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1.
ACS Appl Mater Interfaces ; 16(22): 28928-28937, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38795031

RESUMO

Two-dimensional (2D) mesoporous transition metal oxides are highly desired in various applications, but their fast and low-cost synthesis remains a great challenge. Herein, a Maillard reaction inspired microexplosion approach is applied to rapidly synthesize ultrathin 2D mesoporous tin oxide (mSnO2). During the microexplosion between granular ammonia nitrate with melanoidin at high temperature, the organic species can be carbonized and expanded rapidly due to the instantaneous release of gases, thus producing ultrathin carbonaceous templates with rich functional groups to effectively anchor SnO2 nanoparticles on the surface. The subsequent removal of carbonaceous templates via calcination in air results in the formation of 2D mSnO2 due to the confinement effect of the templates. Pd nanoparticles are controllably deposited on the surface of 2D mSnO2 via in situ reduction, forming ultrathin 2D Pd/mSnO2 nanocomposites with thicknesses of 6-8 nm. Owing to the unique 2D mesoporous structure with rich oxygen defects and highly exposed metal-metal oxide interfaces, 2D Pd/mSnO2 exhibits excellent sensing performance toward acetone with high sensitivity, a short response time, and good selectivity under low working temperature (100 °C). This fast and convenient microexplosion synthesis strategy opens up the possibility of constructing 2D porous functional materials for various applications including high-performance gas sensors.

2.
Natl Sci Rev ; 11(6): nwae152, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38741714
3.
Small ; : e2311659, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38747005

RESUMO

The performance consistency of the gas sensor is strongly dependent on the interface binding between the sensitive materials and the electrodes. Traditional powder coating methods can inevitably lead to differences in terms of substrate-film interface interaction and device performance, affecting the stability and lifetime. Thus, efficient growth of sensitive materials on device substrates is crucial and essential to enhance the sensing performance, especially for stability. Herein, hierarchically ordered macro/mesoporous WO3 films are in situ synthesized on the electrode via a facile soft/hard dual-template strategy. Orderly arrayed uniform polystyrene (PS) microspheres with tailored size (ca. 1.2 µm) are used as a hard template, and surfactant Pluronic F127 as a soft template can co-assemble with tungsten precursor into ordered mesostructure in the interstitials of PS colloidal crystal induced by solvent evaporation. Benefiting from its rich porosity and high stability, the macro/mesoporous WO3-based sensor shows high sensitivity (Rair/Rgas = 307), fast response/recovery speed (5/9 s), and excellent selectivity (SH2S/Smax > 7) toward 50 ppm H2S gas (a biomarker for halitosis). Significantly, the sensors exhibit an extended service life with a negligible change in sensing performance within 60 days. This lab-on-device synthesis provides a platform method for constructing stable nanodevices with good consistency and high stability, which are highly desired for developing high-performance sensors.

4.
Adv Mater ; : e2313920, 2024 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-38634436

RESUMO

Polymer cubosomes (PCs) have well-defined inverse bicontinuous cubic mesophases formed by amphiphilic block copolymer bilayers. The open hydrophilic channels, large periods, and robust physical properties of PCs are advantageous to many host-guest interactions and yet not fully exploited, especially in the fields of functional nanomaterials. Here, the self-assembly of poly(ethylene oxide)-block-polystyrene block copolymers is systematically investigated and a series of robust PCs is developed via a cosolvent method. Ordered nanoporous metal oxide particles are obtained by selectively filling the hydrophilic channels of PCs via an impregnation strategy, followed by a two-step thermal treatment. Based on this versatile PC platform, the general synthesis of a library of ordered porous particles with different pore structures 3 ¯ $\bar{3}$ 3 ¯ $\bar{3}$ , tunable large pore size (18-78 nm), high specific surface areas (up to 123.3 m2 g-1 for WO3) and diverse framework compositions, such as transition and non-transition metal oxides, rare earth chloride oxides, perovskite, pyrochlore, and high-entropy metal oxides is demonstrated. As typical materials obtained via this method, ordered porous WO3 particles have the advantages of open continuous structure and semiconducting properties, thus showing superior gas sensing performances toward hydrogen sulfide.

5.
Nano Lett ; 24(15): 4554-4561, 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38573122

RESUMO

Three-dimensionally (3D) integrated metallic nanomaterials composed of two or more different types of nanostructures make up a class of advanced materials due to the multidimensional and synergistic effects between different components. However, designing and synthesizing intricate, well-defined metallic 3D nanomaterials remain great challenges. Here, a novel single-particle soft-enveloping strategy using a core-shell Au NP@mSiO2 particle as a template was proposed to synthesize 3D nanomaterials, namely, a Au nanoparticle@center-radial nanorod-Au-Pt nanoparticle (Au NP@NR-NP-Pt NP) superstructure. Taking advantage of the excellent plasmonic properties of Au NP@NR-NP by the synergistic plasmonic coupling of the outer Au NPs and inner Au nanorods, we can enhance the catalytic performance for 4-nitrophenol hydrogenation using Au NP@NR-NP-Pt NP as a photocatalyst with plasmon-excited hot electrons from Au NP@NR-NP under light irradiation, which is 2.76 times higher than in the dark. This process opens a door for the design of a new generation of 3D metallic nanomaterials for different fields.

6.
Micromachines (Basel) ; 15(3)2024 Mar 18.
Artigo em Inglês | MEDLINE | ID: mdl-38542655

RESUMO

In response to the increasing demand for high-performance capacitors, with a simultaneous emphasis on minimizing their physical size, a common practice involves etching deep vias and coating them with functional layers to enhance operational efficiency. However, these deep vias often cause warpages during the processing stage. This study focuses on the numerical modeling of wafer warpage that occurs during the deposition of three thin layers onto these vias. A multi-step mechanical and thermal homogenization approach is proposed to estimate the warpage of the silicon wafer. The efficiency and accuracy of this numerical homogenization strategy are validated by comparing detailed and homogenized models. The multi-step homogenization method yields more accurate results compared to the conventional direct homogenization method. Theoretical analysis is also conducted to predict the shape of the wafer warpage, and this study further explores the impact of via depth and substrate thickness.

7.
ACS Appl Mater Interfaces ; 16(14): 17563-17573, 2024 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-38551503

RESUMO

Hydrogen generation is one of the crucial technologies to realize sustainable energy development, and the design of advanced catalysts with efficient interfacial sites and fast mass transfer is significant for hydrogen evolution. Herein, an in situ coassembly strategy was proposed to engineer a cerium-doped ordered mesoporous titanium oxide (mpCe/TiO2), of which the abundant oxygen vacancies (Ov) and highly exposed active pore walls contribute to good stability of ultrasmall Pt nanoclusters (NCs, ∼ 1.0 nm in diameter) anchored in the uniform mesopores (ca. 20 nm). Consequently, the tailored mpCe/TiO2 with 0.5 mol % Ce-doping-supported Pt NCs (Pt-mpCe/TiO2-0.5) exhibits superior H2 evolution performance toward the water-gas shift reaction with a 0.73 molH2·s-1·molPt-1 H2 evolution rate at 200 °C, which is almost 6-fold higher than the Pt-mpTiO2 (0.13 molH2·s-1·molPt-1 H2). Density functional theory calculations confirm that the structure of Ce-doped TiO2 with Ce coordinated to six O atoms by substituting Ti atoms is thermodynamically favorable without the deformation of Ti-O bonds. The Ov generated by the six O atom-coordinated Ce doping is highly active for H2O dissociation with an energy barrier of 2.18 eV, which is obviously lower than the 2.37 eV for the control TiO2. In comparison with TiO2, the resultant Ce/TiO2 support acts as a superior electron acceptor for Pt NCs and causes electron deficiency at the Pt/support interface with a 0.17 eV downshift of the Pt d-band center, showing extremely obvious electronic metal-support interaction (EMSI). As a result, abundant and hyperactive Ti3+-Ov(-Ce3+)-Ptδ+ interfacial sites are formed to significantly promote the generation of CO2 and H2 evolution. In addition, the stronger EMSI between Pt NCs and mpCe/TiO2-0.5 than that between Pt and mpTiO2 contributes to the superior self-enhanced catalytic performance during the cyclic test, where the CO conversion at 200 °C increases from 72% for the fresh catalyst to 99% for the used one. These findings reveal the subtle relationship between the mesoporous metal oxide-metal composite catalysts with unique chemical microenvironments and their catalytic performance, which is expected to inspire the design of efficient heterogeneous catalysts.

8.
Small ; : e2310534, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38326097

RESUMO

The development of high-energy-density solid-state lithium metal battery has been hindered by the unstable cycling of Ni-rich cathodes at high rate and limited wide-temperatures adoptability. In this study, an ionic liquid functionalized quasi-solid-state electrolyte (FQSE) is prepared to address these challenges. The FQSE features a semi-immobilized ionic liquid capable of anchoring solvent molecules through electrostatic interactions, which facilitates Li+ desolvation and reduces deleterious solvent-cathode reactions. The FQSE exhibits impressive electrochemical characteristics, including high ionic conductivity (1.9 mS cm-1 at 30 °C and 0.2 mS cm-1 at -30 °C) and a Li+ transfer number of 0.7. Consequently, Li/NCM811 cells incorporating FQSE demonstrate exceptional stability during high-rate cycling, enduring 700 cycles at 1 C. Notably, the Li/LFP cells with FQSE maintain high capacity across a wide temperature range, from -30 to 60 °C. This research provides a new way to promote the practical application of high-energy lithium metal batteries.

9.
Nat Commun ; 14(1): 8493, 2023 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-38129402

RESUMO

Organic-inorganic molecular assembly has led to numerous nano/mesostructured materials with fantastic properties, but it is dependent on and limited to the direct interaction between host organic structure-directing molecules and guest inorganic species. Here, we report a "solvent-pair surfactants" enabled assembly (SPEA) method to achieve a general synthesis of mesostructured materials requiring no direct host-guest interaction. Taking the synthesis of mesoporous metal oxides as an example, the dimethylformamide/water solvent pairs behave as surfactants and induce the formation of mesostructured polyoxometalates/copolymers nanocomposites, which can be converted into metal oxides. This SPEA method enables the synthesis of functional ordered mesoporous metal oxides with different pore sizes, structures, compositions and tailored pore-wall microenvironments that are difficult to access via conventional direct organic-inorganic assembly. Typically, nitrogen-doped mesoporous ε-WO3 with high specific surface area, uniform mesopores and stable framework is obtained and exhibits great application potentials such as gas sensing.

10.
ACS Sens ; 8(10): 3723-3732, 2023 10 27.
Artigo em Inglês | MEDLINE | ID: mdl-37610721

RESUMO

Glutaraldehyde disinfectant has been widely applied in aquaculture, farming, and medical treatment. Excessive concentrations of glutaraldehyde in the environment can lead to serious health hazards. Therefore, it is extremely important to develop high-performance glutaraldehyde sensors with low cost, high sensitivity, rapid response, fabulous selectivity, and low limit of detection. Herein, mesoporous lanthanum (La) doped SnO2 spheres with high specific surface area (52-59 m2 g-1), uniform mesopores (with a pore size concentrated at 5.7 nm), and highly crystalline frameworks are designed to fabricate highly sensitive gas sensors toward gaseous glutaraldehyde. The mesoporous lanthanum-doped SnO2 spheres exhibit excellent glutaraldehyde-sensing performance, including high response (13.5@10 ppm), rapid response time (28 s), and extremely low detection limit of 0.16 ppm. The excellent sensing performance is ascribed to the high specific surface area, high contents of chemisorbed oxygen species, and lanthanum doping. DFT calculations suggest that lanthanum doping in the SnO2 lattice can effectively improve the adsorption energy toward glutaraldehyde compared to pure SnO2 materials. Moreover, the fabricated gas sensors can effectively detect commercial glutaraldehyde disinfectants, indicating a potential application in aquaculture, farming, and medical treatment.


Assuntos
Desinfetantes , Glutaral , Lantânio , Agricultura , Adsorção , Gases
11.
ACS Nano ; 17(16): 15763-15775, 2023 08 22.
Artigo em Inglês | MEDLINE | ID: mdl-37556610

RESUMO

Highly porous sensitive materials with well-defined structures and morphologies are extremely desirable for developing high-performance chemiresistive gas sensors. Herein, inspired by the classical alkaloid precipitant reaction, a robust and reliable active mesoporous nitrogen polymer sphere-directed synthesis method was demonstrated for the controllable construction of heteroatom-doped mesoporous tungsten oxide spheres. In the typical synthesis, P-doped mesoporous WO3 monodisperse spheres with radially oriented channels (P-mWO3-R) were obtained with a diameter of ∼180 nm, high specific surface area, and crystalline skeleton. The in situ-introduced P atoms could effectively adjust the coordination environment of W atoms (Wδ+-Ov), giving rise to dramatically enhanced active surface-adsorbed oxygen species and unusual metastable ε-WO3 crystallites. The P-mWO3-R spheres were applied for the sensing of 3-hydroxy-2-butanone (3H2B), a biomarker of foodborne pathogenic bacteria Listeria monocytogenes (LM). The sensor exhibited high sensitivity (Ra/Rg = 29 to 3 ppm), fast response dynamics (26/7 s), outstanding selectivity, and good long-term stability. Furthermore, the device was integrated into a wireless sensing module to realize remote real-time and precise detection of LM in practical applications, making it possible to evaluate food quality using gas sensors conveniently.


Assuntos
Alcaloides , Listeria monocytogenes , Óxidos/química , Tungstênio/química , Biomarcadores , Nitrogênio
12.
Small ; 19(45): e2304631, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37438544

RESUMO

Chemiluminescence immunoassay exhibits high sensitivity and signal-to-noise ratio, thus attracting great attention in the early diagnosis and dynamic monitoring of diseases. However, the collection of conventional flash-type chemiluminescence signal (<5 s) relies heavily on automatic sampling and reading instrument. Herein, a novel core-satellite multifunctional chemiluminescence immunosensor is designed for the efficient enrichment and highly sensitive determination of cancer biomarker carcinoembryonic antigen (CEA) with enhanced and long-lasting output signal that can be conveniently recorded by a simple microplate plate reading instrument. Anti-CEA monoclonal antibody 2 (Ab2) modified Fe3 O4 @SiO2 microspheres (Fe3 O4 @SiO2 -Ab2, 370 nm in diameter) are synthesized as the core for selectively capturing and enriching target CEA in solution, and anti-human CEA monoclonal antibody 1 (Ab1) and horseradish peroxidase (HRP) co-immobilized dendritic large-mesoporous silica nanospheres (MSNs-HRP/Ab1, 80 nm in diameter, pore size: 17 nm) are synthesized as the satellite for efficient immunological recognition and signal amplification. The as-designed core-satellite magnetic chemiluminescence immunosensors exhibit a broad linear range of 0.01-20 ng mL-1 and a low detection limit of 3.0 pg mL-1 for the convenient, highly specific, and sensitive determination of CEA in human serum. Such core-satellite chemiluminescence immunosensors are expected to act as a powerful tool for in vitro detection of various biomarkers, overcome the defect of conventional chemiluminescence relying heavily on expensive and bulky automatic instruments and popularize chemiluminescence analysis to primary medical institutions and remote areas.


Assuntos
Técnicas Biossensoriais , Nanopartículas Metálicas , Humanos , Biomarcadores Tumorais , Antígeno Carcinoembrionário , Imunoensaio , Luminescência , Dióxido de Silício , Anticorpos Monoclonais , Limite de Detecção , Ouro , Técnicas Eletroquímicas
13.
Small ; 19(39): e2302327, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37259638

RESUMO

Methane (CH4 ), as the vital energy resource and industrial chemicals, is highly flammable and explosive for concentrations above the explosive limit, triggering potential risks to personal and production safety. Therefore, exploiting smart gas sensors for real-time monitoring of CH4 becomes extremely important. Herein, the Pt-Pd nanoalloy functionalized mesoporous SnO2 microspheres (Pt-Pd/SnO2 ) were synthesized, which show uniform diameter (≈500 nm), high surface area (40.9-56.5 m2 g-1 ), and large mesopore size (8.8-15.8 nm). The highly dispersed Pt-Pd nanoalloys are confined in the mesopores of SnO2 , causing the generation ofoxygen defects and increasing the carrier concentration of sensitive materials. The representative Pt1 -Pd4 /SnO2 exhibits superior CH4 sensing performance with ultrahigh response (Ra /Rg = 21.33 to 3000 ppm), fast response/recovery speed (4/9 s), as well as outstanding stability. Spectroscopic analyses imply that such an excellent CH4 sensing process involves the fast conversion of CH4 into formic acid and CO intermediates, and finally into CO2 . Density functional theory (DFT) calculations reveal that the attractive covalent bonding interaction and rapid electron transfer between the Pt-Pd nanoalloys and SnO2 support, dramatically promote the orbital hybridization of Pd4 sites and adsorbed CH4 molecules, enhancing the catalytic activation of CH4 over the sensing layer.

14.
Small ; 19(32): e2301011, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37066705

RESUMO

Site-selective and partial decoration of supported metal nanoparticles (NPs) with transition metal oxides (e.g., FeOx ) can remarkably improve its catalytic performance and maintain the functions of the carrier. However, it is challenging to selectively deposit transition metal oxides on the metal NPs embedded in the mesopores of supporting matrix through conventional deposition method. Herein, a restricted in situ site-selective modification strategy utilizing poly(ethylene oxide)-block-polystyrene (PEO-b-PS) micellar nanoreactors is proposed to overcome such an obstacle. The PEO shell of PEO-b-PS micelles interacts with the hydrolyzed tungsten salts and silica precursors, while the hydrophobic organoplatinum complex and ferrocene are confined in the hydrophobic PS core. The thermal treatment leads to mesoporous SiO2 /WO3-x framework, and meanwhile FeOx nanolayers are in situ partially deposited on the supported Pt NPs due to the strong metal-support interaction between FeOx and Pt. The selective modification of Pt NPs with FeOx makes the Pt NPs present an electron-deficient state, which promotes the mobility of CO and activates the oxidation of CO. Therefore, mesoporous SiO2 /WO3-x -FeOx /Pt based gas sensors show a high sensitivity (31 ± 2 in 50 ppm of CO), excellent selectivity, and fast response time (3.6 s to 25 ppm) to CO gas at low operating temperature (66 °C, 74% relative humidity).

15.
Small Methods ; 7(7): e2201687, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-37116102

RESUMO

Compared with nanomaterials-based sensors with single function, the development of multifunctional sensors shows high potential in comprehensive monitoring of personal health and environment, intelligent human-machine interfaces, and realistic imitation of human skin in prosthetics. Ordered macro-microporous metal-organic frameworks (MOFs)-enabled flexible and stretchable electronics are promising candidates for integrated multifunctional sensing systems. Herein, a three-dimensional ordered macro-microporous zeolite imidazolate framework-8 (3DOM ZIF-8) for humidity sensing and the derived ZnO within a hierarchically ordered macroporous-mesoporous-microporous carbon matrix (ZnO@HOMC) for gas sensor is constructed. Benefit from hierarchically ordered macroporous-mesoporous-microporous structure, the active site is fully exposed, and the charge transfer is accelerated. As a result, the multifunctional sensing systems show ultrafast response and recovery speed (10 s and 34 s), high sensitivity (Rair /Rgas = 38.6@50 ppm) to acetone, rapid humidity response speed (0.23 s) within changing humidity (RH 21%-99%), excellent stability and repeatability. Furthermore, in order to realize real-time monitoring of gas concentrations and humidity on mobile devices, an intelligent and portable sensor module is fabricated and wirelessly connected to a smartphone to effectively detect acetone concentration and humidity. This sensing technology shows fascinating applications in personal health, fitness tracking, electronic skins, artificial nervous systems, and human-machine interactions.

16.
ACS Appl Mater Interfaces ; 15(12): 15721-15731, 2023 Mar 29.
Artigo em Inglês | MEDLINE | ID: mdl-36917766

RESUMO

Hydrogen as an important clean energy source with a high energy density has attracted extensive attention in fuel cell vehicles and industrial production. However, considering its flammable and explosive property, gas sensors are desperately desired to efficiently monitor H2 concentration in practical applications. Herein, a facile polymerization-induced aggregation strategy was proposed to synthesize uniform Si-doped mesoporous WO3 (Si-mWO3) microspheres with tunable sizes. The polymerization of the melamine-formaldehyde resin prepolymer (MF prepolymer) in the presence of silicotungstic acid hydrate (abbreviated as H4SiW) leads to uniform MF/H4SiW hybrid microspheres, which can be converted into Si-mWO3 microspheres through a simple thermal decomposition treatment process. In addition, benefiting from the pore confinement effect, monodispersed Pd-decorated Si-mWO3 microspheres (Pd/Si-mWO3) were subsequently synthesized and applied as sensitive materials for the sensing and detection of hydrogen. Owing to the oxygen spillover effect of Pd nanoparticles, Pd/Si-mWO3 enables adsorption of more oxygen anions than pure mWO3. These Pd nanoparticles dispersed on the surface of Si-mWO3 accelerated the dissociation of hydrogen and promoted charge transfer between Pd nanoparticles and WO3 crystal particles, which enhanced the sensing sensitivity toward H2. As a result, the gas sensor based on Pd/Si-mWO3 microspheres exhibited excellent selectivity and sensitivity (Rair/Rgas = 33.5) to 50 ppm H2 at a relatively low operating temperature (210 °C), which was 30 times higher than that of the pure Si-mWO3 sensor. To develop intelligent sensors, a portable sensor module based on Pd/Si-mWO3 in combination with wireless Bluetooth connection was designed, which achieved real-time monitoring of H2 concentration, opening up the possibility for use as intelligent H2 sensors.

17.
Int J Nanomedicine ; 18: 437-453, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36718193

RESUMO

Background: Ocular vascular diseases are the major causes of visual impairment, which are characterized by retinal vascular dysfunction and robust inflammatory responses. Traditional anti-angiogenic or anti-inflammatory drugs still have limitations due to the short-acting effects. To improve the anti-angiogenic or anti-inflammatory efficiency, a dual-drug nanocomposite formulation was proposed for combined anti-angiogenic and anti-inflammatory treatment of ocular vascular diseases. Methods : CBC-MCC@hMSN(SM) complex nanoformulation was prepared by integrating conbercept (CBC, an anti-angiogenic drug) and MCC950 (MCC, an inhibitor of inflammation) into the surface-modified hollow mesoporous silica nanoparticles (hMSN(SM)). CBC-MCC@hMSN(SM) complex nanoformulation was then characterized by Fourier transform infrared spectroscopy, transmission electron microscopy, zeta potentials, and nitrogen adsorption-desorption measurement. CBC and MCC release profile, cytotoxicity, tissue toxicity, anti-angiogenic effects, and anti-inflammatory effects of CBC-MCC@hMSN(SM) were estimated using the in vitro and in vivo experiments. Results:  CBC-MCC@hMSN(SM) complex had no obvious cytotoxicity and tissue toxicity and did not cause a detectable ocular inflammatory responses. CBC-MCC@hMSN(SM) complex was more effective than free CBC or MCC in suppressing endothelial angiogenic effects and inflammatory responses in vitro. A single intraocular injection of CBC-MCC@hMSN(SM) complex potently suppressed diabetes-induced retinal vascular dysfunction, choroidal neovascularization, and inflammatory responses for up to 6 months. Conclusion : Combined CBC and MCC nanoformulation provides a promising strategy for sustained suppression of pathological angiogenesis and inflammatory responses to improve the treatment outcomes of ocular vascular diseases.


Assuntos
Oftalmopatias , Doenças Vasculares , Humanos , Neovascularização Patológica/tratamento farmacológico , Neovascularização Patológica/patologia , Inibidores da Angiogênese/farmacologia , Anti-Inflamatórios/farmacologia
18.
Bioact Mater ; 19: 487-498, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-35600973

RESUMO

The regeneration of articular cartilage remains a great challenge due to the difficulty in effectively enhancing spontaneous healing. Recently, the combination of implanted stem cells, suitable biomaterials and bioactive molecules has attracted attention for tissue regeneration. In this study, a novel injectable nanocomposite was rationally designed as a sustained release platform for enhanced cartilage regeneration through integration of a chitosan-based hydrogel, articular cartilage stem cells (ACSCs) and mesoporous SiO2 nanoparticles loaded with anhydroicaritin (AHI). The biocompatible engineered nanocomposite acting as a novel 3D biomimetic extracellular matrix exhibited a remarkable sustained release effect due to the synergistic regulation of the organic hydrogel framework and mesopore channels of inorganic mSiO2 nanoparticles (mSiO2 NPs). Histological assessment and biomechanical tests showed that the nanocomposites exhibited superior performance in inducing ACSCs proliferation and differentiation in vitro and promoting extracellular matrix (ECM) production and cartilage regeneration in vivo. Such a novel multifunctional biocompatible platform was demonstrated to significantly enhance cartilage regeneration based on the sustained release of AHI, an efficient bioactive natural small molecule for ACSCs chondrogenesis, within the hybrid matrix of hydrogel and mSiO2 NPs. Hence, the injectable nanocomposite holds great promise for use as a 3D biomimetic extracellular matrix for tissue regeneration in clinical diagnostics.

19.
ACS Sens ; 7(12): 3963-3972, 2022 12 23.
Artigo em Inglês | MEDLINE | ID: mdl-36511787

RESUMO

Formaldehyde (HCHO) is a prevalent indoor gas pollutant that has been seriously endangering human health. Developing semiconductor metal oxide (SMO) gas sensors for selective measurement of formaldehyde at low working temperatures remains a great challenge. In this work, silver/tin-polyphenol hybrid spheres are applied as a sacrificial template for the fabrication of spherical mesoporous Ag2O/SnO2 sensing materials. The obtained mesoporous Ag2O/SnO2 spheres have a uniform particle size (∼80 nm), large pore size (5.8 nm), and high specific surface area (71.3 m2 g-1). The response is 140 toward formaldehyde (10 ppm) at a low working temperature (75 °C). The detection limit reaches a low level of 23.6 ppb. Most importantly, it has excellent selectivity toward interfering gases. When the concentration of the interfering gas (e.g., ethanol) is 5 times as high as that of formaldehyde, the response is little affected. Theoretical calculations suggest that the addition of Ag2O can significantly enhance the adsorption energy toward formaldehyde, thus improving formaldehyde sensing performance. This work demonstrates an efficient self-template synthesis strategy for noble metal catalyst-decorated mesoporous metal oxide spheres, which could boost gas sensing performance at a lower working temperature.


Assuntos
Nanosferas , Humanos , Temperatura , Temperatura Baixa , Formaldeído , Gases , Óxidos
20.
Nat Commun ; 13(1): 6673, 2022 Nov 05.
Artigo em Inglês | MEDLINE | ID: mdl-36335188

RESUMO

Controlled growth of well-oriented metal-organic framework nanoarrays on requisite surfaces is of prominent significance for a broad range of applications such as catalysis, sensing, optics and electronics. Herein, we develop a highly flexible soft nanobrush-directed synthesis approach for precise in situ fabrication of MOF nanoarrays on diverse substrates. The soft nanobrushes are constructed via surface-initiated living crystallization-driven self-assembly and their active poly(2-vinylpyridine) corona captures abundant metal cations through coordination interactions. This allows the rapid heterogeneous growth of MOF nanoparticles and the subsequent formation of MIL-100 (Fe), HKUST-1 and CUT-8 (Cu) nanoarrays with tailored heights of 220~1100 nm on silicon wafer, Ni foam and ceramic tube. Auxiliary functional components including metal oxygen clusters and precious metal nanoparticles can be readily incorporated to finely fabricate hybrid structures with synergistic features. Remarkably, the MIL-100 (Fe) nanoarrays doped with Keggin H3PMo10V2O40 dramatically boost formaldehyde selectivity up to 92.8% in catalytic oxidation of methanol. Moreover, the HKUST-1 nanoarrays decorated with Pt nanoparticles show exceptional sensitivity to H2S with a ppb-level detection limit.

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