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1.
Adv Sci (Weinh) ; : e2402824, 2024 May 05.
Artigo em Inglês | MEDLINE | ID: mdl-38704682

RESUMO

Creatures, such as Venus flytrap and hummingbirds, capable of rapid predation through snap-through transition, provide paradigms for the design of soft actuators and robots with fast actions. However, these artificial "snappers" usually need contact stimulations to trigger the flipping. Reported here is a constrained anisotropic poly(N-isopropylacrylamide) hydrogel showing fast snapping upon light stimulation. This hydrogel is prepared by flow-induced orientation of nanosheets (NSs) within a rectangular tube. The precursor containing gold nanoparticles is immediately exposed to UV light for photopolymerization to fix the ordered structure of NSs. Two ends of the slender gel are clamped to form a buckle with bistability nature, which snaps to the other side upon laser irradiation. Systematic experiments are conducted to investigate the influences of power intensity and irradiation angle of the laser, as well as thickness and buckle height of the gel, on the snapping behaviors. The fast snapping is further used to kick a plastic bead and control the switch state. Furthermore, synergetic or oscillated snapping of the gel with two buckles of opposite directions is realized by inclined irradiation of a laser or horizontal irradiation with two lasers, respectively. Such light-steered snapping of hydrogels should merit designing soft robots, energy harvests, etc.

2.
Small ; : e2308570, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38716740

RESUMO

Soft-lithography is widely used to fabricate microstructured surfaces on plastics and elastomers for designable physical properties such as wetting and adhesions. However, it remains a big challenge to construct high-aspect-ratio microstructures on the surface of hydrogels due to the difficulty in demolding from the gel with low strength and stiffness. Demonstrated here is the engineering of tough hydrogels by soft-lithography to form well-defined micropillars. The mechanical properties of poly(acrylamide-co-methacrylic acid) hydrogels with dense hydrogen-bond associations severely depend on temperature, with Young's modulus increasing from 8.1 MPa at 15 °C to 821.8 MPa at -30 °C, enabling easy demolding at low temperatures. Arrays of micropillars are maintained on the surface of the gel, and can be used at room temperature when the gel restores soft and stretchable. The hydrogel also exhibits good shape-memory property, favoring tailoring the morphology with a switchable tilt angle of micropillars. Consequently, the hydrogel shows tunable wetting and adhesion properties, as manifested by varying contact angles and adhesion strengths. These surface properties can also be tuned by geometry and arrangement of micropillars. This facile strategy by harnessing tunable viscoelasticity of supramolecular hydrogels should be applicable to other soft materials, and broaden their applications in biomedical and engineering fields.

3.
Am J Chin Med ; : 1-42, 2024 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-38654507

RESUMO

The pathogenesis of Alzheimer's disease (AD), a degenerative disease of the central nervous system, remains unclear. The main manifestations of AD include cognitive and behavioral disorders, neuropsychiatric symptoms, neuroinflammation, amyloid plaques, and neurofibrillary tangles. However, current drugs for AD once the dementia stage has been reached only treat symptoms and do not delay progression, and the research and development of targeted drugs for AD have reached a bottleneck. Thus, other treatment options are needed. Bioactive ingredients derived from plants are promising therapeutic agents. Specifically, Ginkgo biloba (Gb) extracts exert anti-oxidant, anticancer, neuroplastic, neurotransmitter-modulating, blood fluidity, and anti-inflammatory effects, offering alternative options in the treatment of cardiovascular, metabolic, and neurodegenerative diseases. The main chemical components of Gb include flavonoids, terpene lactones, proanthocyanidins, organic acids, polysaccharides, and amino acids. Gb and its extracts have shown remarkable therapeutic effects on various neurodegenerative diseases, including AD, with few adverse reactions. Thus, high-quality Gb extracts are a well-established treatment option for AD. In this review, we summarize the insights derived from traditional Chinese medicine, experimental models, and emerging clinical trials on the role of Gb and its chemical components in the treatment of the main clinical manifestations of AD.

4.
Membranes (Basel) ; 14(3)2024 Feb 25.
Artigo em Inglês | MEDLINE | ID: mdl-38535278

RESUMO

The hydrogen flux inhibition of Pd-Ru membranes under exposure to 1-10% NH3 at 673-773 K was investigated. The Pd-Ru membranes were characterized by XRD, SEM, XPS, and hydrogen permeation tests. The results show that when exposed to 1-10% NH3 at 723 K for 6 h, the hydrogen flux of Pd-Ru membranes sharply decreases by 15-33%, and the decline in hydrogen flux becomes more significant with increasing temperatures. After the removal of 1-10% NH3, 100% recovery of hydrogen flux is observed. XPS results show that nitrogenous species appear on the membrane surface after NH3 exposure, and the hydrogen flux inhibition may be related to the competitive adsorption of nitrogenous species. By comparing the hydrogen flux of Pd-Ru membranes exposed to 10% NH3 with 10% N2, it is indicated that the rapid decrease in hydrogen flux is due to the concentration polarization and competitive adsorption of nitrogenous species. The competitive adsorption effect is attenuated, while the concentration polarization effect becomes more pronounced with increasing temperature.

5.
J Transl Med ; 22(1): 183, 2024 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-38378668

RESUMO

BACKGROUND: Myasthenia gravis (MG) and the experimental autoimmune MG (EAMG) animal model are characterized by T-cell-induced and B-cell-dominated autoimmune diseases that affect the neuromuscular junction. Several subtypes of CD4+ T cells, including T helper (Th) 17 cells, follicular Th cells, and regulatory T cells (Tregs), contribute to the pathogenesis of MG. However, increasing evidence suggests that CD8+ T cells also play a critical role in the pathogenesis and treatment of MG. MAIN BODY: Herein, we review the literature on CD8+ T cells in MG, focusing on their potential effector and regulatory roles, as well as on relevant evidence (peripheral, in situ, cerebrospinal fluid, and under different treatments), T-cell receptor usage, cytokine and chemokine expression, cell marker expression, and Treg, Tc17, CD3+CD8+CD20+ T, and CXCR5+ CD8+ T cells. CONCLUSIONS: Further studies on CD8+ T cells in MG are necessary to determine, among others, the real pattern of the Vß gene usage of autoantigen-specific CD8+ cells in patients with MG, real images of the physiology and function of autoantigen-specific CD8+ cells from MG/EAMG, and the subset of autoantigen-specific CD8+ cells (Tc1, Tc17, and IL-17+IFN-γ+CD8+ T cells). There are many reports of CD20-expressing T (or CD20 + T) and CXCR5+ CD8 T cells on autoimmune diseases, especially on multiple sclerosis and rheumatoid arthritis. Unfortunately, up to now, there has been no report on these T cells on MG, which might be a good direction for future studies.


Assuntos
Linfócitos T CD8-Positivos , Miastenia Gravis Autoimune Experimental , Animais , Humanos , Linfócitos T Auxiliares-Indutores/metabolismo , Miastenia Gravis Autoimune Experimental/metabolismo , Linfócitos T Reguladores , Autoantígenos/metabolismo
6.
Small ; : e2311431, 2024 Feb 16.
Artigo em Inglês | MEDLINE | ID: mdl-38366284

RESUMO

Renewable electricity-driven seawater splitting presents a green, effective, and promising strategy for building hydrogen (H2 )-based energy systems (e.g., storing wind power as H2 ), especially in many coastal cities. The abundance of Cl- in seawater, however, will cause severe corrosion of anode catalyst during the seawater electrolysis, and thus affect the long-term stability of the catalyst. Herein, seawater oxidation performances of NiFe layered double hydroxides (LDH), a classic oxygen (O2 ) evolution material, can be boosted by employing tungstate (WO4 2- ) as the intercalated guest. Notably, insertion of WO4 2- to LDH layers upgrades the reaction kinetics and selectivity, attaining higher current densities with ≈100% O2 generation efficiency in alkaline seawater. Moreover, after a 350 h test at 1000 mA cm-2 , only trace active chlorine can be detected in the electrolyte. Additionally, O2 evolution follows lattice oxygen mechanism on NiFe LDH with intercalated WO4 2- .

7.
ACS Appl Mater Interfaces ; 16(5): 6433-6446, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38289030

RESUMO

Marine biofouling, resulting from the adhesion of marine organisms to ship surfaces, has long been a significant issue in the maritime industry. In this paper, we focused on utilizing soft and hydrophilic hydrogels as a potential approach for antifouling (AF) coatings. Acrylic acid (AA) with a polyelectrolyte effect and N-(3-sulfopropyl)-N-(methacryloxyethyl)-N,N-dimethylammonium betaine (SBMA) with an antipolyelectrolyte effect were selected as monomers. By adjusting the monomer ratio, we were able to create hydrogel coatings that exhibited low swelling ratio in both fresh water and seawater. The Al(OH)3 nanoparticle, as a physical cross-linker, provided better mechanical properties (higher tensile strength and larger elongation at break) than the chemical cross-linker through the dynamic coordination bonds and plentiful hydrogen bonds. Additionally, we incorporated trehalose into the hydrogel, enabling the repair of the hydrogel network through covalent-like hydrogen bonding. The zwitterion compound SBMA endowed the hydrogel with excellent AF performance. It was found that the highest SBMA content did not lead to the best antibacterial performance, as bacterial adhesion quantity was also influenced by the charge of the hydrogel. The hydrogel with appropriate SBMA content being close to electrical neutrality exhibits the strongest zwitterionic property of PSBMA chains, resulting in the best antibacterial adhesion performance. Furthermore, the pronounced hydrophilicity of SBMA enhanced the lubrication of the hydrogel surface, thereby reducing the friction resistance when applied to the hull surface during ship navigation.

8.
Small ; : e2310468, 2024 Jan 11.
Artigo em Inglês | MEDLINE | ID: mdl-38213023

RESUMO

The production of hydrogen peroxide (H2 O2 ) via the two-electron electrochemical oxygen reduction reaction (2e- ORR) is an essential alteration in the current anthraquinone-based method. Herein, a single-atom Co─O4 electrocatalyst is embedded in a defective and porous graphene-like carbon layer (Co─O4 @PC). The Co─O4 @PC electrocatalyst shows promising potential in H2 O2 electrosynthesis via 2e- ORR, providing a high H2 O2 selectivity of 98.8% at 0.6 V and a low onset potential of 0.73 V for generating H2 O2 . In situ surface-sensitive attenuated total reflection Fourier transform infrared spectra and density functional theory calculations reveal that the electronic and geometric modification of Co─O4 induced by defective carbon sites result in decreased d-band center of Co atoms, providing the optimum adsorption energies of OOH* intermediate. The H-cell and flow cell assembled using Co─O4 @PC as the cathode present long-term stability and high efficiency for H2 O2 production. Particularly, a high H2 O2 production rate of 0.25 mol g-1 cat  h-1 at 0.6 V can be obtained by the flow cell. The in situ-generated H2 O2 can promote the degradation of rhodamine B and sterilize Staphylococcus aureus via the Fenton process. This work can pave the way for the efficient production of H2 O2 by using Co─O4 single atom electrocatalyst and unveil the electrocatalytic mechanism.

9.
Anim Biosci ; 37(1): 50-60, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37641828

RESUMO

OBJECTIVE: Testicular fat deposition has been reported to affect animal reproduction. However, the underlying mechanism remains poorly understood. The present study explored whether sperm meiosis and testosterone synthesis contribute to mouse testicular fat depositioninduced reproductive performance. METHODS: High fat diet (HFD)-induced obesity CD1 mice (DIO) were used as a testicular fat deposition model. The serum hormone test was performed by agent kit. The quality of sperm was assessed using a Sperm Class Analyzer. Testicular tissue morphology was analyzed by histochemical methods. The expression of spermatocyte marker molecules was monitored by an immuno-fluorescence microscope during meiosis. Analysis of the synthesis of testosterone was performed by real-time polymerase chain reaction and reagent kit. RESULTS: It was found that there was a significant increase in body weight among DIO mice, however, the food intake showed no difference compared to control mice fed a normal diet (CTR). The number of offspring in DIO mice decreased, but there was no significant difference from the CTR group. The levels of follicle-stimulating hormone were lower in DIO mice and their luteinizing hormone levels were similar. The results showed a remarkable decrease in sperm density and motility among DIO mice. We also found that fat accumulation affected the meiosis process, mainly reflected in the cross-exchange of homologous chromosomes. In addition, overweight increased fat deposition in the testis and reduced the expression of testosterone synthesis-related enzymes, thereby affecting the synthesis and secretion of testosterone by testicular Leydig cells. CONCLUSION: Fat accumulation in the testes causes testicular cell dysfunction, which affects testosterone hormone synthesis and ultimately affects sperm formation.

10.
Small ; 20(11): e2306273, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-37936322

RESUMO

A novel semiconductive Co/Fe-MOF embedded with Fe2 O3 nanocrystals (Fe2 O3 @CoFe-MOF) is developed as a trifunctional electrocatalyst for the urea oxidation reaction (UOR), oxygen evolution reaction (OER), and hydrogen evolution reaction for enhancing the efficiency of the hydrogen production via the urea-assisted overall water splitting. Fe2 O3 @CoFe-TPyP-MOF comprises unsaturated metal-nitrogen coordination sites, affording enriched defects, self-tuned d-band centers, and efficient π-π interaction between different layers. Density functional theory calculation confirms that the adsorption of urea can be optimized at Fe2 O3 @CoFe-TPyP-MOF, realizing the efficient adsorption of intermediates and desorption of the final product of CO2 and N2 characterized by the in situ Fourier transform infrared spectroscopy. The two-electrode urea-assisted water splitting device-assembled with Fe2 O3 @CoFe-TPyP-MOF illustrates a low cell voltage of 1.41 V versus the reversible hydrogen electrode at the current density of 10 mA cm-2 , attaining the hydrogen production rate of 13.13 µmol min-1 in 1 m KOH with 0.33 m urea. The in situ electrochemical Raman spectra and other basic characterizations of the used electrocatalyst uncover that Fe2 O3 @CoFe-TPyP-MOF undergoes the reversible structural reconstruction after the UOR test, while it demonstrates the irreversible reconstruction after the OER measurement. This work redounds the progress of urea-assisted water spitting for hydrogen production.

11.
Front Neurol ; 14: 1209302, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37859648

RESUMO

Stiff person syndrome (SPS) is a rare central nervous system disorder associated with malignancies. In this review, we retrieved information from PubMed, up until August 2023, using various search terms and their combinations, including SPS, stiff person syndrome spectrum disorders (SPSSDs), paraneoplastic, cancer, and malignant tumor. Data from peer-reviewed journals printed in English were organized to explain the possible relationships between different carcinomas and SPSSD subtypes, as well as related autoantigens. From literature searching, it was revealed that breast cancer was the most prevalent carcinoma linked to SPSSDs, followed by lung cancer and lymphoma. Furthermore, classic SPS was the most common SPSSD subtype, followed by stiff limb syndrome and progressive encephalomyelitis with rigidity and myoclonus. GAD65 was the most common autoantigen in patients with cancer and SPSSDs, followed by amphiphysin and GlyR. Patients with cancer subtypes might have multiple SPSSD subtypes, and conversely, patients with SPSSD subtypes might have multiple carcinoma subtypes. The first aim of this review was to highlight the complex nature of the relationships among cancers, autoantigens, and SPSSDs as new information in this field continues to be generated globally. The adoption of an open-minded approach to updating information on new cancer subtypes, autoantigens, and SPSSDs is recommended to renew our database. The second aim of this review was to discuss SPS animal models, which will help us to understand the mechanisms underlying the pathogenesis of SPS. In future, elucidating the relationship among cancers, autoantigens, and SPSSDs is critical for the early prediction of cancer and discovery of new therapeutic modalities.

12.
Proc Natl Acad Sci U S A ; 120(45): e2308035120, 2023 Nov 07.
Artigo em Inglês | MEDLINE | ID: mdl-37883417

RESUMO

Metallic nickel (Ni) is a promising candidate to substitute Pt-based catalysts for hydrogen oxidation reaction (HOR), but huge challenges still exist in precise modulation of the electronic structure to boost the electrocatalytic performances. Herein, we present the use of single-layer Ti3C2Tx MXene to deliberately tailor the electronic structure of Ni nanoparticles via interfacial oxygen bridges, which affords Ni/Ti3C2Tx electrocatalyst with exceptional performances for HOR in an alkaline medium. Remarkably, it shows a high kinetic current of 16.39 mA cmdisk-2 at the overpotential of 50 mV for HOR [78 and 2.7 times higher than that of metallic Ni and Pt/C (20%), respectively], also with good durability and CO antipoisoning ability (1,000 ppm) that are not available for conventional Pt/C (20%) catalyst. The ultrahigh conductivity of single-layer Ti3C2Tx provides fast transmission of electrons for Ni nanoparticles, of which the uniform and small sizes endow them with high-density active sites. Further, the terminated -O/-OH functional groups on Ti3C2Tx directionally capture electrons from Ni nanoparticles via interfacial Ni-O bridges, leading to obvious electronic polarization. This could enhance the Nids-O2p interaction and weaken Nids-H1s interaction of Ni sites in Ni/Ti3C2Txenabling a suitable H-/OH-binding energy and thus enhancing the HOR activity.

13.
Infect Drug Resist ; 16: 6567-6586, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37823028

RESUMO

Objective: This paper explores the drug resistance, genome and proteome expression characteristics of Salmonella from a food poisoning event. Methods: A multidrug-resistant Salmonella Enteritidis strain, labeled as 27A, was isolated and identified from a food poisoning patient. Antimicrobial susceptibility testing determined the resistance of 27A strain to 14 antibiotics. Then, WGS analysis and comparative genomics analysis were performed on 27A, and the functional annotation of resistance genes, virulence genes were performed based on VFDB, ARDB, COG, CARD, GO, KEGG, and CAZY databases. Meanwhile, based on iTRAQ technology, quantitative proteomic analysis was conducted on 27A to analyze the functions and interactions of differentially expressed proteins related to bacterial resistance and pathogenicity. Results: Strain 27A belonged to ST11 S. Enteritidis and was resistant to levofloxacin, ciprofloxacin, ampicillin, piperacillin, and ampicillin/sulbactam. There were 33 drug resistance genes, 384 virulence genes and 2 plasmid replicon, IncFIB(S) and IncFII(S), annotated by WGS. Proteomic analysis revealed significant changes in virulence and drug proteins, which were mainly involved in bacterial pathogenicity and metabolic processes. PPI prediction showed the relationship between virulence proteins and T3SS proteins, and PagN cooperated with proteins related to T3SS to jointly mediate the invasion of 27A strain on the human body. Phylogenetic analysis indicated that S. Enteritidis has potential transmission in humans, food, and animals. Conclusion: This study comprehensively analyzed the drug resistance and virulence phenotypes of S. Enteritidis 27A using genomic and proteomic approaches. These helps reveal the drug resistance and virulence mechanisms of S. Enteritidis, and provides important information for the source tracing and the prevention of related diseases, which lays a foundation for research on food safety, public health monitoring, and the drug resistance and pathogenicity of S. Enteritidis.

14.
Front Aging Neurosci ; 15: 1206572, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37600514

RESUMO

Alzheimer's disease (AD) is the most common chronic neurodegenerative disease worldwide. It causes cognitive dysfunction, such as aphasia and agnosia, and mental symptoms, such as behavioral abnormalities; all of which place a significant psychological and economic burden on the patients' families. No specific drugs are currently available for the treatment of AD, and the current drugs for AD only delay disease onset and progression. The pathophysiological basis of AD involves abnormal deposition of beta-amyloid protein (Aß), abnormal tau protein phosphorylation, decreased activity of acetylcholine content, glutamate toxicity, autophagy, inflammatory reactions, mitochondria-targeting, and multi-targets. The US Food and Drug Administration (FDA) has approved five drugs for clinical use: tacrine, donepezil, carbalatine, galantamine, memantine, and lecanemab. We have focused on the newer drugs that have undergone clinical trials, most of which have not been successful as a result of excessive clinical side effects or poor efficacy. Although aducanumab received rapid approval from the FDA on 7 June 2021, its long-term safety and tolerability require further monitoring and confirmation. In this literature review, we aimed to explore the possible pathophysiological mechanisms underlying the occurrence and development of AD. We focused on anti-Aß and anti-tau drugs, mitochondria-targeting and multi-targets, commercially available drugs, bottlenecks encountered in drug development, and the possible targets and therapeutic strategies for future drug development. We hope to present new concepts and methods for future drug therapies for AD.

15.
Molecules ; 28(11)2023 May 26.
Artigo em Inglês | MEDLINE | ID: mdl-37298849

RESUMO

High-purity hydrogen is extensively employed in chemical vapor deposition, and the existence of methane impurity significantly impacts the device performance. Therefore, it is necessary to purify hydrogen to remove methane. The ZrMnFe getter commonly used in the industry reacts with methane at a temperature as high as 700 ∘C, and the removal depth is not sufficient. To overcome these limitations, Co partially substitutes Fe in the ZrMnFe alloy. The alloy was prepared by suspension induction melting method, and was characterized by means of XRD, ICP, SEM and XPS. The concentration of methane at the outlet was detected by gas chromatography to characterize the hydrogen purification performance of the alloy. The removal effect of the alloy on methane in hydrogen increases first and then decreases with the increase in substitution amount, and increases with the increase in temperature. Specifically, the ZrMnFe0.7Co0.3 alloy reduces methane levels in hydrogen from 10 ppm to 0.215 ppm at 500 ∘C. ZrMnFe0.7Co0.3 alloy can remove 50 ppm of methane in helium to less than 0.01 ppm at 450 ∘C, demonstrating its excellent methane reactivity. Moreover, Co substitution reduces the formation energy barrier of ZrC, and Co in the electron-rich state demonstrates superior catalytic activity for methane decomposition.


Assuntos
Ligas , Metano , Ligas/química , Metano/química , Gases , Temperatura , Hidrogênio
16.
ACS Nano ; 17(12): 11290-11308, 2023 06 27.
Artigo em Inglês | MEDLINE | ID: mdl-37276377

RESUMO

Cancer phototheranostics have the potential for significantly improving the therapeutic effectiveness, as it can accurately diagnose and treat cancer. However, the current phototheranostic platforms leave much to be desired and are often limited by tumor hypoxia. Herein, a Schottky junction nanozyme has been established between a manganese-bridged cobalt-phthalocyanines complex and Ti3C2Tx MXene nanosheets (CoPc-Mn/Ti3C2Tx), which can serve as an integrative type I and II photosensitizer for enhancing cancer therapeutic efficacy via a photoacoustic imaging-guided multimodal chemodynamic/photothermal/photodynamic therapy strategy under near-infrared (808 nm) light irradiation. The Schottky junction not only possessed a narrow-bandgap, enhanced electron-hole separation ability and exhibited a potent redox potential but also enabled improved H2O2 and O2 supplying performances in vitro. Accordingly, the AS1411 aptamer-immobilized CoPc-Mn/Ti3C2Tx nanozyme illustrated high accuracy and excellent anticancer efficiency through a multimodal therapy strategy in in vitro and in vivo experiments. This work presents a valuable method for designing and constructing a multifunctional nanocatalytic medicine platform for synergistic cancer therapy of solid tumors.


Assuntos
Nanopartículas , Neoplasias , Fotoquimioterapia , Humanos , Fotoquimioterapia/métodos , Peróxido de Hidrogênio , Titânio/uso terapêutico , Neoplasias/diagnóstico por imagem , Neoplasias/tratamento farmacológico , Linhagem Celular Tumoral , Microambiente Tumoral , Nanopartículas/uso terapêutico
17.
Small ; 19(42): e2302600, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37322392

RESUMO

An n-n type heterojunction comprising with CuN and BN dual active sites is synthesized via in situ growth of a conductive metal-organic framework (MOF) [Cu3 (HITP)2 ] (HITP = 2,3,6,7,10,11-hexaiminotriphenylene) on hexagonal boron nitride (h-BN) nanosheets (hereafter denoted as Cu3 (HITP)2 @h-BN) for the electrocatalytic nitrogen reduction reaction (eNRR). The optimized Cu3 (HITP)2 @h-BN shows the outstanding eNRR performance with the NH3 production of 146.2 µg h-1 mgcat -1 and the Faraday efficiency of 42.5% due to high porosity, abundant oxygen vacancies, and CuN/BN dual active sites. The construction of the n-n heterojunction efficiently modulates the state density of active metal sites toward the Fermi level, facilitating the charge transfer at the interface between the catalyst and reactant intermediates. Additionally, the pathway of NH3 production catalyzed by the Cu3 (HITP)2 @h-BN heterojunction is illustrated by in situ FT-IR spectroscopy and density functional theory calculation. This work presents an alternative approach to design advanced electrocatalysts based on conductive MOFs.

18.
Chemistry ; 29(38): e202300969, 2023 Jul 06.
Artigo em Inglês | MEDLINE | ID: mdl-37098764

RESUMO

Energy dissipation based on dynamic fracture of metal ligands is an effective way to toughen hydrogels for specific applications in biomedical and engineering fields. Exploration of new kinds of metal-ligand coordinates with robust bonding strength is crucial for the facile synthesis of tough gels. Here a hydrogel toughening strategy based on the formation of robust coordination complexes between the hydrazide ligands and zinc ions is reported. The resultant hydrogels exhibit high strength and toughness at room temperature. Their mechanical properties show temperature dependence due to the dynamic nature of coordination bonds. In addition, the amine group of hydrazides in the gel matrix provides a reactive site for Schiff's base reaction, enabling surface modification without influence on overall mechanical performances of the gel. The hydrazide ligands are easy to synthesize and can coordinate very well with several transition metals. Such a metal-ligand coordination should be suitable to develop tough soft materials with versatile applications.


Assuntos
Complexos de Coordenação , Hidrogéis , Hidrogéis/química , Ligantes , Hidrazinas , Metais , Zinco
19.
Adv Sci (Weinh) ; 10(15): e2206933, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36995064

RESUMO

Electrocatalytic nitrogen reduction reaction (NRR) represents a promising sustainable approach for NH3 synthesis. However, the poor NRR performance of electrocatalysts is a great challenge at this stage, mainly owing to their low activity and the competitive hydrogen evolution reaction (HER). Herein, 2D ferric covalent organic framework/MXene (COF-Fe/MXene) nanosheets with controllable hydrophobic behaviors are successfully prepared via a multiple-in-one synthetic strategy. The boosting hydrophobicity of COF-Fe/MXene can effectively repel water molecules to inhibit the HER for enhanced NRR performances. By virtue of the ultrathin nanostructure, well-defined single Fe sites, nitrogen enrichment effect, and high hydrophobicity, the 1H,1H,2H,2H-perfluorodecanethiol modified COF-Fe/MXene hybrid shows a NH3 yield of 41.8 µg h-1 mgcat. -1 and a Faradaic efficiency of 43.1% at -0.5 V versus RHE in a 0.1 m Na2 SO4 water solution, which are vastly superior to the known Fe-based catalysts and even to the noble metal catalysts. This work provides a universal strategy to design and synthesis of non-precious metal electrocatalysts for high-efficiency N2 reduction to NH3 .

20.
Nanotechnology ; 34(20)2023 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-36745917

RESUMO

With the rapid development of sodium-ion batteries (SIBs), it is urgent to exploit the cathode materials with good rate capability, attractive high energy density and considerable long cycle performance. Na3V2(PO4)3(NVP), as a NASICON-type electrode material, is one of the cathode materials with great potential for application because of its good thermal stability and stable. However, NVP has the inherent problem of low electronic conductivity, and various strategies are proposed to improve it, moreover, nanotechnology or nanostructure are involved in these strategies, the construction of nanostructured active particles and nanocomposites with conductive carbon networks have been shown to be effective in improving the electrical conductivity of NVP. Herein, we review the research progress of NVP performance improvement strategies from the perspective of nanostructures and classifies the prepared nanomaterials according to their different nano-dimension. In addition, NVP nanocomposites are reviewed in terms of both preparation methods and promotion effects, and examples of NVP nanocomposites at different nano-dimension are given. Finally, some personal views are presented to provide reasonable guidance for the research and design of high-performance polyanionic cathode materials of SIBs.

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