The rational design and precise synthesis of multifunctional hybrid nanostructures with a tailored active core and a large, dendritic, modified mesoporous structured shell can promote catalysis, energy storage, and bi...The rational design and precise synthesis of multifunctional hybrid nanostructures with a tailored active core and a large, dendritic, modified mesoporous structured shell can promote catalysis, energy storage, and biological applications. Here, an oil-water biphase stratification coating strategy has been developed to prepare monodisperse magnetic dendritic mesoporous silica core-shell structured nano- spheres. These sophisticated Fe3O4@SiO2@dendritic-mSiO2 nanospheres feature large dendritic open pores （2.7 and 10.3 nm）. Significantly, the silica shells can be converted into dendritic mesoporous aluminosilicate frameworks with unchanged porosity, a Si/Al molar ratio of 14, and remarkably strong acidic sites, through a post-synthesis approach. In addition, the resultant magnetic dendritic mesoporous aluminosilicate nanospheres exhibit outstanding properties and promising application in phosphate removal from wastewater.展开更多
Cross-linkedβ-cyclodextrin polymer/Fe3O4 composite nanoparticles with core-shell structures were prepared via cross linking reaction on the surface of carboxymethylβ-cyclodextrin（CM-β-CD） modified Fe3O4 nanoparti...Cross-linkedβ-cyclodextrin polymer/Fe3O4 composite nanoparticles with core-shell structures were prepared via cross linking reaction on the surface of carboxymethylβ-cyclodextrin（CM-β-CD） modified Fe3O4 nanoparticles inβ-cyclodextrin alkaline solution by using epichlorohydrin as crosslinking agent.The morphology,structure and magnetic properties of the prepared composite nanoparticles were investigated by transmission electron microscopy（TEM）,Fourier transform infrared（FTIR） spectrometry,X-ray diffraction（XRD） measurement,thermogravimetric analysis（TGA） and Vibrating sample magnetometry （VSM）,respectively.展开更多
A focus of the current nanotechnology has shifted from routine fabrication of nanostructures to designing functional electronic devices and realizing their immense potentials for applications. Due to infusion of multi...A focus of the current nanotechnology has shifted from routine fabrication of nanostructures to designing functional electronic devices and realizing their immense potentials for applications. Due to infusion of multi-functionality into a single system, the utilization of hetero-, core/shell and hierarchical nanostructures has become the key issue for building such devices. ZnS, due to its direct wide bandgap, high index of refraction, high transparency in the visible range and intrinsic polarity, is one of the most useful semiconductors for a wide range of electronics applications. This article provides a dense review of the state-of-the-art research activities in one-dimensional （1D） ZnS-based hetero-, core/shell and hierarchical nanostructures. The particular emphasis is put on their syntheses and applications.展开更多
Direct formic acid fuel cells （DFAFCs） allow highly efficient low temperature conversion of chemical energy into electricity and are expected to play a vital role in our future sustainable society. However, the mass...Direct formic acid fuel cells （DFAFCs） allow highly efficient low temperature conversion of chemical energy into electricity and are expected to play a vital role in our future sustainable society. However, the massive precious metal usage in current membrane electrode assembly （MEA） technology greatly inhibits their actual applications. Here we demonstrate a new type of anode constructed by confining highly active nanoengineered catalysts into an ultra-thin catalyst layer with thickness around 100 nm. Specifically, an atomic layer of platinum is first deposited onto nanoporous gold （NPG） leaf to achieve high utilization of Pt and easy accessibility of both reactants and electrons to active sites. These NPG-Pt core/shell nanostructures are further decorated by a sub-monolayer of Bi to create highly active reaction sites for formic acid electro-oxidation. Thus obtained layer-structured NPG-Pt-Bi thin films allow a dramatic decrease in Pt usage down to 3 ~tg.cm-2, while maintaining very high electrode activity and power performance at sufficiently low overall precious metal loading. Moreover, these electrode materials show superior durability during half-year test in actual DFAFCs, with remarkable resistance to common impurities in formic acid, which together imply their great potential in applications in actual devices.展开更多
Developing non-precious metal-based bifunctional electrocatalysts capable for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is essential to achieve efficient water electrolysis for mass hydrog...Developing non-precious metal-based bifunctional electrocatalysts capable for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is essential to achieve efficient water electrolysis for mass hydrogen production,however it remains challenging.Here,we report the synthesis of hierarchical nanorod arrays comprising core-shell structured P-doped NiMoO4@NiFe-coordination polymer(denoted as P-NiMoO4@NiFeCP)as bifunctional electrocatalysts for water electrolysis.Furthermore,we systematically investigate the influence of NiFeCP shell thickness on electrocatalytic activity,manifesting the presence of strong interfacial synergetic effect between P-NiMoO4 and NiFeCP for boosting both the HER and OER.With advantageous hierarchical architectures and unique core-shell structures,optimized P-NiMoO_(4)@NiFeCP-7.3(7.3 is the shell thickness in nm)requires overpotentials of merely 256 and 297 mV to yield a current density of 1000 mA·cm^(−2)for the HER and OER in 1 M KOH,respectively.More importantly,it can serve as a bifunctional electrocatalyst for efficient and sustainable overall water electrolysis,delivering large current densities of 500 and 1000 mA·cm^(−2)at low cell voltages of 1.804 and 1.865 V,along with high stability of over 500 h at 1000 mA·cm−2,demonstrating the great potential of this electrocatalyst towards practical applications.展开更多
The rotator cuff tear has emerged as a significant global health concern.However,existing therapies fail to fully restore the intricate bone-to-tendon gradients,resulting in compromised biomechanical functionalities o...The rotator cuff tear has emerged as a significant global health concern.However,existing therapies fail to fully restore the intricate bone-to-tendon gradients,resulting in compromised biomechanical functionalities of the reconstructed enthesis tissues.Herein,a tri-layered core–shell microfibrous scaffold with layer-specific growth factors(GFs)release is developed using coaxial electrohydrodynamic(EHD)printing for in situ cell recruitment and differentiation to facilitate gradient enthesis tissue repair.Stromal cell-derived factor-1(SDF-1)is loaded in the shell,while basic fibroblast GF,transforming GF-beta,and bone morphogenetic protein-2 are loaded in the core of the EHD-printed microfibrous scaffolds in a layer-specific manner.Correspondingly,the tri-layered microfibrous scaffolds have a core–shell fiber size of(25.7±5.1)μm,with a pore size sequentially increasing from(81.5±4.6)μm to(173.3±6.9)μm,and to(388.9±6.9μm)for the tenogenic,chondrogenic,and osteogenic instructive layers.A rapid release of embedded GFs is observed within the first 2 d,followed by a faster release of SDF-1 and a slightly slower release of differentiation GFs for approximately four weeks.The coaxial EHD-printed microfibrous scaffolds significantly promote stem cell recruitment and direct their differentiation toward tenocyte,chondrocyte,and osteocyte phenotypes in vitro.When implanted in vivo,the tri-layered core–shell microfibrous scaffolds rapidly restored the biomechanical functions and promoted enthesis tissue regeneration with native-like bone-to-tendon gradients.Our findings suggest that the microfibrous scaffolds with layer-specific GFs release may offer a promising clinical solution for enthesis regeneration.展开更多
Catechol-formaldehyde resin(CFR)is very attractive for H_(2)O_(2) production via the catalytic process.However,the H2O2 formation is accompanied by the oxidation of catechol groups to o-benzoquinone groups on CFR,whic...Catechol-formaldehyde resin(CFR)is very attractive for H_(2)O_(2) production via the catalytic process.However,the H2O2 formation is accompanied by the oxidation of catechol groups to o-benzoquinone groups on CFR,which will cause irreversible damage to CFR and greatly limit its long-term stable catalytic activity.Herein,CdS/CFR composite photocatalyst with a core-shell structure was synthesized by hydrothermal method.The photogenerated electrons of Cds are used as a powerful driving force for the reversible redox conversion between catechol groups and o-benzoquinone groups on the CFR.展开更多
NdFeB magnets are third-generation permanent magnets that are employed as indispensable components in various industries.Notably,rare-earth elements(REEs)such as Dy and Nd must be efficiently recovered from end-of-lif...NdFeB magnets are third-generation permanent magnets that are employed as indispensable components in various industries.Notably,rare-earth elements(REEs)such as Dy and Nd must be efficiently recovered from end-of-life magnets to enable resource circulation and reinforce unstable supply chains.To that end,this paper reports synergistically performing core/shell-structured composite fibers(CSCFs)containing sodium polyacrylate and nanoporous zeolitic imidazolate framework-8(NPZIF-8)nanocrystals as a readily recoverable adsorbent with an exceptional REE-adsorbing ability.The CSCF core forms an NPZIF-8 nanocrystal shell on the fiber surface as well as draws REEs using its dense sodium carboxylate groups into the NPZIF-8 nanocrystal lattice with high specific surface area.The CSCFs exhibit significantly higher maximum adsorption capacities(468.60 and 435.13 mg·g-1)and kinetic rate constants(2.02 and 1.92 min-1)for the Nd3+and Dy3+REEs than those of previously reported REE adsorbents.Additionally,the simple application of the CSCFs to an adsorption reactor considerably mitigates the adsorbent-shape-induced pressure drop,thereby directly influencing the energy efficiency of the recovery.Moreover,the high REE-recovery ability,tractability,and recyclability of the CSCFs offers a pragmatic pathway to achieving cost-effective REE recovery.Overall,this study provides new insights into designing synergistically performing core/shell architectures for feasible REE recovery.展开更多
The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by ...The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by increasing its bactericidal performance,the emergence of drug resistance is certainly delayed,so that there's not enough time for developing drug resistance during treatment.Therefore,we selected typical representative materials of metal Ag and semiconductor ZnO nano-bactericides to design and synthesize Ag/ZnO hollow core-shell structures(AZ for short).Antibiotics are grafted on the surface of AZ through rational modification to form a composite sterilization system.The research results show that the antibacterial efficiency of the composite system is significantly increased,from the sum(34.7%+22.8%-57.5%)of the antibacterial efficiency of AZ and gentamicin to 80.2%,net synergizes 22.7%,which fully reflects the effect of 1+1>2.Therefore,the dosage of antibiotics can be drastically reduced in this way,which makes both the possibility of bacterial resistance and medical expenses remarkably decrease.Subsequently,residual antibiotics can be degraded under simple illumination using AZ-self as a photocatalyst,which cuts off the path of environmental pollution.In short,such an innovative route has guiding significance for drug resistance.展开更多
Confined nanospace pyrolysis(CNP)has attracted increasing attention as a general strategy to prepare task-specific hollow structured porous carbons(HSPCs)in the past decade.The unique advantages of the CNP strategy in...Confined nanospace pyrolysis(CNP)has attracted increasing attention as a general strategy to prepare task-specific hollow structured porous carbons(HSPCs)in the past decade.The unique advantages of the CNP strategy include its outstanding ability in control of the monodispersity,porosity and internal cavity of HSPCs.As a consequence,the obtained HSPCs perform exceptionally well in applications where a high dispersibility and tailored cavity are particularly required,such as drug delivery,energy storage,catalysis and so on.In this review,the fundamentals of the CNP strategy and its advances in structural alternation is first summarized,then typical applications are discussed by exemplifying specific synthesis examples.In addition,this review offers insights into future developments for advanced task-specific hollow structured porous materials prepared by the CNP strategy.展开更多
基金We acknowledge the financial support from State Key Laboratory of Pollution Control and Resource Reuse Foundation （No. PCRRF14017）, the National Natural Science Foundation of China （No. 21210004） and the China Postdoctoral Science Foundation （No. 2014M551455）. J. P. Y. appreciates the funding supported by the Commonwealth of Australia through the Automotive Australia 2020 Cooperative Research Centre （Auto CRC） and DP120101194. The authors would like to thank Dr. T. Silver for critical reading of this manuscript.
文摘The rational design and precise synthesis of multifunctional hybrid nanostructures with a tailored active core and a large, dendritic, modified mesoporous structured shell can promote catalysis, energy storage, and biological applications. Here, an oil-water biphase stratification coating strategy has been developed to prepare monodisperse magnetic dendritic mesoporous silica core-shell structured nano- spheres. These sophisticated Fe3O4@SiO2@dendritic-mSiO2 nanospheres feature large dendritic open pores （2.7 and 10.3 nm）. Significantly, the silica shells can be converted into dendritic mesoporous aluminosilicate frameworks with unchanged porosity, a Si/Al molar ratio of 14, and remarkably strong acidic sites, through a post-synthesis approach. In addition, the resultant magnetic dendritic mesoporous aluminosilicate nanospheres exhibit outstanding properties and promising application in phosphate removal from wastewater.
基金financially supported by the Guangdong Natural Science Foundation(No.020891)
文摘Cross-linkedβ-cyclodextrin polymer/Fe3O4 composite nanoparticles with core-shell structures were prepared via cross linking reaction on the surface of carboxymethylβ-cyclodextrin（CM-β-CD） modified Fe3O4 nanoparticles inβ-cyclodextrin alkaline solution by using epichlorohydrin as crosslinking agent.The morphology,structure and magnetic properties of the prepared composite nanoparticles were investigated by transmission electron microscopy（TEM）,Fourier transform infrared（FTIR） spectrometry,X-ray diffraction（XRD） measurement,thermogravimetric analysis（TGA） and Vibrating sample magnetometry （VSM）,respectively.
基金World Premier International Research Center Initiative(WPI Initiative)on Materials Nanoarchitronics,MEXT,Japanthe Japan Society for the Promotion of Science (JSPS)for a support in the form of a fellowship tenable at the National Institute for Materials Science,Tsukuba,Japan.
文摘A focus of the current nanotechnology has shifted from routine fabrication of nanostructures to designing functional electronic devices and realizing their immense potentials for applications. Due to infusion of multi-functionality into a single system, the utilization of hetero-, core/shell and hierarchical nanostructures has become the key issue for building such devices. ZnS, due to its direct wide bandgap, high index of refraction, high transparency in the visible range and intrinsic polarity, is one of the most useful semiconductors for a wide range of electronics applications. This article provides a dense review of the state-of-the-art research activities in one-dimensional （1D） ZnS-based hetero-, core/shell and hierarchical nanostructures. The particular emphasis is put on their syntheses and applications.
文摘Direct formic acid fuel cells （DFAFCs） allow highly efficient low temperature conversion of chemical energy into electricity and are expected to play a vital role in our future sustainable society. However, the massive precious metal usage in current membrane electrode assembly （MEA） technology greatly inhibits their actual applications. Here we demonstrate a new type of anode constructed by confining highly active nanoengineered catalysts into an ultra-thin catalyst layer with thickness around 100 nm. Specifically, an atomic layer of platinum is first deposited onto nanoporous gold （NPG） leaf to achieve high utilization of Pt and easy accessibility of both reactants and electrons to active sites. These NPG-Pt core/shell nanostructures are further decorated by a sub-monolayer of Bi to create highly active reaction sites for formic acid electro-oxidation. Thus obtained layer-structured NPG-Pt-Bi thin films allow a dramatic decrease in Pt usage down to 3 ~tg.cm-2, while maintaining very high electrode activity and power performance at sufficiently low overall precious metal loading. Moreover, these electrode materials show superior durability during half-year test in actual DFAFCs, with remarkable resistance to common impurities in formic acid, which together imply their great potential in applications in actual devices.
基金the Shenzhen Science and Technology Program(Nos.SGDX20201103095802006,RCYX20200714114535052,JCYJ20190808150001775,and JCYJ20190808143007479)the National Natural Science Foundation of China(Nos.U21A20312 and 21975162).
文摘Developing non-precious metal-based bifunctional electrocatalysts capable for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is essential to achieve efficient water electrolysis for mass hydrogen production,however it remains challenging.Here,we report the synthesis of hierarchical nanorod arrays comprising core-shell structured P-doped NiMoO4@NiFe-coordination polymer(denoted as P-NiMoO4@NiFeCP)as bifunctional electrocatalysts for water electrolysis.Furthermore,we systematically investigate the influence of NiFeCP shell thickness on electrocatalytic activity,manifesting the presence of strong interfacial synergetic effect between P-NiMoO4 and NiFeCP for boosting both the HER and OER.With advantageous hierarchical architectures and unique core-shell structures,optimized P-NiMoO_(4)@NiFeCP-7.3(7.3 is the shell thickness in nm)requires overpotentials of merely 256 and 297 mV to yield a current density of 1000 mA·cm^(−2)for the HER and OER in 1 M KOH,respectively.More importantly,it can serve as a bifunctional electrocatalyst for efficient and sustainable overall water electrolysis,delivering large current densities of 500 and 1000 mA·cm^(−2)at low cell voltages of 1.804 and 1.865 V,along with high stability of over 500 h at 1000 mA·cm−2,demonstrating the great potential of this electrocatalyst towards practical applications.
基金financially supported by the National Key Research and Development Program of China(2018YFA0703003)National Natural Science Foundation of China(82072429,52125501,82371590)+6 种基金the Program for Innovation Team of Shaanxi Province(2023-CX-TD-17)the Key Research&Development Program of Shaanxi Province(2024SF-YBXM-355,2020SF-093,2021LLRH-08)the Natural Science Foundation of Henan Province(222300420358)the Postdoctoral Project of Shaanxi Province(2023BSHYDZZ30)the Postdoctoral Fellowship Program of CPSF(GZB20230573)the Institutional Foundation of the First Affiliated Hospital of Xi’an Jiaotong University(2019ZYTS-02)the Fundamental Research Funds for the Central Universities.
文摘The rotator cuff tear has emerged as a significant global health concern.However,existing therapies fail to fully restore the intricate bone-to-tendon gradients,resulting in compromised biomechanical functionalities of the reconstructed enthesis tissues.Herein,a tri-layered core–shell microfibrous scaffold with layer-specific growth factors(GFs)release is developed using coaxial electrohydrodynamic(EHD)printing for in situ cell recruitment and differentiation to facilitate gradient enthesis tissue repair.Stromal cell-derived factor-1(SDF-1)is loaded in the shell,while basic fibroblast GF,transforming GF-beta,and bone morphogenetic protein-2 are loaded in the core of the EHD-printed microfibrous scaffolds in a layer-specific manner.Correspondingly,the tri-layered microfibrous scaffolds have a core–shell fiber size of(25.7±5.1)μm,with a pore size sequentially increasing from(81.5±4.6)μm to(173.3±6.9)μm,and to(388.9±6.9μm)for the tenogenic,chondrogenic,and osteogenic instructive layers.A rapid release of embedded GFs is observed within the first 2 d,followed by a faster release of SDF-1 and a slightly slower release of differentiation GFs for approximately four weeks.The coaxial EHD-printed microfibrous scaffolds significantly promote stem cell recruitment and direct their differentiation toward tenocyte,chondrocyte,and osteocyte phenotypes in vitro.When implanted in vivo,the tri-layered core–shell microfibrous scaffolds rapidly restored the biomechanical functions and promoted enthesis tissue regeneration with native-like bone-to-tendon gradients.Our findings suggest that the microfibrous scaffolds with layer-specific GFs release may offer a promising clinical solution for enthesis regeneration.
基金the financial support for this work provided by the Jilin Provincial Natural Science Foundation of China(No.20210101404JC)National Natural Science Foundation of China(22271044).
文摘Catechol-formaldehyde resin(CFR)is very attractive for H_(2)O_(2) production via the catalytic process.However,the H2O2 formation is accompanied by the oxidation of catechol groups to o-benzoquinone groups on CFR,which will cause irreversible damage to CFR and greatly limit its long-term stable catalytic activity.Herein,CdS/CFR composite photocatalyst with a core-shell structure was synthesized by hydrothermal method.The photogenerated electrons of Cds are used as a powerful driving force for the reversible redox conversion between catechol groups and o-benzoquinone groups on the CFR.
基金supported by grants from the National R&D program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(MSIT)(nos.2020M3H4A3106366 and RS-2023-00209565)by an institutional program grant(2E33081)From the Korea Institute of Science and Technology.
文摘NdFeB magnets are third-generation permanent magnets that are employed as indispensable components in various industries.Notably,rare-earth elements(REEs)such as Dy and Nd must be efficiently recovered from end-of-life magnets to enable resource circulation and reinforce unstable supply chains.To that end,this paper reports synergistically performing core/shell-structured composite fibers(CSCFs)containing sodium polyacrylate and nanoporous zeolitic imidazolate framework-8(NPZIF-8)nanocrystals as a readily recoverable adsorbent with an exceptional REE-adsorbing ability.The CSCF core forms an NPZIF-8 nanocrystal shell on the fiber surface as well as draws REEs using its dense sodium carboxylate groups into the NPZIF-8 nanocrystal lattice with high specific surface area.The CSCFs exhibit significantly higher maximum adsorption capacities(468.60 and 435.13 mg·g-1)and kinetic rate constants(2.02 and 1.92 min-1)for the Nd3+and Dy3+REEs than those of previously reported REE adsorbents.Additionally,the simple application of the CSCFs to an adsorption reactor considerably mitigates the adsorbent-shape-induced pressure drop,thereby directly influencing the energy efficiency of the recovery.Moreover,the high REE-recovery ability,tractability,and recyclability of the CSCFs offers a pragmatic pathway to achieving cost-effective REE recovery.Overall,this study provides new insights into designing synergistically performing core/shell architectures for feasible REE recovery.
基金supported by the National Natural Science Foundation of China(Nos.22176145,82172612)the State Key Laboratory of Fine Chemicals,Dalian University of Technology(KF 2001)the Fundamental Research Funds for the Central Universities(22120210137).
文摘The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by increasing its bactericidal performance,the emergence of drug resistance is certainly delayed,so that there's not enough time for developing drug resistance during treatment.Therefore,we selected typical representative materials of metal Ag and semiconductor ZnO nano-bactericides to design and synthesize Ag/ZnO hollow core-shell structures(AZ for short).Antibiotics are grafted on the surface of AZ through rational modification to form a composite sterilization system.The research results show that the antibacterial efficiency of the composite system is significantly increased,from the sum(34.7%+22.8%-57.5%)of the antibacterial efficiency of AZ and gentamicin to 80.2%,net synergizes 22.7%,which fully reflects the effect of 1+1>2.Therefore,the dosage of antibiotics can be drastically reduced in this way,which makes both the possibility of bacterial resistance and medical expenses remarkably decrease.Subsequently,residual antibiotics can be degraded under simple illumination using AZ-self as a photocatalyst,which cuts off the path of environmental pollution.In short,such an innovative route has guiding significance for drug resistance.
基金financially supported by the National Natural Science Foundation of China(Nos.20873014 and 21073026)National Natural Science Foundation for Distinguished Young Scholars(No.21225312)the Cheung Kong Scholars Program of China(No.T2015036).
文摘Confined nanospace pyrolysis(CNP)has attracted increasing attention as a general strategy to prepare task-specific hollow structured porous carbons(HSPCs)in the past decade.The unique advantages of the CNP strategy include its outstanding ability in control of the monodispersity,porosity and internal cavity of HSPCs.As a consequence,the obtained HSPCs perform exceptionally well in applications where a high dispersibility and tailored cavity are particularly required,such as drug delivery,energy storage,catalysis and so on.In this review,the fundamentals of the CNP strategy and its advances in structural alternation is first summarized,then typical applications are discussed by exemplifying specific synthesis examples.In addition,this review offers insights into future developments for advanced task-specific hollow structured porous materials prepared by the CNP strategy.
