Synthesis of functionalized mesoporous carbon by an easy-accessed method is of great importance towards its practical applications.Herein,an evaporation induced self-assembly/carbonization（EISAC）method was developed...Synthesis of functionalized mesoporous carbon by an easy-accessed method is of great importance towards its practical applications.Herein,an evaporation induced self-assembly/carbonization（EISAC）method was developed and applied to the synthesis of sulfonic acid group functionalized mesoporous carbon（SMC）.The final mesoporous carbon obtained by EISAC method possesses wormlike mesoporous structure,uniform pore size（3.6 nm）,large surface area of 735 m^2/g,graphitic pore walls and rich sulfonic acid group.Moreover,the resultant mesoporous carbon achieves a superior electrochemical capacitive performances（216 F/g） to phenolic resin derived mesoporous carbon（OMC,152 F/g） and commercial activated carbon（AC,119 F/g）.展开更多
Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-...Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-C_(3)N_(4) suffers from limited visible-light absorption and low charge-carrier mobility.In this study,a phosphorus-doped tubular carbon nitride(5P-TCN)was synthesized via a precursor self-assembly method using phosphoric acid and melamine as raw materials,eliminating the need for organic solvents or templates.The 5P-TCN catalyst demonstrated enhanced visible-light absorption,improved charge transfer capability,and a 5.25-fold increase in specific surface area(31.092 m^(2)/g),which provided abundant active sites to efficiently drive the PMS-assisted photocatalytic reaction.The 5P-TCN/vis/PMS system exhibited exceptional degradation performance for organic pollutants across a broad pH range(3–9),achieving over 92%degradation of Rhodamine B(RhB)within 15 min.Notably,the system retained>98%RhB degradation efficiency after three consecutive operational cycles,demonstrating robust operational stability and reusability.Moreover,key parameters influencing,active radi-cals,degradation pathways,and potential mechanisms for RhB degradation were systematically investigated.This work proposes a green and cost-effective strategy for developing high-efficiency photocatalysts,while demon-strating the exceptional capability of a PMS-assisted photocatalytic system for rapid degradation of RhB.展开更多
Recently,hollow carbon nanospheres(HCSs)have garnered significant attention as potential Li metal hosts owing to their unique large voids and ease of fabrication.However,similar to other nanoscale hosts,their practica...Recently,hollow carbon nanospheres(HCSs)have garnered significant attention as potential Li metal hosts owing to their unique large voids and ease of fabrication.However,similar to other nanoscale hosts,their practical performance is limited by inhomogeneous agglomeration,increased binder requirements,and high tortuosity within the electrode.To overcome these problems and high tortuosity within the electrode,this study introduces a pomegranate-like carbon microcluster composed of primary HCSs(P-CMs)as a novel Li metal host.This unique nanostructure can be easily prepared using the spray-drying technique,enabling its mass production.Comprehensive analyses with various tools demonstrate that compared with HCS hosts,the P-CM host requires a smaller amount of binder to fabricate a sufficiently robust and even surface electrode.Furthermore,owing to reduced tortuosity,the well-designed P-CM electrode can provide continuous and shortened pathways for electron/ion transport,accelerating the Li-ion transfer kinetics and prohibiting preferential Li plating at the upper region of the electrode.Due to these characteristics,Li metal can be effectively encapsulated in the large inner voids of the primary HCSs constituting the P-CM,thereby enhancing the electrochemical performance of P-CM hosts in Li metal batteries.Specifically,the Coulombic efficiency of the P-CM host can be maintained at 97%over 100 cycles,with a high Li deposition areal capacity of 3 mAh·cm^(-2)and long cycle life(1000 h,1 mA·cm^(-2),and 1.0 mAh·cm^(-2)).Furthermore,a full cell incorporating a LiFePO4 cathode exhibits excellent cycle life.展开更多
Shape control of mesoporous carbon microparticles(MCMPs)is of critical importance;in particular,asymmetric shapes that can yield unique properties have attracted significant attention.However,the tailored synthesis of...Shape control of mesoporous carbon microparticles(MCMPs)is of critical importance;in particular,asymmetric shapes that can yield unique properties have attracted significant attention.However,the tailored synthesis of asymmetric MCMPs with ordered structures remains challenging.Herein,we report a facile route to prepare asymmetric MCMPs by dynamic neutral interface-guided 3D-confined self-assembly(3D-CSA)of block copolymer/homopolymer(BCP/hP)blends,followed by a self-templated selective direct carbonization strategy.BCP/h P Janus microparticles with ordered hierarchical mesostructures were prepared with emulsion solvent evaporation-induced 3D-CSA.The continuous phase of BCP domains was then crosslinked.Composite asymmetric MCMPs are successfully generated after selective carbonization of the crosslinked continuous phase.This method allows tuning the shape of MCMPs easily by varying the blending ratio of BCP/h P.The composite asymmetric MCMPs combine the advantages of asymmetric shape,ordered structure,high specific surface area,chemical inertness and thermal stability and could provide great possibilities for applications in catalysis,drug delivery,energy conversion and storage.展开更多
The self-assembly of block copolymer in solution has proven to be an effective strategy for building up a wide range of nanomaterials with diverse structures and applications.This paper reports a facile self-assembly ...The self-assembly of block copolymer in solution has proven to be an effective strategy for building up a wide range of nanomaterials with diverse structures and applications.This paper reports a facile self-assembly approach towards two-dimensional(2D)sandwich-like mesoporous nitrogen-doped carbon/reduced graphene oxide nanocomposites(denoted as mNC/rGO)with well-defined large mesopores.The strategy involves the synergistic self-assembly ofpolystyrene-block-poly(ethylene oxide)(PS-b-PEO)spherical micelles,m-phenylenediamine(mPD)monomers and GO in solution and the subsequent carbonization at 900~C.The resultant mNC/rGO nanosheets have an average pore size of 19 nm,a high specific surface of 812 m^(2)'g^(-1)and a nitrogen content of 2.2 wt%.As an oxygen reduction reaction(ORR)catalyst,the unique structural features render the metal-free nanosheets excellent electrocatalytic performance.In a 0.1 mol.L-~KOH alkaline medium,mNC/rGO exhibits a four-electron transfer pathway with a high half-wave-potential(El/2)of+0.77 V versus reversible hydrogen electrode(RHE)and a limiting current density(JL)of 5.2 mA'cm^(-2),which are well comparable with those of the commercial Pt/C catalysts.展开更多
Self-assembled nanostructure arrays integrating the advantages of the intrinsic characters of nanostructure as well as the array stability are appealing in advanced materials.However,the precise bottom-up synthesis of...Self-assembled nanostructure arrays integrating the advantages of the intrinsic characters of nanostructure as well as the array stability are appealing in advanced materials.However,the precise bottom-up synthesis of nanostructure arrays without templates or substrates is quite challenging because of the general occurrence of homogeneous nucleation and the difficult manipulation of noncovalent interactions.Herein,we first report the precisely manipulated synthesis of well-defined louver-like P-doped carbon nitride nanowire arrays(L-PCN)via a supramolecular self-assembly method by regulating the noncovalent interactions through hydrogen bond.With this strategy,CN nanowires align in the outer frame with the separation and spatial location achieving ultrastability and outstanding photoelectricity properties.Significantly,this self-assembly L-PCN exhibits a superior visible light-driven hydrogen evolution activity of 1872.9μmol h^−1 g^−1,rendering a^25.6-fold enhancement compared to bulk CN,and high photostability.Moreover,an apparent quantum efficiency of 6.93%is achieved for hydrogen evolution at 420±15 nm.The experimental results and first-principles calculations demonstrate that the remarkable enhancement of photocatalytic activity of L-PCN can be attributed to the synergetic effect of structural topology and dopant.These findings suggest that we are able to design particular hierarchical nanostructures with desirable performance using hydrogen-bond engineering.展开更多
Carbon nanotubes(CNTs)have garnered significant attention in the fields of science,engineering,and medicine due to their numerous advantages.The initial step towards harnessing the potential of CNTs involves their mac...Carbon nanotubes(CNTs)have garnered significant attention in the fields of science,engineering,and medicine due to their numerous advantages.The initial step towards harnessing the potential of CNTs involves their macroscopic assembly.The present study employed a gentle and direct self-assembly technique,wherein controlled growth of CNT sheaths occurred on the metal wire’s surface,followed by etching of the remaining metal to obtain the hollow tubes composed of CNTs.By controlling the growth time and temperature,it is possible to alter the thickness of the CNTs sheath.After immersing in a solution containing 1 g/L of CNTs at 60℃ for 24 h,the resulting CNTs layer achieved a thickness of up to 60μm.These hollow CNTs tubes with varying inner diameters were prepared through surface reinforcement using polymers and sacrificing metal wires,thereby exhibiting exceptional attributes such as robustness,flexibility,air tightness,and high adsorption capacity that effectively capture CO_(2) from the gas mixture.展开更多
The interfacial property of carbon fiber(CF)reinforced composites is crucial to facilitate the application of high-strength composites.Utilizing the electrostatic and hydrogen bond properties of diazo resin,carbon nan...The interfacial property of carbon fiber(CF)reinforced composites is crucial to facilitate the application of high-strength composites.Utilizing the electrostatic and hydrogen bond properties of diazo resin,carbon nanotubes(CNTs)and graphene oxide(GO)could be quickly grafted onto the surface of the CF via the layer-by-layer self-assembly technique.The results showed that CNTs and GO were uniformly coated onto the CF surface,and the chemical activity and roughness of the modified CF surface were improved signif-icantly.The modified CF surface can significantly augment the interaction between the epoxy resin and the fiber.Remarkably,due to the good interfacial property,the impact performance of the composites re-inforced with the nanomaterial-modified CF was improved obviously.In addition,the interface properties of the composites are studied in depth.This method is expected to achieve rapid surface modification of carbon fiber.展开更多
Lignin has been proved to be a promising precursor for producing carbon foam.The thermal and chemistry properties of lignin during its thermal conversion make it quite unique comparing with other precursors,and the co...Lignin has been proved to be a promising precursor for producing carbon foam.The thermal and chemistry properties of lignin during its thermal conversion make it quite unique comparing with other precursors,and the conversion parameters can clearly affect the properties of the derived products.Therefore,this study systematically investigated the effects of key carbonization parameters on the properties of the resulting carbon foam materials.The findings demonstrate that the performance of the self-shaping lignin-derived carbon foam is simultaneously influenced by the factors that carbonization temperature,heating rate,and carbonization duration.Specifically,the carbonization temperature and carbonization duration have a significant impact on the mechanical performance,where higher temperatures and long carbonization time improve compressive strength and specific strength.Moreover,the data revealed that elevated temperatures,rapid heating rates,and shortened carbonization periods collectively promoted the development of higher porosities and larger pore diameters within the carbon foam structure.Conversely,lower carbonization temperatures,slower heating rates,and extended carbonization durations facilitated the formation of microporous in the carbon foam.This study provides a scientific foundation for optimizing the production of lignin-derived carbon foam with tailored properties and performance characteristics.展开更多
Four glycoluril-based amphiphilic molecular clips(AMCs)M1~M4 have been prepared for intracellular delivery of short DNA.M1~M4 have two methyl groups on its convex surface and four cations on its aromatic side arm,whic...Four glycoluril-based amphiphilic molecular clips(AMCs)M1~M4 have been prepared for intracellular delivery of short DNA.M1~M4 have two methyl groups on its convex surface and four cations on its aromatic side arm,which can be used to construct self-assembled nanoparticles in aqueous solution driven by hydrophobic interaction.Dynamic light scattering experiments show that M1 and M2 can be driven hydrophobically to aggregate into extremely stable nanoparticles in water at the micromolar concentrations.Fluorescence titration and zeta potential experiments support that the nanoparticles formed by M1 and M2 are able to efficiently encapsulate short DNA(sDNA).Fluorescence imaging and flow cytometry studies reveal that their nano sizes enable intracellular delivery of the encapsulated sDNA into both normal and cancer cells,with delivery percentage reaching up to 94%,while in vitro experiments indicate that the two compounds have excellent biocompatibility and low cytotoxicity.展开更多
A facile one-pot synthesis of solid polymer electrolytes(SPEs), composed of carbonate terminated poly(ethylene glycol)(CH3O-PEG-IC), poly(ethylene glycol)-block-polystyrene(PEG-b-PS) block copolymer nanoparticles cont...A facile one-pot synthesis of solid polymer electrolytes(SPEs), composed of carbonate terminated poly(ethylene glycol)(CH3O-PEG-IC), poly(ethylene glycol)-block-polystyrene(PEG-b-PS) block copolymer nanoparticles containing a conductive PEG corona, fumed SiO2 and Li TFSI salt via polymerization-induced self-assembly is proposed. This method to prepare SPEs has the advantages of one-pot convenient synthesis, avoiding use of organic solvent and conveniently adding inorganic additives. CH3O-PEG-IC combines advantages of PEG and polycarbonate, the in situ synthesized PEG-b-PS nanoparticles containing a rigid polystyrene(PS) core and a PEG corona guarantee continuous lithium ion transport in the synthesized SPEs, and the fumed SiO2 optimizes the interfacial properties and improves the electrochemical stability, all of which afford SPEs a well considerable room temperature ionic conductivity of 1.73 × 10^-4S/cm, high lithium transference number of 0.53, and wide electrochemical stability window of 5.5 V(vs. Li^+/Li). By employing these SPEs, the assembled solid state cells of Li FePO4 |SPEs|Li exhibit considerable cell performance.展开更多
Carbon-based films were synthesized by self-assembly of chitosan-encapsulated carbon microsphere （CMS@CS） composite. First, carbon microspheres （CMSs） prepared by chemical vapor deposition were modified by HNO3 an...Carbon-based films were synthesized by self-assembly of chitosan-encapsulated carbon microsphere （CMS@CS） composite. First, carbon microspheres （CMSs） prepared by chemical vapor deposition were modified by HNO3 and H2O2. Second, oxidized CMSs were modified by chitosan （CS）. Finally, CMS@CS was self-assembled by vertical deposition, in which suspension concentration and deposition temperature on the quality of self-assembling film were investigated. Field emission scanning electron microscopy, atomic force microscopy, X-ray diffraction, thermogravimetry, and Fourier transformation infrared spectrometry were employed to characterize the morphology and structure of the samples. The results show that CMSs modified by CS had uniform particle size and good dispersion, CMS@CS was self-assembled into a dense film, the film thickened with increasing suspension concentration at fixed temperature, and more ordered film was obtained at 1 wt% of suspension concentration and 50 ℃. The ultraviolet-visible absorption spectra show that the absorbance of CMS@CS film grew steadily with increasing suspension concentration and that the CMSs with oxygen-containing groups have a good assembling performance to form composite films with CS.展开更多
To clarify the preparation mechanisms of uorinated ordered mesoporous carbon materials (FOMCs), the dissipative par- ticle dynamics method was used to simulate the self-assembly process of the amphiphilic triblock pol...To clarify the preparation mechanisms of uorinated ordered mesoporous carbon materials (FOMCs), the dissipative par- ticle dynamics method was used to simulate the self-assembly process of the amphiphilic triblock poly(ethylene oxide)- poly(propylene oxide)-poly(ethylene oxide) copolymer Pluronic F127 in the aqueous system. The self-assembly mechanisms in aqueous phase and the formation mechanisms of micropores and mesopores were investigated. It was found that the mesoporous structure of the FOMCs was formed by the hydrophobic segments of F127, while the pore wall was formed by both the hydrophilic segments and the carbon precursor in the system. The microporous structure on the pore wall was con- structed by the carbon source in the hydrophilic segments’ spaces after the template was removed. Our ndings could provide understanding and knowledge for the synthesis of mesoporous carbon by the self-assembly method on the mesoscopic scale.展开更多
Van der Waals heterostructures composed of low-dimensional atomic layers host rich physics for new device applications,such as magic-angle twisted bilayer graphene and coaxial multi-walled hetero-nanotubes.Aside from ...Van der Waals heterostructures composed of low-dimensional atomic layers host rich physics for new device applications,such as magic-angle twisted bilayer graphene and coaxial multi-walled hetero-nanotubes.Aside from exploring their abnormal physical behavior,fabrication of such structures also presents a great challenge to this area,owing to the subtle and sensitive interactions among neighboring layers.Here we show by molecular dynamics simulations that narrow blue phosphorene nanoribbons can be encapsulated into carbon nanotubes driven by van der Waals interactions and form one-dimensional heterostructures.It shows that by varying carbon nanotube diameters and nanoribbon width,the nanoribbons can either retain their original straight structures or twist into tubular structures.Wrapping phases are also observed for large-sized blue phosphorus.It is found that the underlying mechanism originates from the competition between van der Waals energy and bending energy induced by tube curvature.A phase diagram of the resultant 1D structure is thus obtained based on a simple analysis of energetics.The results are expected to stimulate further experimental efforts in fabricating one-dimensional van der Waals heterostructues with desired functionality.展开更多
Nowadays,high-stable and ultrasensitive heavy metal detection is of utmost importance in water quality monitoring.Nanoparticle-enhanced laser-induced breakdown spectroscopy(NELIBS)shows high potential in hazardous met...Nowadays,high-stable and ultrasensitive heavy metal detection is of utmost importance in water quality monitoring.Nanoparticle-enhanced laser-induced breakdown spectroscopy(NELIBS)shows high potential in hazardous metal detection,however,encounters unstable and weak signals due to nonuniform distribution of analytes.Herein,we developed an interface self-assembly(ISA)method to create a uniformly distributed gold nanolayer at a liquid-liquid interface for positive heavy metal ions capture and NELIBS analysis.The electrostatically selfassembled Au nanoparticles(NPs)-analytes membrane was prepared at the oil-water interface by injecting ethanol into the mixture of cyclohexane and Au NPs-analytes water solution.Then,the interface self-assembled Au NPs-analytes membrane was transformed onto a laser-processed superhydrophilic Si slide for detection.Three heavy metals(cadmium(Cd),barium(Ba),and chromium(Cr))were analyzed to evaluate the stability and sensitivity of the ISA method for NELIBS.The results(Cd:RSD=3.6%,LoD=0.654 mg/L;Ba:RSD=3.4%,LoD=0.236 mg/L;Cr:RSD=7.7%,LoD=1.367 mg/L)demonstrated signal enhancement and high-stable and ultrasensitive detection.The actual sample detection(Cd:RE=7.71%,Ba:RE=6.78%)illustrated great reliability.The ISA method,creating a uniform distribution of NP-analytes at the interface,has promising prospects in NELIBS.展开更多
Diphenylalanine and its analogs cause many concerns owing to their perfect self-assembly properties in the fields of biology,medicine,and nanotechnology.Experimental research has shown that diphenylalanine-based analo...Diphenylalanine and its analogs cause many concerns owing to their perfect self-assembly properties in the fields of biology,medicine,and nanotechnology.Experimental research has shown that diphenylalanine-based analogs with ethylenediamine linkers(PA,P=phenylalanine,and A=analog)can self-assemble into spherical assemblies,which can serve as novel anticancer drug carriers.In this work,to understand the assembly pathways,drug loading behavior,and formation mechanism of PA aggregates at the molecular level,we carried out dissipative particle dynamics(DPD)simulations of PA molecule systems.Our simulation results demonstrate that PA molecules spontaneously assemble into nanospheres and can self-assemble into drug-loaded nanospheres upon addition of the cancer chemotherapeutic agent doxorubicin(DOX).We also found that the hydrophobic side chain beads of PA molecules exhibited a unique onion-like distribution inside the nanospheres,which was not observed in the experiment.The onion-like nanospheres were verified by calculating the radial distribution function(RDF)of the DPD beads.Furthermore,based on the analysis of the percentages of different interaction components in the total nonbonded energies,main chain-side chain interactions between PA molecules may be important in the formation of onion-like nanospheres,and the synergistic effects of main chain-side chain,main chain-drug,side chain-drug,and main chain-solvent interactions are significant in the formation of drug-loaded nanospheres.These findings provide new insights into the structure and self-assembly pathway of PA assemblies,which may be helpful for the design of efficient and effective drug delivery systems.展开更多
The potential of metal nanoclusters in biomedical applications is limited due to aggregation-caused quenching(ACQ).In this study,an in situ self-assembled pitaya structure was proposed to obtain stable fluorescence em...The potential of metal nanoclusters in biomedical applications is limited due to aggregation-caused quenching(ACQ).In this study,an in situ self-assembled pitaya structure was proposed to obtain stable fluorescence emission through protein coronas-controlled distance between gold nanoclusters(Au NCs).Interestingly,the gold ion complexes coated with proteins of low isoelectric point(pI)nucleate at the secondary structure of proteins with high p I through ionic exchange within cells,generating fluorescent Au NCs.It is worth noting that due to the steric hindrance formed by the protein coronas on the surface of Au NCs,the distance between Au NCs can be controlled,avoiding electron transfer caused by close proximity of Au NCs and inhibiting fluorescence ACQ.This strategy can achieve fluorescence imaging of clinical tissue samples without observable side effects.Therefore,this study proposes a distance-controllable self-assembled pitaya structure to provide a new approach for Au NCs with stable fluorescence.展开更多
For efficient solar energy conversion,the morphology engineering of hollow graphitic carbon nitride(gC3 N4)is one of the promising approachs benefiting from abundant exposed active sites and short photocarrier transpo...For efficient solar energy conversion,the morphology engineering of hollow graphitic carbon nitride(gC3 N4)is one of the promising approachs benefiting from abundant exposed active sites and short photocarrier transport distances,but is difficult to control on account of easy structural collapse.Herein,a facile supramolecular electrostatic self-assembly strategy has been developed for the first time to fabricate mesoporous thin-walled g-C3N4 microtubes(mtw-CNT)with shell thickness of ca.13 nm.The morphological control of g-C3N4 enhances specific surface area by 12 times,induces stronger optical absorption,widens bandgap by 0.18 e V,improves photocurrent density by 2.5 times,and prolongs lifetimes of charge carriers from bulk to surface,compared with those of bulk g-C3N4.As a consequence,the transformed g-C3N4 exhibits the optimum photocatalytic H2-production rate of 3.99 mmol·h^-1·g^-1(λ>420 nm)with remarkable apparent quantum efficiency of 8.7%(λ=420±15 nm)and long-term stability.Moreover,mtw-CNT also achieves high photocatalytic CO2-to-CO selectivity of 96%(λ>420 nm),much better than those on the most previously reported porous g-C3N4 photocatalysts prepared by the conventional hard-templating and soft-templating methods.展开更多
The development of new and efficient extractants plays a key role in the separation and recovery of rare earth elements.In this pape r,the extractant(N,N-methyl py ridineethyl-N',N'-dicyclohexyl-3-oxadiglycola...The development of new and efficient extractants plays a key role in the separation and recovery of rare earth elements.In this pape r,the extractant(N,N-methyl py ridineethyl-N',N'-dicyclohexyl-3-oxadiglycolamide,MPyEDChDGA) with a new structure was synthesized,and the pyridine group was successfully grafted onto the 3-oxadiglycolamide structure.Using MPyEDChDGA for efficient enrichment of rare earth ions,the self-assembled solids were recovered by simple filtration without further backextraction and final precipitation,achieving a one-step strategy for the recovery of rare earth ions.Several important parameters affecting the self-assembly extraction,including pH,diluent,temperature,and extractant concentration,were systematically evaluated using La(NO_(3))_(3),Tb(NO_(3))_(3),and Lu(NO_(3))_(3) as representatives.The self-assembled solids were investigated in detail by X-ray diffraction(XRD),scanning electron microscopy(SEM),1H nuclear magnetic resonance(1H NMR),Fourier transform infrared spectroscopy(FT-IR),Raman,and X-ray photoelectron spectroscopy(XPS) analyses.The stoichiometry of the extraction species was characterized using the Job's method and electrospray ionization mass spectrometry(ESI-MS).In addition,MPyEDChDGA was applied to the recovery of Sm in SmCoCu simulated liquid,and the results show that MPyEDChDGA has good selectivity of Sm from transition metals(Co,Cu).The separation factor of Sm/Co can reach 6281±117,which provides a new approach to recovering Sm from SmCoCu scrap magnets.This study presents an efficient and convenient new strategy for the recovery and separation of rare earth elements.展开更多
The calcium-containing rare earth solution is generated during the recovery processes of NdFeB waste,which is treated as wastewater by enterprises.In this paper,the carbon dioxide carbonization method was applied to t...The calcium-containing rare earth solution is generated during the recovery processes of NdFeB waste,which is treated as wastewater by enterprises.In this paper,the carbon dioxide carbonization method was applied to the separation of rare earths and calcium in the solution,as well as the preparation of rare earth oxides with a large specific surface.It is shown that the process of CO_(2)carbonization of solution includes reactions such as the dissolution,diffusion and ionization of CO_(2),the carbonate precipitation of rare earth ions,and the neutralization of hydrogen ions.At a pH of 4.5,the carbonization precipitation rate is effectively controlled,enabling homogeneous precipitation and ensuring both high precipitation yield and rare earth oxides purity.In this way,the crystallization of carbonization products is a process dominated by the oriented attachment theory and coexisting with the Ostwald ripening theory,resulting in abundant pores formed by multiple layers of stacking in the products.With the optimal carbonization conditions,the rare earth precipitation yield solution reaches 99.32%.The obtained carbonization products are crystalline(LaCe)(CO_(3))_(3)·8H_(2)O,and the purity of the rare earth oxides is as high as 99.22 wt%.The specific surface area of the rare earth oxides reaches 94.7 m^(2)/g,and its adsorption efficiency for tetracycline hydrochloride in solution can reach 92.6%in a short time.The rare earth oxides are expected to be used as an adsorption material for wastewater treatment and other adsorption environments.展开更多
基金supported by the Ministry of Science and Technology of China(No.2009CB623504)the National Science Foundation of China(Nos.20773062,20773063,21173119,and21273109)the Fundamental Research Funds for the Central Universities
文摘Synthesis of functionalized mesoporous carbon by an easy-accessed method is of great importance towards its practical applications.Herein,an evaporation induced self-assembly/carbonization（EISAC）method was developed and applied to the synthesis of sulfonic acid group functionalized mesoporous carbon（SMC）.The final mesoporous carbon obtained by EISAC method possesses wormlike mesoporous structure,uniform pore size（3.6 nm）,large surface area of 735 m^2/g,graphitic pore walls and rich sulfonic acid group.Moreover,the resultant mesoporous carbon achieves a superior electrochemical capacitive performances（216 F/g） to phenolic resin derived mesoporous carbon（OMC,152 F/g） and commercial activated carbon（AC,119 F/g）.
文摘Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-C_(3)N_(4) suffers from limited visible-light absorption and low charge-carrier mobility.In this study,a phosphorus-doped tubular carbon nitride(5P-TCN)was synthesized via a precursor self-assembly method using phosphoric acid and melamine as raw materials,eliminating the need for organic solvents or templates.The 5P-TCN catalyst demonstrated enhanced visible-light absorption,improved charge transfer capability,and a 5.25-fold increase in specific surface area(31.092 m^(2)/g),which provided abundant active sites to efficiently drive the PMS-assisted photocatalytic reaction.The 5P-TCN/vis/PMS system exhibited exceptional degradation performance for organic pollutants across a broad pH range(3–9),achieving over 92%degradation of Rhodamine B(RhB)within 15 min.Notably,the system retained>98%RhB degradation efficiency after three consecutive operational cycles,demonstrating robust operational stability and reusability.Moreover,key parameters influencing,active radi-cals,degradation pathways,and potential mechanisms for RhB degradation were systematically investigated.This work proposes a green and cost-effective strategy for developing high-efficiency photocatalysts,while demon-strating the exceptional capability of a PMS-assisted photocatalytic system for rapid degradation of RhB.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.2020R1C1C1003375)。
文摘Recently,hollow carbon nanospheres(HCSs)have garnered significant attention as potential Li metal hosts owing to their unique large voids and ease of fabrication.However,similar to other nanoscale hosts,their practical performance is limited by inhomogeneous agglomeration,increased binder requirements,and high tortuosity within the electrode.To overcome these problems and high tortuosity within the electrode,this study introduces a pomegranate-like carbon microcluster composed of primary HCSs(P-CMs)as a novel Li metal host.This unique nanostructure can be easily prepared using the spray-drying technique,enabling its mass production.Comprehensive analyses with various tools demonstrate that compared with HCS hosts,the P-CM host requires a smaller amount of binder to fabricate a sufficiently robust and even surface electrode.Furthermore,owing to reduced tortuosity,the well-designed P-CM electrode can provide continuous and shortened pathways for electron/ion transport,accelerating the Li-ion transfer kinetics and prohibiting preferential Li plating at the upper region of the electrode.Due to these characteristics,Li metal can be effectively encapsulated in the large inner voids of the primary HCSs constituting the P-CM,thereby enhancing the electrochemical performance of P-CM hosts in Li metal batteries.Specifically,the Coulombic efficiency of the P-CM host can be maintained at 97%over 100 cycles,with a high Li deposition areal capacity of 3 mAh·cm^(-2)and long cycle life(1000 h,1 mA·cm^(-2),and 1.0 mAh·cm^(-2)).Furthermore,a full cell incorporating a LiFePO4 cathode exhibits excellent cycle life.
基金financially supported by the National Natural Science Foundation of China(Nos.52003094 and 52273010)。
文摘Shape control of mesoporous carbon microparticles(MCMPs)is of critical importance;in particular,asymmetric shapes that can yield unique properties have attracted significant attention.However,the tailored synthesis of asymmetric MCMPs with ordered structures remains challenging.Herein,we report a facile route to prepare asymmetric MCMPs by dynamic neutral interface-guided 3D-confined self-assembly(3D-CSA)of block copolymer/homopolymer(BCP/hP)blends,followed by a self-templated selective direct carbonization strategy.BCP/h P Janus microparticles with ordered hierarchical mesostructures were prepared with emulsion solvent evaporation-induced 3D-CSA.The continuous phase of BCP domains was then crosslinked.Composite asymmetric MCMPs are successfully generated after selective carbonization of the crosslinked continuous phase.This method allows tuning the shape of MCMPs easily by varying the blending ratio of BCP/h P.The composite asymmetric MCMPs combine the advantages of asymmetric shape,ordered structure,high specific surface area,chemical inertness and thermal stability and could provide great possibilities for applications in catalysis,drug delivery,energy conversion and storage.
基金financially supported by the National Natural Science Foundation of China(Nos.51573091,21774076,21320102006 and 91527304)Program of the Shanghai Committee of Science and Technology(Nos.17JC1403200 and 16JC1400703)Program for Shanghai Eastern Scholar
文摘The self-assembly of block copolymer in solution has proven to be an effective strategy for building up a wide range of nanomaterials with diverse structures and applications.This paper reports a facile self-assembly approach towards two-dimensional(2D)sandwich-like mesoporous nitrogen-doped carbon/reduced graphene oxide nanocomposites(denoted as mNC/rGO)with well-defined large mesopores.The strategy involves the synergistic self-assembly ofpolystyrene-block-poly(ethylene oxide)(PS-b-PEO)spherical micelles,m-phenylenediamine(mPD)monomers and GO in solution and the subsequent carbonization at 900~C.The resultant mNC/rGO nanosheets have an average pore size of 19 nm,a high specific surface of 812 m^(2)'g^(-1)and a nitrogen content of 2.2 wt%.As an oxygen reduction reaction(ORR)catalyst,the unique structural features render the metal-free nanosheets excellent electrocatalytic performance.In a 0.1 mol.L-~KOH alkaline medium,mNC/rGO exhibits a four-electron transfer pathway with a high half-wave-potential(El/2)of+0.77 V versus reversible hydrogen electrode(RHE)and a limiting current density(JL)of 5.2 mA'cm^(-2),which are well comparable with those of the commercial Pt/C catalysts.
基金the National Natural Science Foundation of China(Nos.51772085 and U1830138)Hunan Provincial Innovation Foundation for Postgraduate(No.CX20190311)
文摘Self-assembled nanostructure arrays integrating the advantages of the intrinsic characters of nanostructure as well as the array stability are appealing in advanced materials.However,the precise bottom-up synthesis of nanostructure arrays without templates or substrates is quite challenging because of the general occurrence of homogeneous nucleation and the difficult manipulation of noncovalent interactions.Herein,we first report the precisely manipulated synthesis of well-defined louver-like P-doped carbon nitride nanowire arrays(L-PCN)via a supramolecular self-assembly method by regulating the noncovalent interactions through hydrogen bond.With this strategy,CN nanowires align in the outer frame with the separation and spatial location achieving ultrastability and outstanding photoelectricity properties.Significantly,this self-assembly L-PCN exhibits a superior visible light-driven hydrogen evolution activity of 1872.9μmol h^−1 g^−1,rendering a^25.6-fold enhancement compared to bulk CN,and high photostability.Moreover,an apparent quantum efficiency of 6.93%is achieved for hydrogen evolution at 420±15 nm.The experimental results and first-principles calculations demonstrate that the remarkable enhancement of photocatalytic activity of L-PCN can be attributed to the synergetic effect of structural topology and dopant.These findings suggest that we are able to design particular hierarchical nanostructures with desirable performance using hydrogen-bond engineering.
基金Project(ZCLTGS24B0101)supported by Zhejiang Provincial Natural Science Foundation of ChinaProject(Y202250501)supported by Scientific Research Fund of Zhejiang Provincial Education Department,ChinaProject supported by SRT Research Project of Jiaxing Nanhu University,China。
文摘Carbon nanotubes(CNTs)have garnered significant attention in the fields of science,engineering,and medicine due to their numerous advantages.The initial step towards harnessing the potential of CNTs involves their macroscopic assembly.The present study employed a gentle and direct self-assembly technique,wherein controlled growth of CNT sheaths occurred on the metal wire’s surface,followed by etching of the remaining metal to obtain the hollow tubes composed of CNTs.By controlling the growth time and temperature,it is possible to alter the thickness of the CNTs sheath.After immersing in a solution containing 1 g/L of CNTs at 60℃ for 24 h,the resulting CNTs layer achieved a thickness of up to 60μm.These hollow CNTs tubes with varying inner diameters were prepared through surface reinforcement using polymers and sacrificing metal wires,thereby exhibiting exceptional attributes such as robustness,flexibility,air tightness,and high adsorption capacity that effectively capture CO_(2) from the gas mixture.
基金This work was financially supported by the National Nat-ural Science Foundation of China(Grant Nos.52072193 and U22A20131)the Shandong Provincial Natural Science Foundation(Grant Nos.ZR2021JQ16 and ZR2019YQ19)+2 种基金the Project of Shan-dong Province Higher Educational Science and Technology Program(Grant No.2019KJA026)the State Key Laboratory for Modification of Chemical Fibers and Polymer Materials(Grant No.KF2217)the Science Fund of Shandong Laboratory of Yantai Advanced Materials and Green Manufacturing(Grant No.AMGM2021F11).
文摘The interfacial property of carbon fiber(CF)reinforced composites is crucial to facilitate the application of high-strength composites.Utilizing the electrostatic and hydrogen bond properties of diazo resin,carbon nanotubes(CNTs)and graphene oxide(GO)could be quickly grafted onto the surface of the CF via the layer-by-layer self-assembly technique.The results showed that CNTs and GO were uniformly coated onto the CF surface,and the chemical activity and roughness of the modified CF surface were improved signif-icantly.The modified CF surface can significantly augment the interaction between the epoxy resin and the fiber.Remarkably,due to the good interfacial property,the impact performance of the composites re-inforced with the nanomaterial-modified CF was improved obviously.In addition,the interface properties of the composites are studied in depth.This method is expected to achieve rapid surface modification of carbon fiber.
基金funding support from Taishan Scholars Program of Shandong Province(tsqn201909132)National Natural Science Foundation of China(22208183)+1 种基金Startup Foundation from Qingdao Agricultural University(663-1120040,665-1119020)Technology development project from Jinan Shengquan Company(20233702031771)。
文摘Lignin has been proved to be a promising precursor for producing carbon foam.The thermal and chemistry properties of lignin during its thermal conversion make it quite unique comparing with other precursors,and the conversion parameters can clearly affect the properties of the derived products.Therefore,this study systematically investigated the effects of key carbonization parameters on the properties of the resulting carbon foam materials.The findings demonstrate that the performance of the self-shaping lignin-derived carbon foam is simultaneously influenced by the factors that carbonization temperature,heating rate,and carbonization duration.Specifically,the carbonization temperature and carbonization duration have a significant impact on the mechanical performance,where higher temperatures and long carbonization time improve compressive strength and specific strength.Moreover,the data revealed that elevated temperatures,rapid heating rates,and shortened carbonization periods collectively promoted the development of higher porosities and larger pore diameters within the carbon foam structure.Conversely,lower carbonization temperatures,slower heating rates,and extended carbonization durations facilitated the formation of microporous in the carbon foam.This study provides a scientific foundation for optimizing the production of lignin-derived carbon foam with tailored properties and performance characteristics.
文摘Four glycoluril-based amphiphilic molecular clips(AMCs)M1~M4 have been prepared for intracellular delivery of short DNA.M1~M4 have two methyl groups on its convex surface and four cations on its aromatic side arm,which can be used to construct self-assembled nanoparticles in aqueous solution driven by hydrophobic interaction.Dynamic light scattering experiments show that M1 and M2 can be driven hydrophobically to aggregate into extremely stable nanoparticles in water at the micromolar concentrations.Fluorescence titration and zeta potential experiments support that the nanoparticles formed by M1 and M2 are able to efficiently encapsulate short DNA(sDNA).Fluorescence imaging and flow cytometry studies reveal that their nano sizes enable intracellular delivery of the encapsulated sDNA into both normal and cancer cells,with delivery percentage reaching up to 94%,while in vitro experiments indicate that the two compounds have excellent biocompatibility and low cytotoxicity.
基金supported by the National Science Foundation for Distinguished Young Scholars (No. 21525419)the National Natural Science Foundation of China (No. 21474054)the National Key Research and Development Program of China (No. 2016YFA0202503)
文摘A facile one-pot synthesis of solid polymer electrolytes(SPEs), composed of carbonate terminated poly(ethylene glycol)(CH3O-PEG-IC), poly(ethylene glycol)-block-polystyrene(PEG-b-PS) block copolymer nanoparticles containing a conductive PEG corona, fumed SiO2 and Li TFSI salt via polymerization-induced self-assembly is proposed. This method to prepare SPEs has the advantages of one-pot convenient synthesis, avoiding use of organic solvent and conveniently adding inorganic additives. CH3O-PEG-IC combines advantages of PEG and polycarbonate, the in situ synthesized PEG-b-PS nanoparticles containing a rigid polystyrene(PS) core and a PEG corona guarantee continuous lithium ion transport in the synthesized SPEs, and the fumed SiO2 optimizes the interfacial properties and improves the electrochemical stability, all of which afford SPEs a well considerable room temperature ionic conductivity of 1.73 × 10^-4S/cm, high lithium transference number of 0.53, and wide electrochemical stability window of 5.5 V(vs. Li^+/Li). By employing these SPEs, the assembled solid state cells of Li FePO4 |SPEs|Li exhibit considerable cell performance.
基金Funded by Program for Changjiang Scholar and Innovative Research Team in University (No.IRT0972)National Natural Science Foundation of China (Nos.20971094, 21176169, 51152001, and 51002102)+2 种基金 Natural Science Foundation of Shanxi Province (No.2009011012-4)PhD Programs Foundation of Ministry of Education of China (No.20101402110007)International S&T Co-operation Program of Shanxi Province(No.2010081017)
文摘Carbon-based films were synthesized by self-assembly of chitosan-encapsulated carbon microsphere （CMS@CS） composite. First, carbon microspheres （CMSs） prepared by chemical vapor deposition were modified by HNO3 and H2O2. Second, oxidized CMSs were modified by chitosan （CS）. Finally, CMS@CS was self-assembled by vertical deposition, in which suspension concentration and deposition temperature on the quality of self-assembling film were investigated. Field emission scanning electron microscopy, atomic force microscopy, X-ray diffraction, thermogravimetry, and Fourier transformation infrared spectrometry were employed to characterize the morphology and structure of the samples. The results show that CMSs modified by CS had uniform particle size and good dispersion, CMS@CS was self-assembled into a dense film, the film thickened with increasing suspension concentration at fixed temperature, and more ordered film was obtained at 1 wt% of suspension concentration and 50 ℃. The ultraviolet-visible absorption spectra show that the absorbance of CMS@CS film grew steadily with increasing suspension concentration and that the CMSs with oxygen-containing groups have a good assembling performance to form composite films with CS.
基金supported by the National Natural Science Foundation of China (No. 21104035)
文摘To clarify the preparation mechanisms of uorinated ordered mesoporous carbon materials (FOMCs), the dissipative par- ticle dynamics method was used to simulate the self-assembly process of the amphiphilic triblock poly(ethylene oxide)- poly(propylene oxide)-poly(ethylene oxide) copolymer Pluronic F127 in the aqueous system. The self-assembly mechanisms in aqueous phase and the formation mechanisms of micropores and mesopores were investigated. It was found that the mesoporous structure of the FOMCs was formed by the hydrophobic segments of F127, while the pore wall was formed by both the hydrophilic segments and the carbon precursor in the system. The microporous structure on the pore wall was con- structed by the carbon source in the hydrophilic segments’ spaces after the template was removed. Our ndings could provide understanding and knowledge for the synthesis of mesoporous carbon by the self-assembly method on the mesoscopic scale.
基金supported by the National Natural Science Foundation of China via Grant Nos.12072134 and 22073048Jiangsu Province NSF via Grant No.BK20191426supported by Jiangsu Province Research Innovation Program Project for University Postgraduates (#KYCX21_3325).
文摘Van der Waals heterostructures composed of low-dimensional atomic layers host rich physics for new device applications,such as magic-angle twisted bilayer graphene and coaxial multi-walled hetero-nanotubes.Aside from exploring their abnormal physical behavior,fabrication of such structures also presents a great challenge to this area,owing to the subtle and sensitive interactions among neighboring layers.Here we show by molecular dynamics simulations that narrow blue phosphorene nanoribbons can be encapsulated into carbon nanotubes driven by van der Waals interactions and form one-dimensional heterostructures.It shows that by varying carbon nanotube diameters and nanoribbon width,the nanoribbons can either retain their original straight structures or twist into tubular structures.Wrapping phases are also observed for large-sized blue phosphorus.It is found that the underlying mechanism originates from the competition between van der Waals energy and bending energy induced by tube curvature.A phase diagram of the resultant 1D structure is thus obtained based on a simple analysis of energetics.The results are expected to stimulate further experimental efforts in fabricating one-dimensional van der Waals heterostructues with desired functionality.
基金supported by the National Natural Science Foundation of China(No.62075069 and 52303092)the Water Conservancy Technology project of Hunan Province,China(XSKJ2021000-32)+1 种基金the City University of Hong Kong(#7005507)the Open Project of Yunnan Precious Metals Laboratory Co.,Ltd(grant number YPML-2023050278).
文摘Nowadays,high-stable and ultrasensitive heavy metal detection is of utmost importance in water quality monitoring.Nanoparticle-enhanced laser-induced breakdown spectroscopy(NELIBS)shows high potential in hazardous metal detection,however,encounters unstable and weak signals due to nonuniform distribution of analytes.Herein,we developed an interface self-assembly(ISA)method to create a uniformly distributed gold nanolayer at a liquid-liquid interface for positive heavy metal ions capture and NELIBS analysis.The electrostatically selfassembled Au nanoparticles(NPs)-analytes membrane was prepared at the oil-water interface by injecting ethanol into the mixture of cyclohexane and Au NPs-analytes water solution.Then,the interface self-assembled Au NPs-analytes membrane was transformed onto a laser-processed superhydrophilic Si slide for detection.Three heavy metals(cadmium(Cd),barium(Ba),and chromium(Cr))were analyzed to evaluate the stability and sensitivity of the ISA method for NELIBS.The results(Cd:RSD=3.6%,LoD=0.654 mg/L;Ba:RSD=3.4%,LoD=0.236 mg/L;Cr:RSD=7.7%,LoD=1.367 mg/L)demonstrated signal enhancement and high-stable and ultrasensitive detection.The actual sample detection(Cd:RE=7.71%,Ba:RE=6.78%)illustrated great reliability.The ISA method,creating a uniform distribution of NP-analytes at the interface,has promising prospects in NELIBS.
基金financially supported by the National Natural Science Foundation of China(Nos.20904047 and 12074151)the Natural Science Foundation of Zhejiang Province(Nos.LY17A040001 and LY19F03004)。
文摘Diphenylalanine and its analogs cause many concerns owing to their perfect self-assembly properties in the fields of biology,medicine,and nanotechnology.Experimental research has shown that diphenylalanine-based analogs with ethylenediamine linkers(PA,P=phenylalanine,and A=analog)can self-assemble into spherical assemblies,which can serve as novel anticancer drug carriers.In this work,to understand the assembly pathways,drug loading behavior,and formation mechanism of PA aggregates at the molecular level,we carried out dissipative particle dynamics(DPD)simulations of PA molecule systems.Our simulation results demonstrate that PA molecules spontaneously assemble into nanospheres and can self-assemble into drug-loaded nanospheres upon addition of the cancer chemotherapeutic agent doxorubicin(DOX).We also found that the hydrophobic side chain beads of PA molecules exhibited a unique onion-like distribution inside the nanospheres,which was not observed in the experiment.The onion-like nanospheres were verified by calculating the radial distribution function(RDF)of the DPD beads.Furthermore,based on the analysis of the percentages of different interaction components in the total nonbonded energies,main chain-side chain interactions between PA molecules may be important in the formation of onion-like nanospheres,and the synergistic effects of main chain-side chain,main chain-drug,side chain-drug,and main chain-solvent interactions are significant in the formation of drug-loaded nanospheres.These findings provide new insights into the structure and self-assembly pathway of PA assemblies,which may be helpful for the design of efficient and effective drug delivery systems.
基金supported by the National Natural Science Foundation of China(Nos.82061148012,82027806,21974019)SEU Innovation Capability Enhancement Plan for Doctoral Students(No.CXJH_SEU 24138)Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX24_0469)。
文摘The potential of metal nanoclusters in biomedical applications is limited due to aggregation-caused quenching(ACQ).In this study,an in situ self-assembled pitaya structure was proposed to obtain stable fluorescence emission through protein coronas-controlled distance between gold nanoclusters(Au NCs).Interestingly,the gold ion complexes coated with proteins of low isoelectric point(pI)nucleate at the secondary structure of proteins with high p I through ionic exchange within cells,generating fluorescent Au NCs.It is worth noting that due to the steric hindrance formed by the protein coronas on the surface of Au NCs,the distance between Au NCs can be controlled,avoiding electron transfer caused by close proximity of Au NCs and inhibiting fluorescence ACQ.This strategy can achieve fluorescence imaging of clinical tissue samples without observable side effects.Therefore,this study proposes a distance-controllable self-assembled pitaya structure to provide a new approach for Au NCs with stable fluorescence.
基金financially supported by the National Natural Science Foundation of China(21902051)the Natural Science Foundation of Fujian Province(2017J01014 and 2019J05090)the Graphene Power and Composite Research Center of Fujian Province(2017H2001)。
文摘For efficient solar energy conversion,the morphology engineering of hollow graphitic carbon nitride(gC3 N4)is one of the promising approachs benefiting from abundant exposed active sites and short photocarrier transport distances,but is difficult to control on account of easy structural collapse.Herein,a facile supramolecular electrostatic self-assembly strategy has been developed for the first time to fabricate mesoporous thin-walled g-C3N4 microtubes(mtw-CNT)with shell thickness of ca.13 nm.The morphological control of g-C3N4 enhances specific surface area by 12 times,induces stronger optical absorption,widens bandgap by 0.18 e V,improves photocurrent density by 2.5 times,and prolongs lifetimes of charge carriers from bulk to surface,compared with those of bulk g-C3N4.As a consequence,the transformed g-C3N4 exhibits the optimum photocatalytic H2-production rate of 3.99 mmol·h^-1·g^-1(λ>420 nm)with remarkable apparent quantum efficiency of 8.7%(λ=420±15 nm)and long-term stability.Moreover,mtw-CNT also achieves high photocatalytic CO2-to-CO selectivity of 96%(λ>420 nm),much better than those on the most previously reported porous g-C3N4 photocatalysts prepared by the conventional hard-templating and soft-templating methods.
基金Project supported by the Natural Science Foundation of Shandong Province (ZR2022QB067)。
文摘The development of new and efficient extractants plays a key role in the separation and recovery of rare earth elements.In this pape r,the extractant(N,N-methyl py ridineethyl-N',N'-dicyclohexyl-3-oxadiglycolamide,MPyEDChDGA) with a new structure was synthesized,and the pyridine group was successfully grafted onto the 3-oxadiglycolamide structure.Using MPyEDChDGA for efficient enrichment of rare earth ions,the self-assembled solids were recovered by simple filtration without further backextraction and final precipitation,achieving a one-step strategy for the recovery of rare earth ions.Several important parameters affecting the self-assembly extraction,including pH,diluent,temperature,and extractant concentration,were systematically evaluated using La(NO_(3))_(3),Tb(NO_(3))_(3),and Lu(NO_(3))_(3) as representatives.The self-assembled solids were investigated in detail by X-ray diffraction(XRD),scanning electron microscopy(SEM),1H nuclear magnetic resonance(1H NMR),Fourier transform infrared spectroscopy(FT-IR),Raman,and X-ray photoelectron spectroscopy(XPS) analyses.The stoichiometry of the extraction species was characterized using the Job's method and electrospray ionization mass spectrometry(ESI-MS).In addition,MPyEDChDGA was applied to the recovery of Sm in SmCoCu simulated liquid,and the results show that MPyEDChDGA has good selectivity of Sm from transition metals(Co,Cu).The separation factor of Sm/Co can reach 6281±117,which provides a new approach to recovering Sm from SmCoCu scrap magnets.This study presents an efficient and convenient new strategy for the recovery and separation of rare earth elements.
基金Project supported by the National Key Research and Development Project of China(2022YFC2905202)Natural Science Foundation of Jiangxi Province(20232ACB204014)Youth Jinggang Scholars Program in Jiangxi Province(QNJG2019056)。
文摘The calcium-containing rare earth solution is generated during the recovery processes of NdFeB waste,which is treated as wastewater by enterprises.In this paper,the carbon dioxide carbonization method was applied to the separation of rare earths and calcium in the solution,as well as the preparation of rare earth oxides with a large specific surface.It is shown that the process of CO_(2)carbonization of solution includes reactions such as the dissolution,diffusion and ionization of CO_(2),the carbonate precipitation of rare earth ions,and the neutralization of hydrogen ions.At a pH of 4.5,the carbonization precipitation rate is effectively controlled,enabling homogeneous precipitation and ensuring both high precipitation yield and rare earth oxides purity.In this way,the crystallization of carbonization products is a process dominated by the oriented attachment theory and coexisting with the Ostwald ripening theory,resulting in abundant pores formed by multiple layers of stacking in the products.With the optimal carbonization conditions,the rare earth precipitation yield solution reaches 99.32%.The obtained carbonization products are crystalline(LaCe)(CO_(3))_(3)·8H_(2)O,and the purity of the rare earth oxides is as high as 99.22 wt%.The specific surface area of the rare earth oxides reaches 94.7 m^(2)/g,and its adsorption efficiency for tetracycline hydrochloride in solution can reach 92.6%in a short time.The rare earth oxides are expected to be used as an adsorption material for wastewater treatment and other adsorption environments.
