Energy determines the ability of matter to work. However, in the given environment, the real usefulness to perform work is determined by exergy. This study covers not only solar, but also any monochromatic thermal rad...Energy determines the ability of matter to work. However, in the given environment, the real usefulness to perform work is determined by exergy. This study covers not only solar, but also any monochromatic thermal radiation. The value of such radiation was determined by its exergy and the ratio of its exergy-to-energy. A novelty in this work is to demonstrate by means of exergy that the usefulness of thermal polychromatic radiation can be increased by its dispersion to monochromatic radiation. This effect is the greater, the lower the temperature of the radiation. Analogies of this effect to the exergetic effect of gas separation have been indicated. The effect of the increase in exergy in the process of radiation dispersion was interpreted by means of a cylinder-piston system that explains this effect with the influence of environmental radiation. The concept of quasi-monochromatic and cumulated radiation was introduced into dispersion considerations and the change in the energetic, entropic and environmental components of the exergy of radiation beams was analyzed. Considerations were illustrated with appropriate examples of calculations considering dispersion of high-temperature radiation, such as extraterrestrial solar radiation and dispersion of low-temperature radiation from water vapor.展开更多
High-viscosity dispersing system is formed by dispersing the solid particles in the high-viscosity continuous medium.It is very easy to form the three-dimensional network structure for solid particles in the system an...High-viscosity dispersing system is formed by dispersing the solid particles in the high-viscosity continuous medium.It is very easy to form the three-dimensional network structure for solid particles in the system and the rheology behavior becomes complicated.The apparent viscosity of this dispersing system always has the connection with the volume ratio and the shear rate.In order to discuss the rheology behavior and put up the viscosity model,the suspension of silicon dioxide and silicon oil were prepared.Through testing the viscosity,the solid concentration and the shear rate,the effects of the ratio and the shear rate on viscosity was analyzed,the model of the high-viscosity dispersing system was designed and the model with the printing ink were validated.The experiment results show that the model is applicable to the high-viscosity dispersing systems.展开更多
A systematic investigation on the mechanism of dynamic liquid dispersing process via theoretical and experimental approach is presented.The experiments include weak and strong constrained scenarios using the high-spee...A systematic investigation on the mechanism of dynamic liquid dispersing process via theoretical and experimental approach is presented.The experiments include weak and strong constrained scenarios using the high-speed camera technique and the flash X-ray radiography technique.Based on dynamic analysis,one-dimensional characteristics analysis and some numerical simulations on the propagating processes of blast waves before the container shell rupturing,further and detailed analyses of the experimental results are presented.The effects of the liquid viscosity on the dynamic dispersing flow are also analyzed,and the spall fracture mechanism is explored.Thus,the dominating forces determining the dispersing liquid flow are revealed,that is,the stretching and shearing action due to the interaction of two reflecting rarefaction waves in opposite propagating directions.The influence of container shell strength on the dispersing liquid flow is also investigated,and the characters of cavitation layered in liquid before shell rupturing are uncovered.Results revealed that different shell material results in different cavitating layers.Then the different cavitating layers drive the different dynamic liquid dispersing process coming into being.The metastable liquid states caused by pressure drop and cavitation generation are discussed.展开更多
In our relevant paper[Zhao S X(2021)Chin.Phys.B 30055201],a delta distribution of negative ions is given by fluid simulation and preliminarily explained by decomposed anions transport equation.In the present work,firs...In our relevant paper[Zhao S X(2021)Chin.Phys.B 30055201],a delta distribution of negative ions is given by fluid simulation and preliminarily explained by decomposed anions transport equation.In the present work,first,the intrinsic connection between the electropositive plasma transport equation and spring oscillator dynamic equation is established.Inspired by this similarity,reformed“spring oscillator”equation with dispersing instead of restoring force that gives quasi-delta solution is devised according to the math embodied in the anion equation,which is of potential significance to the disciplines of atomic physics and astronomy as well.For solving the“diffusion confusion”the physics that determines the delta profile within the continuity equation is explored on the basis that recombination loss source term plays the role of drift flux,which is applicable for fluid model of low temperature plasma,but not the ordinary fluid dynamics.Besides,the math and physics revealed in this work predict that the ratio of recombination or attachment(for electrons)frequency versus the species diffusion coefficient is a very important parameter in determining the delta distribution,as it acts as the acceleration of object,according to the reformed oscillator equation.With this theory,the analogous delta profile of electrons density in the famous drift and ambi-polar diffusion heating mechanism of electronegative capacitively coupled plasma is interpreted.展开更多
We added Cellulase into the SDS solution for enhancing its dispersion ability to CuPc in terms of their synergistic actions. The optimal mass ratio of SDS/cellulase was determined to be 9 : 1 by dispersibility measure...We added Cellulase into the SDS solution for enhancing its dispersion ability to CuPc in terms of their synergistic actions. The optimal mass ratio of SDS/cellulase was determined to be 9 : 1 by dispersibility measurement. The surface modification of CuPc of SDS/cellulase was confirmed by TG analysis.展开更多
Geographical background and dispersal ability may strongly influence assemblage dissimilarity;however,these aspects have generally been overlooked in previous large-scale beta diversity studies.Here,we examined whethe...Geographical background and dispersal ability may strongly influence assemblage dissimilarity;however,these aspects have generally been overlooked in previous large-scale beta diversity studies.Here,we examined whether the patterns and drivers of taxonomic beta diversity(TBD)and phylogenetic beta diversity(PBD)of breeding birds in China vary across(1)regions on both sides of the Hu Line,which demarcates China’s topographical,climatic,economic,and social patterns,and(2)species with different dispersal ability.TBD and PBD were calculated and partitioned into turnover and nestedness components using a moving window approach.Variables representing climate,habitat heterogeneity,and habitat quality were employed to evaluate the effects of environmental filtering.Spatial distance was considered to assess the impact of dispersal limitation.Variance partitioning analysis was applied to assess the relative roles of these variables.In general,the values of TBD and PBD were high in mountainous areas and were largely determined by environmental filtering.However,different dominant environmental filters on either side of the Hu Line led to divergent beta diversity patterns.Specifically,climate-driven species turnover and habitat heterogeneity-related species nestedness dominated the regions east and west of the line,respectively.Additionally,bird species with stronger dispersal ability were more susceptible to environmental filtering,resulting in more homogeneous assemblages.Our results indicated that regions with distinctive geographical backgrounds may present different ecological factors that lead to divergent assemblage dissimilarity patterns,and dispersal ability determines the response of assemblages to these ecological factors.Identifying a single universal explanation for the observed pattern without considering these aspects may lead to simplistic or incomplete conclusions.Consequently,a comprehensive understanding of large-scale beta diversity patterns and effective planning of conservation strategies necessitate the consideration of both geographical background and species dispersal ability.展开更多
The impact of alkyl dimethyl betaine (ADB) on the collection capacity of sodium oleate (NaOl) at low temperatures was evaluated using flotation tests at various scales. The low-temperature synergistic mechanism of ADB...The impact of alkyl dimethyl betaine (ADB) on the collection capacity of sodium oleate (NaOl) at low temperatures was evaluated using flotation tests at various scales. The low-temperature synergistic mechanism of ADB and NaOl was explored by infrared spectroscopy, X-ray photoelectron spectroscopy, surface tension measurement, foam performance test, and flotation reagent size measurement.The flotation tests revealed that the collector mixed with octadecyl dimethyl betaine (ODB) and NaOl in a mass ratio of 4:96 exhibited the highest collection capacity. The combined collector could increase the scheelite recovery by 3.48% at low temperatures of 8–12℃. This is particularly relevant in the Luanchuan area, which has the largest scheelite concentrate output in China. The results confirmed that ODB enhanced the collection capability of NaOl by improving the dispersion and foaming performance. Betaine can be introduced as an additive to NaOl to improve the recovery of scheelite at low temperatures.展开更多
Proposed agroforestry options should begin with the species that farmers are most familiar with,which would be the native multipurpose trees that have evolved under smallholder farms and socioeconomic conditions.The A...Proposed agroforestry options should begin with the species that farmers are most familiar with,which would be the native multipurpose trees that have evolved under smallholder farms and socioeconomic conditions.The African birch(Anogeissus leiocarpa(DC.)Guill.&Perr.)and pink jacaranda(Stereospermum kunthianum Cham.)trees are the dominant species in the agroforestry parkland system in the drylands of Tigray,Ethiopia.Smallholder farmers highly value these trees for their multifunctional uses including timber,firewood,charcoal,medicine,etc.These trees also could improve soil fertility.However,the amount of soil physical and chemical properties enhanced by the two species must be determined to maintain the sustainable conservation of the species in the parklands and to scale up to similar agroecological systems.Hence,we selected twelve isolated trees,six from each species that had similar dendrometric characteristics and were growing in similar environmental conditions.We divided the canopy cover of each tree into three radial distances:mid-canopy,canopy edge,and canopy gap(control).At each distance,we took soil samples from three different depths.We collected 216 soil samples(half disturbed and the other half undisturbed)from each canopy position and soil depth.Bulk density(BD),soil moisture content(SMC),soil organic carbon(SOC),total nitrogen(TN),available phosphorus(AP),available potassium(AK),p H,electrical conductivity(EC),and cation exchange capacity(CEC)were analysed.Results revealed that soil physical and chemical properties significantly improved except for soil texture and EC under both species,CEC under A.leiocarpus,and soil p H under S.kunthianum,all the studied soils were improved under both species canopy as compared with canopy gap.SMC,TN,AP,and AK under canopy of these trees were respectively 24.1%,11.1%,55.0%,and 9.3% higher than those soils under control.The two parkland agroforestry species significantly enhanced soil fertility near the canopy of topsoil through improving soil physical and chemical properties.These two species were recommended in the drylands with similar agro-ecological systems.展开更多
We theoretically investigate the propagation characteristics of spin waves in skyrmion-based magnonic crystals. It is found that the dispersion relation can be manipulated by strains through magneto-elastic coupling. ...We theoretically investigate the propagation characteristics of spin waves in skyrmion-based magnonic crystals. It is found that the dispersion relation can be manipulated by strains through magneto-elastic coupling. Especially, the allowed bands and forbidden bands in dispersion relations shift to higher frequency with strain changing from compressive to tensile,while shifting to lower frequency with strain changing from tensile to compressive. We also confirm that the spin wave with specific frequency can pass the magnonic crystal or be blocked by tuning the strains. The result provides an advanced platform for studying the tunable skyrmion-based spin wave devices.展开更多
The study of non-axisymmetric fuel dispersal and detonation can provide reference for the prevention of industrial cloud explosion accidents and the design of fuel air explosive(FAE).The concentration and detonation f...The study of non-axisymmetric fuel dispersal and detonation can provide reference for the prevention of industrial cloud explosion accidents and the design of fuel air explosive(FAE).The concentration and detonation fields of 85 kg cylindrical and fan-shaped fuel are investigated by experiments and numerical simulations.A dynamic model of the whole process for fuel dispersal and detonation is built.The concentration distribution of fuel is used as the initial condition to calculate the detonation stage,thus solving the initial value problem of detonation field.The phase and component changes of fuel cloud at different locations are compared.The fuel cloud is divided into directions of 0°,90°,135°and 180°.The results show that the maximum cloud radius is 20.94 m in 135°and the minimum is 12.04 m in 0°.The diameter of the detonation fireball is 53.6 m,and the peak temperature is 3455 K.The highest peak overpressure is 3.44 MPa in 0°and the lowest is 2.97 MPa in 135°.The proportion of liquid phase in 0°is22.90%,and the fuel loss is 11.8% and 9% higher than that in 135°and cylindrical charge,respectively.The stable propagation distance of blast wave in 135°is 42.50% longer than 0°and 28.37% longer than cylindrical charge.展开更多
Lithium–oxygen battery with ultrahigh theoretical energy density is considered a highly competitive next-generation energy storage device,but its practical application is severely hindered by issues such as difficult...Lithium–oxygen battery with ultrahigh theoretical energy density is considered a highly competitive next-generation energy storage device,but its practical application is severely hindered by issues such as difficult decomposition of discharge products at present.Here,we have developed N-doped carbon anchored atomically dispersed Ru sites cathode catalyst with open hollow structure(h-RuNC)for Lithium–oxygen battery.On one hand,the abundance of atomically dispersed Ru sites can effectively catalyze the formation and decomposition of discharge products,thereby greatly enhancing the redox kinetics.On the other hand,the open hollow structure not only enhances the mass activity of atomically dispersed Ru sites but also improves the diffusion efficiency of catalytic molecules.Therefore,the excellent activity from atomically dispersed Ru sites and the enhanced diffusion from open hollow structure respectively improve the redox kinetics and cycling stability,ultimately achieving a high-performance lithium–oxygen battery.展开更多
A trigger system is typically employed in active seismic testing to trigger and synchronize multichannel surface wave data acquisition.The effect of the trigger system on the dispersion image of surface waves is empir...A trigger system is typically employed in active seismic testing to trigger and synchronize multichannel surface wave data acquisition.The effect of the trigger system on the dispersion image of surface waves is empirically known to be negligible,however,theoretical explanation regarding the effect of the trigger system is insufficient.This study systematically examines the theory for surface wave dispersion analysis and proves that the effect of the trigger system on a dispersion image is negligible via a solid theoretical explanation.Subsequently,based on the new theoretical explanation,an alternative method that uses only the relative phase difference between sensors to extract dispersion characteristics with better conceptual clarity is proposed.Two active surface wave testing cases are considered to validate the theory and method.The results indicate that(1)an accurate trigger system is not necessary for surface wave data acquisition,and(2)it is unnecessary to assume that the impact point is the generation point of the surface waves for the experimental dispersion analysis.展开更多
Biological invasion is triggered by human development activities such as the construction and expansion of road networks.Road verges serve as important habitats and corridors for the distribution of invasive alien pla...Biological invasion is triggered by human development activities such as the construction and expansion of road networks.Road verges serve as important habitats and corridors for the distribution of invasive alien plant species(IAPS)between geographically distant habitats.However,the trajectory of plant invasion and the data regarding the impact of roads on IAPS distribution are relatively poor in Nepal.Here,we surveyed two road types(main roads and feeder road)in the Middle Mountain region of central Nepal in order to investigate how different road types are driving the dispersal of IAPS along road verges and the adjacent natural habitats.Systematic sampling was conducted at ca 2.5 km intervals along the roads.At each sampling site,paired plots(25 m×4 m)were sampled:one adjacent to and along the road,and another 20 m away and parallel to it in the interior habitat.Our results revealed that the main road verges had a higher cover(33%)and a larger number of IAPS(14 species)than the feeder road(25%;10 species).The IAPS cover and richness were significantly higher along verges than in the adjacent interior habitats for both road types,indicating that roads are contributing as corridors for the dispersal of IAPS in the Middle Mountain areas of central Nepal.Further,elevation,tree canopy,and disturbances(grazing/mowing/trampling)were found to be the key factors that determine spatial distribution of IAPS along road verges.We emphasize that regular monitoring of vegetation along the road verges can help with the early detection and control of potential IAPS in the region before they become problematic.展开更多
The maintenance of sand-fixing vegetation is important for the stability of artificial sand-fixing systems in which seed dispersal plays a key role.Based on field wind tunnel experiments using 11 common plant species ...The maintenance of sand-fixing vegetation is important for the stability of artificial sand-fixing systems in which seed dispersal plays a key role.Based on field wind tunnel experiments using 11 common plant species on the southeastern edge of the Tengger Desert,China,we studied the secondary seed dispersal in the fixed and semi-fixed sand dunes as well as in the mobile dunes in order to understand the limitations of vegetation regeneration and the maintenance of its stability.Our results indicated that there were significant variations among the selected 11 plant species in the threshold of wind speed(TWS).The TWS of Caragana korshinskii was the highest among the 11 plant species,whereas that of Echinops gmelinii was the lowest.Seed morphological traits and underlying surface could generally explain the TWS.During the secondary seed dispersal processes,the proportions of seeds that did not disperse(no dispersal)and only dispersed over short distance(short-distance dispersal within the wind tunnel test section)were significantly higher than those of seeds that were buried(including lost seeds)and dispersed over long distance(long-distance dispersal beyond the wind tunnel test section).Compared with other habitats,the mobile dunes were the most difficult places for secondary seed dispersal.Buried seeds were the easiest to be found in the semi-fixed sand dunes,whereas fixed sand dunes were the best sites for seeds that dispersed over long distance.The results of linear mixed models showed that after controlling the dispersal distance,smaller and rounder seeds dispersed farther.Shape index and wind speed were the two significant influencing factors on the burial of seeds.The explanatory power of wind speed,underlying surface,and seed morphological traits on the seeds that did not disperse and dispersed over short distance was far greater than that on the seeds that were buried and dispersed over long distance,implying that the processes and mechanisms of burial and long-distance dispersal are more complex.In summary,most seeds in the study area either did not move,were buried,or dispersed over short distance,promoting local vegetation regeneration.展开更多
Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utiliz...Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic functionality.Furthermore,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains elusive.Here,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom sites.Then the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed catalysts.Finally,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered.展开更多
In this paper,layered periodic foundations(LPFs)are numerically examined for their responses to longitudinal and transverse modes in the time and frequency domains.Three different unit-cells,i.e.,2-layer,4-layer,and 6...In this paper,layered periodic foundations(LPFs)are numerically examined for their responses to longitudinal and transverse modes in the time and frequency domains.Three different unit-cells,i.e.,2-layer,4-layer,and 6-layer unit-cells,comprising concrete/rubber,concrete/rubber/steel/rubber,and concrete/rubber/steel/rubber/lead/rubber materials,respectively,are taken into account.Also,the viscoelasticity behavior of the rubber is modeled with two factors,i.e.,a frequency-independent(FI)loss factor and a linear frequency-dependent(FD)loss factor.Following the extraction of the complex dispersion curves and the identification of the band gaps(BGs),the simulations of wave transmission in the time and frequency domains are performed using the COMSOL software.Subsequent parametric studies evaluate the effects of the rubber viscoelasticity models on the dispersion curves and the wave transmission for the longitudinal and transverse modes.The results show that considering the rubber viscoelasticity enhances the wave attenuation performance.Moreover,the transverse-mode damping is more sensitive to the viscoelasticity model than its longitudinal counterpart.The 6-layer unit-cell LPF exhibits the lowest BG,ranging from 4.8 Hz to 6.5 Hz.展开更多
Antimony(Sb)-ba sed anode materials are feasible candidates for sodium-ion batteries(SIBs) due to their high theoretical specific capacity and excellent electrical conductivity.However,they still suffer from volume di...Antimony(Sb)-ba sed anode materials are feasible candidates for sodium-ion batteries(SIBs) due to their high theoretical specific capacity and excellent electrical conductivity.However,they still suffer from volume distortion,structural collapse,and ionic conduction interruption upon cycling.Herein,a hierarchical array-like nanofiber structure was designed to address these limitations by combining architecture engineering and anion tuning strategy,in which SbPO_(4-x) with oxygen vacancy nanosheet arrays are anchored on the surface of interwoven carbon nanofibers(SbPO_(4-x)@CNFs).In particular,bulky PO_(4)^(3-) anions mitigate the large volume distortion and generate Na_(3)PO_(4) with high ionic conductivity,collectively improving cyclic stability and ionic transport efficiency.The abundant oxygen vacancies substantially boost the intrinsic electronic conductivity of SbPO_4,further accelerating the reaction dynamics.In addition,hierarchical fibrous structures provide abundant active sites,construct efficient conducting networks,and enhance the electron/ion transport capacity.Benefiting from the advanced structural design,the SbPO_(4-x)@CNFs electrodes exhibit outstanding cycling stability(1000 cycles at 1.0 A g^(-1) with capacity decay of 0.05% per cycle) and rapid sodium storage performance(293.8 mA h g^(-1) at 5.0 A g^(-1)).Importantly,systematic in-/ex-situ techniques have revealed the "multi-step conversion-alloying" reaction process and the "battery-capacitor dual-mode" sodium-storage mechanism.This work provides valuable insights into the design of anode materials for advanced SIBs with elevated stability and superior rate performance.展开更多
Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites...Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites with atomically dispersed oxygen(O)coordination on bacterial cellulose-converted graphitic carbon(Mn-O-C).Evidence of the atomically dispersed Mn-(O-C_(2))_(4)moieties embedding in the exposed basal plane of carbon surface is confirmed by X-ray absorption spectroscopy.As a result,the as-synthesized Mn-O-C catalyst exhibits superior NitRR activity with an NH_(3)yield rate(RNH_(3))of 1476.9±62.6μg h^(−1)cm^(−2)at−0.7 V(vs.reversible hydrogen electrode,RHE)and a faradaic efficiency(FE)of 89.0±3.8%at−0.5 V(vs.RHE)under ambient conditions.Further,when evaluated with a practical flow cell,Mn-O-C shows a high RNH_(3)of 3706.7±552.0μg h^(−1)cm^(−2)at a current density of 100 mA cm−2,2.5 times of that in the H cell.The in situ FT-IR and Raman spectroscopic studies combined with theoretical calculations indicate that the Mn-(O-C_(2))_(4)sites not only effectively inhibit the competitive hydrogen evolution reaction,but also greatly promote the adsorption and activation of nitrate(NO_(3)^(−)),thus boosting both the FE and selectivity of NH_(3)over Mn-(O-C_(2))_(4)sites.展开更多
Clays have considerable influence on the electrical properties of hydrate-bearing sediments.It is desirable to understand the electrical properties of hydrate-bearing clayey sediments and to build hydrate saturation(S...Clays have considerable influence on the electrical properties of hydrate-bearing sediments.It is desirable to understand the electrical properties of hydrate-bearing clayey sediments and to build hydrate saturation(S_(h))models for reservoir evaluation and monitoring.The electrical properties of tetrahydrofuran-hydrate-bearing sediments with montmorillonite are characterized by complex conductivity at frequencies from 0.01 Hz to 1 kHz.The effects of clay and Sh on the complex conductivity were analyzed.A decrease and increase in electrical conductance result from the clay-swelling-induced blockage and ion migration in the electrical double layer(EDL),respectively.The quadrature conductivity increases with the clay content up to 10%because of the increased surface site density of counterions in EDL.Both the in-phase conductivity and quadrature conductivity decrease consistently with increasing Sh from 0.50 to 0.90.Three sets of models for Sh evaluation were developed.The model based on the Simandoux equation outperforms Archie’s formula,with a root-mean-square error(E_(RMS))of 1.8%and 3.9%,respectively,highlighting the clay effects on the in-phase conductivity.The fre-quency effect correlations based on in-phase and quadrature conductivities exhibit inferior performance(E_(RMS)=11.6%and 13.2%,re-spectively)due to the challenge of choosing an appropriate pair of frequencies and intrinsic uncertainties from two measurements.The second-order Cole-Cole formula can be used to fit the complex-conductivity spectra.One pair of inverted Cole-Cole parameters,i.e.,characteristic time and chargeability,is employed to predict S_(h) with an E_(RMS) of 5.05%and 9.05%,respectively.展开更多
Electrochemical carbon dioxide reduction reaction(CO_(2)RR)involves a variety of intermediates with highly correlated reaction and ad-desorption energies,hindering optimization of the catalytic activity.For example,in...Electrochemical carbon dioxide reduction reaction(CO_(2)RR)involves a variety of intermediates with highly correlated reaction and ad-desorption energies,hindering optimization of the catalytic activity.For example,increasing the binding of the*COOH to the active site will generally increase the*CO desorption energy.Breaking this relationship may be expected to dramatically improve the intrinsic activity of CO_(2)RR,but remains an unsolved challenge.Herein,we addressed this conundrum by constructing a unique atomic dispersed hetero-pair consisting of Mo-Fe di-atoms anchored on N-doped carbon carrier.This system shows an unprecedented CO_(2)RR intrinsic activity with TOF of 3336 h−1,high selectivity toward CO production,Faradaic efficiency of 95.96%at−0.60 V and excellent stability.Theoretical calculations show that the Mo-Fe diatomic sites increased the*COOH intermediate adsorption energy by bridging adsorption of*COOH intermediates.At the same time,d-d orbital coupling in the Mo-Fe di-atom results in electron delocalization and facilitates desorption of*CO intermediates.Thus,the undesirable correlation between these steps is broken.This work provides a promising approach,specifically the use of di-atoms,for breaking unfavorable relationships based on understanding of the catalytic mechanisms at the atomic scale.展开更多
文摘Energy determines the ability of matter to work. However, in the given environment, the real usefulness to perform work is determined by exergy. This study covers not only solar, but also any monochromatic thermal radiation. The value of such radiation was determined by its exergy and the ratio of its exergy-to-energy. A novelty in this work is to demonstrate by means of exergy that the usefulness of thermal polychromatic radiation can be increased by its dispersion to monochromatic radiation. This effect is the greater, the lower the temperature of the radiation. Analogies of this effect to the exergetic effect of gas separation have been indicated. The effect of the increase in exergy in the process of radiation dispersion was interpreted by means of a cylinder-piston system that explains this effect with the influence of environmental radiation. The concept of quasi-monochromatic and cumulated radiation was introduced into dispersion considerations and the change in the energetic, entropic and environmental components of the exergy of radiation beams was analyzed. Considerations were illustrated with appropriate examples of calculations considering dispersion of high-temperature radiation, such as extraterrestrial solar radiation and dispersion of low-temperature radiation from water vapor.
文摘High-viscosity dispersing system is formed by dispersing the solid particles in the high-viscosity continuous medium.It is very easy to form the three-dimensional network structure for solid particles in the system and the rheology behavior becomes complicated.The apparent viscosity of this dispersing system always has the connection with the volume ratio and the shear rate.In order to discuss the rheology behavior and put up the viscosity model,the suspension of silicon dioxide and silicon oil were prepared.Through testing the viscosity,the solid concentration and the shear rate,the effects of the ratio and the shear rate on viscosity was analyzed,the model of the high-viscosity dispersing system was designed and the model with the printing ink were validated.The experiment results show that the model is applicable to the high-viscosity dispersing systems.
基金the support of National Nature Science Foundation of China, the support numbers are No. 10572149 and No.10676120the National Key Research and Development program of China (subject no. 2017YFC0209901) for its support to the work of this paper
文摘A systematic investigation on the mechanism of dynamic liquid dispersing process via theoretical and experimental approach is presented.The experiments include weak and strong constrained scenarios using the high-speed camera technique and the flash X-ray radiography technique.Based on dynamic analysis,one-dimensional characteristics analysis and some numerical simulations on the propagating processes of blast waves before the container shell rupturing,further and detailed analyses of the experimental results are presented.The effects of the liquid viscosity on the dynamic dispersing flow are also analyzed,and the spall fracture mechanism is explored.Thus,the dominating forces determining the dispersing liquid flow are revealed,that is,the stretching and shearing action due to the interaction of two reflecting rarefaction waves in opposite propagating directions.The influence of container shell strength on the dispersing liquid flow is also investigated,and the characters of cavitation layered in liquid before shell rupturing are uncovered.Results revealed that different shell material results in different cavitating layers.Then the different cavitating layers drive the different dynamic liquid dispersing process coming into being.The metastable liquid states caused by pressure drop and cavitation generation are discussed.
文摘In our relevant paper[Zhao S X(2021)Chin.Phys.B 30055201],a delta distribution of negative ions is given by fluid simulation and preliminarily explained by decomposed anions transport equation.In the present work,first,the intrinsic connection between the electropositive plasma transport equation and spring oscillator dynamic equation is established.Inspired by this similarity,reformed“spring oscillator”equation with dispersing instead of restoring force that gives quasi-delta solution is devised according to the math embodied in the anion equation,which is of potential significance to the disciplines of atomic physics and astronomy as well.For solving the“diffusion confusion”the physics that determines the delta profile within the continuity equation is explored on the basis that recombination loss source term plays the role of drift flux,which is applicable for fluid model of low temperature plasma,but not the ordinary fluid dynamics.Besides,the math and physics revealed in this work predict that the ratio of recombination or attachment(for electrons)frequency versus the species diffusion coefficient is a very important parameter in determining the delta distribution,as it acts as the acceleration of object,according to the reformed oscillator equation.With this theory,the analogous delta profile of electrons density in the famous drift and ambi-polar diffusion heating mechanism of electronegative capacitively coupled plasma is interpreted.
文摘We added Cellulase into the SDS solution for enhancing its dispersion ability to CuPc in terms of their synergistic actions. The optimal mass ratio of SDS/cellulase was determined to be 9 : 1 by dispersibility measurement. The surface modification of CuPc of SDS/cellulase was confirmed by TG analysis.
基金supported by the National Natural Science Foundation of China(31901220)Science and Technology Planning Project of Guangdong Province,China(2019B121202004)+1 种基金Guangdong Basic and Applied Basic Research Foundation(2021A1515110744)Forestry Administration of Guangdong Province(DFGP Project of Fauna of Guangdong-202115)。
文摘Geographical background and dispersal ability may strongly influence assemblage dissimilarity;however,these aspects have generally been overlooked in previous large-scale beta diversity studies.Here,we examined whether the patterns and drivers of taxonomic beta diversity(TBD)and phylogenetic beta diversity(PBD)of breeding birds in China vary across(1)regions on both sides of the Hu Line,which demarcates China’s topographical,climatic,economic,and social patterns,and(2)species with different dispersal ability.TBD and PBD were calculated and partitioned into turnover and nestedness components using a moving window approach.Variables representing climate,habitat heterogeneity,and habitat quality were employed to evaluate the effects of environmental filtering.Spatial distance was considered to assess the impact of dispersal limitation.Variance partitioning analysis was applied to assess the relative roles of these variables.In general,the values of TBD and PBD were high in mountainous areas and were largely determined by environmental filtering.However,different dominant environmental filters on either side of the Hu Line led to divergent beta diversity patterns.Specifically,climate-driven species turnover and habitat heterogeneity-related species nestedness dominated the regions east and west of the line,respectively.Additionally,bird species with stronger dispersal ability were more susceptible to environmental filtering,resulting in more homogeneous assemblages.Our results indicated that regions with distinctive geographical backgrounds may present different ecological factors that lead to divergent assemblage dissimilarity patterns,and dispersal ability determines the response of assemblages to these ecological factors.Identifying a single universal explanation for the observed pattern without considering these aspects may lead to simplistic or incomplete conclusions.Consequently,a comprehensive understanding of large-scale beta diversity patterns and effective planning of conservation strategies necessitate the consideration of both geographical background and species dispersal ability.
基金financially supported by the National Natural Science Foundation of China (Nos.51904339 and No.51974364)the Key Laboratory of Hunan Province for Clean and Efficient Utilization of Strategic Calcium-containing Mineral Resources,China (No.2018TP1002)the Co-Innovation Centre for Clean and Efficient Utilization of Strategic Metal Mineral Resources,and the Postgraduate Independent Exploration and Innovation Project of Central South University,China (No.2018zzts224)。
文摘The impact of alkyl dimethyl betaine (ADB) on the collection capacity of sodium oleate (NaOl) at low temperatures was evaluated using flotation tests at various scales. The low-temperature synergistic mechanism of ADB and NaOl was explored by infrared spectroscopy, X-ray photoelectron spectroscopy, surface tension measurement, foam performance test, and flotation reagent size measurement.The flotation tests revealed that the collector mixed with octadecyl dimethyl betaine (ODB) and NaOl in a mass ratio of 4:96 exhibited the highest collection capacity. The combined collector could increase the scheelite recovery by 3.48% at low temperatures of 8–12℃. This is particularly relevant in the Luanchuan area, which has the largest scheelite concentrate output in China. The results confirmed that ODB enhanced the collection capability of NaOl by improving the dispersion and foaming performance. Betaine can be introduced as an additive to NaOl to improve the recovery of scheelite at low temperatures.
基金supported by the Sustainable Forest Management Project with the Local Communities in Tigray,northern Ethiopia,which was funded by the Norwegian Agency for Development Cooperation(NORAD)under the Norwegian Programme for Capacity Development in Higher EducationResearch for Development(NORHED)Programme(ETH 13/0018)+4 种基金the Ecological Organic Agriculture Project,Mekelle University,Ethiopiathe Institute of International Education-Scholars Rescue Fund(IIE-SRF)Norwegian University of Life Sciences(NMBU)Faculty of Environmental Sciences and Natural Resource Management(MINA)NORGLOBAL 2 Project in Ethiopia(303600)for supporting the research。
文摘Proposed agroforestry options should begin with the species that farmers are most familiar with,which would be the native multipurpose trees that have evolved under smallholder farms and socioeconomic conditions.The African birch(Anogeissus leiocarpa(DC.)Guill.&Perr.)and pink jacaranda(Stereospermum kunthianum Cham.)trees are the dominant species in the agroforestry parkland system in the drylands of Tigray,Ethiopia.Smallholder farmers highly value these trees for their multifunctional uses including timber,firewood,charcoal,medicine,etc.These trees also could improve soil fertility.However,the amount of soil physical and chemical properties enhanced by the two species must be determined to maintain the sustainable conservation of the species in the parklands and to scale up to similar agroecological systems.Hence,we selected twelve isolated trees,six from each species that had similar dendrometric characteristics and were growing in similar environmental conditions.We divided the canopy cover of each tree into three radial distances:mid-canopy,canopy edge,and canopy gap(control).At each distance,we took soil samples from three different depths.We collected 216 soil samples(half disturbed and the other half undisturbed)from each canopy position and soil depth.Bulk density(BD),soil moisture content(SMC),soil organic carbon(SOC),total nitrogen(TN),available phosphorus(AP),available potassium(AK),p H,electrical conductivity(EC),and cation exchange capacity(CEC)were analysed.Results revealed that soil physical and chemical properties significantly improved except for soil texture and EC under both species,CEC under A.leiocarpus,and soil p H under S.kunthianum,all the studied soils were improved under both species canopy as compared with canopy gap.SMC,TN,AP,and AK under canopy of these trees were respectively 24.1%,11.1%,55.0%,and 9.3% higher than those soils under control.The two parkland agroforestry species significantly enhanced soil fertility near the canopy of topsoil through improving soil physical and chemical properties.These two species were recommended in the drylands with similar agro-ecological systems.
文摘We theoretically investigate the propagation characteristics of spin waves in skyrmion-based magnonic crystals. It is found that the dispersion relation can be manipulated by strains through magneto-elastic coupling. Especially, the allowed bands and forbidden bands in dispersion relations shift to higher frequency with strain changing from compressive to tensile,while shifting to lower frequency with strain changing from tensile to compressive. We also confirm that the spin wave with specific frequency can pass the magnonic crystal or be blocked by tuning the strains. The result provides an advanced platform for studying the tunable skyrmion-based spin wave devices.
基金supported by the National Key Research and Development Program of China (Grant No.2021YFC3001204)。
文摘The study of non-axisymmetric fuel dispersal and detonation can provide reference for the prevention of industrial cloud explosion accidents and the design of fuel air explosive(FAE).The concentration and detonation fields of 85 kg cylindrical and fan-shaped fuel are investigated by experiments and numerical simulations.A dynamic model of the whole process for fuel dispersal and detonation is built.The concentration distribution of fuel is used as the initial condition to calculate the detonation stage,thus solving the initial value problem of detonation field.The phase and component changes of fuel cloud at different locations are compared.The fuel cloud is divided into directions of 0°,90°,135°and 180°.The results show that the maximum cloud radius is 20.94 m in 135°and the minimum is 12.04 m in 0°.The diameter of the detonation fireball is 53.6 m,and the peak temperature is 3455 K.The highest peak overpressure is 3.44 MPa in 0°and the lowest is 2.97 MPa in 135°.The proportion of liquid phase in 0°is22.90%,and the fuel loss is 11.8% and 9% higher than that in 135°and cylindrical charge,respectively.The stable propagation distance of blast wave in 135°is 42.50% longer than 0°and 28.37% longer than cylindrical charge.
基金This work was supported by National Key R&D Program of China(2021YFF0500503)National Natural Science Foundation of China(21925202,U22B2071)International Joint Mission on Climate Change and Carbon Neutrality.
文摘Lithium–oxygen battery with ultrahigh theoretical energy density is considered a highly competitive next-generation energy storage device,but its practical application is severely hindered by issues such as difficult decomposition of discharge products at present.Here,we have developed N-doped carbon anchored atomically dispersed Ru sites cathode catalyst with open hollow structure(h-RuNC)for Lithium–oxygen battery.On one hand,the abundance of atomically dispersed Ru sites can effectively catalyze the formation and decomposition of discharge products,thereby greatly enhancing the redox kinetics.On the other hand,the open hollow structure not only enhances the mass activity of atomically dispersed Ru sites but also improves the diffusion efficiency of catalytic molecules.Therefore,the excellent activity from atomically dispersed Ru sites and the enhanced diffusion from open hollow structure respectively improve the redox kinetics and cycling stability,ultimately achieving a high-performance lithium–oxygen battery.
基金Natural Science Foundation of Hubei Province of China for Distinguished Young Scholars (2023AFA099)Natural Science Foundation of Hubei Province of China for Key Projects (Innovation Group) (2023AFA030)National Natural Science Foundation of China (52178471)。
文摘A trigger system is typically employed in active seismic testing to trigger and synchronize multichannel surface wave data acquisition.The effect of the trigger system on the dispersion image of surface waves is empirically known to be negligible,however,theoretical explanation regarding the effect of the trigger system is insufficient.This study systematically examines the theory for surface wave dispersion analysis and proves that the effect of the trigger system on a dispersion image is negligible via a solid theoretical explanation.Subsequently,based on the new theoretical explanation,an alternative method that uses only the relative phase difference between sensors to extract dispersion characteristics with better conceptual clarity is proposed.Two active surface wave testing cases are considered to validate the theory and method.The results indicate that(1)an accurate trigger system is not necessary for surface wave data acquisition,and(2)it is unnecessary to assume that the impact point is the generation point of the surface waves for the experimental dispersion analysis.
文摘Biological invasion is triggered by human development activities such as the construction and expansion of road networks.Road verges serve as important habitats and corridors for the distribution of invasive alien plant species(IAPS)between geographically distant habitats.However,the trajectory of plant invasion and the data regarding the impact of roads on IAPS distribution are relatively poor in Nepal.Here,we surveyed two road types(main roads and feeder road)in the Middle Mountain region of central Nepal in order to investigate how different road types are driving the dispersal of IAPS along road verges and the adjacent natural habitats.Systematic sampling was conducted at ca 2.5 km intervals along the roads.At each sampling site,paired plots(25 m×4 m)were sampled:one adjacent to and along the road,and another 20 m away and parallel to it in the interior habitat.Our results revealed that the main road verges had a higher cover(33%)and a larger number of IAPS(14 species)than the feeder road(25%;10 species).The IAPS cover and richness were significantly higher along verges than in the adjacent interior habitats for both road types,indicating that roads are contributing as corridors for the dispersal of IAPS in the Middle Mountain areas of central Nepal.Further,elevation,tree canopy,and disturbances(grazing/mowing/trampling)were found to be the key factors that determine spatial distribution of IAPS along road verges.We emphasize that regular monitoring of vegetation along the road verges can help with the early detection and control of potential IAPS in the region before they become problematic.
基金supported by the Key R&D Program of Ningxia Hui Autonomous Region,China(2021BEG03008)the Natural Science Foundation of Ningxia Hui Autonomous Region,China(2021AAC03083).
文摘The maintenance of sand-fixing vegetation is important for the stability of artificial sand-fixing systems in which seed dispersal plays a key role.Based on field wind tunnel experiments using 11 common plant species on the southeastern edge of the Tengger Desert,China,we studied the secondary seed dispersal in the fixed and semi-fixed sand dunes as well as in the mobile dunes in order to understand the limitations of vegetation regeneration and the maintenance of its stability.Our results indicated that there were significant variations among the selected 11 plant species in the threshold of wind speed(TWS).The TWS of Caragana korshinskii was the highest among the 11 plant species,whereas that of Echinops gmelinii was the lowest.Seed morphological traits and underlying surface could generally explain the TWS.During the secondary seed dispersal processes,the proportions of seeds that did not disperse(no dispersal)and only dispersed over short distance(short-distance dispersal within the wind tunnel test section)were significantly higher than those of seeds that were buried(including lost seeds)and dispersed over long distance(long-distance dispersal beyond the wind tunnel test section).Compared with other habitats,the mobile dunes were the most difficult places for secondary seed dispersal.Buried seeds were the easiest to be found in the semi-fixed sand dunes,whereas fixed sand dunes were the best sites for seeds that dispersed over long distance.The results of linear mixed models showed that after controlling the dispersal distance,smaller and rounder seeds dispersed farther.Shape index and wind speed were the two significant influencing factors on the burial of seeds.The explanatory power of wind speed,underlying surface,and seed morphological traits on the seeds that did not disperse and dispersed over short distance was far greater than that on the seeds that were buried and dispersed over long distance,implying that the processes and mechanisms of burial and long-distance dispersal are more complex.In summary,most seeds in the study area either did not move,were buried,or dispersed over short distance,promoting local vegetation regeneration.
基金supported by the National Natural Science Foundation of China(22234005,21974070)the Natural Science Foundation of Jiangsu Province(BK20222015)。
文摘Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic functionality.Furthermore,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains elusive.Here,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom sites.Then the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed catalysts.Finally,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered.
文摘In this paper,layered periodic foundations(LPFs)are numerically examined for their responses to longitudinal and transverse modes in the time and frequency domains.Three different unit-cells,i.e.,2-layer,4-layer,and 6-layer unit-cells,comprising concrete/rubber,concrete/rubber/steel/rubber,and concrete/rubber/steel/rubber/lead/rubber materials,respectively,are taken into account.Also,the viscoelasticity behavior of the rubber is modeled with two factors,i.e.,a frequency-independent(FI)loss factor and a linear frequency-dependent(FD)loss factor.Following the extraction of the complex dispersion curves and the identification of the band gaps(BGs),the simulations of wave transmission in the time and frequency domains are performed using the COMSOL software.Subsequent parametric studies evaluate the effects of the rubber viscoelasticity models on the dispersion curves and the wave transmission for the longitudinal and transverse modes.The results show that considering the rubber viscoelasticity enhances the wave attenuation performance.Moreover,the transverse-mode damping is more sensitive to the viscoelasticity model than its longitudinal counterpart.The 6-layer unit-cell LPF exhibits the lowest BG,ranging from 4.8 Hz to 6.5 Hz.
基金financially supported by the National Natural Science Foundation of China(52102223,51920105004)。
文摘Antimony(Sb)-ba sed anode materials are feasible candidates for sodium-ion batteries(SIBs) due to their high theoretical specific capacity and excellent electrical conductivity.However,they still suffer from volume distortion,structural collapse,and ionic conduction interruption upon cycling.Herein,a hierarchical array-like nanofiber structure was designed to address these limitations by combining architecture engineering and anion tuning strategy,in which SbPO_(4-x) with oxygen vacancy nanosheet arrays are anchored on the surface of interwoven carbon nanofibers(SbPO_(4-x)@CNFs).In particular,bulky PO_(4)^(3-) anions mitigate the large volume distortion and generate Na_(3)PO_(4) with high ionic conductivity,collectively improving cyclic stability and ionic transport efficiency.The abundant oxygen vacancies substantially boost the intrinsic electronic conductivity of SbPO_4,further accelerating the reaction dynamics.In addition,hierarchical fibrous structures provide abundant active sites,construct efficient conducting networks,and enhance the electron/ion transport capacity.Benefiting from the advanced structural design,the SbPO_(4-x)@CNFs electrodes exhibit outstanding cycling stability(1000 cycles at 1.0 A g^(-1) with capacity decay of 0.05% per cycle) and rapid sodium storage performance(293.8 mA h g^(-1) at 5.0 A g^(-1)).Importantly,systematic in-/ex-situ techniques have revealed the "multi-step conversion-alloying" reaction process and the "battery-capacitor dual-mode" sodium-storage mechanism.This work provides valuable insights into the design of anode materials for advanced SIBs with elevated stability and superior rate performance.
基金the financial support from the Natural Science Foundation of China(Grant No.52172106)Anhui Provincial Natural Science Foundation(Grant Nos.2108085QB60 and 2108085QB61)China Postdoctoral Science Foundation(Grant Nos.2020M682057 and 2023T160651).
文摘Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites with atomically dispersed oxygen(O)coordination on bacterial cellulose-converted graphitic carbon(Mn-O-C).Evidence of the atomically dispersed Mn-(O-C_(2))_(4)moieties embedding in the exposed basal plane of carbon surface is confirmed by X-ray absorption spectroscopy.As a result,the as-synthesized Mn-O-C catalyst exhibits superior NitRR activity with an NH_(3)yield rate(RNH_(3))of 1476.9±62.6μg h^(−1)cm^(−2)at−0.7 V(vs.reversible hydrogen electrode,RHE)and a faradaic efficiency(FE)of 89.0±3.8%at−0.5 V(vs.RHE)under ambient conditions.Further,when evaluated with a practical flow cell,Mn-O-C shows a high RNH_(3)of 3706.7±552.0μg h^(−1)cm^(−2)at a current density of 100 mA cm−2,2.5 times of that in the H cell.The in situ FT-IR and Raman spectroscopic studies combined with theoretical calculations indicate that the Mn-(O-C_(2))_(4)sites not only effectively inhibit the competitive hydrogen evolution reaction,but also greatly promote the adsorption and activation of nitrate(NO_(3)^(−)),thus boosting both the FE and selectivity of NH_(3)over Mn-(O-C_(2))_(4)sites.
基金supported by the Fundamental Research Funds for the Central Universities(No.20CX05005A)the Major Scientific and Technological Projects of CNPC(No.ZD2019-184-001)+2 种基金the PetroChina Innovation Foundation(No.2018D-5007-0214)the Shandong Provincial Natural Science Foundation(No.ZR2019MEE095)the National Natural Science Foundation of China(No.42174141).
文摘Clays have considerable influence on the electrical properties of hydrate-bearing sediments.It is desirable to understand the electrical properties of hydrate-bearing clayey sediments and to build hydrate saturation(S_(h))models for reservoir evaluation and monitoring.The electrical properties of tetrahydrofuran-hydrate-bearing sediments with montmorillonite are characterized by complex conductivity at frequencies from 0.01 Hz to 1 kHz.The effects of clay and Sh on the complex conductivity were analyzed.A decrease and increase in electrical conductance result from the clay-swelling-induced blockage and ion migration in the electrical double layer(EDL),respectively.The quadrature conductivity increases with the clay content up to 10%because of the increased surface site density of counterions in EDL.Both the in-phase conductivity and quadrature conductivity decrease consistently with increasing Sh from 0.50 to 0.90.Three sets of models for Sh evaluation were developed.The model based on the Simandoux equation outperforms Archie’s formula,with a root-mean-square error(E_(RMS))of 1.8%and 3.9%,respectively,highlighting the clay effects on the in-phase conductivity.The fre-quency effect correlations based on in-phase and quadrature conductivities exhibit inferior performance(E_(RMS)=11.6%and 13.2%,re-spectively)due to the challenge of choosing an appropriate pair of frequencies and intrinsic uncertainties from two measurements.The second-order Cole-Cole formula can be used to fit the complex-conductivity spectra.One pair of inverted Cole-Cole parameters,i.e.,characteristic time and chargeability,is employed to predict S_(h) with an E_(RMS) of 5.05%and 9.05%,respectively.
基金the National Natural Science Foundation of China(22279044,12034002,and 22202080)the Project for Self-Innovation Capability Construction of Jilin Province Development and Reform Commission(2021C026)+1 种基金Jilin Province Science and Technology Development Program(20210301009GX)the Fundamental Research Funds for the Central Universities.
文摘Electrochemical carbon dioxide reduction reaction(CO_(2)RR)involves a variety of intermediates with highly correlated reaction and ad-desorption energies,hindering optimization of the catalytic activity.For example,increasing the binding of the*COOH to the active site will generally increase the*CO desorption energy.Breaking this relationship may be expected to dramatically improve the intrinsic activity of CO_(2)RR,but remains an unsolved challenge.Herein,we addressed this conundrum by constructing a unique atomic dispersed hetero-pair consisting of Mo-Fe di-atoms anchored on N-doped carbon carrier.This system shows an unprecedented CO_(2)RR intrinsic activity with TOF of 3336 h−1,high selectivity toward CO production,Faradaic efficiency of 95.96%at−0.60 V and excellent stability.Theoretical calculations show that the Mo-Fe diatomic sites increased the*COOH intermediate adsorption energy by bridging adsorption of*COOH intermediates.At the same time,d-d orbital coupling in the Mo-Fe di-atom results in electron delocalization and facilitates desorption of*CO intermediates.Thus,the undesirable correlation between these steps is broken.This work provides a promising approach,specifically the use of di-atoms,for breaking unfavorable relationships based on understanding of the catalytic mechanisms at the atomic scale.