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
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
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
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
Although nanozymes have been widely developed,accurate design of highly active sites at the atomic level to mimic the electronic and geometrical structure of enzymes and the exploration of underlying mechanisms still ...Although nanozymes have been widely developed,accurate design of highly active sites at the atomic level to mimic the electronic and geometrical structure of enzymes and the exploration of underlying mechanisms still face significant challenges.Herein,two functional groups with opposite electron modulation abilities(nitro and amino)were introduced into the metal–organic frameworks(MIL-101(Fe))to tune the atomically dispersed metal sites and thus regulate the enzymelike activity.Notably,the functionalization of nitro can enhance the peroxidase(POD)-like activity of MIL-101(Fe),while the amino is poles apart.Theoretical calculations demonstrate that the introduction of nitro can not only regulate the geometry of adsorbed intermediates but also improve the electronic structure of metal active sites.Benefiting from both geometric and electronic effects,the nitro-functionalized MIL-101(Fe)with a low reaction energy barrier for the HO*formation exhibits a superior POD-like activity.As a concept of the application,a nitro-functionalized MIL-101(Fe)-based biosensor was elaborately applied for the sensitive detection of acetylcholinesterase activity in the range of 0.2–50 mU mL−1 with a limit of detection of 0.14 mU mL−1.Moreover,the detection of organophosphorus pesticides was also achieved.This work not only opens up new prospects for the rational design of highly active nanozymes at the atomic scale but also enhances the performance of nanozyme-based biosensors.展开更多
The corrosion resistance behavior of a highly dispersed MgO-MgAl2O4-ZrO2 composite refractory material is examined by testing with high-basicity and low-basicity RH(Ruhrstahl-Hereaeus)slags.The composite material exhi...The corrosion resistance behavior of a highly dispersed MgO-MgAl2O4-ZrO2 composite refractory material is examined by testing with high-basicity and low-basicity RH(Ruhrstahl-Hereaeus)slags.The composite material exhibits greater resistance to the RH slags than the traditional MgO-Cr2O3 composite,MgO-ZrO2 composite,and MgO-MgAl2O4-ZrO2 composite.On the basis of the microstructural analysis and mechanisms calculations,the corrosion resistance behavior of the MgO-MgAl2O4-ZrO2 composite is attributable to its highly dispersed structure,which helps protect the high activity of ZrO2.When in contact with the slag,ZrO2 reacts with CaO to form the stable phase CaZrO3,which protects MgAl2O4 against corrosion,thereby enhancing the corrosion resistance of the composite.展开更多
We have prepared novel coated particles, with a conductor graphite core and a dielectric TiO2 coating, as the dispersed phase of electrorheological fluids. One order of magnitude enhancement in the shear stress is obt...We have prepared novel coated particles, with a conductor graphite core and a dielectric TiO2 coating, as the dispersed phase of electrorheological fluids. One order of magnitude enhancement in the shear stress is obtained by using such composite particles, when it is compared with that of TiO2 particles. The experimental results show a way to get excellent ER system.展开更多
The deformation behavior of dispersion strengthened copper alloy Cu-Al2O3 was studied by TEM. The results show that nano-scaled dispersed second phase not only increases dislocation density in matrix, but also has an ...The deformation behavior of dispersion strengthened copper alloy Cu-Al2O3 was studied by TEM. The results show that nano-scaled dispersed second phase not only increases dislocation density in matrix, but also has an important influence on the dislocation substructure. The presence of fine dispersed Al2 O3 particles results in a uniform and random dislocation distribution in matrix copper and causes the difficulty in formation of dislocation cell structure and the decrease in the amount of cell structure during deformation. Deformation gives rise to much more dislocations and dislocation cells form more difficultly and the decrease in the cell size with the increase of dispersion degree.展开更多
Hydrodynamic characteristics of rotating perforated disk contactor(RPDC)were studied with emulsionwater system.The emulsion was dispcrsed in water and its holdup was measured.The effects of columndimensions and operat...Hydrodynamic characteristics of rotating perforated disk contactor(RPDC)were studied with emulsionwater system.The emulsion was dispcrsed in water and its holdup was measured.The effects of columndimensions and operating conditions on holdup and characteristic velocity were studied.By using the methodof dimensional analysis,the authors obtained two experimental correlations for estimating holdup and characteristic velocity respectively.Drop size distribution was studied photographically.The experimental results showedthat drop size distribuiion could be described by upper-limit log-normal distribution.展开更多
Replacement of precious single metal catalysts with cost-effective,highly-dispersed composite catalysts for catalytic hydrothermal conversion of residue holds tremendous promise for the residue upgrading technologies....Replacement of precious single metal catalysts with cost-effective,highly-dispersed composite catalysts for catalytic hydrothermal conversion of residue holds tremendous promise for the residue upgrading technologies.Organic metals were added to the feed as the oil-soluble precursors,and were transformed into the catalytic active phases in this work.Physical properties and structures of the composite catalysts had been investigated by X-ray fluorescence spectroscopy,X-ray photoelectron spectroscopy,X-ray diffraction,scanning electron microscopy and transmission electron microscopy.The composite catalysts were found to be highly efficient in the catalytic hydrothermal conversion of both the model compound and the residue.Increased metal dispersion and synergistic effects of two metals played indispensable roles in such catalytic system.Results showed that under the test conditions specified in the article,the catalyst had the best catalytic performance when the mass ratio of molybdenum to iron was 1.5.展开更多
Rechargeable zinc-air batteries(ZABs)are currently receiving extensive attention because of their extremely high theoretical specific energy density,low manufacturing costs,and environmental friendliness.Exploring bif...Rechargeable zinc-air batteries(ZABs)are currently receiving extensive attention because of their extremely high theoretical specific energy density,low manufacturing costs,and environmental friendliness.Exploring bifunctional catalysts with high activity and stability to overcome sluggish kinetics of oxygen reduction reaction and oxygen evolution reaction is critical for the development of rechargeable ZABs.Atomically dispersed metal-nitrogen-carbon(M-N-C)catalysts possessing prominent advantages of high metal atom utilization and electrocatalytic activity are promising candidates to promote oxygen electrocatalysis.In this work,general principles for designing atomically dispersed M-N-C are reviewed.Then,strategies aiming at enhancing the bifunctional catalytic activity and stability are presented.Finally,the challenges and perspectives of M-N-C bifunctional oxygen catalysts for ZABs are outlined.It is expected that this review will provide insights into the targeted optimization of atomically dispersed M-N-C catalysts in rechargeable ZABs.展开更多
The slurry-bed hydrocracking of Karamay VGO with water-soluble dispersed catalyst was studied and the catalyst after being separated from the reaction products was analyzed by using LRS, XRD and XPS to identify the cr...The slurry-bed hydrocracking of Karamay VGO with water-soluble dispersed catalyst was studied and the catalyst after being separated from the reaction products was analyzed by using LRS, XRD and XPS to identify the crystal structure of the catalyst. In this paper, the catalytic functions of molybdenum, nickel and iron were studied respectively during the slurry-phase hydrocracking while using diphenylmethane as the model compound and VGO from Karamay crude as the feedstock. The test results showed that, during the slurry-phase hydrocracking of heavy oil, the metal sulfides entered into chemical reactions with the free- radical intermediate H·formed on the catalyst surface. The free-radical intermediate H· formed on the catalyst surface could react with the free-radicals of big molecules and could suppress coke deposition.展开更多
Highly dispersed Cu-base catalyst has been prepared via thermal decomposition of layered double hydroxides precursors. The XRD pattern and the HRTEM images of the as prepared catalyst confirmed the high dispersion of ...Highly dispersed Cu-base catalyst has been prepared via thermal decomposition of layered double hydroxides precursors. The XRD pattern and the HRTEM images of the as prepared catalyst confirmed the high dispersion of Cu and Fe ions. Results show that the catalyst has a relatively high selectivity of alkanes at low temperature.展开更多
Considering high temperature and high salinity in the reservoirs, a dispersed particle gel soft heterogeneous compound(SHC) flooding system was prepared to improve the micro-profile control and displacement efficiency...Considering high temperature and high salinity in the reservoirs, a dispersed particle gel soft heterogeneous compound(SHC) flooding system was prepared to improve the micro-profile control and displacement efficiency. The characteristics and displacement mechanisms of the system were investigated via core flow tests and visual simulation experiments. The SHC flooding system composed of DPG particles and surfactants was suitable for the reservoirs with the temperature of 80-110 °C and the salinity of 1×10~4-10×10~4 mg/L. The system presented good characteristics: low viscosity, weak negatively charged, temperature and salinity resistance, particles aggregation capacity, wettability alteration on oil wet surface, wettability weaken on water wet surface, and interfacial tension(IFT) still less than 1×10^(-1) mN/m after aging at high temperature. The SHC flooding system achieved the micro-profile control by entering formations deeply and the better performance was found in the formation with the higher permeability difference existing between the layers, which suggested that the flooding system was superior to the surfactants, DPG particles, and polymer/surfactant compound flooding systems. The system could effectively enhance the micro-profile control in porous media through four behaviors, including direct plugging, bridging, adsorption, and retention. Moreover, the surfactant in the system magnified the deep migration capability and oil displacement capacity of the SHC flooding system, and the impact was strengthened through the mechanisms of improved displacement capacity, synergistic emulsification, enhanced wettability alteration ability and coalescence of oil belts. The synergistic effect of the two components of SHC flooding system improved oil displacement efficiency and subsequently enhanced oil recovery.展开更多
Ferro nematic suspensions are the prominent materials to enhance the electro optical performance of liquid crystal displays. Electro optical properties of polymer dispersed liquid crystal (PDLC) display with the intro...Ferro nematic suspensions are the prominent materials to enhance the electro optical performance of liquid crystal displays. Electro optical properties of polymer dispersed liquid crystal (PDLC) display with the introduction of Barium Titanate nanoparticles have been investigated in this article and it is shown that there is a considerable enhancement in electro-optical response of the displays. The nanoparticles lower the switch-on electric field and thereby increase the optical transmission at certain voltages of the displays. The electro-optical characteristics of the PDLC cells were investigated with a He-Ne laser followed by MatLab calculations.展开更多
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.
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The authors gratefully acknowledge the financial support of the Fundamental Research Funds for the Central Universities(CCNU20TS013)the National Natural Science Foundation of China(No.21503273)the Program of Introducing Talents of Discipline to Universities of China(111 program,B17019)and the Recruitment Program of Global Youth Experts of China.
文摘Although nanozymes have been widely developed,accurate design of highly active sites at the atomic level to mimic the electronic and geometrical structure of enzymes and the exploration of underlying mechanisms still face significant challenges.Herein,two functional groups with opposite electron modulation abilities(nitro and amino)were introduced into the metal–organic frameworks(MIL-101(Fe))to tune the atomically dispersed metal sites and thus regulate the enzymelike activity.Notably,the functionalization of nitro can enhance the peroxidase(POD)-like activity of MIL-101(Fe),while the amino is poles apart.Theoretical calculations demonstrate that the introduction of nitro can not only regulate the geometry of adsorbed intermediates but also improve the electronic structure of metal active sites.Benefiting from both geometric and electronic effects,the nitro-functionalized MIL-101(Fe)with a low reaction energy barrier for the HO*formation exhibits a superior POD-like activity.As a concept of the application,a nitro-functionalized MIL-101(Fe)-based biosensor was elaborately applied for the sensitive detection of acetylcholinesterase activity in the range of 0.2–50 mU mL−1 with a limit of detection of 0.14 mU mL−1.Moreover,the detection of organophosphorus pesticides was also achieved.This work not only opens up new prospects for the rational design of highly active nanozymes at the atomic scale but also enhances the performance of nanozyme-based biosensors.
基金financially supported by the National Natural Science Foundation of China (No.51872023)
文摘The corrosion resistance behavior of a highly dispersed MgO-MgAl2O4-ZrO2 composite refractory material is examined by testing with high-basicity and low-basicity RH(Ruhrstahl-Hereaeus)slags.The composite material exhibits greater resistance to the RH slags than the traditional MgO-Cr2O3 composite,MgO-ZrO2 composite,and MgO-MgAl2O4-ZrO2 composite.On the basis of the microstructural analysis and mechanisms calculations,the corrosion resistance behavior of the MgO-MgAl2O4-ZrO2 composite is attributable to its highly dispersed structure,which helps protect the high activity of ZrO2.When in contact with the slag,ZrO2 reacts with CaO to form the stable phase CaZrO3,which protects MgAl2O4 against corrosion,thereby enhancing the corrosion resistance of the composite.
基金the National Natural Science Foundation of China! (No.19834020).
文摘We have prepared novel coated particles, with a conductor graphite core and a dielectric TiO2 coating, as the dispersed phase of electrorheological fluids. One order of magnitude enhancement in the shear stress is obtained by using such composite particles, when it is compared with that of TiO2 particles. The experimental results show a way to get excellent ER system.
文摘The deformation behavior of dispersion strengthened copper alloy Cu-Al2O3 was studied by TEM. The results show that nano-scaled dispersed second phase not only increases dislocation density in matrix, but also has an important influence on the dislocation substructure. The presence of fine dispersed Al2 O3 particles results in a uniform and random dislocation distribution in matrix copper and causes the difficulty in formation of dislocation cell structure and the decrease in the amount of cell structure during deformation. Deformation gives rise to much more dislocations and dislocation cells form more difficultly and the decrease in the cell size with the increase of dispersion degree.
文摘Hydrodynamic characteristics of rotating perforated disk contactor(RPDC)were studied with emulsionwater system.The emulsion was dispcrsed in water and its holdup was measured.The effects of columndimensions and operating conditions on holdup and characteristic velocity were studied.By using the methodof dimensional analysis,the authors obtained two experimental correlations for estimating holdup and characteristic velocity respectively.Drop size distribution was studied photographically.The experimental results showedthat drop size distribuiion could be described by upper-limit log-normal distribution.
基金This work is financially supported by the China Petroleum and Chemical Corporation(SINOPEC 120063-1).
文摘Replacement of precious single metal catalysts with cost-effective,highly-dispersed composite catalysts for catalytic hydrothermal conversion of residue holds tremendous promise for the residue upgrading technologies.Organic metals were added to the feed as the oil-soluble precursors,and were transformed into the catalytic active phases in this work.Physical properties and structures of the composite catalysts had been investigated by X-ray fluorescence spectroscopy,X-ray photoelectron spectroscopy,X-ray diffraction,scanning electron microscopy and transmission electron microscopy.The composite catalysts were found to be highly efficient in the catalytic hydrothermal conversion of both the model compound and the residue.Increased metal dispersion and synergistic effects of two metals played indispensable roles in such catalytic system.Results showed that under the test conditions specified in the article,the catalyst had the best catalytic performance when the mass ratio of molybdenum to iron was 1.5.
基金This work is supported by the Natural Sciences and Engineering Research Council of Canada(NSERC)Centre Québéco is sur les Materiaux Fonctionnels(CQMF),Fonds de Recherche du Québec-Nature et Technologies(FRQNT)+2 种基金Institut National de la Recherche Scientifique(INRS)This work is also supported by the National Natural Science Foundation of China(21972017)the“Scientific and Technical Innovation Action Plan”Hong Kong,Macao and Taiwan Science&Technology Cooperation Project of Shanghai Science and Technology Committee(19160760600).F.Dong gratefully acknowledges scholarships from the China Scholarship Council(CSC).
文摘Rechargeable zinc-air batteries(ZABs)are currently receiving extensive attention because of their extremely high theoretical specific energy density,low manufacturing costs,and environmental friendliness.Exploring bifunctional catalysts with high activity and stability to overcome sluggish kinetics of oxygen reduction reaction and oxygen evolution reaction is critical for the development of rechargeable ZABs.Atomically dispersed metal-nitrogen-carbon(M-N-C)catalysts possessing prominent advantages of high metal atom utilization and electrocatalytic activity are promising candidates to promote oxygen electrocatalysis.In this work,general principles for designing atomically dispersed M-N-C are reviewed.Then,strategies aiming at enhancing the bifunctional catalytic activity and stability are presented.Finally,the challenges and perspectives of M-N-C bifunctional oxygen catalysts for ZABs are outlined.It is expected that this review will provide insights into the targeted optimization of atomically dispersed M-N-C catalysts in rechargeable ZABs.
文摘The slurry-bed hydrocracking of Karamay VGO with water-soluble dispersed catalyst was studied and the catalyst after being separated from the reaction products was analyzed by using LRS, XRD and XPS to identify the crystal structure of the catalyst. In this paper, the catalytic functions of molybdenum, nickel and iron were studied respectively during the slurry-phase hydrocracking while using diphenylmethane as the model compound and VGO from Karamay crude as the feedstock. The test results showed that, during the slurry-phase hydrocracking of heavy oil, the metal sulfides entered into chemical reactions with the free- radical intermediate H·formed on the catalyst surface. The free-radical intermediate H· formed on the catalyst surface could react with the free-radicals of big molecules and could suppress coke deposition.
文摘Highly dispersed Cu-base catalyst has been prepared via thermal decomposition of layered double hydroxides precursors. The XRD pattern and the HRTEM images of the as prepared catalyst confirmed the high dispersion of Cu and Fe ions. Results show that the catalyst has a relatively high selectivity of alkanes at low temperature.
基金Supported by the National Key Basic Research and Development Program,China(2015CB250904)
文摘Considering high temperature and high salinity in the reservoirs, a dispersed particle gel soft heterogeneous compound(SHC) flooding system was prepared to improve the micro-profile control and displacement efficiency. The characteristics and displacement mechanisms of the system were investigated via core flow tests and visual simulation experiments. The SHC flooding system composed of DPG particles and surfactants was suitable for the reservoirs with the temperature of 80-110 °C and the salinity of 1×10~4-10×10~4 mg/L. The system presented good characteristics: low viscosity, weak negatively charged, temperature and salinity resistance, particles aggregation capacity, wettability alteration on oil wet surface, wettability weaken on water wet surface, and interfacial tension(IFT) still less than 1×10^(-1) mN/m after aging at high temperature. The SHC flooding system achieved the micro-profile control by entering formations deeply and the better performance was found in the formation with the higher permeability difference existing between the layers, which suggested that the flooding system was superior to the surfactants, DPG particles, and polymer/surfactant compound flooding systems. The system could effectively enhance the micro-profile control in porous media through four behaviors, including direct plugging, bridging, adsorption, and retention. Moreover, the surfactant in the system magnified the deep migration capability and oil displacement capacity of the SHC flooding system, and the impact was strengthened through the mechanisms of improved displacement capacity, synergistic emulsification, enhanced wettability alteration ability and coalescence of oil belts. The synergistic effect of the two components of SHC flooding system improved oil displacement efficiency and subsequently enhanced oil recovery.
文摘Ferro nematic suspensions are the prominent materials to enhance the electro optical performance of liquid crystal displays. Electro optical properties of polymer dispersed liquid crystal (PDLC) display with the introduction of Barium Titanate nanoparticles have been investigated in this article and it is shown that there is a considerable enhancement in electro-optical response of the displays. The nanoparticles lower the switch-on electric field and thereby increase the optical transmission at certain voltages of the displays. The electro-optical characteristics of the PDLC cells were investigated with a He-Ne laser followed by MatLab calculations.
