TiO_(2)is the dominant and most widely researched photocatalyst for environmental remediation,however,the drawbacks,such as only responding to UV light(<5%of sunlight),low charge separation efficiency,and difficult...TiO_(2)is the dominant and most widely researched photocatalyst for environmental remediation,however,the drawbacks,such as only responding to UV light(<5%of sunlight),low charge separation efficiency,and difficulties in recycling,have severely hindered its practical application.Herein,we synthesized magnetically separable Fe_(3)O_(4)@MoS_(2)@mesoporous TiO_(2)(FMmT)photocatalysts via a simple,green,and template-free solvothermal method combined with ultrasonic hydrolysis.It is found that FMmT possesses a high specific surface area(55.09 m2·g−1),enhanced visible-light responsiveness(~521 nm),and remarkable photogenerated charge separation efficiency.In addition,the photocatalytic degradation efficiencies of FMmT for methylene blue(MB),rhodamine B(RhB),and tetracycline(TC)are 99.4%,98.5%,and 89.3%within 300 min,respectively.The corresponding degradation rates are 4.5,4.3,and 3.1 times higher than those of pure TiO_(2)separately.Owing to the high saturation magnetization(43.1 A·m^(2)·kg^(−1)),FMmT can achieve effective recycling with an applied magnetic field.The improved photocatalytic activity is closely related to the effective transport of photogenerated electrons by the active interlayer MoS_(2) and the electron–hole separation caused by the MoS_(2)@TiO_(2)heterojunction.Meanwhile,the excellent light-harvesting ability and abundant reactive sites of the mesoporous TiO_(2)shell further boost the photocatalytic efficiency of FMmT.This work provides a new approach and some experimental basis for the design and performance improvement of magnetic photocatalysts by innovatively incorporating MoS2 as the active interlayer and integrating it with a mesoporous shell.展开更多
Developing metal-organic framework(MOF)materials with the moisture-resistant feature is highly desirable for CO_(2)capture from highly humid flue gas.In this work,a new core-shell MOF@MOF composite using Mg-MOF-74 wit...Developing metal-organic framework(MOF)materials with the moisture-resistant feature is highly desirable for CO_(2)capture from highly humid flue gas.In this work,a new core-shell MOF@MOF composite using Mg-MOF-74 with high CO_(2)capture capacity as a functional core and hydrophobic zeolitic imidazolate framework-8(ZIF-8)as a protective shell is fabricated by the epitaxial growth method.Experimental results show that the CO_(2)adsorption performance of the core-shell structured Mg-MOF-74@ZIF-8 composites from water-containing flue gas is enhanced along with their improved hydrophobicity.The dynamic breakthrough results show that the Mg-MOF-74@ZIF-8 with three assembled layers(Mg-MOF-74@ZIF-8-3)can capture 3.56 mmol-g^(-1)CO_(2)from wet CO_(2)/N_(2)(VCO_(2):V_(N_(2))=15:85)mixtures,which outperforms Mg-MOF-74(0.37 mmol·g^(-1))and most of the reported physisorbents.展开更多
To achieve efficient photocatalytic H_(2) generation from water using earth-abundant and cost-effective materials,a simple synthesis method for carbon-doped CdS particles wrapped with graphene(C-doped CdS@G)is reporte...To achieve efficient photocatalytic H_(2) generation from water using earth-abundant and cost-effective materials,a simple synthesis method for carbon-doped CdS particles wrapped with graphene(C-doped CdS@G)is reported.The doping effect and the application of graphene as cocatalyst for CdS is studied for photocatalytic H_(2) generation.The most active sample consists of CdS and graphene(CdS-0.15G)exhibits promising photocatalytic activity,producing 3.12 mmol g^-(1) h^-(1) of H_(2) under simulated solar light which is^4.6 times superior than pure CdS nanoparticles giving an apparent quantum efficiency(AQY)of 11.7%.The enhanced photocatalytic activity for H_(2) generation is associated to the narrowing of the bandgap,enhanced light absorption,fast interfacial charge transfer,and higher carrier density(N_(D))in C-doped CdS@G samples.This is achieved by C doping in CdS nanoparticles and the formation of a graphene shell over the C-doped CdS nanoparticles.After stability test,the spent catalysts sample was also characterized to investigate the nanostructure.展开更多
PS/SiO2 particles with core-shell structure were synthesized by coating silica on surface of polystyrene(PS) colloidal particles.The reaction parameters,such as initial tetraethyl orthosilicate(TEOS) concentration,wat...PS/SiO2 particles with core-shell structure were synthesized by coating silica on surface of polystyrene(PS) colloidal particles.The reaction parameters,such as initial tetraethyl orthosilicate(TEOS) concentration,water concentration and reaction temperature,have been investigated to control the thickness of silica shells.The shell thickness was prepositional to the square root of the initial concentration of TEOS and first increased with increasing water concentration,reached a maximum at about 2.0 mol/L and then started decreasing beyond that concentration.It was also found that the shell thickness decreased firstly with the reaction temperature added,then tended to a constant.The so-synthesized PS/SiO2 core-shell particles were directly crystallized into 3-D ordered thin film,then sintered at 570℃ into the ordered macroporous thin film.Compared with the conditional method,the present approach avoids repeatedly filling the precursor in the templetes and save time more.展开更多
A facile method for preparing monodisperse NaYF4@SiO2@Au core-shell nanocomposite was developed. Transmission electron microscopy(TEM) as well as EDX(energy dispersive X-ray) was used to characterize the samples. The ...A facile method for preparing monodisperse NaYF4@SiO2@Au core-shell nanocomposite was developed. Transmission electron microscopy(TEM) as well as EDX(energy dispersive X-ray) was used to characterize the samples. The TEM showed the composite was a core-shell structure, spherical,with the uniform size of about 100 nm. TEM and EDX revealed that the NPs were coated with a layer of SiO2 and Au shell. The core shell structure of NaYF4@SiO2@Au nanocomposite could dispersed in water easily. More importantly,after being coated with SiO2 and Au, it was feasible for function by-SH and-NH2 groups, respectively. The forming process of the Au shell was monitored with TEM. The mechanism of coating Au shell was discussed in detail. It is expected that the core shell nanoparticle will act as multifunctional molecular imaging probes, such as positron emission tomography(PET), magnetic resonance imaging(MRI), optical imaging(OI), or contrast agent for sensing and detection.展开更多
The vertically aligned one-dimensional(1 D)core-shell structure can maximize the exposure and use of the functionally active surface while maintaining the geometric effects caused by the underlying structure.Herein,we...The vertically aligned one-dimensional(1 D)core-shell structure can maximize the exposure and use of the functionally active surface while maintaining the geometric effects caused by the underlying structure.Herein,we have fabricated 1 D vertically aligned ZnO/V2O5 core-shell hetero-nanostructure nanorod arrays(NRs)for photoelectrochemical(PEC)water splitting.ZnO/V2O5 NRs were prepared through the hydrothermal growing of ZnO NRs and then radio frequency(RF)magnetron sputtering deposition of V2O5 for 300,600 and 900 s.The photocurrent density of ZnO/V2O5-based photoanodes was gradually increased with the sputtering time,reaching the maximum value of 1.21 m A/cm^2 at 1.23 V vs.reversible hydrogen electrode(RHE)for ZnO/V2O5-600,whereas for pure ZnO-based photoanode was 0.42 mA/cm^2.The incident photon to electron conversion efficiency(IPCE)of ZnO/V2O5-600 evaluated to be 82.3%which was 2.3 times higher than that of ZnO(36.4%).The improved PEC performance of ZnO/V2O5-600 is because the core-shell structure with a moderate thickness of the V2O5 layer has the extremely high carrier density,largest electrochemically active surface area(ECSA),largest carrier density,lowest charge recombination rate,and the longest lifetime of e-h pairs due to the formation of the staggered gap junction.This study provides an effective way to design and fabrication of hetero-nanostructures for highefficiency photoelectrodes.展开更多
Ru@RuO2 core-shell nanorods were successfully synthesized by heat-treating Ru nanorods with air oxidation through an accurate control of the temperature and time. The structure, composition, dimension, and adsorption ...Ru@RuO2 core-shell nanorods were successfully synthesized by heat-treating Ru nanorods with air oxidation through an accurate control of the temperature and time. The structure, composition, dimension, and adsorption property of the core-shell nanorods were well characterized with XRD and TEM. The catalytic activity and stability were electrochemically evaluated with a rotating disk electrode, a rotating ring-disk electrode, and chronopotentiometric methods. The Ru@RuO2 nanorods reveal excellent bifunctional catalytic activity and robust stability for both oxygen evolution reaction(OER) and hydrogen evolution reaction(HER). The overpotentials for OER and HER are 320 m V and 137 m V at the current density of10 m A cm-2, respectively. The catalytic activity of Ru@RuO2 nanorods for OER is 6.5 times higher than that of the state-of-the-art catalyst IrO2 according to the catalytic current density measured at 1.60 V(versus RHE).The catalytic activity of Ru@RuO2 nanorods for HER is comparable to 40%Pt/C by comparing the catalytic current densities at à0.2 V.展开更多
Inactive elemental doping is commonly used to improve the structural stability of high-voltage layered transition-metal oxide cathodes.However,the one-step co-doping strategy usually results in small grain size since ...Inactive elemental doping is commonly used to improve the structural stability of high-voltage layered transition-metal oxide cathodes.However,the one-step co-doping strategy usually results in small grain size since the low diffusivity ions such as Ti^(4+)will be concentrated on grain boundaries,which hinders the grain growth.In order to synthesize large single-crystal layered oxide cathodes,considering the different diffusivities of different dopant ions,we propose a simple two-step multi-element co-doping strategy to fabricate core–shell structured LiCoO_(2)(CS-LCO).In the current work,the high-diffusivity Al^(3+)/Mg^(2+)ions occupy the core of single-crystal grain while the low diffusivity Ti^(4+)ions enrich the shell layer.The Ti^(4+)-enriched shell layer(~12 nm)with Co/Ti substitution and stronger Ti–O bond gives rise to less oxygen ligand holes.In-situ XRD demonstrates the constrained contraction of c-axis lattice parameter and mitigated structural distortion.Under a high upper cut-off voltage of 4.6 V,the single-crystal CS-LCO maintains a reversible capacity of 159.8 mAh g^(−1)with a good retention of~89%after 300 cycles,and reaches a high specific capacity of 163.8 mAh g^(−1)at 5C.The proposed strategy can be extended to other pairs of low-(Zr^(4+),Ta^(5+),and W6+,etc.)and high-diffusivity cations(Zn^(2+),Ni^(2+),and Fe^(3+),etc.)for rational design of advanced layered oxide core–shell structured cathodes for lithium-ion batteries.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 (M<sub>n</sub> = 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 CO<sub>2</sub> 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
Photodegradation has emerged as an environmentally friendly method of decomposing harmful dyes in wastewater. In this study, core-shell Fe3O4/SiO2/ TiO2 nanospheres with magnetic cores were obtained from synthesised m...Photodegradation has emerged as an environmentally friendly method of decomposing harmful dyes in wastewater. In this study, core-shell Fe3O4/SiO2/ TiO2 nanospheres with magnetic cores were obtained from synthesised magnetic Fe3O4 nanoparticles through the precipitation method, the surface of the magnetic Fe3O4 nanoparticles was coated with a silica (SiO2) layer by hydrolysis of tetramethoxysilane (TMOS) as a silica source, and finally, Fe3O4/SiO2 nanospheres were coated with titanium (TiO2) layer using tetrabutyltitanate (TBT) as a precursor through the sol-gel process. The morphology and structure of the prepared materials were characterised by X-ray diffraction (XRD) analysis, scanning electron microscopy (SEM), X-ray energy dispersive spectrometry (EDAX), Fourier transform infrared spectroscopy (FT-IR), and atomic force microscopy (AFM). The photocatalytic activities of the prepared core-shell nanospheres were studied using binary azo dyes, namely methyl orange (anionic dye, MO) and methylene blue (cationic dye, MB) in aqueous solution under UV light irradiation (365 nm), and UV-Vis spectrophotometer was utilised to monitor the amount of each dye in the mixture. It was found that 90.2% and 100% of binary MO and MB were removed for 5 h, respectively. The results revealed that the efficiency of the photocatalytic degradation of the core-shell nanospheres was not degreased after five runs that can be used as recyclable photocatalysts. The results show that the performance of the prepared core-shell nanospheres was better than that of commercial TiO2 nanoparticles. Moreover, the magnetic separation properties of the core-shell Fe3O4/SiO2/TiO2 nanospheres can enable the prepared materials to have wider application prospects.展开更多
Graphene has been extensively utilized in the domain of electromagnetic wave(EMW)absorption ma-terials because of its excellent electrical conductivity.However,the inferior impedance matching per-formance and the sing...Graphene has been extensively utilized in the domain of electromagnetic wave(EMW)absorption ma-terials because of its excellent electrical conductivity.However,the inferior impedance matching per-formance and the single loss mechanism vastly restrict the application.Hence,it’s an effective strat-egy to solve these issues by introducing magnetic components.Notably,layer double hydroxide(LDH)is an appropriate template to obtain magnetic component materials.Considering that ferromagnetic met-als such as Fe,Co,Ni,and their corresponding metal oxides are usually treated as magnetic compo-nents which are promising candidates for EMW absorption materials.Therefore,in this work,a FeNi-layered double hydroxide-reduced graphene oxide(FeNi-LDH-rGO)aerogel was synthesized through a series of processes such as electrostatic self-assembly,hydrothermal,freeze-drying,and annealing.The magnetic NiFe_(2)O_(4)@FeNi_(3)core-shell nanospheres were obtained from FeNi-LDH precursor,anchoring on rGO nanosheets after the annealing treatment.Furthermore,the effects of different mass ratios of LDH to GO as well as different annealing temperatures of LDH-rGO aerogel on the EMW absorption prop-erty and impedance matching performance were explored.As a consequence,the fabricated ultralight 600LDH-rGO 2:1 aerogel shows a broad effective absorption bandwidth(EAB)of 7.04 GHz at a thickness of 2.3 mm with a low filling content of only 6 wt%and a low density of 4.4 mg/cm^(3).In conclusion,the synthetic LDH-rGO aerogels offer an effective strategy for preparing EMW absorption materials that own three-dimensional porous network structure and unique magnetic NiFe_(2)O_(4)@FeNi_(3)core-shell struc-ture nanospheres.展开更多
Manganese-based cathode materials are considered as a promising candidate for rechargeable aqueous zinc-ion batteries(ZIBs).Suffering from poor conductive and limited structure tolerance,various carbon matrix,especial...Manganese-based cathode materials are considered as a promising candidate for rechargeable aqueous zinc-ion batteries(ZIBs).Suffering from poor conductive and limited structure tolerance,various carbon matrix,especially N-doped carbon,were employed to incorporate with MnO_(2)for greatly promoted electrochemical performances.However,the related underlying mechanism is still unknown,which is unfavorable to guide the design of high performance electrode.Herein,by incorporating layered MnO_(2)with N-doped carbon nanowires,a free-standing cathode with hierarchical core-shell structure(denoted as MnO_(2)@NC)is prepared.Benefiting from the N-doped carbon and rational architecture,the MnO_(2)@NC electrode shows an enhanced specific capacity(325 mAh g^(−1)at 0.1 A g^(−1))and rate performance(90 mAh g^(−1)at 2 A g^(−1)),as well as improved cycling stability.Furthermore,the performance improvement mechanism of MnO_(2)incorporated by N-doped carbon is investigated by X-ray photoelectron spectroscopy(XPS),Raman spectrums and density functional theory(DFT)calculation.The N atom elongates the Mn-O bond and reduces the valence of Mn^(4+)ion in MnO_(2)crystal by delocalizing its electron clouds.Thus,the electrostatic repulsion will be weakened when Zn^(2+)/H^(+)insert into the host MnO_(2)lattices,which is profitable to more cation insertion and faster ion transfer kinetics for higher capacity and rate capability.This work elucidates a fundamental understanding of the functions of N-doped carbon in composite materials and shed light on a practical pathway to optimize other electrode materials.展开更多
Semiconductor-based photocatalysts have been extensively studied for oxidative photodestruction of organic pollutants in wastewaters, releasing non-toxic substances such as Azo dyes. Various synthesized catalyst speci...Semiconductor-based photocatalysts have been extensively studied for oxidative photodestruction of organic pollutants in wastewaters, releasing non-toxic substances such as Azo dyes. Various synthesized catalyst specimens were characterized to determine the correlation between preparation conditions (catalyst type, dopant, microstructure, preparation routs, optical and physico-chemical properties) on the photocatalytic activity. Some researchers focused on the process parameters to optimize them to reach higher photoactivity. The specific surface areas, crystalline size, charge and pretreatment of the surface have significant effects on the physical and photocatalytic properties of the semiconductors. The surface sites of catalyst (TiO2) were modified by doping ZnS nanoparticles in the form of Core-Shell structure and the photocatalytic activities were determined by using color degradation and hydrogen production tests. The dye adsorption isotherms of photocatalyst were determined using UV-Vis spectroscopy. The specific surface properties were determined from BET, Zeta meter and Particle size analyzer tests. Photocatalytic decolorization of AR and water splitting test were applied to understand the relation between the surface properties and the photocatalytic activity. The result indicated that core-shell prepared samples had different surface suitable sites to cooperate in photocatalytic reaction.展开更多
Copper(Cu)-based materials are known as the most attractive catalysts for electrochemical carbon dioxide reduction reaction(CO_(2)RR),especially the Cu^(+) species(e.g.,Cu_(2)O),which show excellent capability for cat...Copper(Cu)-based materials are known as the most attractive catalysts for electrochemical carbon dioxide reduction reaction(CO_(2)RR),especially the Cu^(+) species(e.g.,Cu_(2)O),which show excellent capability for catalyzing CO_(2) to C_(2+) chemicals because of their unique electronic structure.However,the active Cu^(+) species are prone to be reduced to metallic Cu under an electroreduction environment,thus resulting in fast deactivation and poor selectivity.Here,we developed an advanced surface modification strategy to maintain the active Cu^(+) species via assembling a protective layer of metal-organic framework(copper benzenetricarboxylate,CuBTC) on the surface of Cu_(2)O octahedron(Cu_(2)O@CuBTC).It's encouraging to see that the Cu_(2)O@CuBTC heterostructure outperforms the bare Cu_(2)O octahedron in catalyzing CO_(2) to C_(2+) chemicals and dramatically enhances the ratio of C_(2)H_(4)/CH_(4) products.A systematic study reveals that the introduced CuBTC shell plays a critical role in maintaining the active Cu^(+) species in Cu_(2)O@CuBTC heterostructure under reductive conditions.This work offers a practical strategy for improving the catalytic performance of CO_(2)RR over copper oxides and also establishes a route to maintain the state of valence-sensitive catalysts.展开更多
The nano-iron nitride soft magnetic material has excellent magnetic properties and is expected to be a brilliant electromagnetic wave absorber.However,how to fully exploit its wave-absorbing potential re-mains a thoug...The nano-iron nitride soft magnetic material has excellent magnetic properties and is expected to be a brilliant electromagnetic wave absorber.However,how to fully exploit its wave-absorbing potential re-mains a thought-provoking question.Here,we have synthesized Fe/Fe_(4)N@SiO_(2)nanomagnetic core-shell materials with different Fe/Fe_(4)N ratios by performing nitridation reactions at different temperatures.Then,the flower-like core-shell Fe/Fe_(4)N@SiO_(2)structure was obtained by the etching method.Finally,with the synergy of the excellent magnetic and dielectric losses,an outstanding absorption performance could be achieved with a minimum refection loss(RL min)of−71.31 dB at the matching thickness of 1.4 mm,and the widest effective absorption bandwidth(EAB max)of 6.1 GHz less than−10 dB was realized at 1.16 mm.Moreover,this material also shows a preeminent advance in corrosion resistance to adapt to harsh environments.Hence,this iron nitride flower-like core-shell structure exhibits great potential in microwave absorption in harsh conditions.展开更多
基金financially supported by the National Key R & D Projects (Nos. 2021YFC1910504, 2019YFC1907101, 2019YFC1907103, and 2017YFB0702304)the Key R & D Project in Ningxia Hui Autonomous Region, China (No. 2020BCE01001)+6 种基金the Key and Normal Projects National Natural Science Foundation of China (Nos. U2002212 and 51672024)the Xijiang Innovation and Entrepreneurship Team (No. 2017A0109004)the Fundamental Research Funds for the Central Universities (Nos. FRF-BD-20-24A, FRF-TP-20-031A1, FRF-IC-19-017Z, FRF-GF-19-032B, and 06500141)the Integration of Green Key Process Systems MIIT, Natural Science Foundation of Beijing Municipality (No. 2214073)the Guangdong Basic and Applied Research Foundation, China (No. 2020A1515110408)the Foshan Science and Technology Innovation Special Foundation, China (No. BK21BE002)the Postdoctor Research Foundation of Shunde Graduate School of University of Science and Technology Beijing (No. 2020BH004)
文摘TiO_(2)is the dominant and most widely researched photocatalyst for environmental remediation,however,the drawbacks,such as only responding to UV light(<5%of sunlight),low charge separation efficiency,and difficulties in recycling,have severely hindered its practical application.Herein,we synthesized magnetically separable Fe_(3)O_(4)@MoS_(2)@mesoporous TiO_(2)(FMmT)photocatalysts via a simple,green,and template-free solvothermal method combined with ultrasonic hydrolysis.It is found that FMmT possesses a high specific surface area(55.09 m2·g−1),enhanced visible-light responsiveness(~521 nm),and remarkable photogenerated charge separation efficiency.In addition,the photocatalytic degradation efficiencies of FMmT for methylene blue(MB),rhodamine B(RhB),and tetracycline(TC)are 99.4%,98.5%,and 89.3%within 300 min,respectively.The corresponding degradation rates are 4.5,4.3,and 3.1 times higher than those of pure TiO_(2)separately.Owing to the high saturation magnetization(43.1 A·m^(2)·kg^(−1)),FMmT can achieve effective recycling with an applied magnetic field.The improved photocatalytic activity is closely related to the effective transport of photogenerated electrons by the active interlayer MoS_(2) and the electron–hole separation caused by the MoS_(2)@TiO_(2)heterojunction.Meanwhile,the excellent light-harvesting ability and abundant reactive sites of the mesoporous TiO_(2)shell further boost the photocatalytic efficiency of FMmT.This work provides a new approach and some experimental basis for the design and performance improvement of magnetic photocatalysts by innovatively incorporating MoS2 as the active interlayer and integrating it with a mesoporous shell.
基金supported by the National Natural Science Foundation of China(51772329,51972340,and 51825201)。
文摘Developing metal-organic framework(MOF)materials with the moisture-resistant feature is highly desirable for CO_(2)capture from highly humid flue gas.In this work,a new core-shell MOF@MOF composite using Mg-MOF-74 with high CO_(2)capture capacity as a functional core and hydrophobic zeolitic imidazolate framework-8(ZIF-8)as a protective shell is fabricated by the epitaxial growth method.Experimental results show that the CO_(2)adsorption performance of the core-shell structured Mg-MOF-74@ZIF-8 composites from water-containing flue gas is enhanced along with their improved hydrophobicity.The dynamic breakthrough results show that the Mg-MOF-74@ZIF-8 with three assembled layers(Mg-MOF-74@ZIF-8-3)can capture 3.56 mmol-g^(-1)CO_(2)from wet CO_(2)/N_(2)(VCO_(2):V_(N_(2))=15:85)mixtures,which outperforms Mg-MOF-74(0.37 mmol·g^(-1))and most of the reported physisorbents.
基金support from the Research Council of Norway provided by the Norwegian Center for Transmission Electron Microscopy,NORTEM(197405/F50)NTNU NanoLab(grant number 245963)which have provided the characterization toolsthe strategic funding support provided by Department of Chemical Engineering,NTNU,Trondheim,Norway.
文摘To achieve efficient photocatalytic H_(2) generation from water using earth-abundant and cost-effective materials,a simple synthesis method for carbon-doped CdS particles wrapped with graphene(C-doped CdS@G)is reported.The doping effect and the application of graphene as cocatalyst for CdS is studied for photocatalytic H_(2) generation.The most active sample consists of CdS and graphene(CdS-0.15G)exhibits promising photocatalytic activity,producing 3.12 mmol g^-(1) h^-(1) of H_(2) under simulated solar light which is^4.6 times superior than pure CdS nanoparticles giving an apparent quantum efficiency(AQY)of 11.7%.The enhanced photocatalytic activity for H_(2) generation is associated to the narrowing of the bandgap,enhanced light absorption,fast interfacial charge transfer,and higher carrier density(N_(D))in C-doped CdS@G samples.This is achieved by C doping in CdS nanoparticles and the formation of a graphene shell over the C-doped CdS nanoparticles.After stability test,the spent catalysts sample was also characterized to investigate the nanostructure.
基金Supported by the National Natural Science Foundation of China(No.:20221603)
文摘PS/SiO2 particles with core-shell structure were synthesized by coating silica on surface of polystyrene(PS) colloidal particles.The reaction parameters,such as initial tetraethyl orthosilicate(TEOS) concentration,water concentration and reaction temperature,have been investigated to control the thickness of silica shells.The shell thickness was prepositional to the square root of the initial concentration of TEOS and first increased with increasing water concentration,reached a maximum at about 2.0 mol/L and then started decreasing beyond that concentration.It was also found that the shell thickness decreased firstly with the reaction temperature added,then tended to a constant.The so-synthesized PS/SiO2 core-shell particles were directly crystallized into 3-D ordered thin film,then sintered at 570℃ into the ordered macroporous thin film.Compared with the conditional method,the present approach avoids repeatedly filling the precursor in the templetes and save time more.
基金Funded by the Natural Science Foundation of Shaanxi Province(No.2018JQ2057)the Ph D Research Foundation Project of Shaanxi University of Technology(No.209020195)the Scientific Research Program of Shaanxi Provincial Education Department(No.17JK0151)
文摘A facile method for preparing monodisperse NaYF4@SiO2@Au core-shell nanocomposite was developed. Transmission electron microscopy(TEM) as well as EDX(energy dispersive X-ray) was used to characterize the samples. The TEM showed the composite was a core-shell structure, spherical,with the uniform size of about 100 nm. TEM and EDX revealed that the NPs were coated with a layer of SiO2 and Au shell. The core shell structure of NaYF4@SiO2@Au nanocomposite could dispersed in water easily. More importantly,after being coated with SiO2 and Au, it was feasible for function by-SH and-NH2 groups, respectively. The forming process of the Au shell was monitored with TEM. The mechanism of coating Au shell was discussed in detail. It is expected that the core shell nanoparticle will act as multifunctional molecular imaging probes, such as positron emission tomography(PET), magnetic resonance imaging(MRI), optical imaging(OI), or contrast agent for sensing and detection.
基金supported by National Research Foundation(NRF)of Korean grant funded by the Korea government(MSIP)(Grant number:2017R1E1A1A01074550)。
文摘The vertically aligned one-dimensional(1 D)core-shell structure can maximize the exposure and use of the functionally active surface while maintaining the geometric effects caused by the underlying structure.Herein,we have fabricated 1 D vertically aligned ZnO/V2O5 core-shell hetero-nanostructure nanorod arrays(NRs)for photoelectrochemical(PEC)water splitting.ZnO/V2O5 NRs were prepared through the hydrothermal growing of ZnO NRs and then radio frequency(RF)magnetron sputtering deposition of V2O5 for 300,600 and 900 s.The photocurrent density of ZnO/V2O5-based photoanodes was gradually increased with the sputtering time,reaching the maximum value of 1.21 m A/cm^2 at 1.23 V vs.reversible hydrogen electrode(RHE)for ZnO/V2O5-600,whereas for pure ZnO-based photoanode was 0.42 mA/cm^2.The incident photon to electron conversion efficiency(IPCE)of ZnO/V2O5-600 evaluated to be 82.3%which was 2.3 times higher than that of ZnO(36.4%).The improved PEC performance of ZnO/V2O5-600 is because the core-shell structure with a moderate thickness of the V2O5 layer has the extremely high carrier density,largest electrochemically active surface area(ECSA),largest carrier density,lowest charge recombination rate,and the longest lifetime of e-h pairs due to the formation of the staggered gap junction.This study provides an effective way to design and fabrication of hetero-nanostructures for highefficiency photoelectrodes.
基金the U.S.Department of the ArmyU.S.Army Materiel Command for supporting this work
文摘Ru@RuO2 core-shell nanorods were successfully synthesized by heat-treating Ru nanorods with air oxidation through an accurate control of the temperature and time. The structure, composition, dimension, and adsorption property of the core-shell nanorods were well characterized with XRD and TEM. The catalytic activity and stability were electrochemically evaluated with a rotating disk electrode, a rotating ring-disk electrode, and chronopotentiometric methods. The Ru@RuO2 nanorods reveal excellent bifunctional catalytic activity and robust stability for both oxygen evolution reaction(OER) and hydrogen evolution reaction(HER). The overpotentials for OER and HER are 320 m V and 137 m V at the current density of10 m A cm-2, respectively. The catalytic activity of Ru@RuO2 nanorods for OER is 6.5 times higher than that of the state-of-the-art catalyst IrO2 according to the catalytic current density measured at 1.60 V(versus RHE).The catalytic activity of Ru@RuO2 nanorods for HER is comparable to 40%Pt/C by comparing the catalytic current densities at à0.2 V.
基金the Hong Kong Polytechnic University(Q-CDBG),the Science and Technology Program of Guangdong Province of China(2020A0505090001)the Research Grants Council of the Hong Kong Special Administrative Region,China(Project No.PolyU152178/20E)+2 种基金the National Natural Science Foundation of China(22379052)the Natural Science Foundation of Guangdong(No.2022A1515011667)China Postdoctoral Science Foundation(2021T140268).
文摘Inactive elemental doping is commonly used to improve the structural stability of high-voltage layered transition-metal oxide cathodes.However,the one-step co-doping strategy usually results in small grain size since the low diffusivity ions such as Ti^(4+)will be concentrated on grain boundaries,which hinders the grain growth.In order to synthesize large single-crystal layered oxide cathodes,considering the different diffusivities of different dopant ions,we propose a simple two-step multi-element co-doping strategy to fabricate core–shell structured LiCoO_(2)(CS-LCO).In the current work,the high-diffusivity Al^(3+)/Mg^(2+)ions occupy the core of single-crystal grain while the low diffusivity Ti^(4+)ions enrich the shell layer.The Ti^(4+)-enriched shell layer(~12 nm)with Co/Ti substitution and stronger Ti–O bond gives rise to less oxygen ligand holes.In-situ XRD demonstrates the constrained contraction of c-axis lattice parameter and mitigated structural distortion.Under a high upper cut-off voltage of 4.6 V,the single-crystal CS-LCO maintains a reversible capacity of 159.8 mAh g^(−1)with a good retention of~89%after 300 cycles,and reaches a high specific capacity of 163.8 mAh g^(−1)at 5C.The proposed strategy can be extended to other pairs of low-(Zr^(4+),Ta^(5+),and W6+,etc.)and high-diffusivity cations(Zn^(2+),Ni^(2+),and Fe^(3+),etc.)for rational design of advanced layered oxide core–shell structured cathodes for lithium-ion batteries.
文摘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 (M<sub>n</sub> = 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 CO<sub>2</sub> 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.
文摘Photodegradation has emerged as an environmentally friendly method of decomposing harmful dyes in wastewater. In this study, core-shell Fe3O4/SiO2/ TiO2 nanospheres with magnetic cores were obtained from synthesised magnetic Fe3O4 nanoparticles through the precipitation method, the surface of the magnetic Fe3O4 nanoparticles was coated with a silica (SiO2) layer by hydrolysis of tetramethoxysilane (TMOS) as a silica source, and finally, Fe3O4/SiO2 nanospheres were coated with titanium (TiO2) layer using tetrabutyltitanate (TBT) as a precursor through the sol-gel process. The morphology and structure of the prepared materials were characterised by X-ray diffraction (XRD) analysis, scanning electron microscopy (SEM), X-ray energy dispersive spectrometry (EDAX), Fourier transform infrared spectroscopy (FT-IR), and atomic force microscopy (AFM). The photocatalytic activities of the prepared core-shell nanospheres were studied using binary azo dyes, namely methyl orange (anionic dye, MO) and methylene blue (cationic dye, MB) in aqueous solution under UV light irradiation (365 nm), and UV-Vis spectrophotometer was utilised to monitor the amount of each dye in the mixture. It was found that 90.2% and 100% of binary MO and MB were removed for 5 h, respectively. The results revealed that the efficiency of the photocatalytic degradation of the core-shell nanospheres was not degreased after five runs that can be used as recyclable photocatalysts. The results show that the performance of the prepared core-shell nanospheres was better than that of commercial TiO2 nanoparticles. Moreover, the magnetic separation properties of the core-shell Fe3O4/SiO2/TiO2 nanospheres can enable the prepared materials to have wider application prospects.
文摘Graphene has been extensively utilized in the domain of electromagnetic wave(EMW)absorption ma-terials because of its excellent electrical conductivity.However,the inferior impedance matching per-formance and the single loss mechanism vastly restrict the application.Hence,it’s an effective strat-egy to solve these issues by introducing magnetic components.Notably,layer double hydroxide(LDH)is an appropriate template to obtain magnetic component materials.Considering that ferromagnetic met-als such as Fe,Co,Ni,and their corresponding metal oxides are usually treated as magnetic compo-nents which are promising candidates for EMW absorption materials.Therefore,in this work,a FeNi-layered double hydroxide-reduced graphene oxide(FeNi-LDH-rGO)aerogel was synthesized through a series of processes such as electrostatic self-assembly,hydrothermal,freeze-drying,and annealing.The magnetic NiFe_(2)O_(4)@FeNi_(3)core-shell nanospheres were obtained from FeNi-LDH precursor,anchoring on rGO nanosheets after the annealing treatment.Furthermore,the effects of different mass ratios of LDH to GO as well as different annealing temperatures of LDH-rGO aerogel on the EMW absorption prop-erty and impedance matching performance were explored.As a consequence,the fabricated ultralight 600LDH-rGO 2:1 aerogel shows a broad effective absorption bandwidth(EAB)of 7.04 GHz at a thickness of 2.3 mm with a low filling content of only 6 wt%and a low density of 4.4 mg/cm^(3).In conclusion,the synthetic LDH-rGO aerogels offer an effective strategy for preparing EMW absorption materials that own three-dimensional porous network structure and unique magnetic NiFe_(2)O_(4)@FeNi_(3)core-shell struc-ture nanospheres.
基金supported by National Natural Science Foundation of China(Nos.U20A20246,51872108)the Fundamental Research Funds for the Central Universities(Nos.30106200463 and CCNU20TS006)Graduate Education Innovation Grant from Central China Normal University(No.2020CXZZ101).
文摘Manganese-based cathode materials are considered as a promising candidate for rechargeable aqueous zinc-ion batteries(ZIBs).Suffering from poor conductive and limited structure tolerance,various carbon matrix,especially N-doped carbon,were employed to incorporate with MnO_(2)for greatly promoted electrochemical performances.However,the related underlying mechanism is still unknown,which is unfavorable to guide the design of high performance electrode.Herein,by incorporating layered MnO_(2)with N-doped carbon nanowires,a free-standing cathode with hierarchical core-shell structure(denoted as MnO_(2)@NC)is prepared.Benefiting from the N-doped carbon and rational architecture,the MnO_(2)@NC electrode shows an enhanced specific capacity(325 mAh g^(−1)at 0.1 A g^(−1))and rate performance(90 mAh g^(−1)at 2 A g^(−1)),as well as improved cycling stability.Furthermore,the performance improvement mechanism of MnO_(2)incorporated by N-doped carbon is investigated by X-ray photoelectron spectroscopy(XPS),Raman spectrums and density functional theory(DFT)calculation.The N atom elongates the Mn-O bond and reduces the valence of Mn^(4+)ion in MnO_(2)crystal by delocalizing its electron clouds.Thus,the electrostatic repulsion will be weakened when Zn^(2+)/H^(+)insert into the host MnO_(2)lattices,which is profitable to more cation insertion and faster ion transfer kinetics for higher capacity and rate capability.This work elucidates a fundamental understanding of the functions of N-doped carbon in composite materials and shed light on a practical pathway to optimize other electrode materials.
文摘Semiconductor-based photocatalysts have been extensively studied for oxidative photodestruction of organic pollutants in wastewaters, releasing non-toxic substances such as Azo dyes. Various synthesized catalyst specimens were characterized to determine the correlation between preparation conditions (catalyst type, dopant, microstructure, preparation routs, optical and physico-chemical properties) on the photocatalytic activity. Some researchers focused on the process parameters to optimize them to reach higher photoactivity. The specific surface areas, crystalline size, charge and pretreatment of the surface have significant effects on the physical and photocatalytic properties of the semiconductors. The surface sites of catalyst (TiO2) were modified by doping ZnS nanoparticles in the form of Core-Shell structure and the photocatalytic activities were determined by using color degradation and hydrogen production tests. The dye adsorption isotherms of photocatalyst were determined using UV-Vis spectroscopy. The specific surface properties were determined from BET, Zeta meter and Particle size analyzer tests. Photocatalytic decolorization of AR and water splitting test were applied to understand the relation between the surface properties and the photocatalytic activity. The result indicated that core-shell prepared samples had different surface suitable sites to cooperate in photocatalytic reaction.
基金the Fundamental Research Funds for Central Universities (BLX202151)the National Natural Science Foundation of China (22208021, 52225003, 22109004)。
文摘Copper(Cu)-based materials are known as the most attractive catalysts for electrochemical carbon dioxide reduction reaction(CO_(2)RR),especially the Cu^(+) species(e.g.,Cu_(2)O),which show excellent capability for catalyzing CO_(2) to C_(2+) chemicals because of their unique electronic structure.However,the active Cu^(+) species are prone to be reduced to metallic Cu under an electroreduction environment,thus resulting in fast deactivation and poor selectivity.Here,we developed an advanced surface modification strategy to maintain the active Cu^(+) species via assembling a protective layer of metal-organic framework(copper benzenetricarboxylate,CuBTC) on the surface of Cu_(2)O octahedron(Cu_(2)O@CuBTC).It's encouraging to see that the Cu_(2)O@CuBTC heterostructure outperforms the bare Cu_(2)O octahedron in catalyzing CO_(2) to C_(2+) chemicals and dramatically enhances the ratio of C_(2)H_(4)/CH_(4) products.A systematic study reveals that the introduced CuBTC shell plays a critical role in maintaining the active Cu^(+) species in Cu_(2)O@CuBTC heterostructure under reductive conditions.This work offers a practical strategy for improving the catalytic performance of CO_(2)RR over copper oxides and also establishes a route to maintain the state of valence-sensitive catalysts.
基金supported by the National Natural Science Foun-dation of China(Nos.52071294 and U1809215)Natural Science Foundation of Zhejiang Province(Grant LY20E020015)National Key Research and Development Program(No.2019YFE012862).
文摘The nano-iron nitride soft magnetic material has excellent magnetic properties and is expected to be a brilliant electromagnetic wave absorber.However,how to fully exploit its wave-absorbing potential re-mains a thought-provoking question.Here,we have synthesized Fe/Fe_(4)N@SiO_(2)nanomagnetic core-shell materials with different Fe/Fe_(4)N ratios by performing nitridation reactions at different temperatures.Then,the flower-like core-shell Fe/Fe_(4)N@SiO_(2)structure was obtained by the etching method.Finally,with the synergy of the excellent magnetic and dielectric losses,an outstanding absorption performance could be achieved with a minimum refection loss(RL min)of−71.31 dB at the matching thickness of 1.4 mm,and the widest effective absorption bandwidth(EAB max)of 6.1 GHz less than−10 dB was realized at 1.16 mm.Moreover,this material also shows a preeminent advance in corrosion resistance to adapt to harsh environments.Hence,this iron nitride flower-like core-shell structure exhibits great potential in microwave absorption in harsh conditions.