Cu2O@Cu2O core-shell nanoparticles (NPs) were prepared by using solution phase strategy. It was found that Cu2O@Cu2O NPs were easily converted to Cu2O@Cu NPs with the help of polyvinylpyrrolidine (PVP) and excessive a...Cu2O@Cu2O core-shell nanoparticles (NPs) were prepared by using solution phase strategy. It was found that Cu2O@Cu2O NPs were easily converted to Cu2O@Cu NPs with the help of polyvinylpyrrolidine (PVP) and excessive ascorbic acid (AA) in air at room temperature, which was an interesting phenomenon. The features of the two kinds of NPs were characterized by XRD, TEM and extinction spectra. Cu2O@Cu NPs with different shell thicknesses showed wide tunable optical properties for the localized surface plasmon (LSP) in metallic Cu. But Cu2O@Cu2O NPs did not indicate this feature. FTIR results reveal that Cu+ ions on the surface of Cu2O shell coordinate with N and O atoms in PVP and are further reduced to metallic Cu by excessive AA and then form a nucleation site on the surface of Cu2O nanocrystalline. PVP binds onto different sites to proceed with the reduction utill all the Cu sources in Cu2O shell are completely assumed.展开更多
Herein,we successfully prepare highly dispersed and uniform small nano-size nickel nanoparticles embedded on core-shell carbon spheres by confined-deposition method.The mesoporous silica layer containing surfactant co...Herein,we successfully prepare highly dispersed and uniform small nano-size nickel nanoparticles embedded on core-shell carbon spheres by confined-deposition method.The mesoporous silica layer containing surfactant coated on the surface of the polymer sphere provides confined space and effectively controls the growth of nickel nanoparticles during pyrolysis.At the same time,the introduction of nickel species has an impact on structure of the obtained carbon spheres,and it can promote the deposition of carbon to realize the adjustment from hollow to core-shell and then to solid spheres.Owing to the uniform distribution of Ni nanoparticles with small size,mesoporous structure,N-doping groups,high specified surface areas,and core-shell structure,the obtained catalyst shows exciting ability for the production of CO by reduction of CO2with a maximum CO Faradaic efficiency of 98%,indicating its promising prospect in electro-reduction of CO2.展开更多
Unlike previous emulsion polymerization, we used grafting reactions in soap-free emulsion systems. In this study, we synthesized grafted PMMA/PEI core-shell nanoparticles by varying the MMA/PEI content and molecular w...Unlike previous emulsion polymerization, we used grafting reactions in soap-free emulsion systems. In this study, we synthesized grafted PMMA/PEI core-shell nanoparticles by varying the MMA/PEI content and molecular weight of PEI (Mn = 600, 8000, and 10,000). The size and morphology of the core-shell nanoparticles were characterized by a particle size analyzer and scanning electron microscopy. The nanoparticles were 178 - 408 nm in diameter and swelled in water or methanol by 30 - 75 nm. The size of the nanoparticles increased with MMA contents, whereas the size distribution progressively became homogeneous with increasing molecular weight of PEI. Lastly, we measured CO2 adsorption capacity of the grafted PMMA/PEI core-shell nanoparticles, and we found the capacity to be limited at a level of 0.69 mg, which occurred for nanoparticles prepared from emulsions at a pH value of 11.展开更多
Ag@Cu2O core-shell metal-semiconductor nanoparticles (NPs) were prepared by using solution phase strategy. The composites, structures, morphologies and absorption properties of Ag@Cu2O core-shell NPs were systematic...Ag@Cu2O core-shell metal-semiconductor nanoparticles (NPs) were prepared by using solution phase strategy. The composites, structures, morphologies and absorption properties of Ag@Cu2O core-shell NPs were systematically characterized by X-ray diffraction (XRD) , transmission electron microscope (TEM) and ultraviolet-visible (UV-VIS) absorption spectra. The Ag@Cu2O core-shell metal-semiconductor NPs indicate tunable light absorption over the visible-light region. Under visible-near-infrared (VIS-NIR) light irradiation, up to 83.0% MO dye could be degraded after 150 min irradiation. The calculated apparent pseudo-first-order reaction rate constant is 0.0038 min-1. The high photocatalytic efficiency attributes to the decreasing recombination of photo-induced electrons and holes for the electron sink of Ag core, the better spectra overlap between the absorption spectra of Ag@Cu2O NPs and the emission spectra of the VIS-NIR lamp, and the good adsorption ability and rich catalytic active points for the poroused shell structure of Cu2O.展开更多
Along with a wide range of applications,the surface-enhanced Raman spectroscopy(SERS)is a promi-nent analytical technique to recognize and detect molecules and materials even at an extremely low mo-lar concentration.I...Along with a wide range of applications,the surface-enhanced Raman spectroscopy(SERS)is a promi-nent analytical technique to recognize and detect molecules and materials even at an extremely low mo-lar concentration.In this work,a unique hybrid SERS platform is demonstrated by the incorporation of molybdenum disulfate(MoS2)nanoparticles(NPs)onto the core-shell AuPt hybrid NPs(HNPs)for the en-hanced molecular Raman vibration of crystal violet(CV).The hybrid platform takes the advantage of both the electromagnetic mechanism(EM)offered by the AuPt HNPs and chemical mechanism(CM)owing to the MoS2NPs.The distinctive core-shell morphology of AuPt HNPs with the high-density background Au NPs is attained by a unique two-step solid-state dewetting method,which can offer a high concentration of electromagnetic hot spots.At the same time,the MoS2NPs can provide an ample charge transfer with abundant active sites.Through the hybrid SERS approach,a dramatic SERS enhancement of CV Raman vibration is demonstrated,and the SERS capability is thoroughly studied.In addition,the finite-difference time-domain(FDTD)simulations provide a deeper understanding of the electromagnetic field distributions for various configurations of nanostructures and their hybrid combinations:i.e.,HNPs,alloy NPs,MoS2/HNPs configurations.展开更多
Functionalized PS/SiO:composite nanoparticles bearing sulfonic groups on the surface were successfully synthesized via emulsion copolymerization using a polymerizable emulsifier ar olefin solfonate(AOS).As demonstrate...Functionalized PS/SiO:composite nanoparticles bearing sulfonic groups on the surface were successfully synthesized via emulsion copolymerization using a polymerizable emulsifier ar olefin solfonate(AOS).As demonstrated by transmission electron microscopy and atomic force microscopy,well-defined core-shel]PS/SiO:composite nanoparticles with a diameter of 50 nm were obtained.Sulfonic groups introduced onto the surface of the composite nanoparticles were quantified by FTIR.and can be controlled to some extent via a two-stage procedure.展开更多
CO2methanation offers a pathway to produce a carbon-neutral methane fuel.Although a number of research efforts have been conducted on this topic,a greater understanding of the mechanism of the reaction,which is sti...CO2methanation offers a pathway to produce a carbon-neutral methane fuel.Although a number of research efforts have been conducted on this topic,a greater understanding of the mechanism of the reaction,which is still under debate,is needed.Here,using in situ transmission electron microscopy,we provide direct insights into the dynamics of a metallic nickel catalyst supported on activated carbon during CO2methanation.The keys to the high performance of the catalyst are the in situ formation and dynamic behavior of a Ni@NiO core@shell nanostructure.Based on the detailed electron microscopy investigation,the mechanism of such nanostructure formation during methanation is proposed.Our studies revealed that the deactivation of the catalyst is not due to the accumulation of carbon coke over nickel nanoparticles,but an increase in the size of the nickel nanoparticles that is responsible for the deactivation of the catalyst over time.展开更多
Multicomponent binary metal oxide-involved hybrid structures with unique physicochemical properties have received extensive attention due to their fascinating electrochemical performance.Herein,a flexible strategy,whi...Multicomponent binary metal oxide-involved hybrid structures with unique physicochemical properties have received extensive attention due to their fascinating electrochemical performance.Herein,a flexible strategy,which involves the preparation of dual-functional heterometallic Fe2M clusters and their subsequent sintering treatment,is developed to engineer novel 3D hierarchical porous structures assembled with MFe2O4(M=Co,Mn,Ni and Zn)nanoparticles confined within carbon outer shell(denoted as MFe2O4@C HPSs).In this intriguing construction,it can be observed that MFe2O4@C HPSs comprised of carbon coated secondary MFe2O4nanoparticles with an interconnected carbon network.The as-prepared MFe2O4@C HPSs possess combined advantages of high capacity of MFe2O4and high conductivity of carbon.As expected,the MFe2O4@C HPSs offer a high reversible capacity,high cycling stability and superior rate performance.The interconnected conductive carbon shells facilitates fast ion and electron transport and accommodates the mechanical strain.In addition,nanosized MFe2O4particles,which shorten the ion-transport path and provide extra electroactive sites,also improve the reaction kinetics.Moreover,these MFe2O4@C HPSs exhibit good structural integrity during repeated charging and discharging.The research perspective and strategy reported here are highly versatile and shed new light on the synthesis of other advanced electrode for various applications.展开更多
Molybdenum disulfide(MoS2)-based nanostructures are highly desirable for applications such as chemical and biological sensing,photo/electrochemical catalysis,and energy storage due to their unique physical and chem...Molybdenum disulfide(MoS2)-based nanostructures are highly desirable for applications such as chemical and biological sensing,photo/electrochemical catalysis,and energy storage due to their unique physical and chemical properties.In this work,MoS2core-shell nanoparticles were first prepared through the liquid-phase processing of bulk MoS2by a femtosecond laser.The core of prepared nanoparticles was incompletely and weakly crystalline MoS2;the shell of prepared nanoparticles was highly crystalline MoS2,which wrapped around the core layer by layer.The femtosecond laser simultaneously achieved liquid-phase ablation and light exfoliation.The formation mechanism of the core-shell nanoparticles is to prepare the nanonuclei first by laser liquid-phase ablation and then the nanosheets by light exfoliation;the nanosheets will wrap the nanonuclei layer by layer through van der Waals forces to form core-shell nanoparticles.The MoS2core-shell nanoparticles,because of Mo-S bond breakage and recombination,have high chemical activity for chemical catalysis.Afterward,the nanoparticles were used as a reducing agent to directly prepare three-dimensional(3D)Au-MoS2microanostructures,which were applied as surface-enhanced Raman spectroscopy(SERS)substrates to explore chemical sensing activity.The ultrahigh enhancement factor(1.06×1011),ultralow detection limit(10-13M),and good SERS adaptability demonstrate highly sensitive SERS activity,great ability of ultralow concentration detection,and ability to detect diverse analytes,respectively.This work reveals the tremendous potential of 3D Au-MoS2composite structures as excellent SERS substrates for chemical and biological sensing.展开更多
A novel core-shell luminol-based SiO2 nanoparticle While these nanoparticles were used as electrogenerated was synthesized by two step micro-emulsion method. chemiluminescence (ECL) reagent, the electrochemical (EC...A novel core-shell luminol-based SiO2 nanoparticle While these nanoparticles were used as electrogenerated was synthesized by two step micro-emulsion method. chemiluminescence (ECL) reagent, the electrochemical (EC) reaction as well as the subsequent chemiluminescence (CL) reaction not only could be separated spatially, but also presented high efficiency for analytical purpose. In this case, the core-shell luminol-based SiO2 nanoparticles offered more potential to avoid the contradiction between the EC and the CL reaction conditions. A new ECL method based on the nanoparticle was developed, and isoniazid was selected as a model analyte to illustrate the characteristics of this new ECL method. Under the selected conditions, the proposed ECL response to isoniazid concentration was linear in the range of 1.0 ×10^-10 to 1.0 × 10^-6 g/mL with 2 × 10^-11g/mL detection limit.展开更多
ZrO2/PMMA nanocomposite particles are synthesized through an in-situ free radical emulsion polymerization based on the silane coupling agent(Z-6030)modified ZrO2nanoparticles,and the morphology,size and its dist...ZrO2/PMMA nanocomposite particles are synthesized through an in-situ free radical emulsion polymerization based on the silane coupling agent(Z-6030)modified ZrO2nanoparticles,and the morphology,size and its distribution of nanocomposite particles are investigated.Scanning electron microscopy(SEM)images demonstrate that the methyl methacrylate(MMA)feeding rate has a significant effect on the particle size and morphology.When the MMA feeding rate decreases from 0.42 ml-min-1 to 0.08 ml.min-1,large particles(about 200-550.nm)will not form,and the size distribution become narrow(36-54 nm).The average nanocomposite particles size increases from 34 nm to 55 nm,as the MMA/ZrO2 nanoparticles mass ratio increased from 4:1 to 16:1.Regular spherical ZrO2/PMMA nanocomposite particles are synthesized when the emulsifier OP-10 concentration is 2 mg.m1-1.The nanocomposite particles could be mixed with VAc-VeoVa10 polymer matrix just by magnetic stirring to prepare the ZrOE/PMMA/VAc-VeoVal0 hybrid coatings.SEM and atomic force microscopy(AFM)photos reveal that the distribution of the ZrO2/PMMA nanocomposite particles in the VAc-VeoVal0 polymer matrix is homogenous and stable.Here,the grafted-PMMA polymer on ZrO2 nanoparticles plays as a bridge which effectively connects the ZrO2 nanoparticles and the VAc-VeoVal0 polymer matrix with improved comparability.In consequence,the hybrid coating with good dispersion stability is obtained.展开更多
Core-shell silica nanoparticles are superior in modifying surface wetting behavior,enhancing nucleation and growth in crystallization,improving dispersion of naked nanoparticles,and thus upgrading the overall properti...Core-shell silica nanoparticles are superior in modifying surface wetting behavior,enhancing nucleation and growth in crystallization,improving dispersion of naked nanoparticles,and thus upgrading the overall properties of organic polymers.The dispersion behavior and morphology of monodisperse core-shell silica particles in several polymers including polyesters are reviewed and their potential applications are discussed.展开更多
Six kinds of terbium ternary complexes with halo-benzoic acids were synthesized. Their compositions were determined by C, H elemental analyzer and EDTA titration. The infrared spectra, ultraviolet absorption spectra, ...Six kinds of terbium ternary complexes with halo-benzoic acids were synthesized. Their compositions were determined by C, H elemental analyzer and EDTA titration. The infrared spectra, ultraviolet absorption spectra, and fluorescence spectra were also measured to identify the complexes. Elemental analysis showed that the compositions of these complexes were Tb(p-BrBA)3- H20, Tb(p-CIBA)3- 2H20, Tb(p-FBA)3- H20, Tb(o-FBA)3·2H20, Tb(o-CIBA)3· H20, and Tb(o-BrBA)3. H20, respectively. The monodispersed Ag@SiO2 core-shell nanoparticles with silica thicknesses of 10, 15, and 25 nm were success- fully prepared and characterized by transmission-electron microscopy. Fluorescence intensities of the complexes were detected before and after Ag@SiO2core-shell nanoparticles were added; the enhancement times were related to the silica-shell thick- ness. The fluorescence enhancement times were largest when the thickness of the silica shell was 25 nm. The mechanism may be attributed to the localized surface-plasmon resonance. Furthermore, the enhancement effect of terbium fluoro-benzoate complexes was the strongest in these complexes. This result may be attributed to the hydrogen bond between the hydroxyl on the surface of the silica shell and the fluorine atom.展开更多
The construction of highly stable and regular nanoreactors is a major challenge.In this work,we use a facile template protection method to obtain ZIF-67@SiO2(JS)and to encapsulate metal oxide nanoparticles(Co3O_...The construction of highly stable and regular nanoreactors is a major challenge.In this work,we use a facile template protection method to obtain ZIF-67@SiO2(JS)and to encapsulate metal oxide nanoparticles(Co3O4)into nanoreactors(SiO2).ZIF-67 crystals provide a cobalt species;SiO2was first used as a protective layer of ZIF-67 and then as a nanoreactor for metastable metal oxide nanoparticles.On this basis,Co3O4@SiO2with dodecahedron morphology were synthesized by calcining JS at different tempe ratures,followed by a hydrothermal reaction to obtain Co3(OH)4Si2O5.Subsequently,CoSx and CoP-SiO2were fabricated through sulfuration and phosphorization.The results in this work show that nanoreactors derived from metal-organic frameworks(MOFs)with a rational structure have broad development prospects.展开更多
Regulating the surface plasmon resonance(SPR)of metallic nanostructures is of great interests for optical and catalytic applications,however,it is still a great challenge for tuning SPR features of small metallic nano...Regulating the surface plasmon resonance(SPR)of metallic nanostructures is of great interests for optical and catalytic applications,however,it is still a great challenge for tuning SPR features of small metallic nanoparticles(<10 nm).In this work,we design a unique dielectric support-urchin-like mesoporous silica nanoparticles(U-SiO2)with ordered long spikes on its surface,which can well enhance the SPR properties of~3 nm gold nanocrystals(AuNCs).The U-SiO2not only realizes the uniform self-assembly of AuNCs,but also prevents their aggregation due to the unique confinement effect.The finite-difference time-domain simulations show that the AuNCs on U-SiO2can generate plasmonic hot spots with highly enhanced electromagnetic field.Moreover,the hot electrons can be effectively and rapidly transferred through the interface junction to TiO2.Thus,a high visible-light-driven photocatalytic activity can be observed,which is 3.8 times higher than that of smooth photocatalysts.The concept of dielectric supports engineering provides a new strategy for tuning SPR of small metallic nanocrystals towards the development of advanced plasmon-based applications.展开更多
基金Projects(41172110,61107090)supported by the National Natural Science Foundation of China
摘要Cu2O@Cu2O core-shell nanoparticles (NPs) were prepared by using solution phase strategy. It was found that Cu2O@Cu2O NPs were easily converted to Cu2O@Cu NPs with the help of polyvinylpyrrolidine (PVP) and excessive ascorbic acid (AA) in air at room temperature, which was an interesting phenomenon. The features of the two kinds of NPs were characterized by XRD, TEM and extinction spectra. Cu2O@Cu NPs with different shell thicknesses showed wide tunable optical properties for the localized surface plasmon (LSP) in metallic Cu. But Cu2O@Cu2O NPs did not indicate this feature. FTIR results reveal that Cu+ ions on the surface of Cu2O shell coordinate with N and O atoms in PVP and are further reduced to metallic Cu by excessive AA and then form a nucleation site on the surface of Cu2O nanocrystalline. PVP binds onto different sites to proceed with the reduction utill all the Cu sources in Cu2O shell are completely assumed.
基金financially supported by the Natural Science Foundation of Hebei(Nos.B02020208088,H2020206514 and B2021208074)S&T Program of Hebei(Nos.20544401D,20314401D,206Z4406G,21314402D,22344402D,22373709D,22284601Z and 21344601D)Tianjin Science and Technology Project(No.19YFSLQY00070)。
摘要Herein,we successfully prepare highly dispersed and uniform small nano-size nickel nanoparticles embedded on core-shell carbon spheres by confined-deposition method.The mesoporous silica layer containing surfactant coated on the surface of the polymer sphere provides confined space and effectively controls the growth of nickel nanoparticles during pyrolysis.At the same time,the introduction of nickel species has an impact on structure of the obtained carbon spheres,and it can promote the deposition of carbon to realize the adjustment from hollow to core-shell and then to solid spheres.Owing to the uniform distribution of Ni nanoparticles with small size,mesoporous structure,N-doping groups,high specified surface areas,and core-shell structure,the obtained catalyst shows exciting ability for the production of CO by reduction of CO2with a maximum CO Faradaic efficiency of 98%,indicating its promising prospect in electro-reduction of CO2.
摘要Unlike previous emulsion polymerization, we used grafting reactions in soap-free emulsion systems. In this study, we synthesized grafted PMMA/PEI core-shell nanoparticles by varying the MMA/PEI content and molecular weight of PEI (Mn = 600, 8000, and 10,000). The size and morphology of the core-shell nanoparticles were characterized by a particle size analyzer and scanning electron microscopy. The nanoparticles were 178 - 408 nm in diameter and swelled in water or methanol by 30 - 75 nm. The size of the nanoparticles increased with MMA contents, whereas the size distribution progressively became homogeneous with increasing molecular weight of PEI. Lastly, we measured CO2 adsorption capacity of the grafted PMMA/PEI core-shell nanoparticles, and we found the capacity to be limited at a level of 0.69 mg, which occurred for nanoparticles prepared from emulsions at a pH value of 11.
基金This work was supported by the National Natural Science Foundation of China (Grant Nos. 41172110 and 61107090) and Shandong Provincial Natural Science Foundation (Grant No. ZR2011BZ007).
摘要Ag@Cu2O core-shell metal-semiconductor nanoparticles (NPs) were prepared by using solution phase strategy. The composites, structures, morphologies and absorption properties of Ag@Cu2O core-shell NPs were systematically characterized by X-ray diffraction (XRD) , transmission electron microscope (TEM) and ultraviolet-visible (UV-VIS) absorption spectra. The Ag@Cu2O core-shell metal-semiconductor NPs indicate tunable light absorption over the visible-light region. Under visible-near-infrared (VIS-NIR) light irradiation, up to 83.0% MO dye could be degraded after 150 min irradiation. The calculated apparent pseudo-first-order reaction rate constant is 0.0038 min-1. The high photocatalytic efficiency attributes to the decreasing recombination of photo-induced electrons and holes for the electron sink of Ag core, the better spectra overlap between the absorption spectra of Ag@Cu2O NPs and the emission spectra of the VIS-NIR lamp, and the good adsorption ability and rich catalytic active points for the poroused shell structure of Cu2O.
基金Financial support from the National Research Foundation of Korea(NRF)Grant funded by the Korean Government(MSIP)(Nos.NRF-2019R1A2C4069438 and NRF-2018R1A6A1A03025242)in part by the research grant of Kwangwoon University in 2021 is gratefully acknowledged。
摘要Along with a wide range of applications,the surface-enhanced Raman spectroscopy(SERS)is a promi-nent analytical technique to recognize and detect molecules and materials even at an extremely low mo-lar concentration.In this work,a unique hybrid SERS platform is demonstrated by the incorporation of molybdenum disulfate(MoS2)nanoparticles(NPs)onto the core-shell AuPt hybrid NPs(HNPs)for the en-hanced molecular Raman vibration of crystal violet(CV).The hybrid platform takes the advantage of both the electromagnetic mechanism(EM)offered by the AuPt HNPs and chemical mechanism(CM)owing to the MoS2NPs.The distinctive core-shell morphology of AuPt HNPs with the high-density background Au NPs is attained by a unique two-step solid-state dewetting method,which can offer a high concentration of electromagnetic hot spots.At the same time,the MoS2NPs can provide an ample charge transfer with abundant active sites.Through the hybrid SERS approach,a dramatic SERS enhancement of CV Raman vibration is demonstrated,and the SERS capability is thoroughly studied.In addition,the finite-difference time-domain(FDTD)simulations provide a deeper understanding of the electromagnetic field distributions for various configurations of nanostructures and their hybrid combinations:i.e.,HNPs,alloy NPs,MoS2/HNPs configurations.
基金supported by the Hi-Tech Research and Development Program of China(863,No2006AA03Z562)
摘要Functionalized PS/SiO:composite nanoparticles bearing sulfonic groups on the surface were successfully synthesized via emulsion copolymerization using a polymerizable emulsifier ar olefin solfonate(AOS).As demonstrated by transmission electron microscopy and atomic force microscopy,well-defined core-shel]PS/SiO:composite nanoparticles with a diameter of 50 nm were obtained.Sulfonic groups introduced onto the surface of the composite nanoparticles were quantified by FTIR.and can be controlled to some extent via a two-stage procedure.
基金support of the German Research Foundation (DFG) for supporting this work under grant number HE 7192/1-2support for the project ‘Electroscopy’ (Grant No. 892916) from the Marie Skłodowska-Curie action+1 种基金the Portuguese Foundation for Science and Technology (FCT) for the Ph D grant (SFRH/BD/128986/2017)supported by national funds through Fundação para a Ciência e a Tecnologia, I.P./MCTES: LSRE-LCM, UID/50020.
摘要CO2methanation offers a pathway to produce a carbon-neutral methane fuel.Although a number of research efforts have been conducted on this topic,a greater understanding of the mechanism of the reaction,which is still under debate,is needed.Here,using in situ transmission electron microscopy,we provide direct insights into the dynamics of a metallic nickel catalyst supported on activated carbon during CO2methanation.The keys to the high performance of the catalyst are the in situ formation and dynamic behavior of a Ni@NiO core@shell nanostructure.Based on the detailed electron microscopy investigation,the mechanism of such nanostructure formation during methanation is proposed.Our studies revealed that the deactivation of the catalyst is not due to the accumulation of carbon coke over nickel nanoparticles,but an increase in the size of the nickel nanoparticles that is responsible for the deactivation of the catalyst over time.
基金the financial support provided by the National Natural Science Foundation of China(No.21871164)the Taishan Scholar Project Foundation of Shandong Province(No.ts20190908)+2 种基金the Natural Science Foundation of Shandong Province(No.ZR2019MB024)the China Postdoctoral Science Foundation(No.2018M632666)the Special Fund for Postdoctoral Innovation Program of Shandong Province(No.201901003)。
摘要Multicomponent binary metal oxide-involved hybrid structures with unique physicochemical properties have received extensive attention due to their fascinating electrochemical performance.Herein,a flexible strategy,which involves the preparation of dual-functional heterometallic Fe2M clusters and their subsequent sintering treatment,is developed to engineer novel 3D hierarchical porous structures assembled with MFe2O4(M=Co,Mn,Ni and Zn)nanoparticles confined within carbon outer shell(denoted as MFe2O4@C HPSs).In this intriguing construction,it can be observed that MFe2O4@C HPSs comprised of carbon coated secondary MFe2O4nanoparticles with an interconnected carbon network.The as-prepared MFe2O4@C HPSs possess combined advantages of high capacity of MFe2O4and high conductivity of carbon.As expected,the MFe2O4@C HPSs offer a high reversible capacity,high cycling stability and superior rate performance.The interconnected conductive carbon shells facilitates fast ion and electron transport and accommodates the mechanical strain.In addition,nanosized MFe2O4particles,which shorten the ion-transport path and provide extra electroactive sites,also improve the reaction kinetics.Moreover,these MFe2O4@C HPSs exhibit good structural integrity during repeated charging and discharging.The research perspective and strategy reported here are highly versatile and shed new light on the synthesis of other advanced electrode for various applications.
基金supported by the National Natural Science Foundation of China(Grant Nos.52105427,U2037205,52005041,51575053,and 51775047)Research Foundation from Ministry of Education of China(Grant No.6141A02033123)+2 种基金Beijing Municipal Commission of Education(Grant No.KM201910005003)Knowledge Innovation Program of Wuhan-Basic Research(Grant No.2022010801010349)Scientific Research Project of Hubei Provincial Department of Education(Grant No.B2022055)。
摘要Molybdenum disulfide(MoS2)-based nanostructures are highly desirable for applications such as chemical and biological sensing,photo/electrochemical catalysis,and energy storage due to their unique physical and chemical properties.In this work,MoS2core-shell nanoparticles were first prepared through the liquid-phase processing of bulk MoS2by a femtosecond laser.The core of prepared nanoparticles was incompletely and weakly crystalline MoS2;the shell of prepared nanoparticles was highly crystalline MoS2,which wrapped around the core layer by layer.The femtosecond laser simultaneously achieved liquid-phase ablation and light exfoliation.The formation mechanism of the core-shell nanoparticles is to prepare the nanonuclei first by laser liquid-phase ablation and then the nanosheets by light exfoliation;the nanosheets will wrap the nanonuclei layer by layer through van der Waals forces to form core-shell nanoparticles.The MoS2core-shell nanoparticles,because of Mo-S bond breakage and recombination,have high chemical activity for chemical catalysis.Afterward,the nanoparticles were used as a reducing agent to directly prepare three-dimensional(3D)Au-MoS2microanostructures,which were applied as surface-enhanced Raman spectroscopy(SERS)substrates to explore chemical sensing activity.The ultrahigh enhancement factor(1.06×1011),ultralow detection limit(10-13M),and good SERS adaptability demonstrate highly sensitive SERS activity,great ability of ultralow concentration detection,and ability to detect diverse analytes,respectively.This work reveals the tremendous potential of 3D Au-MoS2composite structures as excellent SERS substrates for chemical and biological sensing.
基金Project supported by the National Natural Science Foundation of China (No. 2057040).
摘要A novel core-shell luminol-based SiO2 nanoparticle While these nanoparticles were used as electrogenerated was synthesized by two step micro-emulsion method. chemiluminescence (ECL) reagent, the electrochemical (EC) reaction as well as the subsequent chemiluminescence (CL) reaction not only could be separated spatially, but also presented high efficiency for analytical purpose. In this case, the core-shell luminol-based SiO2 nanoparticles offered more potential to avoid the contradiction between the EC and the CL reaction conditions. A new ECL method based on the nanoparticle was developed, and isoniazid was selected as a model analyte to illustrate the characteristics of this new ECL method. Under the selected conditions, the proposed ECL response to isoniazid concentration was linear in the range of 1.0 ×10^-10 to 1.0 × 10^-6 g/mL with 2 × 10^-11g/mL detection limit.
基金Supported by Production,Teaching&Research Combination Project for Universities in Guangdong Province(cgzhzd0904),Department of Education of Guangdong Province,China
摘要ZrO2/PMMA nanocomposite particles are synthesized through an in-situ free radical emulsion polymerization based on the silane coupling agent(Z-6030)modified ZrO2nanoparticles,and the morphology,size and its distribution of nanocomposite particles are investigated.Scanning electron microscopy(SEM)images demonstrate that the methyl methacrylate(MMA)feeding rate has a significant effect on the particle size and morphology.When the MMA feeding rate decreases from 0.42 ml-min-1 to 0.08 ml.min-1,large particles(about 200-550.nm)will not form,and the size distribution become narrow(36-54 nm).The average nanocomposite particles size increases from 34 nm to 55 nm,as the MMA/ZrO2 nanoparticles mass ratio increased from 4:1 to 16:1.Regular spherical ZrO2/PMMA nanocomposite particles are synthesized when the emulsifier OP-10 concentration is 2 mg.m1-1.The nanocomposite particles could be mixed with VAc-VeoVa10 polymer matrix just by magnetic stirring to prepare the ZrOE/PMMA/VAc-VeoVal0 hybrid coatings.SEM and atomic force microscopy(AFM)photos reveal that the distribution of the ZrO2/PMMA nanocomposite particles in the VAc-VeoVal0 polymer matrix is homogenous and stable.Here,the grafted-PMMA polymer on ZrO2 nanoparticles plays as a bridge which effectively connects the ZrO2 nanoparticles and the VAc-VeoVal0 polymer matrix with improved comparability.In consequence,the hybrid coating with good dispersion stability is obtained.
摘要Core-shell silica nanoparticles are superior in modifying surface wetting behavior,enhancing nucleation and growth in crystallization,improving dispersion of naked nanoparticles,and thus upgrading the overall properties of organic polymers.The dispersion behavior and morphology of monodisperse core-shell silica particles in several polymers including polyesters are reviewed and their potential applications are discussed.
基金supported by the National Natural Science Foundation of China(21161013)the Natural Science Foundation of Inner Mongolia(2011MS0202)the Opening Foundation for Significant Fundamental Research of Inner Mongolia(2010KF03)
摘要Six kinds of terbium ternary complexes with halo-benzoic acids were synthesized. Their compositions were determined by C, H elemental analyzer and EDTA titration. The infrared spectra, ultraviolet absorption spectra, and fluorescence spectra were also measured to identify the complexes. Elemental analysis showed that the compositions of these complexes were Tb(p-BrBA)3- H20, Tb(p-CIBA)3- 2H20, Tb(p-FBA)3- H20, Tb(o-FBA)3·2H20, Tb(o-CIBA)3· H20, and Tb(o-BrBA)3. H20, respectively. The monodispersed Ag@SiO2 core-shell nanoparticles with silica thicknesses of 10, 15, and 25 nm were success- fully prepared and characterized by transmission-electron microscopy. Fluorescence intensities of the complexes were detected before and after Ag@SiO2core-shell nanoparticles were added; the enhancement times were related to the silica-shell thick- ness. The fluorescence enhancement times were largest when the thickness of the silica shell was 25 nm. The mechanism may be attributed to the localized surface-plasmon resonance. Furthermore, the enhancement effect of terbium fluoro-benzoate complexes was the strongest in these complexes. This result may be attributed to the hydrogen bond between the hydroxyl on the surface of the silica shell and the fluorine atom.
基金supported by the National Natural Science Foundation of China(NSFC,Nos.21671170,21673203)the Topnotch Academic Programs Project of Jiangsu Higher Education Institutions(TAPP)+2 种基金Program for New Century Excellent Talents of the University in China(NCET,No.13-0645)the Six Talent Plan(No.2015-XCL-030)Qinglan Project。
摘要The construction of highly stable and regular nanoreactors is a major challenge.In this work,we use a facile template protection method to obtain ZIF-67@SiO2(JS)and to encapsulate metal oxide nanoparticles(Co3O4)into nanoreactors(SiO2).ZIF-67 crystals provide a cobalt species;SiO2was first used as a protective layer of ZIF-67 and then as a nanoreactor for metastable metal oxide nanoparticles.On this basis,Co3O4@SiO2with dodecahedron morphology were synthesized by calcining JS at different tempe ratures,followed by a hydrothermal reaction to obtain Co3(OH)4Si2O5.Subsequently,CoSx and CoP-SiO2were fabricated through sulfuration and phosphorization.The results in this work show that nanoreactors derived from metal-organic frameworks(MOFs)with a rational structure have broad development prospects.
基金This work was supported by the National Key Research and Development Program of China(No.2018YFE0201701)the National Natural Science Foundation of China(Nos.21975050,21905052,11975081,and 22105041)+3 种基金Science and Technology Commission of Shanghai Municipality(No.21ZR1408800)Key Basic Research Program of Science and Technology Commission of Shanghai Municipality(No.19JC1410700)the Program of Shanghai Academic Research Leader(No.21XD1420800)Guangdong Basic and Applied Basic Research Foundation(No.2021A1515010108).
摘要Regulating the surface plasmon resonance(SPR)of metallic nanostructures is of great interests for optical and catalytic applications,however,it is still a great challenge for tuning SPR features of small metallic nanoparticles(<10 nm).In this work,we design a unique dielectric support-urchin-like mesoporous silica nanoparticles(U-SiO2)with ordered long spikes on its surface,which can well enhance the SPR properties of~3 nm gold nanocrystals(AuNCs).The U-SiO2not only realizes the uniform self-assembly of AuNCs,but also prevents their aggregation due to the unique confinement effect.The finite-difference time-domain simulations show that the AuNCs on U-SiO2can generate plasmonic hot spots with highly enhanced electromagnetic field.Moreover,the hot electrons can be effectively and rapidly transferred through the interface junction to TiO2.Thus,a high visible-light-driven photocatalytic activity can be observed,which is 3.8 times higher than that of smooth photocatalysts.The concept of dielectric supports engineering provides a new strategy for tuning SPR of small metallic nanocrystals towards the development of advanced plasmon-based applications.