Achieving efficient adsorption and desorption processes by controllably tuning the properties of adsorbents at different technical stages is extremely attractive.However,it is difficult for traditional adsorbents to r...Achieving efficient adsorption and desorption processes by controllably tuning the properties of adsorbents at different technical stages is extremely attractive.However,it is difficult for traditional adsorbents to reach the target because of their fixed active sites.Herein,we report on the fabrication of a smart adsorbent,which was achieved by introducing photoresponsive azobenzene derivatives with cis/trans isomers to Ce-doped mesoporous silica.These photoresponsive groups serve as “molecular switches”by sheltering and exposing active sites,leading to efficient adsorption and desorption.Ce is also doped to provide additional active sites in order to enhance the adsorption performance.The results show that the cis isomers effectively shelter the active sites,leading to the selective adsorption of methylene blue(MB)over brilliant blue(BB),while the trans isomers completely expose the active sites,resulting in the convenient release of the adsorbates.Both selective adsorption and efficient desorption can be realized controllably by these smart adsorbents through photostimulation.Moreover,the performance of the obtained materials is well maintained after five cycles.展开更多
In order to improve the proton conductivity of hollow silica spheres （HSS）/perfluorosulfonic acid ion-exchange （PFSA） composite membranes as proton exchange membrane,sulfonic acid groups were grafted onto the surf...In order to improve the proton conductivity of hollow silica spheres （HSS）/perfluorosulfonic acid ion-exchange （PFSA） composite membranes as proton exchange membrane,sulfonic acid groups were grafted onto the surfaces of HSS via post grafting methods.TEM images and FT-IR spectra of the obtained sulfonic acid groups modified hollow silica spheres （SAMHSS） illustrated that the sulfonic acid groups were successfully grafted onto the surfaces of HSS.Water uptake and swelling degree of SAMHSS/PFSA composite membranes were found much higher than those of HSS/PFSA membranes due to the introduction of hydrophilic sulfonic acid groups.In a range from 50 ℃ to 130 ℃,the highest conductivity of composite membranes was obtained when 5 wt% SAMHSS was loaded.The maximum conductivity reached 7.5×10-2 S·cm-1 at 100 ℃ and 100% relative humidity,even the temperature increased to 130 ℃,the conductivity of composite membranes with 5 wt% SAMHSS could reach 3.7×10-2 S·cm-1 at 100 % relative humidity,while the conductivity of the recast PFSA was only 2.2×10-3 S·cm-1.展开更多
The magnetic hollow silica spheres (MHSS) with uniform cavity size and shell thickness were prepared by a simple and “green” method using functionalized SiO2 spheres as templates. Magnetic particles (Fe3O4) were dep...The magnetic hollow silica spheres (MHSS) with uniform cavity size and shell thickness were prepared by a simple and “green” method using functionalized SiO2 spheres as templates. Magnetic particles (Fe3O4) were deposited on the SiO2 surface by varying the molar ratio of [Fe2+]/[Fe3+] and the molar concentration of iron salts. The obtained magnetic hollow silica spheres exhibited a super-paramagnetic behavior at room temperature. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray powder scattering (XRD) were applied to characterize the MHSS. Besides, their unit cell parameters are calculated according to results indexing to XRD, the MHSS sample prepared at 0.10 M iron salts and 2:1 molar ratio of [Fe2+]/[Fe3+] has a largest cell angle (β) of unit cell. Due to large hollow cavity space and super-paramagnetic characteristics, the inner amino-functionalized MHSS could be labeled with radioisotope 99Tcm to study the MHSS’s magnetic targeting distribution in vivo. These results indicate that the MHSS has potential in the magnetic targeted drug delivery system which reduces the damage to normal cells and improves the therapeutic effect of cancer.展开更多
A self-regulated anti-diabetic drug release device mimicking pancreatic cells is highly desirable for the therapy of diabetes. Herein, a glucose-mediated dual-responsive drug delivery system, which combines pH-and H_(...A self-regulated anti-diabetic drug release device mimicking pancreatic cells is highly desirable for the therapy of diabetes. Herein, a glucose-mediated dual-responsive drug delivery system, which combines pH-and H_(2)O_(2)-responsive block copolymer grafted hollow mesoporous silica nanoparticles(HMSNs)with microneedle(MN) array patch, has been developed to achieve self-regulated administration.The poly[4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)benzyl acrylate]-b-poly[2-(dimethylamino)ethyl methacrylate](PPBEM-b-PDM) polymer serves as gate keeper to prevent drug release from the cavity of HMSNs at normoglycemic level. In contrast, the drug release rate is significantly enhanced upon H_(2)O_(2)and pH stimuli due to the chemical change of H_(2)O_(2)sensitive PPBEM block and acid responsive PDM block. Therefore, incorporation of anti-diabetic drug and glucose oxidase(GOx, which can oxidize glucose to gluconic acid and in-situ produce H_(2)O_(2)) into stimulus polymer coated HMSNs results in a glucose-mediated MN device after depositing the drug-loaded nanoparticles into MN array patch. Both in vitro and in vivo results show this MN device presents a glucose mediated self-regulated drug release characteristic, which possesses a rapid drug release at hyperglycemic level but retarded drug release at normoglycemic level. The result indicates that the fabricated smart drug delivery system is a good candidate for the therapy of diabetes.展开更多
Si/Al composite hollow spheres with a surface hole were prepared with the co-axial microchannel in a one-step method. It is easy to use the technique for size control and continuous operation. At Si/Al ratio between 4...Si/Al composite hollow spheres with a surface hole were prepared with the co-axial microchannel in a one-step method. It is easy to use the technique for size control and continuous operation. At Si/Al ratio between 4 and 5, a hole forms on the surface, due to the fast gelation process and high viscosity of the sol. Scanning electron microscopy, nitrogen adsorption–desorption isotherms, and mercury intrusion method are used to characterize the samples. The hole size is 40–150 μm and the particle size is 450–600 μm. The size can be adjusted by the flow rate of the oil phase.展开更多
Hollow core-shell structure nanomaterials have been broadly used in energy storage, catalysis, reactor,and other fields due to their unique characteristics, including the synergy between different materials,a large sp...Hollow core-shell structure nanomaterials have been broadly used in energy storage, catalysis, reactor,and other fields due to their unique characteristics, including the synergy between different materials,a large specific surface area, small density, large charge carrying capacity and so on. However, their synthesis processes were mostly complicated, and few researches reported one-step encapsulation of different valence states of precious metals in carbon-based materials. Hence, a novel hollow core-shell nanostructure electrode material, RuO_(2)@Ru/HCs, with a lower mass of ruthenium to reduce costs was constructed by one-step hydrothermal method with hard template and co-assembled strategy, consisting of RuO_(2) core and ruthenium nanoparticles(Ru NPs) in carbon shell. The Ru NPs were uniformly assembled in the carbon layer, which not only improved the electronic conductivity but also provided more active centers to enhance the pseudocapacitance. The RuO_(2) core further enhanced the material’s energy storage capacity. Excellent capacitance storage(318.5 F·g^(-1)at 0.5 A·g^(-1)), rate performance(64.4%) from 0.5 A·g^(-1)to 20 A·g^(-1), and cycling stability(92.3% retention after 5000 cycles) were obtained by adjusting Ru loading to 0.92%(mass). It could be attributed to the wider pore size distribution in the micropores which increased the transfer of electrons and protons. The symmetrical supercapacitor device based on RuO_(2)@Ru/HCs could successfully light up the LED lamp. Therefore, our work verified that interfacial modification of RuO_(2) and carbon could bring attractive insights into energy density for nextgeneration supercapacitors.展开更多
3D-printed Porous Titanium Alloy Implants(pTi),owing to their biologically inertness and relatively smooth surface morphology,adversely affect the biological functions of surrounding cells.To address the challenges,co...3D-printed Porous Titanium Alloy Implants(pTi),owing to their biologically inertness and relatively smooth surface morphology,adversely affect the biological functions of surrounding cells.To address the challenges,constructing a bioinspired interface that mimics the hierarchical structure of bone tissue can enhance the cellular functions of cells.In this context,Hollow Mesoporous Silica Nanoparticles(HMSNs),renowned for their unique physicochemical properties and superior biocompatibility,offer a promising direction for this research.In this research,the initially synthesized HMSNs were used to construct a“hollow-mesoporous-macroporous”hierarchical bioinspired coating on the pTi surface through the Layer-by-Layer technique.Simultaneously,diverse morphologies of coatings were established by adjusting the deposition strategy of PDDA/HMSNs on the pTi surface(pTi-HMSN-2,pTi-HMSN-4,pTi-HMSN-6).A range of techniques were employed to investigate the physicochemical properties and regulation of cellular biological functions of the diverse HMSN coating strategies.Notably,the pTi-HMSN-4 and pTi-HMSN-6 groups exhibited the uniform coatings,leading to a substantial enhancement in surface roughness and hydrophilicity.Meantime,the coating constructed strategy of pTi-HMSN-4 possessed commendable stability.Based on the aforementioned findings,both pTi-HMSN-4 and pTi-HMSN-6 facilitated the adhesion,spreading,and pseudopodia extension of BMSCs,which led to a notable upsurge in the expression levels of vinculin protein in BMSCs.Comprehensive analysis indicates that the coating,when PDDA/HMSNs are deposited four times,possesses favorable overall performance.The research will provide a solid theoretical basis for the translation of HMSN bioinspired coatings for orthopedic implants.展开更多
Silica nanoparticles have been one of the most promising nanosystems for biomedical applications due to their facile surface chemistry and non-toxic nature. However, it is still challenging to effectively deliver them...Silica nanoparticles have been one of the most promising nanosystems for biomedical applications due to their facile surface chemistry and non-toxic nature. However, it is still challenging to effectively deliver them into tumor sites and noninvasively visualize their in vivo biodistribution with excellent sensitivity and accuracy for effective cancer diagnosis. In this study, we design a yolk/shell-structured silica nanosystem ^(64) Cu-NOTAQD@HMSN-PEG-TRC105, which can be employed for tumor vasculature targeting and dual-modality PET/optical imaging, leading to superior targeting specificity, excellentimaging capability and more reliable diagnostic outcomes.By combining vasculature targeting, pH-sensitive drug delivery, and dual-modality imaging into a single platform,as-designed yolk/shell-structured silica nanosystems may be employed for the future image-guided tumor-targeted drug delivery, to further enable cancer theranostics.展开更多
Hollow mesoporous silica spheres with magnetite cores(HMSMC) have been fabricated by Vacuum Nano-casting Route. The amount of magnetite cores and saturation magnetization value can be easily adjusted by changing the c...Hollow mesoporous silica spheres with magnetite cores(HMSMC) have been fabricated by Vacuum Nano-casting Route. The amount of magnetite cores and saturation magnetization value can be easily adjusted by changing the concentration of iron nitrate solution used in the synthesis procedure. Furthermore, the as-prepared HMSMCs still maintain narrow mesopore distribution, high surface area and large pore volume after the hollow cores of hollow mesoporous silica spheres were filled with magnetite particles. Specially, when the saturation magnetization value of as-prepared HMSMCs reaches 22.0 emu/g, the surface area and pore volume of corresponding HMSMCs are 149 m^2/g and 0.19 cm^3/g, respectively, and the pore size is 2.30 nm. The corresponding samples are characterized by X-ray diffraction, N_2 sorption isotherms, transmission electron microscopy and vibrating-sample magnetometer.展开更多
基金This work was supported by the National Science Fund for Excellent Young Scholars(21722606)the National Natural Science Foundation of China(21676138,21878149,21808110,and 21576137)+1 种基金the China Postdoctoral Science Foundation(2018M632295)the Six Talent Plan(2016XCL031).
文摘Achieving efficient adsorption and desorption processes by controllably tuning the properties of adsorbents at different technical stages is extremely attractive.However,it is difficult for traditional adsorbents to reach the target because of their fixed active sites.Herein,we report on the fabrication of a smart adsorbent,which was achieved by introducing photoresponsive azobenzene derivatives with cis/trans isomers to Ce-doped mesoporous silica.These photoresponsive groups serve as “molecular switches”by sheltering and exposing active sites,leading to efficient adsorption and desorption.Ce is also doped to provide additional active sites in order to enhance the adsorption performance.The results show that the cis isomers effectively shelter the active sites,leading to the selective adsorption of methylene blue(MB)over brilliant blue(BB),while the trans isomers completely expose the active sites,resulting in the convenient release of the adsorbates.Both selective adsorption and efficient desorption can be realized controllably by these smart adsorbents through photostimulation.Moreover,the performance of the obtained materials is well maintained after five cycles.
基金Funded by National Natural Science Foundation of China(No.50803046)
文摘In order to improve the proton conductivity of hollow silica spheres （HSS）/perfluorosulfonic acid ion-exchange （PFSA） composite membranes as proton exchange membrane,sulfonic acid groups were grafted onto the surfaces of HSS via post grafting methods.TEM images and FT-IR spectra of the obtained sulfonic acid groups modified hollow silica spheres （SAMHSS） illustrated that the sulfonic acid groups were successfully grafted onto the surfaces of HSS.Water uptake and swelling degree of SAMHSS/PFSA composite membranes were found much higher than those of HSS/PFSA membranes due to the introduction of hydrophilic sulfonic acid groups.In a range from 50 ℃ to 130 ℃,the highest conductivity of composite membranes was obtained when 5 wt% SAMHSS was loaded.The maximum conductivity reached 7.5×10-2 S·cm-1 at 100 ℃ and 100% relative humidity,even the temperature increased to 130 ℃,the conductivity of composite membranes with 5 wt% SAMHSS could reach 3.7×10-2 S·cm-1 at 100 % relative humidity,while the conductivity of the recast PFSA was only 2.2×10-3 S·cm-1.
文摘The magnetic hollow silica spheres (MHSS) with uniform cavity size and shell thickness were prepared by a simple and “green” method using functionalized SiO2 spheres as templates. Magnetic particles (Fe3O4) were deposited on the SiO2 surface by varying the molar ratio of [Fe2+]/[Fe3+] and the molar concentration of iron salts. The obtained magnetic hollow silica spheres exhibited a super-paramagnetic behavior at room temperature. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray powder scattering (XRD) were applied to characterize the MHSS. Besides, their unit cell parameters are calculated according to results indexing to XRD, the MHSS sample prepared at 0.10 M iron salts and 2:1 molar ratio of [Fe2+]/[Fe3+] has a largest cell angle (β) of unit cell. Due to large hollow cavity space and super-paramagnetic characteristics, the inner amino-functionalized MHSS could be labeled with radioisotope 99Tcm to study the MHSS’s magnetic targeting distribution in vivo. These results indicate that the MHSS has potential in the magnetic targeted drug delivery system which reduces the damage to normal cells and improves the therapeutic effect of cancer.
基金financially supported by the Zhejiang Provincial Natural Science Foundation of China (LY20E030005)Natural Science Foundation of Zhejiang Education Department (Y201942793)the Opening Project of Jiangxi Province Key Laboratory of Polymer Micro/Nano Manufacturing and Devices (PMND201905)。
文摘A self-regulated anti-diabetic drug release device mimicking pancreatic cells is highly desirable for the therapy of diabetes. Herein, a glucose-mediated dual-responsive drug delivery system, which combines pH-and H_(2)O_(2)-responsive block copolymer grafted hollow mesoporous silica nanoparticles(HMSNs)with microneedle(MN) array patch, has been developed to achieve self-regulated administration.The poly[4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)benzyl acrylate]-b-poly[2-(dimethylamino)ethyl methacrylate](PPBEM-b-PDM) polymer serves as gate keeper to prevent drug release from the cavity of HMSNs at normoglycemic level. In contrast, the drug release rate is significantly enhanced upon H_(2)O_(2)and pH stimuli due to the chemical change of H_(2)O_(2)sensitive PPBEM block and acid responsive PDM block. Therefore, incorporation of anti-diabetic drug and glucose oxidase(GOx, which can oxidize glucose to gluconic acid and in-situ produce H_(2)O_(2)) into stimulus polymer coated HMSNs results in a glucose-mediated MN device after depositing the drug-loaded nanoparticles into MN array patch. Both in vitro and in vivo results show this MN device presents a glucose mediated self-regulated drug release characteristic, which possesses a rapid drug release at hyperglycemic level but retarded drug release at normoglycemic level. The result indicates that the fabricated smart drug delivery system is a good candidate for the therapy of diabetes.
基金Supported by the National Basic Research Foundation of China(2013CB733600)the National Natural Science Foundation(20976096,21036002)the Innovative Science and Technology Foundation of Petro China(2011D-5006-0407)
文摘Si/Al composite hollow spheres with a surface hole were prepared with the co-axial microchannel in a one-step method. It is easy to use the technique for size control and continuous operation. At Si/Al ratio between 4 and 5, a hole forms on the surface, due to the fast gelation process and high viscosity of the sol. Scanning electron microscopy, nitrogen adsorption–desorption isotherms, and mercury intrusion method are used to characterize the samples. The hole size is 40–150 μm and the particle size is 450–600 μm. The size can be adjusted by the flow rate of the oil phase.
基金supported by Jinan Mingzhu Co., Ltd (HX20200364)。
文摘Hollow core-shell structure nanomaterials have been broadly used in energy storage, catalysis, reactor,and other fields due to their unique characteristics, including the synergy between different materials,a large specific surface area, small density, large charge carrying capacity and so on. However, their synthesis processes were mostly complicated, and few researches reported one-step encapsulation of different valence states of precious metals in carbon-based materials. Hence, a novel hollow core-shell nanostructure electrode material, RuO_(2)@Ru/HCs, with a lower mass of ruthenium to reduce costs was constructed by one-step hydrothermal method with hard template and co-assembled strategy, consisting of RuO_(2) core and ruthenium nanoparticles(Ru NPs) in carbon shell. The Ru NPs were uniformly assembled in the carbon layer, which not only improved the electronic conductivity but also provided more active centers to enhance the pseudocapacitance. The RuO_(2) core further enhanced the material’s energy storage capacity. Excellent capacitance storage(318.5 F·g^(-1)at 0.5 A·g^(-1)), rate performance(64.4%) from 0.5 A·g^(-1)to 20 A·g^(-1), and cycling stability(92.3% retention after 5000 cycles) were obtained by adjusting Ru loading to 0.92%(mass). It could be attributed to the wider pore size distribution in the micropores which increased the transfer of electrons and protons. The symmetrical supercapacitor device based on RuO_(2)@Ru/HCs could successfully light up the LED lamp. Therefore, our work verified that interfacial modification of RuO_(2) and carbon could bring attractive insights into energy density for nextgeneration supercapacitors.
基金supported by the National Natural Science Foundation of China(Grant No.82372391,82001971,82102358,82202698,52105343,U21A2099 and U23A20523)Project of“Medical+X”interdisciplinary innovation team of Norman Bethune Health Science Center of Jilin University(Grant No.2022JBGS06)+5 种基金Project of youth interdisciplinary innovation team of Jilin University(Grant No.419070623054)China Postdoctoral Science Foundation(Grant No.2021M701384)Bethune Plan of Jilin University(Grant No.2022B27,2022B03)Wu Jieping Medical Foundation(Grant No.320.6750.18522)Scientific Development Program of Jilin Province(Grant No.20220402067GH)Jilin Province Development and Reform Commission(Grant No.2022C044-2).
文摘3D-printed Porous Titanium Alloy Implants(pTi),owing to their biologically inertness and relatively smooth surface morphology,adversely affect the biological functions of surrounding cells.To address the challenges,constructing a bioinspired interface that mimics the hierarchical structure of bone tissue can enhance the cellular functions of cells.In this context,Hollow Mesoporous Silica Nanoparticles(HMSNs),renowned for their unique physicochemical properties and superior biocompatibility,offer a promising direction for this research.In this research,the initially synthesized HMSNs were used to construct a“hollow-mesoporous-macroporous”hierarchical bioinspired coating on the pTi surface through the Layer-by-Layer technique.Simultaneously,diverse morphologies of coatings were established by adjusting the deposition strategy of PDDA/HMSNs on the pTi surface(pTi-HMSN-2,pTi-HMSN-4,pTi-HMSN-6).A range of techniques were employed to investigate the physicochemical properties and regulation of cellular biological functions of the diverse HMSN coating strategies.Notably,the pTi-HMSN-4 and pTi-HMSN-6 groups exhibited the uniform coatings,leading to a substantial enhancement in surface roughness and hydrophilicity.Meantime,the coating constructed strategy of pTi-HMSN-4 possessed commendable stability.Based on the aforementioned findings,both pTi-HMSN-4 and pTi-HMSN-6 facilitated the adhesion,spreading,and pseudopodia extension of BMSCs,which led to a notable upsurge in the expression levels of vinculin protein in BMSCs.Comprehensive analysis indicates that the coating,when PDDA/HMSNs are deposited four times,possesses favorable overall performance.The research will provide a solid theoretical basis for the translation of HMSN bioinspired coatings for orthopedic implants.
基金supported,in part,by the University of Wisconsin–Madisonthe National Institutes of Health (P30CA014520 and T32CA009206)the American Cancer Society (125246-RSG-13-099-01-CCE)
文摘Silica nanoparticles have been one of the most promising nanosystems for biomedical applications due to their facile surface chemistry and non-toxic nature. However, it is still challenging to effectively deliver them into tumor sites and noninvasively visualize their in vivo biodistribution with excellent sensitivity and accuracy for effective cancer diagnosis. In this study, we design a yolk/shell-structured silica nanosystem ^(64) Cu-NOTAQD@HMSN-PEG-TRC105, which can be employed for tumor vasculature targeting and dual-modality PET/optical imaging, leading to superior targeting specificity, excellentimaging capability and more reliable diagnostic outcomes.By combining vasculature targeting, pH-sensitive drug delivery, and dual-modality imaging into a single platform,as-designed yolk/shell-structured silica nanosystems may be employed for the future image-guided tumor-targeted drug delivery, to further enable cancer theranostics.
基金support of this research by the National Science Foundation of China(Grant No.50702072)Chinese Academy of Science(Grant No.KJCX2.YW.M02)+1 种基金National 863 Projects(Grant No.2007AA03Z317)Shanghai Nano-Science Program(Grant No.0852nm03900)
文摘Hollow mesoporous silica spheres with magnetite cores(HMSMC) have been fabricated by Vacuum Nano-casting Route. The amount of magnetite cores and saturation magnetization value can be easily adjusted by changing the concentration of iron nitrate solution used in the synthesis procedure. Furthermore, the as-prepared HMSMCs still maintain narrow mesopore distribution, high surface area and large pore volume after the hollow cores of hollow mesoporous silica spheres were filled with magnetite particles. Specially, when the saturation magnetization value of as-prepared HMSMCs reaches 22.0 emu/g, the surface area and pore volume of corresponding HMSMCs are 149 m^2/g and 0.19 cm^3/g, respectively, and the pore size is 2.30 nm. The corresponding samples are characterized by X-ray diffraction, N_2 sorption isotherms, transmission electron microscopy and vibrating-sample magnetometer.
