Acetone is a common volatile organic compound that can cause harm to human health when inhaled in small amounts.Therefore,the development of fast response and low detection limit acetone sensors becomes crucial.In thi...Acetone is a common volatile organic compound that can cause harm to human health when inhaled in small amounts.Therefore,the development of fast response and low detection limit acetone sensors becomes crucial.In this study,a core-shell spherical TiO_(2) sensor with a rich pore structure was designed.This sensor exhibited excellent sensing properties,including higher responsiveness(100 ppm acetone,R_(a)/R_(g)=80),lower detection limit(10 ppb)and short response time(8 s).The problem is that the sensing mechanism between TiO_(2) and acetone is not thoroughly analyzed.To gain further insight,the interaction process of TiO_(2) core-shell spheres and acetone under varying oxygen content environments was investigated by dynamic testing,X-ray photoelectron spectroscopy,in-situ Fourier transform infrared spectroscopy and gas chromatography-mass spectrometry.The research results show that acetone not only adsorbs on the surface of the material and reacts with adsorbed oxygen,but also undergoes catalytic oxidation reaction with TiO_(2) core-shell spheres.Significantly,in high oxygen content environments,acetone undergoes oxidation to form intermediates such as acids and anhydrides that are difficult to desorpt on the surface of the material,thus prolonging the recovery time of the sensor.The discovery of this sensing process will provide some guidance for the design of acetone sensing materials in the future.Meanwhile,this also imparts valuable references and insights for the investigation of the mechanism and application of other sensitive metal oxide materials.展开更多
In this work,Dy_(2)O_(3)rods and layered Dy_(2)WO_(6)heterostructure were effectively interconnected by carbon spheres named Dy_(2)O_(3)/Dy_(2)WO_(6)/C-sph nanocomposite with a confined interface and it was fabricated...In this work,Dy_(2)O_(3)rods and layered Dy_(2)WO_(6)heterostructure were effectively interconnected by carbon spheres named Dy_(2)O_(3)/Dy_(2)WO_(6)/C-sph nanocomposite with a confined interface and it was fabricated using a simple solvothermal approach.These ternary nanocomposites were investigated by X-ray diffraction(XRD),UV-visible diffuse-reflectance spectroscopy(UV-DRS),Fourier transform-infrared spectroscopy(FT-IR),Raman,field emission scanning electron microscopy(FESEM)with energy disperse spectroscopy(EDS),high-resolution transmission electron microscopy(HRTEM),and X-ray photoelectron spectroscopy(XPS)analyses systematically.The XRD data expose that the synthesized materials are formed with a virtuous crystalline state.The charge storage properties and electrochemical performances of the as-synthesized nanocomposites and pure components were assessed with the help of cyclic voltammogram(CV),galvanostatic charge-discharge studies(GCD),and electrochemical impedance studies(EIS),respectively.The rare-earth-based novel Dy_(2)O_(3)/Dy_(2)WO_(6)/C-sph nanocomposite as wo rking electrodes established commendable electrochemical perfo rmances with a maximum specific capacitance value of 123 F/g at a current density of 0.4 A/g in 2.0 mol/L aqueous KOH solution.According to the stability measurements,it was observed that the initial capacitance was maintained at~93%even after 2500 cycles,indicating that good electrochemical stability with the lowest internal resistance values was obtained from EIS analysis.The electrochemical measurements suggest that the Dy_(2)O_(3)/Dy_(2)WO_(6)/C-sph nanocomposite enables great competence and can be used as alternative electrode material in supercapacitor devices to avail high energy efficiency in a sustainable approach.展开更多
Exploring efficient and nonprecious metal electrocatalysts of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is crucial for developing rechargeable zinc-air batteries(ZABs).Herein,an alloying-degree c...Exploring efficient and nonprecious metal electrocatalysts of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is crucial for developing rechargeable zinc-air batteries(ZABs).Herein,an alloying-degree control strategy was employed to fabricate nitrogen-doped carbon sphere(NCS)decorated with dual-phase Co/Co_(7)Fe_(3)heterojunctions(CoFe@NCS).The phase composition of materials has been adjusted by controlling the alloying degree.The optimal CoFe_(0.08)@NCS electrocatalyst displays a half-wave potential of 0.80 V for ORR and an overpotential of 283 mV at 10 mA·cm^(-2)for OER in an alkaline electrolyte.The intriguing bifunctional electrocatalytic activity and durability is attributed to the hierarchically porous structure and interfacial electron coupling of highly-active Co_(7)Fe_(3)alloy and metallic Co species.When the CoFe_(0.08)@NCS material is used as air-cathode catalyst of rechargeable liquid-state zinc-air battery(ZAB),the device shows a high peak power-density(157 mW·cm^(-2))and maintains a stable voltage gap over 150 h,outperforming those of the benchmark(Pt/C+RuO_(2))-based device.In particular,the as-fabricated solid-state flexible ZAB delivers a reliable compatibility under different bending conditions.Our work provides a promising strategy to develop metal/alloy-based electrocatalysts for the application in renewable energy conversion technologies.展开更多
Development of efficient and stable metal catalysts for the selective aqueous phase hydrodeoxygenation(HDO)of biomass-derived oxygenates to value-added biofuels is highly desired.An innovative surface microenvironment...Development of efficient and stable metal catalysts for the selective aqueous phase hydrodeoxygenation(HDO)of biomass-derived oxygenates to value-added biofuels is highly desired.An innovative surface microenvironment modulation strategy was used to construct the nitrogen-doped hollow carbon sphere encapsulated with Pd(Pd@NHCS-X,X:600–800)nanoreactors for catalytic HDO of biomass-derived vanillin in water.The specific surface microenvironments of Pd@NHCS catalysts including the electronic property of active Pd centers and the surface wettability and porous structure of NHCS supports could be well-controlled by the calcination temperature of catalysts.Intrinsic kinetic evaluations demonstrated that the Pd@NHCS-600 catalyst presented a high turnover frequency of 337.77 h^(–1)and a low apparent activation energy of 18.63 kJ/mol.The excellent catalytic HDO performance was attributed to the unique surface microenvironment of Pd@NHCS catalyst based on structure-performance relationship analysis and DFT calculations.It revealed that pyridinic N species dominated the electronic property regulation of Pd sites through electronic metal-support interaction(EMSI)and produced numerous electron-rich active Pd centers,which not only intensified the dissociation and activation of H2 molecules,but also substantially improved the activation capability of vanillin via the enhanced adsorption of–C=O group.The fine hydrophilicity and abundant porous structure promoted the uniform dispersion of catalyst and ensured the effective access of reactants to catalytic active centers in water.Additionally,the Pd@NHCS-600 catalyst exhibited excellent catalytic stability and broad substrate applicability for the selective aqueous phase HDO of various biomass-derived carbonyl compounds.The proposed surface microenvironment modulation strategy will provide a new consideration for the rational design of high-performance nitrogen-doped carbon-supported metal catalysts for catalytic biomass transformation.展开更多
Ceramic hollow spheres have great potential for deep-sea applications.However,the irregularity of the conventional molding process,among other reasons,results in low wall thickness uniformity of hollow spheres.To solv...Ceramic hollow spheres have great potential for deep-sea applications.However,the irregularity of the conventional molding process,among other reasons,results in low wall thickness uniformity of hollow spheres.To solve this problem,in this work,we developed a biaxial rotation grouting process for deep-sea ceramic hollow buoyancy spheres,which improves the drawbacks of the traditional rotary grouting method that results in poor wall thickness uniformity of the hollow spheres due to its irregular rotational processing.In this paper,an experimental study was carried out to investigate the effects of different rotational methods,rotational speeds,rotational time,solid phase content,etc.on the wall thickness uniformity of ceramic hollow spheres.The results show that the hollow floating balls prepared by the biaxial rotation method have the lowest wall thickness standard deviation(0.04)when the rotation speed is 60 rpm,the molding time is 8 min,and the solid phase content is 70 wt%.After the hydrostatic pressure test of 120 MPa,the hydrostatic compressive strength of hollow spheres prepared by the biaxial rotation method was increased by 31.67%compared with that of the traditional process.展开更多
This study presents a novel Li metal host material with a unique hollow nano-spherical structure that incorporates Ag nano-seeds into a graphitic carbon nitride(g-C_(3)N_(4))shell layer,referred to as g-C_(3)N_(4)@Ag ...This study presents a novel Li metal host material with a unique hollow nano-spherical structure that incorporates Ag nano-seeds into a graphitic carbon nitride(g-C_(3)N_(4))shell layer,referred to as g-C_(3)N_(4)@Ag hollow spheres.The g-C_(3)N_(4)@Ag spheres provide a managed internal site for Li metal encapsulation and promote stable Li plating.The g-C_(3)N_(4) spheres are uniformly coated using polydopamine,which has an adhesive nature,to enhance lithium plating/stripping stability.The strategic presence of Ag nano-seeds eliminates the nucleation barrier,properly directing Li growth within the hollow spheres.This design facilitates highly reversible and consistent lithium deposition,offering a promising direction for the production of high-performance lithium metal anodes.These well-designed g-C_(3)N_(4)@Ag hollow spheres ensure stable Li plating/stripping kinetics over more than 500 cycles with a high coulombic efficiency of over 97%.Furthermore,a full cell made using LiNi_(0.90)Co_(0.07)Mn_(0.03)O_(2) and Li-g-C_(3)N_(4)@Ag host electrodes demonstrated highly competitive performance over 200 cycles,providing a guide for the implementation of this technology in advanced lithium metal batteries.展开更多
Spherical objects are widely used in target localization applications,and the existing sphere localization methods with cameras or total stations both have some limitations.A new high-precision sphere localization met...Spherical objects are widely used in target localization applications,and the existing sphere localization methods with cameras or total stations both have some limitations.A new high-precision sphere localization method with a theodolite is proposed in this paper.From the view point of the theodolite,the contour points of a sphere with a known radius are measured as latitude-longitude coordinates.It is observed that the center of the target sphere is located on a cylindrical surface constructed with the latitude-longitude coordinates,and therefore the latitude-longitude coordinates of at least three contour points can be used to construct a set of ternary quadratic equations.The Gröbner basis method is used to compute at most four real solutions of the sphere center coordinates.To distinguish the only meaningful solution from the other possible real solutions,a pre-processing of the measured longitude values is also proposed.The factors affecting the positioning accuracy of the sphere center are evaluated in simulation experiments,which are used to obtain an empirical estimation model of the positioning error.Real data experiments are also performed and the results show that the proposed method can achieve high localization precision.展开更多
Lithium-sulfur(Li-S)batteries are one of the most promising energy storage and conversion devices due to the high theoretical capacity and cost-effectiveness of sulfur.However,they still suffer from sluggish redox kin...Lithium-sulfur(Li-S)batteries are one of the most promising energy storage and conversion devices due to the high theoretical capacity and cost-effectiveness of sulfur.However,they still suffer from sluggish redox kinetics and the shuttle effect caused by complex polysulfides.In this work,graphitic carbon nitride(g-C_(3)N_(4))is utilized as a template and further hydrothermally treated with an Mn source and glucose.The pyrolysis of g-C_(3)N_(4)gives rise to N-doped carbon nanotubes,producing abundant sites for physical confinement and chemical adsorption of polysulfides,while glucose carbonization brings forth amorphous carbon and Mn source produces metal spheres.Afterward,polydopamine(PDA)induces N-doped carbon coating and promotes interface connection as well as electron immigration.This synergistic design possesses a high surface area of micropores and mesopores to aggregate sulfur and accelerate redox kinetics.As a result,the N-doped carbon nanotube with Mn spheres and PDA coating@sulfur(CN/Mn-PDA@S)exhibits a high reversible capacity of 813.5 mAh g^(-1)at 1 C with a decay rate of 0.064%per cycle and remarkable capacity retention at 2 C with rate performance up to 4 C.Therefore,the novel design of N-doped carbon nanotubes with Mn spheres and PDA coating serves as an efficient polysulfide immobilizer for Li-S batteries.展开更多
Structural colors originated from Mie scattering of dielectric spheres can be regulated by the coupling effect between them and substrates.Here a rapid visual identification method of silver ornaments was proposed by ...Structural colors originated from Mie scattering of dielectric spheres can be regulated by the coupling effect between them and substrates.Here a rapid visual identification method of silver ornaments was proposed by the coupling effect of Zn O spheres with them.Both simulation and experimental results proved that,by coupling with different metal substrates,the Mie resonance scattering peaks of ZnO spheres with dimeter of 700 nm showed different degrees of redshift,which lead to different structural color appeared when ZnO spheres deposited on different metal surfaces with a similar appearance.A red structural color was displayed on the surface of the real silver ornament and a yellow-green structural color was shown on the surface of the cupronickel ornament.This method is quite simple and low-cost because it only needs to spray the dispersion of ZnO spheres on the ornament surface.Due to the mild chemical properties of the ZnO,covering and erasing ZnO spheres on the surface of silver would not corrode the silver ornament.Finally,an atomizer method was used for portable and daily testing.This work opens new perspectives on the visual identification of silver.展开更多
To solve the long-standing contradiction between the bonding strength and abradability of an abradable seal coating(ASC),a novel spherical closed-pore structure was proposed.The new structure consisted of three discon...To solve the long-standing contradiction between the bonding strength and abradability of an abradable seal coating(ASC),a novel spherical closed-pore structure was proposed.The new structure consisted of three discontinuous phases,including locally enriched metals,hollow thin-shell spheres,and pores.The results show that the bonding strength of the abradable seal coating reaches 25.4 MPa,and the abrasion ratio between the coating and blade tip,as a characteristic of the abradability of ASCs,is>5900.The dewetting kinetics of the metal film on the ceramic sphere were calculated.The size of the shrink metal hemisphere is 3.6 times the metal film thickness.The locally enriched metal enables a high bonding strength,while the fragmentation of the hollow thin-shell spheres enhances the abradability,thus simultaneously improving the strength and abradability.The coating is expected to be used in next-generation turbines to improve efficiency and stability.展开更多
Sodium-sulfur(Na-S)and potassium-sulfur(K-S)batteries for use at room temperature have received widespread attention because of the abundance and low cost of their raw materials and their high energy density.However,t...Sodium-sulfur(Na-S)and potassium-sulfur(K-S)batteries for use at room temperature have received widespread attention because of the abundance and low cost of their raw materials and their high energy density.However,their development is restricted by the shuttling of polysulfides,large volume expansion and poor conductivity.To overcome these obstacles,an effective approach is to use carbon-based materials with abundant space for the sulfur that has sulfiphilic sites to immobilize it,and a high electrical conductivity.Hollow carbon spheres(HCSs)with a controllable structure and composition are promising for this purpose.We consider recent progress in optimizing the electrochemical performance of Na-/K-S batteries by using these materials.First,the advantages of HCSs,their synthesis methods,and strategies for preparing HCSs/sulfur composite materials are reviewed.Second,the use of HCSs in Na-/K-S batteries,along with mechanisms underlying the resulting performance improvement,are discussed.Finally,prospects for the further development of HCSs for metal−S batteries are presented.展开更多
Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challen...Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challenges due to the dissolution of intermediate reaction products.In this work,we aim to harness the advantages of Se while reducing its limitations by preparing a core-shell mesoporous carbon hollow sphere with a titanium nitride(C@TiN)host to load 63.9wt%Se as the positive electrode material for Al-Se batteries.Using the physical and chemical confinement offered by the hollow mesoporous carbon and TiN,the obtained core-shell mesoporous carbon hollow spheres coated with Se(Se@C@TiN)display superior utilization of the active material and remarkable cycling stability.As a result,Al-Se batteries equipped with the as-prepared Se@C@TiN composite positive electrodes show an initial discharge specific capacity of 377 mAh·g^(-1)at a current density of 1000 mA·g^(-1)while maintaining a discharge specific capacity of 86.0 mAh·g^(-1)over 200 cycles.This improved cycling performance is ascribed to the high electrical conductivity of the core-shell mesoporous carbon hollow spheres and the unique three-dimensional hierarchical architecture of Se@C@TiN.展开更多
Collisions between objects are a relatively common phenomenon in nature.Analyses of collision processes can greatly contribute to solving problems such as impact-rub faults and particle impacts.The coefficient of rest...Collisions between objects are a relatively common phenomenon in nature.Analyses of collision processes can greatly contribute to solving problems such as impact-rub faults and particle impacts.The coefficient of restitution is a critical parameter in the analysis of collision processes.Many experiments have shown that the coefficient of restitution is closely related to the plate thickness,and the smaller the plate thickness,the more inaccurate the coefficient of restitution predicted by the existing model,which seriously affects the process of collision analysis.To remedy this shortcoming,this paper proposes a plate thickness influence factor with the ratio of sphere diameter to plate thickness as the variable.The plate thickness influence factor can optimize the coefficient of restitution model to effectively predict the coefficient of restitution of impacting elastoplastic spheres with finite plate thickness.Finally,the validity of the new model is verified using a large amount of experimental data.展开更多
Electrochemical CO_(2) reduction to produce value-added chemicals and fuels is one of the research hotspots in the field of energy conversion.The development of efficient catalysts with high conductivity and readily a...Electrochemical CO_(2) reduction to produce value-added chemicals and fuels is one of the research hotspots in the field of energy conversion.The development of efficient catalysts with high conductivity and readily accessible active sites for CO_(2) electroreduction remains challenging yet indispensable.In this work,a reliable poly(ethyleneimine)(PEI)-assisted strategy is developed to prepare a hollow carbon nanocomposite comprising a single-site Ni-modified carbon shell and confined Ni nanoparticles(NPs)(denoted as Ni@NHCS),where PEI not only functions as a mediator to induce the highly dispersed growth of Ni NPs within hollow carbon spheres,but also as a nitrogen precursor to construct highly active atomically-dispersed Ni-Nx sites.Benefiting from the unique structural properties of Ni@NHCS,the aggregation and exposure of Ni NPs can be effectively prevented,while the accessibility of abundant catalytically active Ni-Nx sites can be ensured.As a result,Ni@NHCS exhibits a high CO partial current density of 26.9 mA cm^(-2) and a Faradaic efficiency of 93.0% at-1.0 V vs.RHE,outperforming those of its PEI-free analog.Apart from the excellent activity and selectivity,the shell confinement effect of the hollow carbon sphere endows this catalyst with long-term stability.The findings here are anticipated to help understand the structure-activity relationship in Ni-based carbon catalyst systems for electrocatalytic CO_(2) reduction.Furthermore,the PEI-assisted synthetic concept is potentially applicable to the preparation of high-performance metal-based nanoconfined materials tailored for diverse energy conversion applications and beyond.展开更多
This study ingeniously synthesized a novel CdS/NiS hollow nanoflower sphere(HNS)using a one-step method to enhance photocatalytic hydrogen production activity.Compared to conventional preparation methods,this approach...This study ingeniously synthesized a novel CdS/NiS hollow nanoflower sphere(HNS)using a one-step method to enhance photocatalytic hydrogen production activity.Compared to conventional preparation methods,this approach features seamlessly interfaced contact that facilitates efficient electron transfer across the interface.The internal hollow structure allows for multiple light reflections,maximizing light absorption,while the exterior shell and inner surfaces simultaneously offer active sites for reactions.The modification with non-noble metal NiS enables the extraction of electrons from CdS to the NiS surface,achieving rapid charge separation.Furthermore,adsorption-free energy calculations reveal that the NiS surface is more conducive to photocatalytic hydrogen generation,providing additional reaction active sites.The results demonstrate a hydrogen production rate of 2.18 mmol g^(-1)h^(-1)for CdS/NiS HNS,which is 9.48 times greater than that of pristine CdS.This work presents a novel approach for synthesizing seamlessly interfaced contacts between photocatalysts and cocatalysts,offering new insight into efficient one-step synthesis for enhanced photocatalytic performance.展开更多
Monoclinic BiVO4 hollow nanospheres were successfully prepared via template-free method using citric acid （C6H8O7） as chelating agent and characterized by X-ray diffraction patterns, transmission electron microscope...Monoclinic BiVO4 hollow nanospheres were successfully prepared via template-free method using citric acid （C6H8O7） as chelating agent and characterized by X-ray diffraction patterns, transmission electron microscope, UV-Vis DRS, and TG-DTA technique. C6H8O7 played an important role in the formation of hollow spheres. Morphology observations revealed that when appropriate amount of C6H8O7 was introduced, the cavity with the diameter of 40 nm was obtained in BiVO4 nanospheres. UV-Vis diffuse reflectance spectra indicated that the samples had absorption in both UV and visible light region. The photocatalytic activities were evaluated by the degradation of methylene blue under Xe lamp irradiation. Hollow spheres endow BiVO4 samples with greatly improved photocatalytic activity. A possible formation mechanism of hollow spheres was proposed.展开更多
It is rather essential to design glorious system with high CO_(2) adsorption capacity and electron migration efficiency for improving selective and effective CO_(2) reduction into solar fuels.Here,as-synthesized pheno...It is rather essential to design glorious system with high CO_(2) adsorption capacity and electron migration efficiency for improving selective and effective CO_(2) reduction into solar fuels.Here,as-synthesized phenolic resin spheres via suspension polymerization were carbonized and activated by water vapor to obtain activated carbon spheres(ACSs).Subsequently,Bi_(2)MoO_(6)/ACSs were prepared via hydrothermal-impregnated method.The systematical characterizations of samples,including XRD,XPS,SEM,EDX,DRS,BET,PL,CO_(2) adsorption isotherm,EIS and transient photocurrent,were analyzed.The results clearly demonstrated that Bi_(2)MoO_(6) with suitable oxidation reduction potentials and bandgap and ACSs with admirable CO_(2) adsorption and electrical conductivity not only enhanced separation efficiency of photoindued electron-hole pair,but also displayed as 1.8 times CO_(2) reduction activity to CO as single Bi_(2)MoO_(6) sample under Xe-lamp irradiation.Finally,a concerned photocatalytic CO_(2) reduction mechanism was proposed and investigated.Our findings should provide innovative guidance for designing a series of photocatalytic CO_(2) reduction materials with highly efficient and selective ability.展开更多
基金supported by the National Natural Science Foundation of China(Nos.21771060 and 61271126)the International Science&Technology Cooperation Program of China(No.2016YFE0115100)+2 种基金Heilongjiang Provincial Natural Science Foundation of China(No.LH_(2)023B021)Reform and Development Fund Project of Local University supported by the Central Government,Heilongjiang Touyan Innovation Team Program,New Era Excellent Master’s and Doctoral Dissertations of Heilongjiang Province(No.LJYXL2023-020)Basic Scientific Research Project for Heilongjiang Provincial Colleges and Universities(No.2023-KYYWF-1482).
文摘Acetone is a common volatile organic compound that can cause harm to human health when inhaled in small amounts.Therefore,the development of fast response and low detection limit acetone sensors becomes crucial.In this study,a core-shell spherical TiO_(2) sensor with a rich pore structure was designed.This sensor exhibited excellent sensing properties,including higher responsiveness(100 ppm acetone,R_(a)/R_(g)=80),lower detection limit(10 ppb)and short response time(8 s).The problem is that the sensing mechanism between TiO_(2) and acetone is not thoroughly analyzed.To gain further insight,the interaction process of TiO_(2) core-shell spheres and acetone under varying oxygen content environments was investigated by dynamic testing,X-ray photoelectron spectroscopy,in-situ Fourier transform infrared spectroscopy and gas chromatography-mass spectrometry.The research results show that acetone not only adsorbs on the surface of the material and reacts with adsorbed oxygen,but also undergoes catalytic oxidation reaction with TiO_(2) core-shell spheres.Significantly,in high oxygen content environments,acetone undergoes oxidation to form intermediates such as acids and anhydrides that are difficult to desorpt on the surface of the material,thus prolonging the recovery time of the sensor.The discovery of this sensing process will provide some guidance for the design of acetone sensing materials in the future.Meanwhile,this also imparts valuable references and insights for the investigation of the mechanism and application of other sensitive metal oxide materials.
基金supported by Selective Excellence Research Initiative-2023,SRM Institute of Science and Technology(SRMIST/R/AR(A)/SERI2023/174/26-3944)。
文摘In this work,Dy_(2)O_(3)rods and layered Dy_(2)WO_(6)heterostructure were effectively interconnected by carbon spheres named Dy_(2)O_(3)/Dy_(2)WO_(6)/C-sph nanocomposite with a confined interface and it was fabricated using a simple solvothermal approach.These ternary nanocomposites were investigated by X-ray diffraction(XRD),UV-visible diffuse-reflectance spectroscopy(UV-DRS),Fourier transform-infrared spectroscopy(FT-IR),Raman,field emission scanning electron microscopy(FESEM)with energy disperse spectroscopy(EDS),high-resolution transmission electron microscopy(HRTEM),and X-ray photoelectron spectroscopy(XPS)analyses systematically.The XRD data expose that the synthesized materials are formed with a virtuous crystalline state.The charge storage properties and electrochemical performances of the as-synthesized nanocomposites and pure components were assessed with the help of cyclic voltammogram(CV),galvanostatic charge-discharge studies(GCD),and electrochemical impedance studies(EIS),respectively.The rare-earth-based novel Dy_(2)O_(3)/Dy_(2)WO_(6)/C-sph nanocomposite as wo rking electrodes established commendable electrochemical perfo rmances with a maximum specific capacitance value of 123 F/g at a current density of 0.4 A/g in 2.0 mol/L aqueous KOH solution.According to the stability measurements,it was observed that the initial capacitance was maintained at~93%even after 2500 cycles,indicating that good electrochemical stability with the lowest internal resistance values was obtained from EIS analysis.The electrochemical measurements suggest that the Dy_(2)O_(3)/Dy_(2)WO_(6)/C-sph nanocomposite enables great competence and can be used as alternative electrode material in supercapacitor devices to avail high energy efficiency in a sustainable approach.
基金financially supported by the National Natural Science Foundation of China(No.22279047)the Instrumental Analysis Center of Jiangsu University of Science and Technology。
文摘Exploring efficient and nonprecious metal electrocatalysts of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is crucial for developing rechargeable zinc-air batteries(ZABs).Herein,an alloying-degree control strategy was employed to fabricate nitrogen-doped carbon sphere(NCS)decorated with dual-phase Co/Co_(7)Fe_(3)heterojunctions(CoFe@NCS).The phase composition of materials has been adjusted by controlling the alloying degree.The optimal CoFe_(0.08)@NCS electrocatalyst displays a half-wave potential of 0.80 V for ORR and an overpotential of 283 mV at 10 mA·cm^(-2)for OER in an alkaline electrolyte.The intriguing bifunctional electrocatalytic activity and durability is attributed to the hierarchically porous structure and interfacial electron coupling of highly-active Co_(7)Fe_(3)alloy and metallic Co species.When the CoFe_(0.08)@NCS material is used as air-cathode catalyst of rechargeable liquid-state zinc-air battery(ZAB),the device shows a high peak power-density(157 mW·cm^(-2))and maintains a stable voltage gap over 150 h,outperforming those of the benchmark(Pt/C+RuO_(2))-based device.In particular,the as-fabricated solid-state flexible ZAB delivers a reliable compatibility under different bending conditions.Our work provides a promising strategy to develop metal/alloy-based electrocatalysts for the application in renewable energy conversion technologies.
文摘Development of efficient and stable metal catalysts for the selective aqueous phase hydrodeoxygenation(HDO)of biomass-derived oxygenates to value-added biofuels is highly desired.An innovative surface microenvironment modulation strategy was used to construct the nitrogen-doped hollow carbon sphere encapsulated with Pd(Pd@NHCS-X,X:600–800)nanoreactors for catalytic HDO of biomass-derived vanillin in water.The specific surface microenvironments of Pd@NHCS catalysts including the electronic property of active Pd centers and the surface wettability and porous structure of NHCS supports could be well-controlled by the calcination temperature of catalysts.Intrinsic kinetic evaluations demonstrated that the Pd@NHCS-600 catalyst presented a high turnover frequency of 337.77 h^(–1)and a low apparent activation energy of 18.63 kJ/mol.The excellent catalytic HDO performance was attributed to the unique surface microenvironment of Pd@NHCS catalyst based on structure-performance relationship analysis and DFT calculations.It revealed that pyridinic N species dominated the electronic property regulation of Pd sites through electronic metal-support interaction(EMSI)and produced numerous electron-rich active Pd centers,which not only intensified the dissociation and activation of H2 molecules,but also substantially improved the activation capability of vanillin via the enhanced adsorption of–C=O group.The fine hydrophilicity and abundant porous structure promoted the uniform dispersion of catalyst and ensured the effective access of reactants to catalytic active centers in water.Additionally,the Pd@NHCS-600 catalyst exhibited excellent catalytic stability and broad substrate applicability for the selective aqueous phase HDO of various biomass-derived carbonyl compounds.The proposed surface microenvironment modulation strategy will provide a new consideration for the rational design of high-performance nitrogen-doped carbon-supported metal catalysts for catalytic biomass transformation.
基金Funded by the Key Research and Development Program of Shandong Province(No.2020JMRH0101)。
文摘Ceramic hollow spheres have great potential for deep-sea applications.However,the irregularity of the conventional molding process,among other reasons,results in low wall thickness uniformity of hollow spheres.To solve this problem,in this work,we developed a biaxial rotation grouting process for deep-sea ceramic hollow buoyancy spheres,which improves the drawbacks of the traditional rotary grouting method that results in poor wall thickness uniformity of the hollow spheres due to its irregular rotational processing.In this paper,an experimental study was carried out to investigate the effects of different rotational methods,rotational speeds,rotational time,solid phase content,etc.on the wall thickness uniformity of ceramic hollow spheres.The results show that the hollow floating balls prepared by the biaxial rotation method have the lowest wall thickness standard deviation(0.04)when the rotation speed is 60 rpm,the molding time is 8 min,and the solid phase content is 70 wt%.After the hydrostatic pressure test of 120 MPa,the hydrostatic compressive strength of hollow spheres prepared by the biaxial rotation method was increased by 31.67%compared with that of the traditional process.
基金supported by the National Research Council of Science&Technology(NST)grant by the Korea government(MSIT)(No.GTL24011-000)supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.RS-2023-00272863)supported by Korea Institute for Advancement of Technology(KIAT)grant funded by the Korea Government(MOTIE)(P0012748,HRD Program for Industrial Innovation)。
文摘This study presents a novel Li metal host material with a unique hollow nano-spherical structure that incorporates Ag nano-seeds into a graphitic carbon nitride(g-C_(3)N_(4))shell layer,referred to as g-C_(3)N_(4)@Ag hollow spheres.The g-C_(3)N_(4)@Ag spheres provide a managed internal site for Li metal encapsulation and promote stable Li plating.The g-C_(3)N_(4) spheres are uniformly coated using polydopamine,which has an adhesive nature,to enhance lithium plating/stripping stability.The strategic presence of Ag nano-seeds eliminates the nucleation barrier,properly directing Li growth within the hollow spheres.This design facilitates highly reversible and consistent lithium deposition,offering a promising direction for the production of high-performance lithium metal anodes.These well-designed g-C_(3)N_(4)@Ag hollow spheres ensure stable Li plating/stripping kinetics over more than 500 cycles with a high coulombic efficiency of over 97%.Furthermore,a full cell made using LiNi_(0.90)Co_(0.07)Mn_(0.03)O_(2) and Li-g-C_(3)N_(4)@Ag host electrodes demonstrated highly competitive performance over 200 cycles,providing a guide for the implementation of this technology in advanced lithium metal batteries.
基金supported in part by the National Natural Science Foundation of China under Grants 61703373,61873246,U1504604in part by the Key research project of Henan Province Universities under Grant 19A413014.
文摘Spherical objects are widely used in target localization applications,and the existing sphere localization methods with cameras or total stations both have some limitations.A new high-precision sphere localization method with a theodolite is proposed in this paper.From the view point of the theodolite,the contour points of a sphere with a known radius are measured as latitude-longitude coordinates.It is observed that the center of the target sphere is located on a cylindrical surface constructed with the latitude-longitude coordinates,and therefore the latitude-longitude coordinates of at least three contour points can be used to construct a set of ternary quadratic equations.The Gröbner basis method is used to compute at most four real solutions of the sphere center coordinates.To distinguish the only meaningful solution from the other possible real solutions,a pre-processing of the measured longitude values is also proposed.The factors affecting the positioning accuracy of the sphere center are evaluated in simulation experiments,which are used to obtain an empirical estimation model of the positioning error.Real data experiments are also performed and the results show that the proposed method can achieve high localization precision.
基金support from the National Natural Science Foundation of China(No.22179109).
文摘Lithium-sulfur(Li-S)batteries are one of the most promising energy storage and conversion devices due to the high theoretical capacity and cost-effectiveness of sulfur.However,they still suffer from sluggish redox kinetics and the shuttle effect caused by complex polysulfides.In this work,graphitic carbon nitride(g-C_(3)N_(4))is utilized as a template and further hydrothermally treated with an Mn source and glucose.The pyrolysis of g-C_(3)N_(4)gives rise to N-doped carbon nanotubes,producing abundant sites for physical confinement and chemical adsorption of polysulfides,while glucose carbonization brings forth amorphous carbon and Mn source produces metal spheres.Afterward,polydopamine(PDA)induces N-doped carbon coating and promotes interface connection as well as electron immigration.This synergistic design possesses a high surface area of micropores and mesopores to aggregate sulfur and accelerate redox kinetics.As a result,the N-doped carbon nanotube with Mn spheres and PDA coating@sulfur(CN/Mn-PDA@S)exhibits a high reversible capacity of 813.5 mAh g^(-1)at 1 C with a decay rate of 0.064%per cycle and remarkable capacity retention at 2 C with rate performance up to 4 C.Therefore,the novel design of N-doped carbon nanotubes with Mn spheres and PDA coating serves as an efficient polysulfide immobilizer for Li-S batteries.
基金supported by the National Natural Science Foundation of China(Nos.22178047 and 21878042)the Dalian Science and Technology Innovation Fund(No.2020JJ26GX046)the Fundamental Research Funds for the Central Universities(Nos.DUT22LAB610 and DUT2022TB10)。
文摘Structural colors originated from Mie scattering of dielectric spheres can be regulated by the coupling effect between them and substrates.Here a rapid visual identification method of silver ornaments was proposed by the coupling effect of Zn O spheres with them.Both simulation and experimental results proved that,by coupling with different metal substrates,the Mie resonance scattering peaks of ZnO spheres with dimeter of 700 nm showed different degrees of redshift,which lead to different structural color appeared when ZnO spheres deposited on different metal surfaces with a similar appearance.A red structural color was displayed on the surface of the real silver ornament and a yellow-green structural color was shown on the surface of the cupronickel ornament.This method is quite simple and low-cost because it only needs to spray the dispersion of ZnO spheres on the ornament surface.Due to the mild chemical properties of the ZnO,covering and erasing ZnO spheres on the surface of silver would not corrode the silver ornament.Finally,an atomizer method was used for portable and daily testing.This work opens new perspectives on the visual identification of silver.
基金financially supported by the National Sci-ence and Technology Major Project(No.2017-VII-0012-0107)the Postdoctoral Innovative Talent Support Program(No.BX2021238)the National Natural Science Foundation of China(No.U22A20110).
文摘To solve the long-standing contradiction between the bonding strength and abradability of an abradable seal coating(ASC),a novel spherical closed-pore structure was proposed.The new structure consisted of three discontinuous phases,including locally enriched metals,hollow thin-shell spheres,and pores.The results show that the bonding strength of the abradable seal coating reaches 25.4 MPa,and the abrasion ratio between the coating and blade tip,as a characteristic of the abradability of ASCs,is>5900.The dewetting kinetics of the metal film on the ceramic sphere were calculated.The size of the shrink metal hemisphere is 3.6 times the metal film thickness.The locally enriched metal enables a high bonding strength,while the fragmentation of the hollow thin-shell spheres enhances the abradability,thus simultaneously improving the strength and abradability.The coating is expected to be used in next-generation turbines to improve efficiency and stability.
文摘Sodium-sulfur(Na-S)and potassium-sulfur(K-S)batteries for use at room temperature have received widespread attention because of the abundance and low cost of their raw materials and their high energy density.However,their development is restricted by the shuttling of polysulfides,large volume expansion and poor conductivity.To overcome these obstacles,an effective approach is to use carbon-based materials with abundant space for the sulfur that has sulfiphilic sites to immobilize it,and a high electrical conductivity.Hollow carbon spheres(HCSs)with a controllable structure and composition are promising for this purpose.We consider recent progress in optimizing the electrochemical performance of Na-/K-S batteries by using these materials.First,the advantages of HCSs,their synthesis methods,and strategies for preparing HCSs/sulfur composite materials are reviewed.Second,the use of HCSs in Na-/K-S batteries,along with mechanisms underlying the resulting performance improvement,are discussed.Finally,prospects for the further development of HCSs for metal−S batteries are presented.
基金supported by the National Natural Science Foundation of China(No.52374350)China Postdoctoral Science Foundation(Nos.2020M680347 and 2021T140051)the Fundamental Research Funds for the Central Universities(No.FRF-TP-20-045A1)。
文摘Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challenges due to the dissolution of intermediate reaction products.In this work,we aim to harness the advantages of Se while reducing its limitations by preparing a core-shell mesoporous carbon hollow sphere with a titanium nitride(C@TiN)host to load 63.9wt%Se as the positive electrode material for Al-Se batteries.Using the physical and chemical confinement offered by the hollow mesoporous carbon and TiN,the obtained core-shell mesoporous carbon hollow spheres coated with Se(Se@C@TiN)display superior utilization of the active material and remarkable cycling stability.As a result,Al-Se batteries equipped with the as-prepared Se@C@TiN composite positive electrodes show an initial discharge specific capacity of 377 mAh·g^(-1)at a current density of 1000 mA·g^(-1)while maintaining a discharge specific capacity of 86.0 mAh·g^(-1)over 200 cycles.This improved cycling performance is ascribed to the high electrical conductivity of the core-shell mesoporous carbon hollow spheres and the unique three-dimensional hierarchical architecture of Se@C@TiN.
基金Supported by Joint Fund of the Ministry of Education of China (Grant No.8091B022203)Youth Talent Support Project (Grant No.2022-JCJQ-QT-059)。
文摘Collisions between objects are a relatively common phenomenon in nature.Analyses of collision processes can greatly contribute to solving problems such as impact-rub faults and particle impacts.The coefficient of restitution is a critical parameter in the analysis of collision processes.Many experiments have shown that the coefficient of restitution is closely related to the plate thickness,and the smaller the plate thickness,the more inaccurate the coefficient of restitution predicted by the existing model,which seriously affects the process of collision analysis.To remedy this shortcoming,this paper proposes a plate thickness influence factor with the ratio of sphere diameter to plate thickness as the variable.The plate thickness influence factor can optimize the coefficient of restitution model to effectively predict the coefficient of restitution of impacting elastoplastic spheres with finite plate thickness.Finally,the validity of the new model is verified using a large amount of experimental data.
文摘Electrochemical CO_(2) reduction to produce value-added chemicals and fuels is one of the research hotspots in the field of energy conversion.The development of efficient catalysts with high conductivity and readily accessible active sites for CO_(2) electroreduction remains challenging yet indispensable.In this work,a reliable poly(ethyleneimine)(PEI)-assisted strategy is developed to prepare a hollow carbon nanocomposite comprising a single-site Ni-modified carbon shell and confined Ni nanoparticles(NPs)(denoted as Ni@NHCS),where PEI not only functions as a mediator to induce the highly dispersed growth of Ni NPs within hollow carbon spheres,but also as a nitrogen precursor to construct highly active atomically-dispersed Ni-Nx sites.Benefiting from the unique structural properties of Ni@NHCS,the aggregation and exposure of Ni NPs can be effectively prevented,while the accessibility of abundant catalytically active Ni-Nx sites can be ensured.As a result,Ni@NHCS exhibits a high CO partial current density of 26.9 mA cm^(-2) and a Faradaic efficiency of 93.0% at-1.0 V vs.RHE,outperforming those of its PEI-free analog.Apart from the excellent activity and selectivity,the shell confinement effect of the hollow carbon sphere endows this catalyst with long-term stability.The findings here are anticipated to help understand the structure-activity relationship in Ni-based carbon catalyst systems for electrocatalytic CO_(2) reduction.Furthermore,the PEI-assisted synthetic concept is potentially applicable to the preparation of high-performance metal-based nanoconfined materials tailored for diverse energy conversion applications and beyond.
基金supported by the National Natural Science Foundation of China(Nos.22278169 and 51973078)the Excellent Scientific Research and Innovation team of the Education Department of Anhui Province(No.2022AH010028)+2 种基金the Major projects of the Education Department of Anhui Province(No.2022AH040068)the Key Foundation of Educational Commission of Anhui Province(Nos.2022AH050396 and 2022AH050376)Anhui Provincial Quality Engineering Project(No.2022sx134).
文摘This study ingeniously synthesized a novel CdS/NiS hollow nanoflower sphere(HNS)using a one-step method to enhance photocatalytic hydrogen production activity.Compared to conventional preparation methods,this approach features seamlessly interfaced contact that facilitates efficient electron transfer across the interface.The internal hollow structure allows for multiple light reflections,maximizing light absorption,while the exterior shell and inner surfaces simultaneously offer active sites for reactions.The modification with non-noble metal NiS enables the extraction of electrons from CdS to the NiS surface,achieving rapid charge separation.Furthermore,adsorption-free energy calculations reveal that the NiS surface is more conducive to photocatalytic hydrogen generation,providing additional reaction active sites.The results demonstrate a hydrogen production rate of 2.18 mmol g^(-1)h^(-1)for CdS/NiS HNS,which is 9.48 times greater than that of pristine CdS.This work presents a novel approach for synthesizing seamlessly interfaced contacts between photocatalysts and cocatalysts,offering new insight into efficient one-step synthesis for enhanced photocatalytic performance.
文摘Monoclinic BiVO4 hollow nanospheres were successfully prepared via template-free method using citric acid （C6H8O7） as chelating agent and characterized by X-ray diffraction patterns, transmission electron microscope, UV-Vis DRS, and TG-DTA technique. C6H8O7 played an important role in the formation of hollow spheres. Morphology observations revealed that when appropriate amount of C6H8O7 was introduced, the cavity with the diameter of 40 nm was obtained in BiVO4 nanospheres. UV-Vis diffuse reflectance spectra indicated that the samples had absorption in both UV and visible light region. The photocatalytic activities were evaluated by the degradation of methylene blue under Xe lamp irradiation. Hollow spheres endow BiVO4 samples with greatly improved photocatalytic activity. A possible formation mechanism of hollow spheres was proposed.
基金The authors are thankful to the National Natural Science Foundation of China(No.21978196,21676178,21706179)Shanxi Province Science Foundation for Youths(201801D211008).
文摘It is rather essential to design glorious system with high CO_(2) adsorption capacity and electron migration efficiency for improving selective and effective CO_(2) reduction into solar fuels.Here,as-synthesized phenolic resin spheres via suspension polymerization were carbonized and activated by water vapor to obtain activated carbon spheres(ACSs).Subsequently,Bi_(2)MoO_(6)/ACSs were prepared via hydrothermal-impregnated method.The systematical characterizations of samples,including XRD,XPS,SEM,EDX,DRS,BET,PL,CO_(2) adsorption isotherm,EIS and transient photocurrent,were analyzed.The results clearly demonstrated that Bi_(2)MoO_(6) with suitable oxidation reduction potentials and bandgap and ACSs with admirable CO_(2) adsorption and electrical conductivity not only enhanced separation efficiency of photoindued electron-hole pair,but also displayed as 1.8 times CO_(2) reduction activity to CO as single Bi_(2)MoO_(6) sample under Xe-lamp irradiation.Finally,a concerned photocatalytic CO_(2) reduction mechanism was proposed and investigated.Our findings should provide innovative guidance for designing a series of photocatalytic CO_(2) reduction materials with highly efficient and selective ability.
