which is conducive to recovering heat for secondary use.As the content of the Ca-rich iron ore increases,sinter agglomeration shifts from localized liquid-phase bonding to a combination of localized liquid-phase bonding and iron oxide crystal connection.Based on an examination of the greater weight value of productivity with grey correlation analysis,the Ca-rich iron ore is beneficial for the comprehensive index of sintering in the range of 0-20wt%content.Therefore,it may be used in sintering with magnetite concentrates as the major ore species.展开更多
River bending is the major effect responsible for bed topography and bank changes.In this study,fluid velocity(measured by a three-dimensional Doppler advanced point current meter)and bed topographical data have been ...River bending is the major effect responsible for bed topography and bank changes.In this study,fluid velocity(measured by a three-dimensional Doppler advanced point current meter)and bed topographical data have been collected in 40 sections of an experimental model.The whole flume was composed of an organic glass bend,upstream and downstream water tanks,two transition straight sections,a circulation pump,and a connection pipeline.Each section has been found to be characterized by a primary circulation and a small reverse circulation,with some sections even presenting three more or more circulation structures.The minimum circulation intensity has been detected in proximity to the top of the curved channel,while a region with small longitudinal velocity has been observed near the concave bank of each bend,corresponding to the flat bed formed after a short period of scouring.The maximum sediment deposition and scour depth in the presence of a uniform distribution of living flexible vegetation within 10 cm of the flume wall have been found to be smaller than those observed in the tests conducted without vegetation.展开更多
Focused exploration of earth-abundant and cost-efficient non-noble metal electrocatalysts with superior hydrogen evolution reaction(HER)performance is very important for large-scale and efficient electrolysis of water...Focused exploration of earth-abundant and cost-efficient non-noble metal electrocatalysts with superior hydrogen evolution reaction(HER)performance is very important for large-scale and efficient electrolysis of water.Herein,a sandwich composite structure(designed as MS-Mo2C@NCNS)ofβ-Mo2C hollow nanotubes(HNT)and N-doped carbon nanosheets(NCNS)is designed and prepared using a binary NaCl–KCl molten salt(MS)strategy for HER.The temperature-dominant Kirkendall formation mechanism is tentatively proposed for such a three-dimensional hierarchical framework.Due to its attractive structure and componential synergism,MS-Mo2C@NCNS exposes more effective active sites,confers robust structural stability,and shows significant electrocatalytic activity/stability in HER,with a current density of 10 mA cm-2 and an overpotential of only 98 mV in 1 M KOH.Density functional theory calculations point to the synergistic effect of Mo2C HNT and NCNS,leading to enhanced electronic transport and suitable adsorption free energies of H*(ΔGH*)on the surface of electroactive Mo2C.More significantly,the MS-assisted synthetic methodology here provides an enormous perspective for the commercial development of highly active non-noble metal electrocatalysts toward efficient hydrogen evolution.展开更多
A three-layer Ta_2O_5-containing coating was successfully fabricated by laser cladding on a pure Ta substrate. The maximum thickness of such a coating is about 1.6 mm. The microstructure, phase constitution and elemen...A three-layer Ta_2O_5-containing coating was successfully fabricated by laser cladding on a pure Ta substrate. The maximum thickness of such a coating is about 1.6 mm. The microstructure, phase constitution and elemental distribution in the coating were investigated. Results show that the coating has been metallurgically bonded to the Ta substrate and the microstructure exhibits a graded change along the deposition direction from Ta substrate to the top of coating. In the layers I and II of the graded coating, the microstructure evolution can be confi rmed as a result of hypomonotectic reaction, but in the layer Ⅲ it was formed by hypermonotectic reaction. At the top of coating, the microstructure was still homogeneous although liquid phase separation had occurred, which can be attributed to the fact that the O-rich droplets do not have enough time to fl oat at high cooling rate. The theoretical calculation results show that during laser cladding, the solidifi cation time of the melt pool was less than 0.1 s, which fi ts well with the results from the experiment.展开更多
The microstructure, chemical composition and morphology evolution of icosahedral quasicrystalline phase of Mg67.4Zn28.9Y3.7 ternary alloy were investigated in detail at different pouring temperatures by X-ray diffract...The microstructure, chemical composition and morphology evolution of icosahedral quasicrystalline phase of Mg67.4Zn28.9Y3.7 ternary alloy were investigated in detail at different pouring temperatures by X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy-dispersive spectrum (EDS). Low interracial energy favors the formation of l-phase. The experimental results show that the primary l-phase reveals petal-shaped with five and six branches, where each branch has facetted growth morphology with the size ranging from 50 to 100μm. As the temperature decreases, the polygon-shaped l-phase forms, attributed to the decomposition of branch of petal-shaped l-phase, and then it grows bigger and some of the fine polygons join together to form large polygons. Besides these, (α-Mg+l-phase) eutectic structures disappear and the relative amount of Mg7Zn3 phase increases as the pouring temperature decreases. The chemical composition and morphology evolution of l-phase were also discussed.展开更多
基金National Natural Science Foundation of China,Grant/Award Numbers:52102260,52171211,51972220,61903235,U22A20145Shandong Provincial Natural Science Foundation,Grant/Award Numbers:ZR2020QB069,ZR2022ME051+4 种基金National Key Research and Development Program of China,Grant/Award Number:2022YFB4002004Scientific and Technological Innovation Ability Improvement Project of Minor Enterprises in Shandong Province,Grant/Award Number:2022TSGC1021Announce the List and Take Charge Project in Jinan,Grant/Award Number:202214012Major innovation project for integrating science,education and industry of Qilu University of Technology (Shandong Academy of Sciences),Grant/Award Numbers:2022JBZ01-07,2022PY044China Postdoctoral Science Foundation,Grant/Award Number:2022M711545。
文摘Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au nanoparticles(NPs)(denoted as HP-Au@CoxSy@ZIF-67)hybrid is synthesized by low-temperature sulfuration treatment.The well-defined macroporous-mesoporous-microporous structure is obtained based on the combination of polystyrene spheres,as-formed CoxSy nanosheets,and ZIF-67 frameworks.This novel three-dimensional hierarchical structure significantly enlarges the three-phase interfaces,accelerating the mass transfer and exposing the active centers for oxygen evolution reaction.The electronic structure of Co is modulated by Au through charge transfer,and a series of experiments,together with theoretical analysis,is performed to ascertain the electronic modulation of Co by Au.Meanwhile,HP-Au@CoxSy@ZIF-67 catalysts with different amounts of Au were synthesized,wherein Au and NaBH4 reductant result in an interesting“competition effect”to regulate the relative ratio of Co^(2+)/Co^(3+),and moderate Au assists the electrochemical performance to reach the highest value.Consequently,the optimized HP-Au@CoxSy@ZIF-67 exhibits a low overpotential of 340 mV at 10 mA cm^(-2)and a Tafel slope of 42 mV dec-1 for OER in 0.1 M aqueous KOH,enabling efficient water splitting and Zn-air battery performance.The work here highlights the pivotal roles of both microstructural and electronic modulation in enhancing electrocatalytic activity and presents a feasible strategy for designing and optimizing advanced electrocatalysts.
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.
文摘The production of renewable fuels through water splitting via photocatalytic hydrogen production holds significant promise.Nonetheless,the sluggish kinetics of hydrogen evolution and the inadequate water adsorption on photocatalysts present notable challenges.In this study,we have devised a straightforward hydrothermal method to synthesize Bi_(2)O_(3)(BO)derived from metal‐organic frameworks(MOFs),loaded with flower-like ZnIn_(2)S_(4)(ZIS).This approach substantially enhances water adsorption and surface catalytic reactions,resulting in a remarkable enhancement of photocatalytic activity.By employing triethanolamine(TEOA)as a sacrificial agent,the hydrogen evolution rate achieved with 15%(mass fraction)ZIS loading on BO reached an impressive value of 1610μmol∙h^(−1)∙g^(−1),marking a 6.34-fold increase compared to that observed for bare BO.Furthermore,through density functional theory(DFT)and ab initio molecular dynamics(AIMD)calculations,we have identified the reactions occurring at the ZIS/BO S-scheme heterojunction interface,including the identification of active sites for water adsorption and catalytic reactions.This study provides valuable insights into the development of high-performance composite photocatalytic materials with tailored electronic properties and wettability.
基金Natural Science Foundation of Hebei ProvinceTangshan Talent Funding Project,Grant/Award Number:E2022209039+1 种基金Key Research Project of North China University of Science and Technology,Grant/Award Number:ZD-YG 202301Tangshan Talent Punding Project,Grant/Award Number:A202202007
文摘A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C_(3)N_(4))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(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 National Natural Science Foundation of China(No.22269010)the Jiangxi Provincial Natural Science Foundation(No.20224BAB214021)+3 种基金the Training Program for Academic and Technical Leaders of Major Disciplines in Jiangxi Province(No.20212BCJ23020)the Science and Technology Project of Jiangxi Provincial Department of Education(No.GJJ211305)the Jingdezhen Science and Technology Planning Project(No.20212GYZD009-04)the Graduate Innovation Fund of Jiangxi Province(YC2022-s880)
文摘Transition metal phosphides with metallic properties are a promising candidate for electrocatalytic water oxidation,and developing highly active and stable metal phosphide-based oxygen evolution reaction catalysts is still challenging.Herein,we present a facile ion exchange and phosphating processes to transform intestine-like CoNiP_(x)@P,N-C into lotus pod-like CoNiFeP_(x)@P,N-C heterostructure in which numerous P,N-codoped carboncoated CoNiFeP_(x)nanoparticles tightly anchors on the 2D carbon matrix.Meanwhile,the as-prepared CoNiFeP_(x)@P,N-C enables a core-shell structure,high specific surface area,and hierarchical pore structure,which present abundant heterointerfaces and fully exposed active sites.Notably,the incorporation of Fe can also induce electron transfer in CoNiP_(x)@P,IM-C,thereby promoting the oxygen evolution reaction.Consequently,CoNiFeP_(x)@P,IM-C delivers a low overpotential of 278 mV(vs RHE)at a current density of10 mA cm^(-1)and inherits excellent long-term stability with no observable current density decay after 30 h of chronoamperometry test.This work not only highlights heteroatom induction to tune the electronic structure but also provides a facile approach for developing advanced and stable oxygen evolution reaction electrocatalysts with abundant heterointerfaces.
基金supported by the National Natural Science Foundation of China(No.22209193)Natural Science Foundation of Shandong Province(Nos.ZR2020ZD10 and ZR2021QB111)+1 种基金the Taishan Scholars Program of Shandong Province(No.tstq20221151)the Innovation Funds of Shandong Energy Institute(No.SEI I202140).
文摘Optimizing the catalytic activity and stability of molybdenum disulfide (MoS_(2)) towards alkaline hydrogen evolution reaction (HER) is significant for sustaining green hydrogen. A moderate localized electronic structure of active sites plays a crucial role in determining the activity and stability of the catalysts, yet how to construct such localized electronic structure still remains indeterminacy. Enlightened by theoretical prediction, herein, the introduction of both single-atom Re and the adjacent S vacancy in MoS_(2) (denoted as Re-MoS_(2)-Vs) exhibits collaborative effect on regulating the localized electronic structure of active sites (viz. Re-(S, Vs)-Mo). Such regulated electronic structure helps to decrease the energy barrier of the water dissociation and optimize hydrogen adsorption energy for enhancing alkaline HER performance. Most importantly, Mo-S bonds in the above local Re-(S, Vs)-Mo configurations are also strengthened for preventing the leaching of Mo and S atoms and then ensuring the long-time stability. Consequently, the deliberately designed Re-MoS_(2)-Vs with a Re coordination number of ~ 5.0 is experimentally verified to exhibit a comparable electrocatalytic performance and robust operational stability over 120 h. This strategy provides a promising guidance for modulating the electronic structure of MoS_(2) based catalysts via double-tuning atomic-scale local configuration for HER applications.
基金Supported by the Key Project of National Natural Science Foundation of China(42330810).
文摘With drilling and seismic data of Transtensional(strike-slip)Fault System in the Ziyang area of the central Sichuan Basin,SW China plane-section integrated structural interpretation,3-D fault framework model building,fault throw analyzing,and balanced profile restoration,it is pointed out that the transtensional fault system in the Ziyang 3-D seismic survey consists of the northeast-trending F_(I)19 and F_(I)20 fault zones dominated by extensional deformation,as well as 3 sets of northwest-trending en echelon normal faults experienced dextral shear deformation.Among them,the F_(I)19 and F_(I)20 fault zones cut through the Neoproterozoic to Lower Triassic Jialingjiang Formation,presenting a 3-D structure of an“S”-shaped ribbon.And before Permian and during the Early Triassic,the F_(I)19 and F_(I)20 fault zones underwent at least two periods of structural superimposition.Besides,the 3 sets of northwest-trending en echelon normal faults are composed of small normal faults arranged in pairs,with opposite dip directions and partially left-stepped arrangement.And before Permian,they had formed almost,restricting the eastward growth and propagation of the F_(I)19 fault zone.The F_(I)19 and F_(I)20 fault zones communicate multiple sets of source rocks and reservoirs from deep to shallow,and the timing of fault activity matches well with oil and gas generation peaks.If there were favorable Cambrian-Triassic sedimentary facies and reservoirs developing on the local anticlinal belts of both sides of the F_(I)19 and F_(I)20 fault zones,the major reservoirs in this area are expected to achieve breakthroughs in oil and gas exploration.
基金Under the auspices of National Natural Science Foundation of China(No.41201473,41371975)。
文摘This study selected the Sino-US route data from the top 30 global container liner companies between December 1,2019,and December 29,2019,as the data source utilizing the complex network research methodology.It constructs a Sino-US container shipping network through voyage weighting and analyzes the essential structural characteristics to explore the network’s complex structural fea-tures.The network’s evolution is examined from three perspectives,namely,time,space,and event influence,aiming to comprehens-ively explore the network’s evolution mechanism.The results revealed that:1)the weighted Sino-US container shipping network exhib-its small-world and scale-free properties.Key hub ports in the United States include NEW YORK NY,SAVANNAH GA,LOS ANGELES CA,and OAKLAND CA,whereas SHANGHAI serving as the hub port in China.The geographical distribution of these hub ports is uneven.2)Concerning the evolution of the weighted Sino-US container shipping network,from a temporal perspective,the evolution of the regional structure of the entire Sino-US region and the Inland United States is in a stage of radiative expansion and de-velopment,with a need for further enhancement in competitiveness and development speed.The evolution of the regional structure of southern China and Europe is transitioning from the stage of radiative expansion and development to an advanced equilibrium stage.The shipping development in Northern China,the Western and Eastern United States,and Asia is undergoing significant changes but faces challenges of fierce competition and imbalances.From a spatial perspective,the rationality and effectiveness of the improved weighted Barrat-Barthelemy-Vespignani(BBV)model are confirmed through theoretical derivation.The applicability of the improved evolution model is verified by simulating the evolution of the weighted Sino-US container shipping network.From an event impact per-spective,the Corona Virus Disease 2019(COVID-19)pandemic has not fundamentally affected the spatial pattern of the weighted Sino-US container shipping network but has significantly impacted the network’s connectivity.The network lacks sufficient resilience and stability in emergency situations.3)Based on the analysis of the structural characteristics and evolution of the weighted Sino-US con-tainer shipping network,recommendations for network development are proposed from three aspects:emphasizing the development of hub ports,focusing on the balanced development of the network,and optimizing the layout of Chinese ports.
基金National Natural Science Foundation of China,Grant/Award Number:51632008。
文摘The establishment of efficient oxygen evolution electrocatalysts is of great value but also challenging.Herein,a durable metal–organic framework(MOF)with minor atomically dispersed ruthenium and an optimized electronic structure is constructed as an efficient electrocatalyst.Significantly,the obtained NiRu_(0.08)-MOF with doping Ru only needs an overpotential of 187 mV at 10 mA cm^(-2) with a Tafel slop of 40 mV dec^(-1) in 0.1M KOH for the oxygen evolution reaction,and can work continuously for more than 300 h.Ultrahigh Ru mass activity is achieved,reaching 56.7 Ag^(-1)_(Ru) at an overpotential of 200 mV,which is 36 times higher than that of commercial RuO_(2).X-ray adsorption spectroscopy and density function theory calculations reveal that atomically dispersed ruthenium on metal sites in MOFs is expected to optimize the electronic structure of nickel sites,thus improving the conductivity of the catalyst and optimizing the adsorption energy of intermediates,resulting in significant optimization of electrocatalytic performance.This study could provide a new avenue for the design of efficient and stable MOF electrocatalysts.
基金supported by the Shanxi Science and Technology Major Project (No.20201102004)the Distinguished Youth Funds of National Natural Science Foundation of China (No.51925402)+2 种基金the National Natural Science Foundation of China (Nos.52174125,52004171,and 51904203)the Outstanding Youth Cultivation Project in Shanxi Province,China (No.202103021222008)the Key Science and Technology Innovation Team of“1331”Project in Shanxi Province,China,and the Open Fund Project of Key Laboratory of Mining Disaster Prevention and Control (No.MDPC202004)。
文摘A backfilling body-coal pillar-backfilling body(BPB)structure formed by pillar-side cemented paste backfilling can bear overburden stress and ensure safe mining.However,the failure response of BPB composite samples must be investigated.This paper examines the deformation characteristics and damage evolution of six types of BPB composite samples using a digital speckle correlation method under uniaxial compression conditions.A new damage evolution equation was established on the basis of the input strain energy and dissipated strain energy at the peak stress.The prevention and control mechanisms of the backfilling body on the coal pillar instability were discussed.The results show that the deformation localization and macroscopic cracks of the BPB composite samples first appeared at the coal-backfilling interface,and then expanded to the backfilling elements,ultimately appearing in the coal elements.The elastic strain energy in the BPB composite samples reached a maximum at the peak stress,whereas the dissipated energy continued to accumulate and increase.The damage evolution curve and equation agree well with the test results,providing further understanding of instability prevention and the control mechanisms of the BPB composite samples.The restraining effect on the coal pillar was gradually reduced with decreasing backfilling body element's volume ratio,and the BPB composite structure became more vulnerable to failure.This research is expected to guide the design,stability monitoring,instability prevention,and control of BPB structures in pillar-side cemented paste backfilling mining.
基金sponsored by the National Natural Science Foundation of China(52176193)the National Key Research and Development Program of China(2019YFD1100602)+1 种基金the Shandong Provincial Natural Science Foundation,China(ZR2020ME184)the SDUT & Zhangdian City Integration Development Project(2021JSCG0013)。
文摘This study aimed to investigate the mechanism of nitrogen doping,migration,and conversion during ammonia torrefaction and also explore the evolution law of the chemical structure of cellulose.The results showed that the ammonia torrefaction pretreatment could significantly optimize the distribution of nitrogen and oxygen elements in cellulose.The carbon skeleton first captured the active nitrogenous radicals to form-NHn-N,and pyridine-N and pyrrole-N originated from the conversion of-NHn-N.The existence of C=O played a major role in the immobilization of nitrogen.The nitrogen in bio-oil exists mainly in the form of five-and six-membered heterocycles.The correlation analysis showed that the main precursors for the formation of nitrogenous heterocyclic compounds were five-membered Oheterocyclic compounds.Finally,the product distribution characteristics in the torrefaction-pyrolysis systems were summarized,and the nitrogen doping and conversion mechanisms were proposed.This study expanded the boundaries of cellulose pretreatment and the production of high-value chemicals.
基金Supported by the National Natural Science Foundation of China(U19B6003-01).
文摘The Tongnan secondary negative structure in central Sichuan Basin has controls and influences on the structural framework and petroleum geological conditions in the Gaoshiti-Moxi area.To clarify the controls and influences,the deformation characteristics,structural attributes and evolution process of the Tongnan negative structure were investigated through a series of qualitative and quantitative methods such as balanced profile restoration,area-depth-strain(ADS)analysis,and structural geometric forward numerical simulation,after comprehensive structural interpretation of high-precision 3D seismic data.The results are obtained in three aspects.First,above and below the P/AnP(Permian/pre-Permian)unconformity,the Tongnan negative structure demonstrates vertical differential structural deformation.It experiences two stages of structural stacking and reworking:extensional depression(from the Sinian Dengying Formation to the Permian),and compressional syncline deformation(after the Jurassic).The multi-phase trishear deformation of the preexisting deep normal faults dominated the extensional depression.The primary depression episodes occurred in the periods from the end of Late Proterozoic to the deposition of the 1st–2nd members of the Dengying Formation,and from the deposition of Lower Cambrian Longwangmiao Formation–Middle–Upper Cambrian until the Ordovician.Second,the multi-stage evolution process of the Tongnan negative structure controlled the oil and gas migration and adjustment and present-day differential gas and water distribution between the Tongnan negative structure and the Gaoshiti and Moxi-Longnüsi structural highs.Third,the Ordovician,which is limitedly distributed in the Tongnan negative structure and is truncated by the P/AnP unconformity on the top,has basic geological conditions for the formation of weathering karst carbonate reservoirs.It is a new petroleum target deserving attention.
基金supported by National MCF Energy R&D Program of China(2018YFE0306105)National Key R&D Program of China(2020YFA0406104,2020YFA0406101)+10 种基金Innovative Research Group Project of the National Natural Science Foundation of China(51821002)National Natural Science Foundation of China(52201269,51725204,21771132,51972216,52041202)Natural Science Foundation of Jiangsu Province(BK20210735)Natural Science Foundation of the Higher Education Institutions of Jiangsu Province(21KJB430043)Collaborative Innovation Center of Suzhou Nano Science&Technologythe 111 ProjectSuzhou Key Laboratory of Functional Nano&Soft MaterialsJiangsu Key Laboratory for Advanced Negative Carbon Technologiesthe funding from Alexander von Humboldt(AvH)FoundationGusu leading talent plan for scientific and technological innovation and entrepreneurship(ZXL2022487)support from the German Federal Ministry of Education and Research in the framework of the project Catlab(03EW0015A/B)。
文摘Efficient and durable oxygen evolution reaction(OER)requires the electrocatalyst to bear abundant active sites,optimized electronic structure as well as robust component and mechanical stability.Herein,a bimetallic lanthanum-nickel oxysulfide with rich oxygen vacancies based on the La_(2)O_(2)S prototype is fabricated as a binder-free precatalyst for alkaline OER.The combination of advanced in situ and ex situ characterizations with theoretical calculation uncovers the synergistic effect among La,Ni,O,and S species during OER,which assures the adsorption and stabilization of the oxyanion SO_(4)^(2-)onto the surface of the deeply reconstructed porous heterostructure composed of confining Ni OOH nanodomains by La(OH)_3 barrier.Such coupling,confinement,porosity and immobilization enable notable improvement in active site accessibility,phase stability,mass diffusion capability and the intrinsic Gibbs free energy of oxygen-containing intermediates.The optimized electrocatalyst delivers exceptional alkaline OER activity and durability,outperforming most of the Ni-based benchmark OER electrocatalysts.
基金financially supported by the National Natural Science Foundation of China(No.52174291)。
文摘In order to study the sintering characteristics of Ca-rich iron ore,chemical analysis,laser diffraction,scanning electron microscopy,XRD-Rietveld method,and micro-sintering were used to analyze the mineralogical properties and sintering pot tests were used to study the sintering behavior.In addition,a grey correlation mathematical model was used to calculate and compare the comprehensive sintering performance under different calcium-rich iron ore contents.The results demonstrate that the Ca-rich iron ore has coarse grain size and strong self-fusing characteristics with Ca element in the form of calcite(CaCO_(3)) and the liquid phase produced by the self-fusing of the calcium-rich iron ore is well crystallized.Its application with a 20wt%content in sintering improves sinter productivity,reduces fuel consumption,enhances reduction index,and improves gas permeability in blast furnace by 0.45 t/(m^(2)·h),6.11 kg/t,6.17%,and 65.39 kPa·℃,respectively.The Ca-rich iron ore sintering can improve the calorific value of sintering flue gas compared with magnetite sintering,which is conducive to recovering heat for secondary use.As the content of the Ca-rich iron ore increases,sinter agglomeration shifts from localized liquid-phase bonding to a combination of localized liquid-phase bonding and iron oxide crystal connection.Based on an examination of the greater weight value of productivity with grey correlation analysis,the Ca-rich iron ore is beneficial for the comprehensive index of sintering in the range of 0-20wt%content.Therefore,it may be used in sintering with magnetite concentrates as the major ore species.
基金supported in part by the Special Fund for Basic Scientific Research Business Expenses of Central Public Welfare Scientific Research Institutes under Grant TKS20210103the Open Fund of Key Laboratory of Ocean Observation Technology,Ministry of Natural Resources of China(2021klootA06).
文摘River bending is the major effect responsible for bed topography and bank changes.In this study,fluid velocity(measured by a three-dimensional Doppler advanced point current meter)and bed topographical data have been collected in 40 sections of an experimental model.The whole flume was composed of an organic glass bend,upstream and downstream water tanks,two transition straight sections,a circulation pump,and a connection pipeline.Each section has been found to be characterized by a primary circulation and a small reverse circulation,with some sections even presenting three more or more circulation structures.The minimum circulation intensity has been detected in proximity to the top of the curved channel,while a region with small longitudinal velocity has been observed near the concave bank of each bend,corresponding to the flat bed formed after a short period of scouring.The maximum sediment deposition and scour depth in the presence of a uniform distribution of living flexible vegetation within 10 cm of the flume wall have been found to be smaller than those observed in the tests conducted without vegetation.
基金the National Natural Science Foundation of China(Nos.52072151,52171211,52102253,52271218,U22A20145)the Jinan Independent Innovative Team(2020GXRC015)+1 种基金the Major Program of Shandong Province Natural Science Foundation(ZR2021ZD05)the Science and Technology Program of University of Jinan(XKY2119).
文摘Focused exploration of earth-abundant and cost-efficient non-noble metal electrocatalysts with superior hydrogen evolution reaction(HER)performance is very important for large-scale and efficient electrolysis of water.Herein,a sandwich composite structure(designed as MS-Mo2C@NCNS)ofβ-Mo2C hollow nanotubes(HNT)and N-doped carbon nanosheets(NCNS)is designed and prepared using a binary NaCl–KCl molten salt(MS)strategy for HER.The temperature-dominant Kirkendall formation mechanism is tentatively proposed for such a three-dimensional hierarchical framework.Due to its attractive structure and componential synergism,MS-Mo2C@NCNS exposes more effective active sites,confers robust structural stability,and shows significant electrocatalytic activity/stability in HER,with a current density of 10 mA cm-2 and an overpotential of only 98 mV in 1 M KOH.Density functional theory calculations point to the synergistic effect of Mo2C HNT and NCNS,leading to enhanced electronic transport and suitable adsorption free energies of H*(ΔGH*)on the surface of electroactive Mo2C.More significantly,the MS-assisted synthetic methodology here provides an enormous perspective for the commercial development of highly active non-noble metal electrocatalysts toward efficient hydrogen evolution.
基金financially supported by the National Key Research and Development Program of China(No.2016YFB0700301,2016YFB1101003)Shaanxi Science&Technology Co-ordination&Innovation Project(No.2016KTZDCY02-02)
文摘A three-layer Ta_2O_5-containing coating was successfully fabricated by laser cladding on a pure Ta substrate. The maximum thickness of such a coating is about 1.6 mm. The microstructure, phase constitution and elemental distribution in the coating were investigated. Results show that the coating has been metallurgically bonded to the Ta substrate and the microstructure exhibits a graded change along the deposition direction from Ta substrate to the top of coating. In the layers I and II of the graded coating, the microstructure evolution can be confi rmed as a result of hypomonotectic reaction, but in the layer Ⅲ it was formed by hypermonotectic reaction. At the top of coating, the microstructure was still homogeneous although liquid phase separation had occurred, which can be attributed to the fact that the O-rich droplets do not have enough time to fl oat at high cooling rate. The theoretical calculation results show that during laser cladding, the solidifi cation time of the melt pool was less than 0.1 s, which fi ts well with the results from the experiment.
基金supported by the National Natural Science Foundation of China (Grant No.50571081)the Aeronautical Science Foundation of China (Grant No.04G53042)
文摘The microstructure, chemical composition and morphology evolution of icosahedral quasicrystalline phase of Mg67.4Zn28.9Y3.7 ternary alloy were investigated in detail at different pouring temperatures by X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy-dispersive spectrum (EDS). Low interracial energy favors the formation of l-phase. The experimental results show that the primary l-phase reveals petal-shaped with five and six branches, where each branch has facetted growth morphology with the size ranging from 50 to 100μm. As the temperature decreases, the polygon-shaped l-phase forms, attributed to the decomposition of branch of petal-shaped l-phase, and then it grows bigger and some of the fine polygons join together to form large polygons. Besides these, (α-Mg+l-phase) eutectic structures disappear and the relative amount of Mg7Zn3 phase increases as the pouring temperature decreases. The chemical composition and morphology evolution of l-phase were also discussed.