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
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
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
With the rapid development of urban rail transit,the existing track detection has some problems such as low efficiency and insufficient detection coverage,so an intelligent and automatic track detectionmethod based on...With the rapid development of urban rail transit,the existing track detection has some problems such as low efficiency and insufficient detection coverage,so an intelligent and automatic track detectionmethod based onUAV is urgently needed to avoid major safety accidents.At the same time,the geographical distribution of IoT devices results in the inefficient use of the significant computing potential held by a large number of devices.As a result,the Dispersed Computing(DCOMP)architecture enables collaborative computing between devices in the Internet of Everything(IoE),promotes low-latency and efficient cross-wide applications,and meets users’growing needs for computing performance and service quality.This paper focuses on examining the resource allocation challenge within a dispersed computing environment that utilizes UAV inspection tracks.Furthermore,the system takes into account both resource constraints and computational constraints and transforms the optimization problem into an energy minimization problem with computational constraints.The Markov Decision Process(MDP)model is employed to capture the connection between the dispersed computing resource allocation strategy and the system environment.Subsequently,a method based on Double Deep Q-Network(DDQN)is introduced to derive the optimal policy.Simultaneously,an experience replay mechanism is implemented to tackle the issue of increasing dimensionality.The experimental simulations validate the efficacy of the method across various scenarios.展开更多
The real structure and in situ evolution of catalysts under working conditions are of paramount importance,especially for bifunctional electrocatalysis.Here,we report asymmetric structural evolution and dynamic hydrog...The real structure and in situ evolution of catalysts under working conditions are of paramount importance,especially for bifunctional electrocatalysis.Here,we report asymmetric structural evolution and dynamic hydrogen-bonding promotion mechanism of an atomically dispersed electrocatalyst.Pyrolysis of Co/Ni-doped MAF-4/ZIF-8 yielded nitrogen-doped porous carbons functionalized by atomically dispersed Co–Ni dual-metal sites with an unprecedented N8V4 structure,which can serve as an efficient bifunctional electrocatalyst for overall water splitting.More importantly,the electrocatalyst showed remarkable activation behavior due to the in situ oxidation of the carbon substrate to form C–OH groups.Density functional theory calculations suggested that the flexible C–OH groups can form reversible hydrogen bonds with the oxygen evolution reaction intermediates,giving a bridge between elementary reactions to break the conventional scaling relationship.展开更多
A series of CeO_(2)-TiO_(2)mixed oxides supports with various Ce/Ti molar ratio were synthesized by modified coprecipitation method. The corresponding Pt loaded(0.5 wt% Pt) catalysts were prepared by electronless depo...A series of CeO_(2)-TiO_(2)mixed oxides supports with various Ce/Ti molar ratio were synthesized by modified coprecipitation method. The corresponding Pt loaded(0.5 wt% Pt) catalysts were prepared by electronless deposition method and evaluated for the deep oxidation of n-hexane as a model VOCs. The results show that the CeO_(2)and TiOxnanoparticles can highly disperse into each other and form Ce_(2)Ti_(2)O_(7)solid solution with appropriate Ce/Ti molar ratio, which significantly improves their redox ability by enhancing the interaction between CeO_(2)and TiO_(x). The dispersibility of Pt species can also be adjusted by altering the Ce/Ti molar ratio, and Pt/CeTi-2/1 catalyst with Ce/Ti molar ratio of 2:1 exhibits the best Pt dispersibility that Pt species mainly exist as Pt single atoms. The high dispersion of Pt species in the Pt/CeO_(2)-TiO_(2)catalysts would promote the catalytic activity of VOCs oxidation with low T90% values(1000 ppm, GHSV = 15,000 h^(-1)), such as for n-hexane degradation with T90% of 139℃. The characterizations reveal that the superior activity is mainly related to possessing the more Pt2+species,adsorbed oxygen species and higher low-temperature reducibility owing to the strong interaction between highly dispersed Pt species and CeO_(2)-TiO_(2)as well as the promoted migration of lattice oxygen by the formation of more Ce_(2)Ti_(2)O_(7)species. Furthermore, the Pt/CeTi-2/1 catalyst also exhibits excellent stability for chlorinated and other non-chlorinated VOCs oxidation, making it very promising for real application under various operating conditions.展开更多
Drilling and blasting methods have been used as a common driving technique for shallow-hole driving and blasting in rock roadways.With the advent of digital electronic detonators and the need for increased production ...Drilling and blasting methods have been used as a common driving technique for shallow-hole driving and blasting in rock roadways.With the advent of digital electronic detonators and the need for increased production efciency,the traditional blasting design is no longer suitable for deep hole blasting.In this paper,a disperse charge cut blasting method was proposed to address the issues of low excavation depth and high block rate in deep hole undercut blasting.First,a blasting model was used to illustrate the mechanism of the deep hole dispersive charge cut blasting process.Then,continuous charge and dispersed charge blasting models were developed using the smooth particle hydrodynamics-fnite element method(SPHFEM).The cutting parameters were determined theoretically,and the cutting efciency was introduced to evaluate the cutting efect.The blasting efects of the two charging models were analyzed utilizing the evolution law of rock damage,the number of rock particles thrown,and the cutting efciency.The results show that using a dispersed charge improves the cutting efciency by about 20%and the rock breakage for the deep hole cut blasting compared to the traditional continuous charge.In addition,important parameters such as cutting hole spacing,cutting hole depth and upper charge proportion also have a signifcant impact on the cutting efect.Finally,the deep hole dispersed charge cut blasting technology is combined with the digital electronic detonator through the feld engineering practice.It provides a reference for the subsequent deep hole cutting blasting and the use of electronic detonators in rock roadways.展开更多
Dispersed computing is a new resourcecentric computing paradigm.Due to its high degree of openness and decentralization,it is vulnerable to attacks,and security issues have become an important challenge hindering its ...Dispersed computing is a new resourcecentric computing paradigm.Due to its high degree of openness and decentralization,it is vulnerable to attacks,and security issues have become an important challenge hindering its development.The trust evaluation technology is of great significance to the reliable operation and security assurance of dispersed computing networks.In this paper,a dynamic Bayesian-based comprehensive trust evaluation model is proposed for dispersed computing environment.Specifically,in the calculation of direct trust,a logarithmic decay function and a sliding window are introduced to improve the timeliness.In the calculation of indirect trust,a random screening method based on sine function is designed,which excludes malicious nodes providing false reports and multiple malicious nodes colluding attacks.Finally,the comprehensive trust value is dynamically updated based on historical interactions,current interactions and momentary changes.Simulation experiments are introduced to verify the performance of the model.Compared with existing model,the proposed trust evaluation model performs better in terms of the detection rate of malicious nodes,the interaction success rate,and the computational cost.展开更多
Graphene as a lubricating additive holds great potential for industrial lubrication. However, its poor dispersity and compatibility with base oils and grease hinder maximizing performance. Here, the infuence of graphe...Graphene as a lubricating additive holds great potential for industrial lubrication. However, its poor dispersity and compatibility with base oils and grease hinder maximizing performance. Here, the infuence of graphene dispersion on the thickening efect and lubrication function is considered. A well-dispersed lubricant additive was obtained via trihexyl tetradecyl phosphonium bis(2-ethylhexyl) phosphate modifed graphene ([P_(66614)][DEHP]-G). Then lithium complex grease was prepared by saponifcation with 12-OH stearic acid, sebacic acid, and lithium hydroxide, using polyalphaolefn (PAO20) as base oil and the modifed-graphene as lubricating additive, with the original graphene as a comparison. The physicochemical properties and lubrication performance of the as-prepared greases were evaluated in detail. The results show that the as-prepared greases have high dropping point and colloidal stability. Furthermore, modifed-graphene lithium complex grease ofered the best friction reduction and anti-wear abilities, manifesting the reduction of friction coefcient and wear volume up to 18.84% and 67.34%, respectively. With base oil overfow and afux, well-dispersed [P_(66614)][DEHP]-G was readily adsorbed to the worn surfaces, resulting in the formation of a continuous and dense graphene deposition flm. The synergy of deposited graphene-flm, spilled oil, and adhesive grease greatly improves the lubrication function of grease. This research paves the way for modulating high-performance lithium complex grease to reduce the friction and wear of movable machinery.展开更多
Degradable industrial packaging foam trays made from cellulose fibers were fabricated using a hot-press baking process.Bleached softwood pulp fibers with a concentration of 30%were dispersed at a high speed under the ...Degradable industrial packaging foam trays made from cellulose fibers were fabricated using a hot-press baking process.Bleached softwood pulp fibers with a concentration of 30%were dispersed at a high speed under the action of a dispersant.The effects of the dispersant dosage of the fibers on the porosity,foam density,and static compression characteristics were discussed.Furthermore,the effects of the reinforcing adhesive including polyvinyl alcohol(PVA),and cassava starch on the physical and mechanical properties of the foam trays were studied,as well as the relationship between these properties and the microstructure of the foam trays.The dispersant enhanced the rheological and blistering properties of the fiber dispersion.As the dispersant dosage increased from 2%to 4%,the foam density gradually increased and the compressive strain performance and residual compressive strain of the foam trays decreased.Under the condition of constant dosage of dispersant,increasing the fiber proportion from 67%to 77%improved the porosity and foam density and slightly reduced the static compression performance.In additioton,the static compression resistance of the foamed materials was improved by increasing the PVA dosage since PVA was beneficial for improving the strength of the foam trays.展开更多
The solubility of disperse dyes and their mixture in supercritical carbon dioxide is an important property in study and development of supercritical fluid dyeing technology.In this study,solubilities of C.I.Disperse R...The solubility of disperse dyes and their mixture in supercritical carbon dioxide is an important property in study and development of supercritical fluid dyeing technology.In this study,solubilities of C.I.Disperse Red 73,C.I.Disperse Blue 183 and their mixture in supercritical CO2 are measured at temperatures from 343.2 to 383.2 K and pressures from 12 to 28 MPa with a static recirculation method.Under the experimental conditions for the binary(C.I.Disperse Red 73+CO2 or C.I.Disperse Blue 183+CO2) and ternary(C.I.Disperse Red 73+C.I.Disperse Blue 183+CO2) systems,the solubilities increase with pressure.The solubility of C.I.Disperse Blue 183 decreases with the increase of temperature when the pressure is lower than 16 MPa,and the trend is opposite when the pressure is higher than 16 MPa.However,there is no crossover pressure for C.I.Disperse Red 73.The solubilities are also affected by molecular polarity of dyes.The co-solvent effect exhibited in the dissolving process of mixed dyes promotes their dissolution in supercritical CO2.The experimental data of solubilities of C.I.Disperse Red 73,C.I.Disperse Blue 183,and their mixture are correlated with the Chrastil model and Mendez-Santiago/Teja model. The former is more accurate.展开更多
Based on previous laser-induced fluorescence excitation spectroscopy work, the vibrational constants of neutral FeS in the X5 △ electronic state were obtained by directly mapping the ground-state vibrational levels u...Based on previous laser-induced fluorescence excitation spectroscopy work, the vibrational constants of neutral FeS in the X5 △ electronic state were obtained by directly mapping the ground-state vibrational levels up to v＂=3 using conventional laser-induced dispersed fluorescence spectroscopy. The vibrational frequency of FeS（X5 △） （518±5 cm-1） agrees well with that reported in a recent PES measurement （520±30 cm-1） [J. Phys. Chem. A 107, 2821 （2003）] which is the only one prior experimental vibrational frequency value for the 5 △ state of FeS. Careful comparisons of our experimental results and those documented in the literature （mainly from theoretical predictions） suggest that the ground state of FeS is 5 △ state.展开更多
For a better understanding of the feasibility of supercritieal fluid dyeing （SFD） and more available information for the process development, the experiments of dyeing PET textile with C.I. disperse red 60 （anthraq...For a better understanding of the feasibility of supercritieal fluid dyeing （SFD） and more available information for the process development, the experiments of dyeing PET textile with C.I. disperse red 60 （anthraquinone type） and C. I. disperse orange 25 （azo type） in supercritieal CO2 were carried out with a high-pressure dyeing apparatus at temperatures from 80 to 130℃ and pressure up to 31 MPa. The effect of operating conditions on color yield （K/S） was investigated in SFD experiment, and the optimum operating conditions for the above two disperse dyes were obtained as follows： the temperature 120℃, the pressure 25 MPa and the dyeing time 100 min. As compared with SFD, the conventional water dyeing （CWD） was carried out with the same dyes and textile. The results show that the better fastness, levelness and apparent color can be achieved in SFD and the SFD process has many significant advantages over the CWD process.展开更多
以C.I.Reactive Red 241、C.I.Disperse Blue 56模拟染料废水为对象,研究了电解法处理该类染料废水的优化条件。考察了起始电压、电解时间、溶液初始p H对处理效果的影响。结果表明,在p H=7,U=14V、I=3.2A、t=30min的条件下,C.I.Reactiv...以C.I.Reactive Red 241、C.I.Disperse Blue 56模拟染料废水为对象,研究了电解法处理该类染料废水的优化条件。考察了起始电压、电解时间、溶液初始p H对处理效果的影响。结果表明,在p H=7,U=14V、I=3.2A、t=30min的条件下,C.I.Reactive Red241模拟染料废水的脱色率可达到86%以上;在p H=7,U=14V、I=3.2A、t=25min的条件下,C.I.Disperse Blue 56模拟染料废水的脱色率可达到79以上%。展开更多
Exploring non‐precious metal catalysts for the oxygen reduction reaction （ORR） is essential for fuel cells and metal–air batteries. Herein, we report a Fe‐N‐C catalyst possessing a high specific surface area （1...Exploring non‐precious metal catalysts for the oxygen reduction reaction （ORR） is essential for fuel cells and metal–air batteries. Herein, we report a Fe‐N‐C catalyst possessing a high specific surface area （1501 m2/g） and uniformly dispersed iron within a carbon matrix prepared via a two‐step pyrolysis process. The Fe‐N‐C catalyst exhibits excellent ORR activity in 0.1 mol/L NaOH electrolyte （onset potential, Eo=1.08 V and half wave potential, E1/2=0.88 V vs. reversible hydrogen electrode） and 0.1 mol/L HClO4 electrolyte （Eo=0.85 V and E1/2=0.75 V vs. reversible hydrogen electrode）. The direct methanol fuel cells employing Fe‐N‐C as the cathodic catalyst displayed promising per‐formance with a maximum power density of 33 mW/cm2 in alkaline media and 47 mW/cm2 in acidic media. The detailed investigation on the composition–structure–performance relationship by X‐ray diffraction, X‐ray photoelectron spectroscopy and Mo-ssbauer spectroscopy suggests that Fe‐N4, together with graphitic‐N and pyridinic‐N are the active ORR components. The promising direct methanol fuel cell performance displayed by the Fe‐N‐C catalyst is related to the intrinsic high catalytic activity, and critically for this application, to the high methanol tolerance.展开更多
The laser-induced fluorescence excitation spectra of jet-cooled NiB radicals have been recorded in the energy range of 19000-22100 cm-1. Eleven bands have been assigned to the [20.77]2П-X2∑＋ transition system for t...The laser-induced fluorescence excitation spectra of jet-cooled NiB radicals have been recorded in the energy range of 19000-22100 cm-1. Eleven bands have been assigned to the [20.77]2П-X2∑＋ transition system for the first time. The dispersed fluorescence spectra related to most of these bands have been investigated. Vibrationally excited levels of the ground electronic state, with v＂ up to 6, have been observed. In addition, the lifetimes for almost all the observed bands have also been measured.展开更多
以Disperse Red 3B染料废水为对象,研究了电催化-光化物化组合技术处理该类染料废水的优化条件。考察了电解温度、电解质NaCl浓度、流速、染液初始pH值对处理效果的影响,且后续加入紫外光汞灯探究物化组合技术对处理效果的影响。结果表...以Disperse Red 3B染料废水为对象,研究了电催化-光化物化组合技术处理该类染料废水的优化条件。考察了电解温度、电解质NaCl浓度、流速、染液初始pH值对处理效果的影响,且后续加入紫外光汞灯探究物化组合技术对处理效果的影响。结果表明,在T=30℃、C_(NaCl)=0.20g/L、V=65.46μl/min、pH=3的条件下,Disperse Red 3B染料废水的脱色率可达到88%以上,继续光照30mins后,COD去除率可以提升3%左右。展开更多
Some disperse dyes were microencapsulated by means of in- situ polymerization. These microencapsulated disperse dyes was extracted respectively by ethanol under certain conditions. The controlled-release properties of...Some disperse dyes were microencapsulated by means of in- situ polymerization. These microencapsulated disperse dyes was extracted respectively by ethanol under certain conditions. The controlled-release properties of disperse dyes through the shell of microcapsules were measured by spectrophotometer. According to the results, it was drawn that the type of disperse dyes, the auxiliaries contained in disperse dyes, the quantity of system controlling medium used and the core/shell ratio of microcapsules play important roles in controlling the release properties of microcapsules. The different controlled- release properties of microcapsules, which were prepared under given conditions, however, would in turn influence the performance of microcapsules in multiple-transfer printing.展开更多
The present study has been undertaken to evaluate the adsorption in batch mode of a disperse dye (Disperse Blue SBL) by poorly crystalline hydroxyapatite synthesized by coprecipitation between Ca(NO3)2and (NH4)2HPO4 r...The present study has been undertaken to evaluate the adsorption in batch mode of a disperse dye (Disperse Blue SBL) by poorly crystalline hydroxyapatite synthesized by coprecipitation between Ca(NO3)2and (NH4)2HPO4 reagents in aqueous solution at room temperature. The adsorption experiments were carried out to investigate the factors that influence the dye uptake by the adsorbent, such as the contact time under agitation, adsorbent dosage, initial dye concentration, solution temperature, and pH. The experimental results show that the percentage of dye removal increases with increasing the amount of adsorbent, until the total discoloration. The adsorption isotherms follow the model of Langmuir with a high adsorption capacity. The adsorption was pH and temperature dependent.展开更多
Mass transfer enhancement of gas absorption by adding a dispersed organic phase has been studied in this work. Various dispersed organic phases （heptanol, octanol, isoamyl alcohol, heptane, octane, and isooctane） we...Mass transfer enhancement of gas absorption by adding a dispersed organic phase has been studied in this work. Various dispersed organic phases （heptanol, octanol, isoamyl alcohol, heptane, octane, and isooctane） were tested respectively in the experiment. According to the theoretical model and experimental data, the overall volumetric mass transfer coefficient and enhancement factor were obtained under different dispersed organic phase volume fraction and stirring speed. The experimental results indicate that gas-liquid mass transfer is enhanced at different level by adding a dispersed organic phase. The best performance of enhancement were achieved with the dispersed organic phase volumetric fraction of 5% and under an intermediate stirring speed of 670 r·min^-1. Among the organic phases tested in the experiment, alcohols show better performance, which gave 20% higher enhance-ment of overall volumetric mass transfer coefficient than adding alkanes.展开更多
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.
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.
文摘With the rapid development of urban rail transit,the existing track detection has some problems such as low efficiency and insufficient detection coverage,so an intelligent and automatic track detectionmethod based onUAV is urgently needed to avoid major safety accidents.At the same time,the geographical distribution of IoT devices results in the inefficient use of the significant computing potential held by a large number of devices.As a result,the Dispersed Computing(DCOMP)architecture enables collaborative computing between devices in the Internet of Everything(IoE),promotes low-latency and efficient cross-wide applications,and meets users’growing needs for computing performance and service quality.This paper focuses on examining the resource allocation challenge within a dispersed computing environment that utilizes UAV inspection tracks.Furthermore,the system takes into account both resource constraints and computational constraints and transforms the optimization problem into an energy minimization problem with computational constraints.The Markov Decision Process(MDP)model is employed to capture the connection between the dispersed computing resource allocation strategy and the system environment.Subsequently,a method based on Double Deep Q-Network(DDQN)is introduced to derive the optimal policy.Simultaneously,an experience replay mechanism is implemented to tackle the issue of increasing dimensionality.The experimental simulations validate the efficacy of the method across various scenarios.
基金supported by the National Key Research and Development Program of China(2021YFA1500401)the National Natural Science Foundation of China(21890380,21975290,21901089,and 21821003)+1 种基金the Foundation of Basic and Applied Basic Research of Guangdong Province(2020B1515120024)C.-T.H.acknowledges the Jiangxi Province(20202ZDB01004 and jxsq2018106041).
文摘The real structure and in situ evolution of catalysts under working conditions are of paramount importance,especially for bifunctional electrocatalysis.Here,we report asymmetric structural evolution and dynamic hydrogen-bonding promotion mechanism of an atomically dispersed electrocatalyst.Pyrolysis of Co/Ni-doped MAF-4/ZIF-8 yielded nitrogen-doped porous carbons functionalized by atomically dispersed Co–Ni dual-metal sites with an unprecedented N8V4 structure,which can serve as an efficient bifunctional electrocatalyst for overall water splitting.More importantly,the electrocatalyst showed remarkable activation behavior due to the in situ oxidation of the carbon substrate to form C–OH groups.Density functional theory calculations suggested that the flexible C–OH groups can form reversible hydrogen bonds with the oxygen evolution reaction intermediates,giving a bridge between elementary reactions to break the conventional scaling relationship.
基金supported by a grant from the National Key Research and Development Program of China (2016YFC0204300)the National Nature Science Foundation of China (21477109)。
文摘A series of CeO_(2)-TiO_(2)mixed oxides supports with various Ce/Ti molar ratio were synthesized by modified coprecipitation method. The corresponding Pt loaded(0.5 wt% Pt) catalysts were prepared by electronless deposition method and evaluated for the deep oxidation of n-hexane as a model VOCs. The results show that the CeO_(2)and TiOxnanoparticles can highly disperse into each other and form Ce_(2)Ti_(2)O_(7)solid solution with appropriate Ce/Ti molar ratio, which significantly improves their redox ability by enhancing the interaction between CeO_(2)and TiO_(x). The dispersibility of Pt species can also be adjusted by altering the Ce/Ti molar ratio, and Pt/CeTi-2/1 catalyst with Ce/Ti molar ratio of 2:1 exhibits the best Pt dispersibility that Pt species mainly exist as Pt single atoms. The high dispersion of Pt species in the Pt/CeO_(2)-TiO_(2)catalysts would promote the catalytic activity of VOCs oxidation with low T90% values(1000 ppm, GHSV = 15,000 h^(-1)), such as for n-hexane degradation with T90% of 139℃. The characterizations reveal that the superior activity is mainly related to possessing the more Pt2+species,adsorbed oxygen species and higher low-temperature reducibility owing to the strong interaction between highly dispersed Pt species and CeO_(2)-TiO_(2)as well as the promoted migration of lattice oxygen by the formation of more Ce_(2)Ti_(2)O_(7)species. Furthermore, the Pt/CeTi-2/1 catalyst also exhibits excellent stability for chlorinated and other non-chlorinated VOCs oxidation, making it very promising for real application under various operating conditions.
基金the State Key Development Program for Basic Research of China(2016YFC0600903)the National Natural Science Foundation of China(51934001).
文摘Drilling and blasting methods have been used as a common driving technique for shallow-hole driving and blasting in rock roadways.With the advent of digital electronic detonators and the need for increased production efciency,the traditional blasting design is no longer suitable for deep hole blasting.In this paper,a disperse charge cut blasting method was proposed to address the issues of low excavation depth and high block rate in deep hole undercut blasting.First,a blasting model was used to illustrate the mechanism of the deep hole dispersive charge cut blasting process.Then,continuous charge and dispersed charge blasting models were developed using the smooth particle hydrodynamics-fnite element method(SPHFEM).The cutting parameters were determined theoretically,and the cutting efciency was introduced to evaluate the cutting efect.The blasting efects of the two charging models were analyzed utilizing the evolution law of rock damage,the number of rock particles thrown,and the cutting efciency.The results show that using a dispersed charge improves the cutting efciency by about 20%and the rock breakage for the deep hole cut blasting compared to the traditional continuous charge.In addition,important parameters such as cutting hole spacing,cutting hole depth and upper charge proportion also have a signifcant impact on the cutting efect.Finally,the deep hole dispersed charge cut blasting technology is combined with the digital electronic detonator through the feld engineering practice.It provides a reference for the subsequent deep hole cutting blasting and the use of electronic detonators in rock roadways.
基金supported in part by the National Science Foundation Project of P.R.China (No.61931001)the Fundamental Research Funds for the Central Universities under Grant (No.FRFAT-19-010)the Scientific and Technological Innovation Foundation of Foshan,USTB (No.BK20AF003)。
文摘Dispersed computing is a new resourcecentric computing paradigm.Due to its high degree of openness and decentralization,it is vulnerable to attacks,and security issues have become an important challenge hindering its development.The trust evaluation technology is of great significance to the reliable operation and security assurance of dispersed computing networks.In this paper,a dynamic Bayesian-based comprehensive trust evaluation model is proposed for dispersed computing environment.Specifically,in the calculation of direct trust,a logarithmic decay function and a sliding window are introduced to improve the timeliness.In the calculation of indirect trust,a random screening method based on sine function is designed,which excludes malicious nodes providing false reports and multiple malicious nodes colluding attacks.Finally,the comprehensive trust value is dynamically updated based on historical interactions,current interactions and momentary changes.Simulation experiments are introduced to verify the performance of the model.Compared with existing model,the proposed trust evaluation model performs better in terms of the detection rate of malicious nodes,the interaction success rate,and the computational cost.
基金Supported by National Natural Science Foundation of China(Grant Nos.52075458 and U2141211).
文摘Graphene as a lubricating additive holds great potential for industrial lubrication. However, its poor dispersity and compatibility with base oils and grease hinder maximizing performance. Here, the infuence of graphene dispersion on the thickening efect and lubrication function is considered. A well-dispersed lubricant additive was obtained via trihexyl tetradecyl phosphonium bis(2-ethylhexyl) phosphate modifed graphene ([P_(66614)][DEHP]-G). Then lithium complex grease was prepared by saponifcation with 12-OH stearic acid, sebacic acid, and lithium hydroxide, using polyalphaolefn (PAO20) as base oil and the modifed-graphene as lubricating additive, with the original graphene as a comparison. The physicochemical properties and lubrication performance of the as-prepared greases were evaluated in detail. The results show that the as-prepared greases have high dropping point and colloidal stability. Furthermore, modifed-graphene lithium complex grease ofered the best friction reduction and anti-wear abilities, manifesting the reduction of friction coefcient and wear volume up to 18.84% and 67.34%, respectively. With base oil overfow and afux, well-dispersed [P_(66614)][DEHP]-G was readily adsorbed to the worn surfaces, resulting in the formation of a continuous and dense graphene deposition flm. The synergy of deposited graphene-flm, spilled oil, and adhesive grease greatly improves the lubrication function of grease. This research paves the way for modulating high-performance lithium complex grease to reduce the friction and wear of movable machinery.
文摘Degradable industrial packaging foam trays made from cellulose fibers were fabricated using a hot-press baking process.Bleached softwood pulp fibers with a concentration of 30%were dispersed at a high speed under the action of a dispersant.The effects of the dispersant dosage of the fibers on the porosity,foam density,and static compression characteristics were discussed.Furthermore,the effects of the reinforcing adhesive including polyvinyl alcohol(PVA),and cassava starch on the physical and mechanical properties of the foam trays were studied,as well as the relationship between these properties and the microstructure of the foam trays.The dispersant enhanced the rheological and blistering properties of the fiber dispersion.As the dispersant dosage increased from 2%to 4%,the foam density gradually increased and the compressive strain performance and residual compressive strain of the foam trays decreased.Under the condition of constant dosage of dispersant,increasing the fiber proportion from 67%to 77%improved the porosity and foam density and slightly reduced the static compression performance.In additioton,the static compression resistance of the foamed materials was improved by increasing the PVA dosage since PVA was beneficial for improving the strength of the foam trays.
基金Supported by the Natural Science Foundation of Zhejiang Province（M203035）
文摘The solubility of disperse dyes and their mixture in supercritical carbon dioxide is an important property in study and development of supercritical fluid dyeing technology.In this study,solubilities of C.I.Disperse Red 73,C.I.Disperse Blue 183 and their mixture in supercritical CO2 are measured at temperatures from 343.2 to 383.2 K and pressures from 12 to 28 MPa with a static recirculation method.Under the experimental conditions for the binary(C.I.Disperse Red 73+CO2 or C.I.Disperse Blue 183+CO2) and ternary(C.I.Disperse Red 73+C.I.Disperse Blue 183+CO2) systems,the solubilities increase with pressure.The solubility of C.I.Disperse Blue 183 decreases with the increase of temperature when the pressure is lower than 16 MPa,and the trend is opposite when the pressure is higher than 16 MPa.However,there is no crossover pressure for C.I.Disperse Red 73.The solubilities are also affected by molecular polarity of dyes.The co-solvent effect exhibited in the dissolving process of mixed dyes promotes their dissolution in supercritical CO2.The experimental data of solubilities of C.I.Disperse Red 73,C.I.Disperse Blue 183,and their mixture are correlated with the Chrastil model and Mendez-Santiago/Teja model. The former is more accurate.
基金Acknowledgment： This work was supported by the National Natural Science Foundation of China （No.20673107 and No.20873133）, the National Basic Research Program of China （No.2007CB815203 and No.2010CB923302）, the Chinese Academy of Sciences （No.KJCX2-YW-N24）, and the Scientific Research Foundation for the Returned Overseas Chinese Scholars, Ministry of Education of China.
文摘Based on previous laser-induced fluorescence excitation spectroscopy work, the vibrational constants of neutral FeS in the X5 △ electronic state were obtained by directly mapping the ground-state vibrational levels up to v＂=3 using conventional laser-induced dispersed fluorescence spectroscopy. The vibrational frequency of FeS（X5 △） （518±5 cm-1） agrees well with that reported in a recent PES measurement （520±30 cm-1） [J. Phys. Chem. A 107, 2821 （2003）] which is the only one prior experimental vibrational frequency value for the 5 △ state of FeS. Careful comparisons of our experimental results and those documented in the literature （mainly from theoretical predictions） suggest that the ground state of FeS is 5 △ state.
基金Supported by National Natural Science Foundation of China(No.20277004)
文摘For a better understanding of the feasibility of supercritieal fluid dyeing （SFD） and more available information for the process development, the experiments of dyeing PET textile with C.I. disperse red 60 （anthraquinone type） and C. I. disperse orange 25 （azo type） in supercritieal CO2 were carried out with a high-pressure dyeing apparatus at temperatures from 80 to 130℃ and pressure up to 31 MPa. The effect of operating conditions on color yield （K/S） was investigated in SFD experiment, and the optimum operating conditions for the above two disperse dyes were obtained as follows： the temperature 120℃, the pressure 25 MPa and the dyeing time 100 min. As compared with SFD, the conventional water dyeing （CWD） was carried out with the same dyes and textile. The results show that the better fastness, levelness and apparent color can be achieved in SFD and the SFD process has many significant advantages over the CWD process.
文摘以C.I.Reactive Red 241、C.I.Disperse Blue 56模拟染料废水为对象,研究了电解法处理该类染料废水的优化条件。考察了起始电压、电解时间、溶液初始p H对处理效果的影响。结果表明,在p H=7,U=14V、I=3.2A、t=30min的条件下,C.I.Reactive Red241模拟染料废水的脱色率可达到86%以上;在p H=7,U=14V、I=3.2A、t=25min的条件下,C.I.Disperse Blue 56模拟染料废水的脱色率可达到79以上%。
基金supported by the“Strategic Priority Research Program”of the Chinese Academy of Sciences(XDA09030104)the National Basic Research Program of China(973 Program,2012CB215500)+1 种基金the National Natural Science Foundation of China(2157625850823008)~~
文摘Exploring non‐precious metal catalysts for the oxygen reduction reaction （ORR） is essential for fuel cells and metal–air batteries. Herein, we report a Fe‐N‐C catalyst possessing a high specific surface area （1501 m2/g） and uniformly dispersed iron within a carbon matrix prepared via a two‐step pyrolysis process. The Fe‐N‐C catalyst exhibits excellent ORR activity in 0.1 mol/L NaOH electrolyte （onset potential, Eo=1.08 V and half wave potential, E1/2=0.88 V vs. reversible hydrogen electrode） and 0.1 mol/L HClO4 electrolyte （Eo=0.85 V and E1/2=0.75 V vs. reversible hydrogen electrode）. The direct methanol fuel cells employing Fe‐N‐C as the cathodic catalyst displayed promising per‐formance with a maximum power density of 33 mW/cm2 in alkaline media and 47 mW/cm2 in acidic media. The detailed investigation on the composition–structure–performance relationship by X‐ray diffraction, X‐ray photoelectron spectroscopy and Mo-ssbauer spectroscopy suggests that Fe‐N4, together with graphitic‐N and pyridinic‐N are the active ORR components. The promising direct methanol fuel cell performance displayed by the Fe‐N‐C catalyst is related to the intrinsic high catalytic activity, and critically for this application, to the high methanol tolerance.
文摘The laser-induced fluorescence excitation spectra of jet-cooled NiB radicals have been recorded in the energy range of 19000-22100 cm-1. Eleven bands have been assigned to the [20.77]2П-X2∑＋ transition system for the first time. The dispersed fluorescence spectra related to most of these bands have been investigated. Vibrationally excited levels of the ground electronic state, with v＂ up to 6, have been observed. In addition, the lifetimes for almost all the observed bands have also been measured.
文摘以Disperse Red 3B染料废水为对象,研究了电催化-光化物化组合技术处理该类染料废水的优化条件。考察了电解温度、电解质NaCl浓度、流速、染液初始pH值对处理效果的影响,且后续加入紫外光汞灯探究物化组合技术对处理效果的影响。结果表明,在T=30℃、C_(NaCl)=0.20g/L、V=65.46μl/min、pH=3的条件下,Disperse Red 3B染料废水的脱色率可达到88%以上,继续光照30mins后,COD去除率可以提升3%左右。
文摘Some disperse dyes were microencapsulated by means of in- situ polymerization. These microencapsulated disperse dyes was extracted respectively by ethanol under certain conditions. The controlled-release properties of disperse dyes through the shell of microcapsules were measured by spectrophotometer. According to the results, it was drawn that the type of disperse dyes, the auxiliaries contained in disperse dyes, the quantity of system controlling medium used and the core/shell ratio of microcapsules play important roles in controlling the release properties of microcapsules. The different controlled- release properties of microcapsules, which were prepared under given conditions, however, would in turn influence the performance of microcapsules in multiple-transfer printing.
文摘The present study has been undertaken to evaluate the adsorption in batch mode of a disperse dye (Disperse Blue SBL) by poorly crystalline hydroxyapatite synthesized by coprecipitation between Ca(NO3)2and (NH4)2HPO4 reagents in aqueous solution at room temperature. The adsorption experiments were carried out to investigate the factors that influence the dye uptake by the adsorbent, such as the contact time under agitation, adsorbent dosage, initial dye concentration, solution temperature, and pH. The experimental results show that the percentage of dye removal increases with increasing the amount of adsorbent, until the total discoloration. The adsorption isotherms follow the model of Langmuir with a high adsorption capacity. The adsorption was pH and temperature dependent.
基金Supported by the National Natural Science Foundation of China （20776086）
文摘Mass transfer enhancement of gas absorption by adding a dispersed organic phase has been studied in this work. Various dispersed organic phases （heptanol, octanol, isoamyl alcohol, heptane, octane, and isooctane） were tested respectively in the experiment. According to the theoretical model and experimental data, the overall volumetric mass transfer coefficient and enhancement factor were obtained under different dispersed organic phase volume fraction and stirring speed. The experimental results indicate that gas-liquid mass transfer is enhanced at different level by adding a dispersed organic phase. The best performance of enhancement were achieved with the dispersed organic phase volumetric fraction of 5% and under an intermediate stirring speed of 670 r·min^-1. Among the organic phases tested in the experiment, alcohols show better performance, which gave 20% higher enhance-ment of overall volumetric mass transfer coefficient than adding alkanes.
