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2.
Small ; 20(30): e2311013, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38372007

RESUMEN

The ability to design halide perovskite nanocrystals (PNCs) with circularly polarized luminescence (CPL) offers exceptional potential in photonic technologies. Despite recent inspiring advances, the creation of PNCs with full-color tailorablity, outstanding CPL, and long-term stability remains a substantial challenge. Herein, a robust strategy to craft CPL-active PNCs is reported, exhibiting appealing full-color tunable wavelengths, enhanced CPL, and prolonged stability. In contrast to conventional methodologies, this strategy utilizes chiral nematic mesoporous silica (CNMS) as host to render in situ confined growth of diverse achiral PNCs. By strategically engineering photonic bandgap, adjusting loading amount of PNCs, and manipulating cations/anion compositions of PNCs, robust CPL responses with tunable wavelength and intensity are successfully obtained. The resulting PNCs-CNMS achieves stable CPL emissions with full-color tunability and impressive luminescent dissymmetric factors up to -0.17. Remarkably, silica-based hosts as a protective barrier confer exceptional resistance to humidity, photodegradation, and thermal stability, even up to 95 °C. Furthermore, the ability to achieve reversible CPL switching within PNCs-CNMS is attainable by leveraging the responsiveness of CNMS matrix or dynamic behavior of impregnated PNCs. Additionally, circularly polarized light-emitting diode devices based on PNCs-CNMS can be conveniently fabricated. This research affords a powerful platform for designing functional chiroptical materials.

3.
Angew Chem Int Ed Engl ; 63(18): e202401924, 2024 Apr 24.
Artículo en Inglés | MEDLINE | ID: mdl-38366134

RESUMEN

Nitrate electroreduction reaction (eNO3 -RR) to ammonia (NH3) provides a promising strategy for nitrogen utilization, while achieving high selectivity and durability at an industrial scale has remained challenging. Herein, we demonstrated that the performance of eNO3 -RR could be significantly boosted by introducing two-dimensional Cu plates as electrocatalysts and eliminating the general carrier gas to construct a steady fluid field. The developed eNO3 -RR setup provided superior NH3 Faradaic efficiency (FE) of 99 %, exceptional long-term electrolysis for 120 h at 200 mA cm-2, and a record-high yield rate of 3.14 mmol cm-2 h-1. Furthermore, the proposed strategy was successfully extended to the Zn-nitrate battery system, providing a power density of 12.09 mW cm-2 and NH3 FE of 85.4 %, outperforming the state-of-the-art eNO3 -RR catalysts. Coupled with the COMSOL multiphysics simulations and in situ infrared spectroscopy, the main contributor for the high-efficiency NH3 production could be the steady fluid field to timely rejuvenate the electrocatalyst surface during the electrocatalysis.

4.
Adv Mater ; 36(19): e2313096, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38308111

RESUMEN

Despite the increasing effort in advancing oxygen electrocatalysts for zinc-air batteries (ZABs), the performance development gradually reaches a plateau via only ameliorating the electrocatalyst materials. Herein, a new class of external field-responsive electrocatalyst comprising Ni0.5Mn0.5Fe2O4 stably dispersed on N-doped Ketjenblack (Ni0.5Mn0.5Fe2O4/N-KB) is developed via polymer-assisted strategy for practical ZABs. Briefly, the activity indicator ΔE is significantly decreased to 0.618 V upon photothermal assistance, far exceeding most reported electrocatalysts (generally >0.680 V). As a result, the photothermal electrocatalyst possesses comprehensive merits of excellent power density (319 mW cm-2), ultralong lifespan (5163 cycles at 25 mA cm-2), and outstanding rate performance (100 mA cm-2) for liquid ZABs, and superb temperature and deformation adaptability for flexible ZABs. Such improvement is attributed to the photothermal-heating-enabled synergy of promoted electrical conductivity, reactant-molecule motion, active area, and surface reconstruction, as revealed by operando Raman and simulation. The findings open vast possibilities toward more-energy-efficient energy applications.

5.
Front Microbiol ; 14: 1273842, 2023.
Artículo en Inglés | MEDLINE | ID: mdl-38075910

RESUMEN

By the end of 2021, the pear yield in Xinjiang reached 1,795,900 tons, accounting for 1/9 of the country. Pear black spot, caused by Alternaria gaisen disease, has had a significant impact on the pear industry. A. gaisen can infect nearly all pear plants, resulting in black spots on the fruit that negatively affect both yield and quality. This study focused on the TRM76323 strain of Streptomyces, which was isolated from the soil of Tamarix chinensis in Xinjiang Province. Through a multiphase classification and identification method, the genetic classification status of the antagonistic strains was determined. The study also identified the antibacterial active components of streptochlorin using modern isolation and purification techniques. The antagonistic activity of Streptomyces against Alternaria was analyzed through in vitro and in vivo experiments. This research not only expanded the resource bank of antagonistic microorganisms in extreme environments in Xinjiang, but also identified active components that could contribute to the development of new drug lead compounds. Additionally, this study presents a novel approach for the prevention and control of pear black spot disease.

6.
Small Methods ; : e2301307, 2023 Dec 13.
Artículo en Inglés | MEDLINE | ID: mdl-38088567

RESUMEN

Despite that extensive efforts have been dedicated to the search for advanced catalysts to boost the electrocatalytic nitrobenzene reduction reaction (eNBRR), its progress is severely hampered by the limited understanding of the relationship between catalyst structure and its catalytic performance. Herein, this review aims to bridge such a gap by first analyzing the eNBRR pathway to present the main influential factors, such as electrolyte feature, applied potential, and catalyst structure. Then, the recent advancements in catalyst design for eNBRR are comprehensively summarized, particularly about the impacts of chemical composition, morphology, and crystal facets on regulating the local microenvironment, electron and mass transport for boosting catalytic performance. Finally, the future research of eNBRR is also proposed from the perspectives of performance enhancement, expansion of product scope, in-depth understanding of the reaction mechanism, and acceleration of the industrialization process through the integration of upstream and downstream technologies.

7.
Chem Commun (Camb) ; 59(95): 14126-14129, 2023 Nov 28.
Artículo en Inglés | MEDLINE | ID: mdl-37947301

RESUMEN

This study presents an optimized co-antisolvent modulation strategy for producing two-dimensional lead-free chiral double perovskite nanomaterial with superior chirality and stability. The chiroptical signals or their dissymmetric factors are significantly influenced by the selection of antisolvent mixture. This research contributes to the advancement of chiral semiconductor materials and expands the understanding of their behavior at the nanoscale.

8.
J Colloid Interface Sci ; 650(Pt B): 1842-1850, 2023 Nov 15.
Artículo en Inglés | MEDLINE | ID: mdl-37515974

RESUMEN

Sluggish kinetics of hydrogen oxidation reaction (HOR) in alkaline solution has restricted the rapid development of hydrogen economy. Constructing catalyst with metal-oxide heterostructures can enhance HOR performance; however, little studies concentrate on charge transfer between them, and the corresponding effects on reactions remain unclear. Herein, we report charge-transfer-adjustable CeO2/Rh interfaces uniformly dispersed on multiwalled carbon nanotube (CNT), which exhibit excellent alkaline HOR performance. Results confirm that the charge transfer from Rh to CeO2 could be conveniently tuned via thermal treatment. Consequently, the adsorption free energies of H* in Rh sites and OH* adsorption strength in CeO2 could be adjusted, as corroborated by density functional theory study. The optimized CeO2/Rh interfaces exhibit an exchange current density and a mass-specific kinetic current of 0.53 mA cmPGM-2 and 830 A gPGM-1 at an overpotential of 50 mV, respectively, which surpasses most of the advanced noble-metal-based electrocatalysts. This work provides a new insight of harnessing charge transfer of heterostructure to enhance catalytic activities.

9.
Small Methods ; 7(4): e2201534, 2023 04.
Artículo en Inglés | MEDLINE | ID: mdl-36813751

RESUMEN

The past several years have witnessed a rapid development of intelligent wearable devices. However, despite the splendid advances, the creation of flexible human-machine interfaces that synchronously possess multiple sensing capabilities, wearability, accurate responsivity, sensitive detectivity, and fast recyclability remains a substantial challenge. Herein, a convenient yet robust strategy is reported to craft flexible transient circuits via stencil printing liquid metal conductor on the water-soluble electrospun film for human-machine interaction. Due to the inherent liquid conductor within porous substrate, the circuits feature high-resolution, customized patterning viability, attractive permeability, excellent electroconductivity, and superior mechanical stability. More importantly, such circuits display appealing noncontact proximity capabilities while maintaining compelling tactile sensing performance, which is unattainable by traditional systems with compromised contact sensing. As such, the flexible circuit is utilized as wearable sensors with practical multifunctionality, including information transfer, smart identification, and trajectory monitoring. Furthermore, an intelligent human-machine interface composed of the flexible sensors is fabricated to realize specific goals such as wireless object control and overload alarm. The transient circuits are quickly and efficiently recycled toward high economic and environmental values. This work opens vast possibilities of generating high-quality flexible and transient electronics for advanced applications in soft and intelligent systems.


Asunto(s)
Percepción del Tacto , Dispositivos Electrónicos Vestibles , Humanos , Electrónica , Metales , Tacto
10.
ACS Appl Mater Interfaces ; 14(40): 45476-45483, 2022 Oct 12.
Artículo en Inglés | MEDLINE | ID: mdl-36190118

RESUMEN

A highly stable composite electrolyte was developed in this research to address the performance decline over time in a solid lithium ion battery (SLIB). It involved the synthesis of bifunctional MOF material (MOF-2) from two different functionalized UiO-66 materials containing carboxyl groups and amine groups, respectively, and the subsequent blending of PEO (polyethylene oxide) with the MOF-2 to form the novel composite solid electrolyte (PEO-MOF-2). The composite electrolytes showed higher ionic conductivity (5.20 × 10-4 S/cm) than that of pristine PEO. The LiFePO4||Li cells constructed with PEO-MOF-2 exhibited 98.45% capacity retention with 149.92 mA h/g after 100 cycles operation at 1.0 C, which was higher than those cells prepared with pristine PEO electrolyte or with PEO-based electrolytes that were only doped by aminated MOF or carboxylated MOF. Furthermore, our experiments showed that there was about a 40% increase in the potential window (from 3.5 to 5.0 V) and 80% increase in the lithium ion transfer number (from 0.20 to 0.36 at 60 °C) as a result of replacing pristine PEO electrolyte with PEO-MOF-2.

11.
Small ; 18(27): e2202194, 2022 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-35665997

RESUMEN

The ability to craft high-efficiency and non-precious bifunctional oxygen catalysts opens an enticing avenue for the real-world implementation of metal-air batteries (MABs). Herein, Co3 O4 encapsulated within nitrogen defect-rich g-C3 N4 (denoted Co3 O4 @ND-CN) as a bifunctional oxygen catalyst for MABs is prepared by graphitizing the zeolitic imidazolate framework (ZIF)-67@ND-CN. Co3 O4 @ND-CN possesses superb bifunctional catalytic performance, which facilitates the construction of high-performance MABs. Concretely, the rechargeable zinc-air battery based on Co3 O4 @ND-CN shows a superior round-trip efficiency of ≈60% with long-term durability (over 340 cycles), exceeding the battery with the state-of-the-art noble metals. The corresponding lithium-oxygen battery using Co3 O4 @ND-CN exhibits an excellent maximum discharge/charge capacity (9838.8/9657.6 mAh g-1 ), an impressive discharge/charge overpotential (1.14 V/0.18 V), and outstanding cycling stability. Such compelling electrocatalytic processes and device performances of Co3 O4 @ND-CN originate from concurrent compositional (i.e., defect-engineering) and structural (i.e., wrinkled morphology with abundant porosity) elaboration as well as the well-defined synergy between Co3 O4 and ND-CN, which produce an advantageous surface electronic environment corroborated by theoretical modeling. By extension, a rich diversity of other metal oxides@ND-CN with adjustable defects, architecture, and enhanced activities may be rationally designed and crafted for both scientific research on catalytic properties and technological development in renewable energy conversion and storage systems.

12.
Front Chem ; 10: 874675, 2022.
Artículo en Inglés | MEDLINE | ID: mdl-35494639

RESUMEN

Large-scale synthesis of graphene-based nanomaterials in stirred tank reactor (STR) often results in serious agglomeration because of the poor control during micromixing process. In this work, reactive impingement mixing is conducted in a two-stage impinging jet microreactor (TS-IJMR) for the controllable and scale-up synthesis of nickel-cobalt boride@borate core-shell nanostructures on RGO flakes (NCBO/RGO). Benefiting from the good process control and improved micromixing efficiency of TS-IJMR, NCBO/RGO nanosheet provides a large BET surface area, abundant of suitable mesopores (2-5 nm), fast ion diffusion, and facile electron transfer within the whole electrode. Therefore, NCBO/RGO electrode exhibits a high specific capacitance of 2383 F g-1 at 1 A g-1, and still retains 1650 F g-1 when the current density is increased to 20 A g-1, much higher than those of nickel boride@borate/RGO (NBO/RGO) and cobalt boride@borate/RGO (CBO/RGO) synthesized in TS-IJMR, as well as NCBO/RGO-S synthesized in STR. In addition, an asymmetric supercapacitor (NCBO/RGO//AC) is constructed with NCBO/RGO and activated carbon (AC), which displays a high energy density of 53.3 W h kg-1 and long cyclic lifespan with 91.8% capacitance retention after 5000 charge-discharge cycles. Finally, NCBO/RGO is used as OER electrocatalyst to possess a low overpotential of 309 mV at a current density of 10 mA cm-2 and delivers a good long-term durability for 10 h. This study opens up the potential of controllable and scale-up synthesis of NCBO/RGO nanosheets for high-performance supercapacitor electrode materials and OER catalysts.

13.
Front Chem ; 9: 724188, 2021.
Artículo en Inglés | MEDLINE | ID: mdl-34307305

RESUMEN

Recently, as our population increasingly ages with more pressure on bone and cartilage diseases, bone/cartilage tissue engineering (TE) have emerged as a potential alternative therapeutic technique accompanied by the rapid development of materials science and engineering. The key part to fulfill the goal of reconstructing impaired or damaged tissues lies in the rational design and synthesis of therapeutic agents in TE. Gold nanomaterials, especially gold nanoparticles (AuNPs), have shown the fascinating feasibility to treat a wide variety of diseases due to their excellent characteristics such as easy synthesis, controllable size, specific surface plasmon resonance and superior biocompatibility. Therefore, the comprehensive applications of gold nanomaterials in bone and cartilage TE have attracted enormous attention. This review will focus on the biomedical applications and molecular mechanism of gold nanomaterials in bone and cartilage TE. In addition, the types and cellular uptake process of gold nanomaterials are highlighted. Finally, the current challenges and future directions are indicated.

14.
Front Chem ; 9: 677821, 2021.
Artículo en Inglés | MEDLINE | ID: mdl-33981678

RESUMEN

Though solar cells are one of the promising technologies to address the energy crisis, this technology is still far from commercialization. Thermoelectric materials offer a novel opportunity to convert energy between thermal and electrical aspects, which show the feasibility to improve the performance of solar cells via heat management and light harvesting. Polymer-inorganic thermoelectric nanocomposites consisting of inorganic nanomaterials and functional organic polymers represent one kind of advanced hybrid nanomaterials with tunable optical and electrical characteristics and fascinating interfacial and surface chemistry. During the past decades, they have attracted extensive research interest due to their diverse composition, easy synthesis, and large surface area. Such advanced nanomaterials not only inherit low thermal conductivity from polymers and high Seebeck coefficient, and high electrical conductivity from inorganic materials, but also benefit from the additional interface between each component. In this review, we provide an overview of interfacial chemistry engineering and electrical feature of various polymer-inorganic thermoelectric hybrid nanomaterials, including synthetic methods, properties, and applications in thermoelectric devices. In addition, the prospect and challenges of polymer-inorganic nanocomposites are discussed in the field of thermoelectric energy.

15.
Nanoscale ; 12(16): 8636-8646, 2020 Apr 30.
Artículo en Inglés | MEDLINE | ID: mdl-32296803

RESUMEN

As an emerging photocatalyst, polymeric carbon nitride (PCN) currently has drawn ever-increasing attention for electrochemical energy conversion and storage due to its graphite-like structure, metal-free characteristic and excellent structural tunability. Nonetheless, its practical applications are still hindered by the poor electrical conductivity induced irreversible capacity loss. Recently, PCN-derived carbon materials with improved conductivity have received increasing interest and made tremendous progress for advanced electrochemical energy conversion and storage. This review highlights the latest research advancements regarding the electrochemical energy conversion (hydrogen evolution reaction, oxygen reduction/evolution reaction, nitrogen reduction reaction, carbon dioxide reduction reaction, etc.) and storage (Li-ion batteries, Li-S batteries, supercapacitors, etc.) application from PCN to PCN-derived carbon materials. A perspective about the challenges and trends in the electrochemical application of PCN and PCN-derived carbon materials is also provided at the end of the review.

16.
Adv Mater ; 32(16): e1908011, 2020 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-32115824

RESUMEN

Designing new hole-transporting materials (HTMs) with desired chemical, electrical, and electronic properties is critical to realize efficient and stable inverted perovskite solar cells (PVSCs) with a p-i-n structure. Herein, the synthesis of a novel 3D small molecule named TPE-S and its application as an HTM in PVSCs are shown. The all-inorganic inverted PVSCs made using TPE-S, processed without any dopant or post-treatment, are highly efficient and stable. Compared to control devices based on the commonly used HTM, PEDOT:PSS, devices based on TPE-S exhibit improved optoelectronic properties, more favorable interfacial energetics, and reduced recombination due to an improved trap passivation effect. As a result, the all-inorganic CsPbI2 Br PVSCs based on TPE-S demonstrate a remarkable efficiency of 15.4% along with excellent stability, which is the one of the highest reported values for inverted all-inorganic PVSCs. Meanwhile, the TPE-S layer can also be generally used to improve the performance of organic/inorganic hybrid inverted PVSCs, which show an outstanding power conversation efficiency of 21.0%, approaching the highest reported efficiency for inverted PVSCs. This work highlights the great potential of TPE-S as a simple and general dopant-free HTM for different types of high-performance PVSCs.

17.
Adv Mater ; 31(32): e1901602, 2019 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-31192498

RESUMEN

Instability of perovskite quantum dots (QDs) toward humidity remains one of the major obstacles for their long-term use in optoelectronic devices. Herein, a general amphiphilic star-like block copolymer nanoreactor strategy for in situ crafting a set of hairy perovskite QDs with precisely tunable size and exceptionally high water and colloidal stabilities is presented. The selective partition of precursors within the compartment occupied by inner hydrophilic blocks of star-like diblock copolymers imparts in situ formation of robust hairy perovskite QDs permanently ligated by outer hydrophobic blocks via coprecipitation in nonpolar solvent. These size- and composition-tunable perovskite QDs reveal impressive water and colloidal stabilities as the surface of QDs is intimately and permanently ligated by a layer of outer hydrophobic polymer hairs. More intriguingly, the readily alterable length of outer hydrophobic polymers renders the remarkable control over the stability enhancement of hairy perovskite QDs.

18.
Angew Chem Int Ed Engl ; 58(34): 11910-11917, 2019 08 19.
Artículo en Inglés | MEDLINE | ID: mdl-31197938

RESUMEN

Thermoresponsive nanoparticles (NPs) represent an important hybrid material comprising functional NPs with temperature-sensitive polymer ligands. Strikingly, significant discrepancies in optical and catalytic properties of thermoresponsive noble-metal NPs have been reported, and have yet to be unraveled. Reported herein is the crafting of Au NPs, intimately and permanently ligated by thermoresponsive poly(N-isopropylacrylamide) (PNIPAM), in situ using a starlike block copolymer nanoreactor as model system to resolve the paradox noted above. As temperature rises, plasmonic absorption of PNIPAM-capped Au NPs red-shifts with increased intensity in the absence of free linear PNIPAM, whereas a greater red-shift with decreased intensity occurs in the presence of deliberately introduced linear PNIPAM. Remarkably, the absence or addition of free linear PNIPAM also accounts for non-monotonic or switchable on/off catalytic performance, respectively, of PNIPAM-capped Au NPs.

19.
Chem Soc Rev ; 48(4): 1194-1228, 2019 Feb 18.
Artículo en Inglés | MEDLINE | ID: mdl-30663742

RESUMEN

The current trend in the miniaturization of electronic devices has driven the investigation into many nanostructured materials. The ferroelectric material barium titanate (BaTiO3) has garnered considerable attention over the past decade owing to its excellent dielectric and ferroelectric properties. This has led to significant progress in synthetic techniques that yield high quality BaTiO3 nanocrystals (NCs) with well-defined morphologies (e.g., nanoparticles, nanorods, nanocubes and nanowires) and controlled crystal phases (e.g., cubic, tetragonal and multi-phase). The ability to produce nanoscale BaTiO3 with controlled properties enables theoretical and experimental studies on the intriguing yet complex dielectric properties of individual BaTiO3 NCs as well as BaTiO3/polymer nanocomposites. Compared with polymer-free individual BaTiO3 NCs, BaTiO3/polymer nanocomposites possess several advantages. The polymeric component enables simple solution processibility, high breakdown strength and light weight for device scalability. The BaTiO3 component enables a high dielectric constant. In this review, we highlight recent advances in the synthesis of high-quality BaTiO3 NCs via a variety of chemical approaches including organometallic, solvothermal/hydrothermal, templating, molten salt, and sol-gel methods. We also summarize the dielectric and ferroelectric properties of individual BaTiO3 NCs and devices based on BaTiO3 NCs via theoretical modeling and experimental piezoresponse force microscopy (PFM) studies. In addition, viable synthetic strategies for novel BaTiO3/polymer nanocomposites and their structure-composition-performance relationship are discussed. Lastly, a perspective on the future direction of nanostructured BaTiO3-based materials is presented.

20.
Nanoscale ; 10(48): 22750-22757, 2018 Dec 13.
Artículo en Inglés | MEDLINE | ID: mdl-30346004

RESUMEN

We report a viable route to plasmonic nanoparticles with well-controlled sizes, shapes, and compositions. A series of monodisperse Ag and Au nanoparticles capped with polystyrene chains (i.e., "hairy" nanoparticles) are crafted by capitalizing on star-like diblock copolymers as nanoreactors. Such monodisperse nanoparticles render an accurate absorption spectrum, providing a strong basis for theoretical investigation into their optical properties. By combining the experimental study with the three-dimensional finite element calculation of electromagnetic field distributions, the contributions of both intra-band and inter-band transitions to plasmonic absorption are revealed. The calculated absorption spectra perfectly reproduce the experimental observations, including the peak positions, shapes, and trends of peak shifting or broadening as a function of nanoparticle sizes. The influences of nanoparticle dimensions and surface ligands on plasmonic absorption of metallic nanoparticles are also systematically explored.

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