Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 84
Filtrar
Mais filtros











Base de dados
Intervalo de ano de publicação
1.
J Colloid Interface Sci ; 677(Pt A): 655-664, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39116563

RESUMO

Germanium based nanomaterials are very promising as the anodes for the lithium ion batteries since their large specific capacity, excellent lithium diffusivity and high conductivity. However, their controllable preparation is still very difficult to achieve. Herein, we facilely prepare a unique carbon coating Ge nanospheres with a cubic hollow structure (Ge@C) via a hydrothermal synthesis and subsequent pyrolysis using low-cost GeO2 as precursors. The hollow Ge@C nanostructure not only provides abundant interior space to alleviate the huge volumetric expansion of Ge upon lithiation, but also facilitates the transmission of lithium ions and electrons. Moreover, experiment analyses and density functional theory (DFT) calculations unveil the excellent lithium adsorption ability, high exchange current density, low activation energy for lithium diffusion of the hollow Ge@C electrode, thus exhibiting significant lithium storage advantages with a large charge capacity (1483 mAh/g under 200 mA g-1), distinguished rate ability (710 mAh/g under 8000 mA g-1) as well as long-term cycling stability (1130 mAh/g after 900 cycles under 1000 mA g-1). Therefore, this work offers new paths for controllable synthesis and fabrication of high-performance Ge based lithium storage nanomaterials.

2.
Chem Asian J ; : e202400896, 2024 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-39384549

RESUMO

Nanoscale framework materials have received much attention due to their diverse morphologies as well as good properties, and synthetic methods to construct different dimensions have been reported. Therefore, the study of the relationship between different sizes, dimensions and properties has become a hot research topic. This article provides a comprehensive examination of the controllable synthesis strategies of nano-metal-organic frameworks (nano-MOFs) and nano-covalent-organic frameworks (nano-COFs) and their applications in energy storage and catalysis. Commences with an overview of the synthetic evolution of nanoscale framework materials, which have garnered attention due to their exceptional specific surface area, regular pores, and tunable structural functionality. Various preparation methods for 0D, 1D, 2D and 3D nanostructures are then highlighted. These synthesis strategies not only improve the stability and activity of the materials, but also provide a basis for the design of novel energy storage and catalytic materials. Furthermore, the article presents an overview of the recent advancements in the field of energy storage and catalysis, with a particular focus on the applications of nano-MOFs/COFs in zinc-, lithium-, and sodium-based batteries as well as supercapacitors. ​.

3.
Materials (Basel) ; 17(17)2024 Aug 31.
Artigo em Inglês | MEDLINE | ID: mdl-39274723

RESUMO

Constructing photonic crystals with core-shell structured nanoparticles is an important means for applications such as secure communication, anti-counterfeiting marking, and structural color camouflage. Nonetheless, the precise synthesis technology for core-shell structured nanoparticles at the hundred-nanometer scale faces significant challenges. This paper proposes a controlled synthesis method for core-shell structured nanoparticles using a template method. By using 100 nm diameter silica nanospheres as templates and coating them with a ferroferric oxide shell layer, SiO2@Fe3O4 core-shell structured nanoparticles with regular morphology and good uniformity can be obtained. The study experimentally investigated the effects of feed amount, modifiers, temperature, and feed order on the coating effect, systematically optimizing the preparation process. Centrifugal driving technology was used to achieve structural colors in the visible wavelength range. Additionally, the method successfully created well-defined and uniform core-shell structured nanoparticles using 200 nm diameter silica nanospheres as templates, demonstrating that this controllable synthesis method can effectively produce core-shell structured nanoparticles over a wide range of particle sizes. The template method proposed in this paper can significantly improve morphological regularity and size uniformity while effectively reducing the preparation cost of core-shell structured nanoparticles.

4.
J Chromatogr A ; 1736: 465398, 2024 Sep 26.
Artigo em Inglês | MEDLINE | ID: mdl-39342731

RESUMO

Sample preparation is crucial in analytical chemistry, impacting result accuracy, sensitivity, and reliability. Solid-phase separation media, especially adsorbents, are vital for preparing of liquid and gas samples, commonly analyzed by most analytical instruments. With the advancements in materials science, covalent organic frameworks (COFs) constructed through strong covalent bonds, have been increasingly employed in sample preparation in recent years. COFs have outstanding selectivity and/or excellent adsorption capacity for a single target or can selectively adsorb multiple targets from complex matrix, due to their large specific surface area, adjustable pore size, easy modification, and stable chemical properties. In this review, we summarize the classification of COFs, such as pristine COFs, COF composite particles, and COFs-based substrates. We aim to provide a comprehensive understanding of the different classifications of COFs in sample preparation within the last three years. The challenges and development trends of COFs in sample preparation are also presented.

5.
Small ; : e2406489, 2024 Sep 28.
Artigo em Inglês | MEDLINE | ID: mdl-39340269

RESUMO

Silicon (Si) has attracted considerable attention as a promising alternative to graphite in lithium-ion batteries (LIBs) because of its high theoretical capacity and voltage. However, the durability and cycling stability of Si-based composites have emerged as major obstacles to their widespread adoption as LIBs anode materials. To tackle these challenges, a hollow core-shell dodecahedra structure of a Si-based composite (HD-Si@C) is developed through a novel double-layer in situ growth approach. This innovative design ensures that the nano-sized Si particles are evenly distributed within a hollow carbon shell, effectively addressing issues like Si fragmentation, volume expansion, and detachment from the carbon layer during cycles. The HD-Si@C composite demonstrates remarkable structural integrity as a LIBs anode, resulting in exceptional electrochemical performance and promising practical applications, as evidenced by tests in pouch-type full cells. Notably, the composite shows outstanding cycling stability, retaining 85% of its initial capacity (713 mAh g-1) even after 3000 cycles at a high current rate of 5000 mA g-1. Additionally, the material achieves a gravimetric energy density of 369 W h kg-1, showcasing its potential for efficient energy storage solutions. This research signifies a significant step toward realizing the practical utilization of Si-based materials in the next generation of LIBs.

6.
Molecules ; 29(15)2024 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-39124863

RESUMO

Hexagonal boron nitride (h-BN) nanoparticles have attracted increasing attention due to their unique structure and properties. However, it is difficult to synthesize h-BN nanoparticles with uniform spherical morphology due to their crystal characteristic. The morphology control by tuning their precursor synthesis is a promising and effective strategy to solve this problem. Especially, the treatment temperature of precursors plays an important role in the morphology and surface area of h-BN nanoparticles. Herein, h-BN nanoparticles with different morphologies were synthesized via regulating the treatment temperature of precursors. The result shows that treatment temperature will affect the microstructure and state of precursor and further influence the morphology of h-BN products. Benefiting from the unique structure, the h-BN obtained using 250 °C precursors shows higher specific surface area (61.1 m2 g-1) than that of 85 °C (36.5 m2 g-1) and 145 °C (27.9 m2 g-1). h-BN products obtained using 250 °C precursors show higher specific surface area than that of 85 °C and 145 °C. The optimal condition for obtaining high-quality spherical h-BN is the pretreatment temperature of 250 °C and sintering temperature of 1300 °C. Importantly, compared with commercial h-BN nanoparticles, the synthesized h-BN nanoparticles show more uniform structure and larger specific surface area, indicating that sintering activity will be greatly improved. Furthermore, the reaction pathway and formation mechanism of h-BN was revealed by DFT calculations. The result shows that the five stationary states and five transition states exist in the reaction pathway, and the energy barrier can be overcome at high temperatures to form a ring h-BN. In view of its simplicity and efficiency, this work is promising for designing and guiding the synthesis of h-BN nanoparticles with uniform morphology.

7.
Small ; : e2402641, 2024 Jul 16.
Artigo em Inglês | MEDLINE | ID: mdl-39011737

RESUMO

The tracking of nanomedicines in their concentration and location inside living systems has a pivotal effect on the understanding of the biological processes, early-stage diagnosis, and therapeutic monitoring of diseases. Nanoscale metal-organic frameworks (nano MOFs) possess high surface areas, definite structure, regulated optical properties, rich functionalized sites, and good biocompatibility that allow them to excel in a wide range of biomedical applications. Controllable syntheses and functionalization endow nano MOFs with better properties as imaging agents and sensing units for the diagnosis and treatment of diseases. This minireview summarizes the tunable synthesis strategies of nano MOFs with controllable size, shape, and regulated luminescent performance, and pinpoints their recent advanced applications as optical elements in bioimaging and biosensing. The current limitations and future development directions of nano MOF-contained materials in bioimaging and biosensing applications are also discussed, aiming to expand the biological applications of nano MOF-based nanomedicine and facilitate their production or clinical translation.

8.
Biosens Bioelectron ; 263: 116613, 2024 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-39084044

RESUMO

The biomimetic enzyme cascade system plays a key role in biosensing as a sophisticated signal transduction and amplification strategy. However, constructing a regulated enzyme cascade sensing system remains challenging due to the mismatch of multiple enzyme activities and poor stability. Herein, we design an efficient dual-enhanced enzyme cascade hybrid system (UFD-DEC) containing DNA-controlled nanozymes (Fe-cdDNA) and enzyme (urease) via combining the electrostatic contact effect with the hydrogel-directed confinement effect. Precise modulation of Fe-cdDNA nanozyme by DNA offers a means to control its catalytic efficiency. This regulated UFD-DEC system accelerates the reaction rate and provides remarkable stability compared with the free enzyme system. Benefiting from the plasticity properties of hydrogels, a "lab-in-a-tube" platform was constructed by encapsulating UFD-DEC in a microcentrifuge tube. Such a UFD-DEC-based hydrogel tube exhibits sufficient adaptability to profile urea when used in conjunction with a smartphone-assisted image processing algorithm, which on-site delivers urea information with a detection limit of 0.12 mmol L-1. This customizable and inexpensive miniaturized biosensor platform for monitoring urea may facilitate point-of-care testing applications.


Assuntos
Técnicas Biossensoriais , Hidrogéis , Limite de Detecção , Urease , Técnicas Biossensoriais/métodos , Hidrogéis/química , Urease/química , Ureia/análise , Ureia/química , DNA Catalítico/química , DNA/química
9.
Acta Biomater ; 183: 30-49, 2024 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-38849022

RESUMO

Bone, an actively metabolic organ, undergoes constant remodeling throughout life. Disturbances in the bone microenvironment can be responsible for pathologically bone diseases such as periodontitis, osteoarthritis, rheumatoid arthritis and osteoporosis. Conventional bone tissue biomaterials are not adequately adapted to complex bone microenvironment. Therefore, there is an urgent clinical need to find an effective strategy to improve the status quo. In recent years, nanotechnology has caused a revolution in biomedicine. Cerium(III, IV) oxide, as an important member of metal oxide nanomaterials, has dual redox properties through reversible binding with oxygen atoms, which continuously cycle between Ce(III) and Ce(IV). Due to its special physicochemical properties, cerium(III, IV) oxide has received widespread attention as a versatile nanomaterial, especially in bone diseases. This review describes the characteristics of bone microenvironment. The enzyme-like properties and biosafety of cerium(III, IV) oxide are also emphasized. Meanwhile, we summarizes controllable synthesis of cerium(III, IV) oxide with different nanostructural morphologies. Following resolution of synthetic principles of cerium(III, IV) oxide, a variety of tailored cerium-based biomaterials have been widely developed, including bioactive glasses, scaffolds, nanomembranes, coatings, and nanocomposites. Furthermore, we highlight the latest advances in cerium-based biomaterials for inflammatory and metabolic bone diseases and bone-related tumors. Tailored cerium-based biomaterials have already demonstrated their value in disease prevention, diagnosis (imaging and biosensors) and treatment. Therefore, it is important to assist in bone disease management by clarifying tailored properties of cerium(III, IV) oxide in order to promote the use of cerium-based biomaterials in the future clinical setting. STATEMENT OF SIGNIFICANCE: In this review, we focused on the promising of cerium-based biomaterials for bone diseases. We reviewed the key role of bone microenvironment in bone diseases and the main biological activities of cerium(III, IV) oxide. By setting different synthesis conditions, cerium(III, IV) oxide nanostructures with different morphologies can be controlled. Meanwhile, tailored cerium-based biomaterials can serve as a versatile toolbox (e.g., bioactive glasses, scaffolds, nanofibrous membranes, coatings, and nanocomposites). Then, the latest research advances based on cerium-based biomaterials for the treatment of bone diseases were also highlighted. Most importantly, we analyzed the perspectives and challenges of cerium-based biomaterials. In future perspectives, this insight has given rise to a cascade of cerium-based biomaterial strategies, including disease prevention, diagnosis (imaging and biosensors) and treatment.


Assuntos
Materiais Biocompatíveis , Doenças Ósseas , Cério , Cério/química , Cério/uso terapêutico , Humanos , Materiais Biocompatíveis/química , Materiais Biocompatíveis/uso terapêutico , Doenças Ósseas/tratamento farmacológico , Animais
10.
Natl Sci Rev ; 11(4): nwae056, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38444985

RESUMO

The absence of efficient and durable catalysts for oxygen evolution reaction (OER) is the main obstacle to hydrogen production through water splitting in an acidic electrolyte. Here, we report a controllable synthesis method of surface IrOx with changing Au/Ir compositions by constructing a range of sub-10-nm-sized core-shell nanocatalysts composed of an Au core and AuxIr1-x alloy shell. In particular, Au@Au0.43Ir0.57 exhibits 4.5 times higher intrinsic OER activity than that of the commercial Ir/C. Synchrotron X-ray-based spectroscopies, electron microscopy and density functional theory calculations revealed a balanced binding of reaction intermediates with enhanced activity. The water-splitting cell using a load of 0.02 mgIr/cm2 of Au@Au0.43Ir0.57 as both anode and cathode can reach 10 mA/cm2 at 1.52 V and maintain activity for at least 194 h, which is better than the cell using the commercial couple Ir/C‖Pt/C (1.63 V, 0.2 h).

11.
J Chromatogr A ; 1720: 464794, 2024 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-38484640

RESUMO

The distinctive morphology of dendritic mesoporous silica nanoparticles (DMSN) has recently attracted considerable attention in scientific community. However, synthesis of DMSN with well-defined structure and uniform size for ultrafast extraction of trace herbicide residues from environmental and food samples remains to be a compelling challenge. In this study, sulfhydryl functionalized dendritic mesoporous silica (SH-DMSN) was synthesized and the SH-DMSN showcases monodisperse microspheres with flower shape and precisely tailored and controllable pore sizes. This distinctive structural configuration accelerates mass transfer within the silica layer, resulting in heightened adsorption efficiencies. Furthermore, the particle sizes (455, 765, and 808) of the adsorbent can be meticulously fine-tuned by introducing distinct templates. Specifically, when the particle size is 765 nm, the optimized SH-DMSN exhibits a substantial specific surface area (691.32 m²/g), outstanding adsorption efficiencies (>90 %), remarkably swift adsorption and desorption kinetics (2 min and 3 min, respectively), and exceptional stability. The superior adsorption capabilities of this novel adsorbent, ranging from 481.65 to 1021.7 µg/g for organochlorine herbicides containing amide groups, can be attributed to the interplay of S-π interactions, halogen bonding, and electrostatic attraction interaction. These interactions involve the lone pair electrons of sulfhydryl and silanol groups with the π-electrons, halogen atoms and amide groups in herbicide molecules. This study not only offers a new perspective on advancing the practical utilization of dendritic mesoporous silica but also provides a pragmatic strategy for the separation and analysis of herbicides in diverse sample matrices.


Assuntos
Herbicidas , Nanosferas , Nanosferas/química , Dióxido de Silício/química , Halogênios , Porosidade
12.
Nanomicro Lett ; 16(1): 163, 2024 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-38546814

RESUMO

In recent years, low-dimensional transition metal chalcogenide (TMC) materials have garnered growing research attention due to their superior electronic, optical, and catalytic properties compared to their bulk counterparts. The controllable synthesis and manipulation of these materials are crucial for tailoring their properties and unlocking their full potential in various applications. In this context, the atomic substitution method has emerged as a favorable approach. It involves the replacement of specific atoms within TMC structures with other elements and possesses the capability to regulate the compositions finely, crystal structures, and inherent properties of the resulting materials. In this review, we present a comprehensive overview on various strategies of atomic substitution employed in the synthesis of zero-dimensional, one-dimensional and two-dimensional TMC materials. The effects of substituting elements, substitution ratios, and substitution positions on the structures and morphologies of resulting material are discussed. The enhanced electrocatalytic performance and photovoltaic properties of the obtained materials are also provided, emphasizing the role of atomic substitution in achieving these advancements. Finally, challenges and future prospects in the field of atomic substitution for fabricating low-dimensional TMC materials are summarized.

13.
Anal Chim Acta ; 1287: 342061, 2024 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-38182368

RESUMO

BACKGROUND: Covalent organic frameworks (COFs) have found promising applications in separation fields due to their large surface area and high adsorption capacity, but the exiting COFs can not be directly used as the packing materials of on-line solid-phase extraction (SPE) coupled to HPLC and HPLC because their nano/submicron size or irregular shapes might cause ultrahigh column back pressure and low column efficiency. To synthesize the large-size spherical COFs larger than 3 µm as sorbents might be able to address these problems, however it is still a great challenge till now. RESULTS: In this work, two large-size spherical 3D COFs (COF-320 and COF-300) were size-controllably synthesized within 10-90 µm via a two-step strategy. These two spherical COFs showed large surface area, fine crystallinity, good chemical/mechanical stability, and good reproducibility. As an application case, when used as the on-line SPE sorbents coupled to HPLC, the large-size spherical COF-320 displayed high binding capacity for bisphenol F (Qmax of 452.49 mg/g), low column back pressure (6-8 psi at flow rate of 1 mL/min), and good reusability (at least 30 cycles). The developed on-line-SPE-HPLC-UV method presented good analytical performance with enrichment factor of 667 folds, linear range of 1.0-400 ng/mL, limit of detection (LOD, S/N = 3) of 0.3 ng/mL, limit of quantification (LOQ, S/N = 10) of 1.0 ng/mL, and recoveries of 100.3-103.2 % (RSDs of 2.0-3.5 %) and 95.2-97.0 % (RSDs of 4.3-5.6 %) for tap water and lake water samples, respectively. SIGNIFICANCE: This is the first case to synthesize the large-size spherical COFs within 10-90 µm, and this work made it possible to directly use COFs as the filling materials of on-line SPE coupled to HPLC and HPLC. The developed analytical method can be potentially applied to the rapid and sensitive detection of trace bisphenol F in environmental water samples.

14.
Mikrochim Acta ; 191(2): 91, 2024 Jan 13.
Artigo em Inglês | MEDLINE | ID: mdl-38216807

RESUMO

Controllable synthesis of micro-flower covalent organic frameworks (MFCOFs) with controllable size, monodisperse, spherical, and beautiful flower shape was realized by using 2,5-diformylfuran (DFF) and p-phenylenediamine (p-PDA) as building blocks at room temperature. High-quality MFCOFs (5 - 7 µm) were synthesized by controlling the kind of solvent, amounts of monomers, catalyst content, and reaction time. The synthesized MFCOFs possessed uniform mesopores deriving from the intrinsic pores of frameworks and wide-distributed pores belonging to the gap between the petals. The MFCOFs-packed solid-phase extraction (SPE) column shows adsorption capacity of about 8.85 mg g-1 for 2,4-dichlorophenol (2,4-DCP). The MFCOF-based SPE combined with the HPLC method was established for the determination of 2,4-DCP in environmental water. The linear range of this method is 20-1000 ng mL-1 (R2 > 0.9994), and limit of detection (S/N = 3) is 10.9 ng mL-1. Spiked recoveries were 94.3-98.5% with relative standard deviations lower than 2.3%.

15.
Small ; 20(15): e2307923, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38009514

RESUMO

Vertical graphene (VG) nanosheets have garnered significant attention in the field of electrochemical energy applications, such as supercapacitors, electro-catalysis, and metal-ion batteries. The distinctive structures of VG, including vertically oriented morphology, exposed, and extended edges, and separated few-layer graphene nanosheets, have endowed VG with superior electrode reaction kinetics and mass/electron transportation compared to other graphene-based nanostructures. Therefore, gaining insight into the structure-activity relationship of VG and VG-based materials is crucial for enhancing device performance and expanding their applications in the energy field. In this review, the authors first summarize the fabrication methods of VG structures, including solution-based, and vacuum-based techniques. The study then focuses on structural modulations through plasma-enhanced chemical vapor deposition (PECVD) to tailor defects and morphology, aiming to obtain desirable architectures. Additionally, a comprehensive overview of the applications of VG and VG-based hybrids d in the energy field is provided, considering the arrangement and optimization of their structures. Finally, the challenges and future prospects of VG-based energy-related applications are discussed.

16.
Talanta ; 270: 125601, 2024 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-38150970

RESUMO

Large-size spherical sorbents with particle size of 10-50 µm are widely applied in separation fields, however it is still a great challenge to synthesize such large-size spherical covalent organic framework (COF). In this work, a type of large-size porous 3D COF was size-controablly synthesized via a two-step strategy, in which a large-size porous 3D spherical polymer was prepared first through a Pickering emulsion polymerization using nano silica as the stabilizer, and subsequently it was converted into porous spherical 3D COF by a solvothermal method. The as-prepared porous spherical COF (COF-320 as a model) showed size-controllable uniform spherical morphology within 15-45 µm, large specific surface area, fine crystalline structure, and good chemical stability. When used as the sorbent for dispersive solid-phase extraction (d-SPE) of bisphenol F (BPF), the porous spherical COF-320 (15 µm) displayed high adsorption capacity (Qmax = 335.6 mg/g), high enrichment factor (80 folds), and good reusability (at least five cycles). By coupling the d-SPE method to HPLC, a new analytical approach was developed and successfully applied to the determination of trace BPF in two water samples, an orange juice and a standard sample with recoveries of 96.0-102.2 % (RSD = 1.1-1.5 %), 95.7-97.4 % (RSD = 1.4-4.4 %) and 98.7 % (RSD = 2.3 %), respectively. The limit of detection (S/N = 3) and limit of quantification (S/N = 10) were 0.1 and 0.3 ng/mL, respectively. The new synthesis strategy opens a viable way to prepare large-size porous spherical COFs, and the developed analytical method can be potentially applied to sensitively detect the trace BPF in water samples and beverages.

17.
Adv Mater ; 36(11): e2308243, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38102967

RESUMO

The development of facile, efficient synthesis method to construct low-cost and high-performance single-atom catalysts (SACs) for oxygen reduction reaction (ORR) is extremely important, yet still challenging. Herein, an atomically dispersed N, S co-doped carbon with abundant vacancy defects (NSC-vd) anchored Fe single atoms (SAs) is reported and a vacancy defects inductive effect is proposed for promoting electrocatalytic ORR. The optimized catalyst featured of stable Fe─N3 S1 active sites exhibits excellent ORR activity with high turnover frequency and mass activity. In situ Raman, attenuated total reflectance surface enhanced infrared absorption spectroscopy reveal the Fe─N3 S1 active sites exhibit different kinetic mechanisms in acidic and alkaline solutions. Operando X-ray absorption spectra reveal the ORR activity of Fe SAs/NSC-vd catalyst in different electrolyte is closely related to the coordination structure. Theoretical calculation reveals the upshifted d band center of Fe─N3 S1 active sites facilitates the adsorption of O2 and accelerates the kinetics process of *OH reduction. The abundant vacancy defects around the Fe─N3 S1 active sites balance the OOH* formation and *OH reduction, thus synergetically promoting the electrocatalytic ORR process.

18.
ACS Appl Mater Interfaces ; 15(42): 49920-49930, 2023 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-37819026

RESUMO

Metal-organic framework (MOF) structures have gained significant attention for their exceptional catalytic performance in ozone degradation, even under high humidity conditions, which is attributed to the presence of unsaturated metal sites (MOF defects). However, the correlation between MOF defects and catalytic ozone remains ambiguous, and a general approach for the controllable synthesis of high-performance MOF structures is currently lacking. Herein, different defective UiO-66 materials with cluster or ligand defects were obtained by precisely controlling small molecular acid modulators. Their catalytic performance can be analyzed in real time through the specific cataluminescence (CTL) signal of ozone at the interface. The presence of ligand defects was found to be crucial for both catalytic degradation and luminescence of ozone, and the CTL signal exhibited a positive correlation with the endogenous hydroxyl group content in the material (R2 = 0.982), while external humidity further supplemented internal water molecules within the material. Furthermore, theoretical calculations were conducted to compare the adsorption behaviors of ozone on the defective UiO-66 under dry/wet conditions, leading to the proposal of two potential reaction pathways. Subsequently, UiO-66-DA with superior catalytic performance was employed to develop a highly efficient CTL sensor capable of accurately detecting ozone (LOD = 23.3 ppb). This study held significant value in elucidating the reaction site of ozone on MOFs and achieving optimal catalytic effects through the careful selection of modulators and humidity levels.

19.
Molecules ; 28(18)2023 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-37764447

RESUMO

In order to improve photocatalytic activity and maximize solar energy use, a new composite material Fe2O3/P2Mo18 was prepared by combining polyoxometalates (P2Mo18) with Fe2O3 nanosheets. FT-IR, XRD, XPS, SEM, TEM, UV-vis, EIS, and PL were used to characterize the composite material, and nano-Fe2O3 of different sizes and morphologies with a controllable absorption range was prepared by adjusting the reaction time, and, when combined with P2Mo18, a composite photocatalyst with efficient visible light response and photocatalytic activity was constructed. The EIS, Bode, and PL spectra analysis results show that the Fe2O3/P2Mo18 composite material has outstanding interfacial charge transfer efficiency and potential photocatalytic application possibilities. Model reactions of methylene blue (MB) and Cr (VI) photodegradation were used to evaluate the redox activity of Fe2O3/P2Mo18 composites under simulated visible light. The photocatalytic degradation rate was as high as 98.98% for MB and 96.86% for Cr (VI) when the composite ratio was Fe2O3/P2Mo18-5%. This research opens up a new avenue for the development of high-performance photocatalysts.

20.
Int J Biol Macromol ; 251: 126325, 2023 Aug 12.
Artigo em Inglês | MEDLINE | ID: mdl-37579896

RESUMO

One more effective measure to solve the energy crisis caused by the shortage of fossil energy is to convert natural renewable resources into high-value chemical products for electrochemical energy storage. Lignin has broad application prospects in this field. In this paper, three kinds of lignin with different molecular weights were obtained by the ethanol/water grading of Kraft lignin (KL). Then, different surface morphology lignin microspheres were prepared by spray drying. Finally, petal-like microspheres were successfully prepared by mixing and grinding the above four kinds of surface morphology lignin microspheres with potassium ferrate and cyanogen chloride and carbonizing at 800 °C and were later used as electrode materials for supercapacitors. Compared with the other microspheres, LMS-F3@Fe3C has the highest specific surface area (1041.42 m2 g-1), the smallest pore size (2.36 nm) and the largest degree of graphitization (ID/IG = 1.06). At a current density of 1 A g-1, the maximum specific capacitance is 786.7 F g-1. At a power density of 1000 W kg-1, the high energy density of 83.3 Wh kg-1 is displayed. This work provides a novel approach to the modulation of surface morphology and structure of lignin microspheres.

SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA