RESUMEN
Light-driven transcription and replication are always subordinate to a delicate chirality transfer. Enabling light work in construction of the helical self-assembly with reversible chiral transformation becomes attractive. Herein we demonstrate that a helical hydrogen-bonded self-assembly is reversibly photoswitched between photochromic open and closed forms upon irradiation with alternative UV and visible light, in which molecular chirality is amplified with the formation of helixes at supramolecular level. The characteristics in these superhelixes such as left-handed or right-handed twist and helical length, height, and pitch are revealed by SEM and AFM. The helical photoswitchable nanostructure provides an easily accessible route to an unprecedented photoreversible modulation in morphology, fluorescence, and helicity, with precise assembly/disassembly architectures similar to biological systems such as protein and DNA.
Asunto(s)
Etilenos/síntesis química , Luz , Procesos Fotoquímicos , Rayos Ultravioleta , ADN/química , Etilenos/química , Enlace de Hidrógeno , Sustancias Macromoleculares/síntesis química , Sustancias Macromoleculares/química , Estructura Molecular , Proteínas/química , EstereoisomerismoRESUMEN
A controllable and scalable strategy is developed to fabricate multiplexed plasmonic nanoparticle structures by mechanical scratching with AFM lithography, which exhibit multiplex plasmonic properties and surface-enhanced Raman scattering responses. It offers an intuitive way to explore the plasmonic effects on the performance of an organic light-emitting diode device integrating with multiplexed plasmonic nanostructures.
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We demonstrated three-dimensional PMMA-based photonic crystal (3D-PC) nanostructures attached to Au nanoparticles (AuNPs), which undergo self-organization into super lattice planes and enhance the fluorescence properties. This new structure exhibited interesting tunable spectral, peak broadening plasmonic behavior because of strong plasmonic interaction at high laser powers. The presented work provides an important tool to improve the efficiency of dye laser applications.
RESUMEN
Electron-photon coupling in metal nanostructures has raised a new trend for active plasmonic switch devices in both fundamental understanding and technological applications. However, low sensitivity switches with an on/off ratio less than 5 have restricted applications. In this work, an electrically modulated plasmonic switch based on a surface-enhanced Raman spectroscopy (SERS) system with a single fivefold stellate polyhedral gold nanoparticle (FSPAuNP) is reported. The reversible switch of the SERS signal shows high sensitivity with an on/off ratio larger than 30. Such a high on/off ratio arises primarily from the plasmonic resonance shift of the FSPAuNP with the incident laser due to the altered free electron density on the nanoparticle under an applied electrochemical potential. This highly sensitive electro-plasmonic switch may enable further development of plasmonic devices.
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The stability of electrocatalysts during the hydrogen evolution reaction (HER) is vital for efficient production of hydrogen energy. Herein, we demonstrate that silver nanowire aerogel-based support (AABS) could facilitate the construction of HER catalysts with extraordinary long-term stability. A full nanostructure catalyst of nickel phosphide based formed on AABS (Ni2P-Ni5P4@AABS) was prepared to achieve an overpotential of 687 mV (without iR compensation) for HER at the current density of 1 A cm-2 in 0.5 M H2SO4. Excitingly, the stable HER performance was kept for 42 days during the long-term stability (i-t) test at high current density (0.5-1 A cm-2). The excellent HER performance of the Ni2P-Ni5P4@AABS catalyst is attributed to rapid electron transport pathways, numerous more accessible active sites, and support induced enhanced catalytic activity. The support effect was highlighted by a proposed phenomenological two-channel model for electron transport, which provides fresh insights into the design strategy for energy storage and delivery.
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The recycling of spent lithium-ion batteries (LIBs) has received increasing attention for environment and resource reclamation. Converting LIBs wastes into high-efficiency catalysts is a win-win strategy for realizing resource reclamation and addressing sustainable energy challenges. Herein, we developed a simple method to upcycle spent-LIBs cathode powder into Co-doped NiFe carbonate hydroxide hydrate (Co/NFCH-FF) as a low-cost and efficient oxygen evolution reaction (OER) electrocatalyst. The optimized Co/NFCH-FF electrode appears very competitive OER performances with low overpotentials of 201 and 249 mV at 10 and 100 mA cm-2, respectively, a small Tafel slope of 48.4 mV dec-1, and a high long-term stability. Moreover, we reveal that the existence of Co atoms leads to the formation of a crystalline/amorphous (c/a) interface at the Co/NFCH nanosheet edge, inducing the nanosheets possess a unique edge effect to enhance electric fields and accumulate hydroxide ions (OH-) at the edge during the OER process. Benefiting from edge effect, Co/NFCH-FF shows outstanding intrinsic activity. Furthermore, Co atoms as dopants stabilize the electronic structure of Co/NFCH-FF, enabling Co/NFCH-FF to exhibit excellent catalytic stability. This work provides an effective strategy for converting the end-life LIBs to high-performance multicomponent OER electrocatalysts and proposes new insights into the mechanism of enhanced catalytic activity of Co/NFCH.
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Development of a composite electrolyte with high ionic conductivity, excellent electrochemical stability and preeminent mechanical strength is beneficial for suppressing Li-dendrite penetration and unstable interfacial reactions in solid-state Li-metal batteries. Herein, a novel composite electrolyte material comprising perovskite Li0.485La0.505TiO3 (LLTO), poly(ethylene oxide) (PEO), and a barium titanate (BTO)-polyimide (PI) composite matrix has been successfully fabricated. Benefiting from the well-defined ion channels, the resulting BTO-PI@LLTO-PEO-FEC-LiTFSI (BP@LPFL) exhibits excellent cycling stability, low interfacial resistance, enhanced mechanical strength, and high ionic conductivity. Particularly, BP@LPFL possesses an excellent ionic conductivity of 3.0 × 10-4 S cm-1 at room temperature and achieves a wide electrochemical window of 5.2 V (vs. Li+/Li). For Li-LiFePO4 batteries, such an ingenious structure yields a discharge capacity of 124 mA h g-1 at 0.1 C after 200 cycles at room temperature and delivers a discharge capacity of 165 mA h g-1 at 0.1 C after 110 cycles at 60 °C. Additionally, the symmetric Li cell remains stable after 700 h at a current density of 0.5 mA cm-2. Furthermore, ex situ X-ray photoelectron spectroscopy and ex situ scanning electron microscopy were used to verify the interface evolution. Besides, a flexible full battery is fabricated, which exhibits impressive performance. These properties presented here provide support for BP@LPFL as a feasible candidate electrolyte for solid-state lithium batteries.
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Recently, silver nanowire-based transparent conductive films (AgNW-based TCFs) with excellent comprehensive performance have aroused wide and great interest. However, it is always difficult to simultaneously improve the performances of TCFs in all aspects. In this work, by introducing silica nanoparticles (SiO2-NPs) with a smaller particle size, several properties of AgNW-based TCFs were optimized successfully. The transmittance and conductivity were improved simultaneously, and smaller particle size was proven to be more suitable to achieve TCFs with excellent optoelectrical properties. Typically, an AgNW/SiO2-based TCF with a sheet resistance of 250 Ω/sq and transmittance of 93.6% (including the poly (ethylene terephthalate) substrate, abbreviated as PET) could be obtained by using SiO2-NPs with a size of â¼21 nm, and this transmittance is even higher than that of the bare PET (91.8%) substrate. We demonstrated that the layer formed through self-assembly of SiO2-NPs can cut down the light scattering on the AgNW surface through total reflection, thus leading to a low haze of AgNW/SiO2-based TCFs. Very interestingly, the SiO2-NPs conducted away most of the heat generated during laser ablation, protecting the AgNWs from excessive melt and PET from empyrosis, and thus ensuring the TCFs with high transmittance and patterning accuracy. Besides, AgNW/SiO2-based TCFs have smaller surface roughness, better flexibility, and adhesive force. To the best of our knowledge, the comprehensive performance of the AgNW/SiO2-based TCFs reaches the highest level among recently reported novel TCFs.
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Plasmonic nanomaterials are excellent and promising building blocks for information encoding and decoding. However, the positioning of multiplexed nanomaterials into recognizable structures remains a major challenge in nanotechnology. Herein, we developed a novel method for fabricating diversified nanostructures through surface charge inversion from amino-modified substrates to carboxyl-modified ones, as well as the corresponding electrostatic-induced assembly of metal nanoparticles. Under optimal conditions, the selected gold nanospheres (NSs) and peanut-like gold nanorods were successively located into patterns of spaced lines on the same substrate. Due to their unique optical properties, these two types of designed nanoarrays exhibited distinct color contrast and spectrum difference under dark-field scattering microscopy. Furthermore, this general strategy can be extended to wide ranges of nanoparticles with different morphologies and compositions for other multifunctional and high-demanding encoding applications.
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The negative differential resistance (NDR) effect observed in conducting polymer/Au nanoparticle composite devices is not yet fully clarified due to the random and disordered incorporation of Au nanoparticles into conducting polymers. It remains a formidable challenge to achieve the sequential arrangement of various components in an optimal manner during the fabrication of Au nanoparticle/conducting polymer composite devices. Here, a novel strategy for fabricating Au nanoparticle/conducting polymer composite devices based on self-assembled Au@PPy core-shell nanoparticle arrays is demonstrated. The interval between the two Au nanoparticles can be precisely programmed by modulating the thickness of the shell and the size of the core. Programmable NDR is achieved by regulating the spacer between two Au nanoparticles. In addition, the Au/conducting polymer composite device exhibits a reproducible memory effect with read-write-erase characteristics. The sequentially controllable assembly of Au@PPy core-shell nanoparticle arrays between two microelectrodes will simplify nanodevice fabrication and will provide a profound impact on the development of new approaches for Au/conducting polymer composite devices.
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Random lasing is desired in plasmonics nanostructures through surface plasmon amplification. In this study, tunable random lasing behavior was observed in dye molecules attached with Au nanorods (NRs), Au nanoparticles (NPs) and Au@Ag nanorods (NRs) respectively. Our experimental investigations showed that all nanostructures i.e., Au@AgNRs, AuNRs & AuNPs have intensive tunable spectral effects. The random lasing has been observed at excitation wavelength 532 nm and varying pump powers. The best random lasing properties were noticed in Au@AgNRs structure, which exhibits broad absorption spectrum, sufficiently overlapping with that of dye Rhodamine B (RhB). Au@AgNRs significantly enhance the tunable spectral behavior through localized electromagnetic field and scattering. The random lasing in Au@AgNRs provides an efficient coherent feedback for random lasers.
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A conductive polymer nanowire embedded with a 1D Au nanoparticle chain with defined size, shape, and interparticle distance is fabricated which demonstrates enhanced photoresponse behavior. The precise and controllable positioning of 1D Au nanoparticle chain in the conductive polymer nanowire plays a critical role in modulating the photoresponse behavior by excitation light wavelength or power due to the coupled-plasmon effect of 1D Au nanoparticle chain.
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We report a new strategy to directly attach Au nanoparticles onto YAG:Ce(3+) phosphor via a chemical preparation method, which yields efficient and quality conversion of blue to yellow light in the presence of a low amount of phosphor. Photoluminescent intensity and quantum yield of YAG:Ce(3+) phosphor are significantly enhanced after Au nanoparticle modification, which can be attributed to the strongly enhanced local surface electromagnetic field of Au nanoparticles on the phosphor particle surface. The CIE color coordinates shifted from the blue light (0.23, 0.23) to the white light region (0.30, 0.33) with a CCT value of 6601 K and a good white light CRI value of 78, which indicates that Au nanoparticles greatly improve the conversion efficiency of low amounts of YAG:Ce(3+) in WLEDs.