The conversion of CO into liquid fuels, using only sunlight and water, offers a promising path to carbon neutrality. An outstanding challenge is to achieve high efficiency and product selectivity. Here, we introduce a wireless photocatalytic architecture for conversion of CO and water into methanol and oxygen.
View Article and Find Full Text PDFPlasmonic nanomaterials such as Au, Ag, and Cu are widely recognized for their strong light-matter interactions, making them promising photothermal materials for solar steam generation. However, their practical use in water evaporation is significantly limited by the trade-off between high costs and poor stability. In this regard, we introduce a novel, nonmetallic dual plasmonic TiN/MoO composite.
View Article and Find Full Text PDFPlasmonic polymeric nanoassemblies offer valuable opportunities in photoconversion applications. Localized surface plasmon mechanisms behind such nanoassemblies govern their functionalities under light illumination. However, an in-depth investigation at the single nanoparticle (NP) level is still challenging, especially when the buried interface is involved, due to the availability of suitable techniques.
View Article and Find Full Text PDFIn this work, we investigate the effects of bends on the surface plasmon resonances in nanowires (NWs) and isolated edges of planar structures using electron energy loss spectroscopy experiments and theoretical calculations. Previous work showed that the sharp bends in NWs do not affect their resonant modes. Here, we study previously overlooked effects and analyze systematically the evolution of resonant modes for several bending angles from 30° to 180°, showing that bending can have a significant effect on the plasmonic response of a nanostructure.
View Article and Find Full Text PDFThe energy resolution in hyperspectral imaging techniques has always been an important matter in data interpretation. In many cases, spectral information is distorted by elements such as instruments' broad optical transfer function, and electronic high frequency noises. In the past decades, advances in artificial intelligence methods have provided robust tools to better study sophisticated system artifacts in spectral data and take steps towards removing these artifacts from the experimentally obtained data.
View Article and Find Full Text PDFElectron ptychography has been implemented in Scanning Transmission Electron Microscopy (STEM) to study materials with higher spatial resolution. High electron dose imposed by data redundancy requirement in electron ptychography is detrimental to the samples well-suited for ptychography, i.e.
View Article and Find Full Text PDFLayered Ni-rich lithium transition metal oxides are promising cathode materials for high-energy-density lithium-ion batteries. These cathodes, however, suffer from rapid performance decay under high-voltage operation. In this work, the electrochemical properties and structural evolution of the LiNi Mn Co O (NMC811) cathode upon high-voltage cycling are investigated.
View Article and Find Full Text PDFNowadays, sub-50 meV atom-wide electron probes are routinely produced for electron energy loss spectroscopy in transmission electron microscopes due to monochromator technology advances. We review how gradual improvements in energy resolution enabled the study of very low-energy excitations such as lattice phonons, molecular vibrations, infrared plasmons and strongly coupled hybrid modes in nanomaterials. Starting with the theoretical framework needed to treat inelastic electron scattering from phonons in solids, we illustrate contributions in detecting optical surface phonons in photonic structures.
View Article and Find Full Text PDFA detailed study aimed at understanding and confirming the reported highly promising performance of a LaSrFeCrO (LSFCr) perovskite catalyst in CO/CO mixtures, for use in reversible solid oxide fuel cells (RSOFCs), is reported in this work, with an emphasis on chemical and performance stability. This work includes an X-ray diffraction (XRD), thermogravimetric analysis (TGA), and electrochemical study in a range of pO atmospheres (pure CO, CO alone (balance N), and a 90-70% CO/10-30% CO containing mixture), related to the different conditions that could be encountered during CO reduction at the cathode. Powdered LSFCr remains structurally stable in 20-100% CO (balance N, pO = 10-10 atm) without any decomposition.
View Article and Find Full Text PDFThe mineral franckeite is a naturally occurring van der Waals superlattice which has recently attracted attention for future applications in optoelectronics, biosensors and beyond. Furthermore, its stacking of incommensurately modulated 2D layers, the pseudo tetragonal Q-layer and the pseudo hexagonal H-layer, is an experimentally accessible prototype for the development of synthetic van der Waals materials and of advanced characterization methods to reveal new insights in their structure and chemistry at the atomic scale that is crucial for deep understanding of its properties. While some experimental studies have been undertaken in the past, much is still unknown on the correlation between local atomic structure and chemical composition within the layers.
View Article and Find Full Text PDFIron oxide nanoparticles (IONPs) are well-known contrast agents for MRI for a wide range of sizes and shapes. Their use as theranostic agents requires a better understanding of their magnetic hyperthermia properties and also the design of a biocompatible coating ensuring their stealth and a good biodistribution to allow targeting of specific diseases. Here, biocompatible IONPs of two different shapes (spherical and octopod) were designed and tested and to evaluate their abilities as high-end theranostic agents.
View Article and Find Full Text PDFNanodiamonds are interesting materials from the point of view of their biocompatibility and their chemical, spectroscopic, and mechanical properties. Current synthetic methods for nanodiamonds involve harsh environments, which are potentially hazardous in addition to being expensive. We report a low-temperature (423 K) hydrothermal approach to form nanodiamonds by using graphene-oxide or nitrated polycyclic aromatic hydrocarbons (naphthalene, anthracene, phenanthrene, or pyrene) as a starting material.
View Article and Find Full Text PDFPlasmonic nanoparticles are ideal candidates for hot-electron-assisted applications, but their narrow resonance region and limited hotspot number hindered the energy utilization of broadband solar energy. Inspired by tree branches, we designed and chemically synthesized silver fractals, which enable self-constructed hotspots and multiple plasmonic resonances, extending the broadband generation of hot electrons for better matching with the solar radiation spectrum. We directly revealed the plasmonic origin, the spatial distribution, and the decay dynamics of hot electrons on the single-particle level by using simulation, dark-field spectroscopy, pump-probe measurements, and electron energy loss spectroscopy.
View Article and Find Full Text PDFThe mechanism of palladium nanoparticles (Pd NPs)-catalyzed cross-coupling reactions has been the subject of intense debate since the recognition of catalytic active sites involving a wide array of dynamic changed Pd species. Here, through the combination of the hot filtration experiment together with the recently developed identical location transmission electron microscopy (IL-TEM) method, the delicate structure evolution of highly dispersed Pd NPs supported on oxygen-functionalized carbon nanotubes (Pd/oCNTs) as well as the kinetics properties of derived dissolved species in liquid phase were systemically investigated in the Suzuki-Miyaura reaction. The result indicates that the leached Pd components caused by the strong adsorption of reactants might have a significant contribution to the coupling products, and the degree for different substrates follows the order of iodobenzene > phenylboronic acid > bromobenzene.
View Article and Find Full Text PDFTo pave the way for InGaN-on-Si integrated photovoltaics, uniform and close-packed n-GaN/(Al)InGaN/p-GaN nanowire (NW) arrays with a ∼0.29 μm thick absorption segment of ∼2.35 eV energy bandgap were fabricated on a Si substrate using Ti-mask selective area growth (SAG) in a molecular beam epitaxy (MBE) chamber.
View Article and Find Full Text PDFThe surface plasmon response of a cross-sectional segment of a wrinkled gold film is studied using electron energy loss spectroscopy (EELS). EELS data demonstrate that wrinkled gold structures act as a suitable substrate for surface plasmons to propagate. The intense surface variations in these structures facilitate the resonance of a wide range of surface plasmons, leading to the broadband surface plasmon response of these geometries from the near-infrared to visible wavelengths.
View Article and Find Full Text PDFWith their ns2 np3 valence electronic configuration, pnictogens are the only system to crystallize in layered van der Waals (vdW) and quasi-vdW structures throughout the group. Light pnictogens crystallize in the A17 phase, and bulk heavier elements prefer the A7 phase. Herein, we demonstrate that the A17 of heavy pnictogens can be stabilized in antimonene grown on weakly interacting surfaces and that it undergoes a spontaneous thickness-driven transformation to the stable A7 phase.
View Article and Find Full Text PDFConfiguring metal single-atom catalysts (SACs) with high electrocatalytic activity and stability is one efficient strategy in achieving the cost-competitive catalyst for fuel cells' applications. Herein, the atomic layer deposition (ALD) strategy for synthesis of Pt SACs on the metal-organic framework (MOF)-derived N-doped carbon (NC) is proposed. Through adjusting the ALD exposure time of the Pt precursor, the size-controlled Pt catalysts, from Pt single atoms to subclusters and nanoparticles, are prepared on MOF-NC support.
View Article and Find Full Text PDFLi- and Mn-rich layered oxides are among the most promising cathode materials for Li-ion batteries with high theoretical energy density. Its practical application is, however, hampered by the capacity and voltage fade after long cycling. Herein, a finite difference method for near-edge structure (FDMNES) code was combined with in situ X-ray absorption spectroscopy (XAS) and transmission electron microscopy/electron energy loss spectroscopy (TEM/EELS) to investigate the evolution of transition metals (TMs) in fresh and heavily cycled electrodes.
View Article and Find Full Text PDFSimultaneously improving energy efficiency (EE) and material stability in electrochemical CO conversion remains an unsolved challenge. Among a series of ternary Sn-Ti-O electrocatalysts, 3D ordered mesoporous (3DOM) Sn Ti O achieves a trade-off between active-site exposure and structural stability, demonstrating up to 71.5 % half-cell EE over 200 hours, and a 94.
View Article and Find Full Text PDFEnhanced electromagnetic fields in nanometer gaps of plasmonic structures increase the optical interaction with matter, including Raman scattering and optical absorption. Quantum electron tunneling across sub-1 nm gaps, however, lowers these effects again. Understanding these phenomena requires controlled variation of gap sizes.
View Article and Find Full Text PDFHerein, we study the effect of adding bismuth to Ni-nanostructured catalysts (NiBi, = 100-90 at. %) for glycerol electro-oxidation in alkaline solution by combining physiochemical, electrochemical, and infrared spectroscopy techniques, as well as continuous electrolysis with HPLC (high-performance liquid chromatography) product analysis. The addition of small quantities of Bi (<20 at.
View Article and Find Full Text PDFDirect electron detectors (DeDs) have been widely used for imaging studies because of their higher beam sensitivity, lower noise, improved pixel resolution, etc. However, there have been limited studies related to the performance in spectroscopic applications for the direct electron detection. Hereby, taking the advantage of the DeD installed on a high-performance electron energy-loss spectrometer, we systematically studied the performance of a DeD (Gatan's K2 IS) fitted on an aberration-corrected transmission electron microscope (TEM) equipped with an electron monochromator.
View Article and Find Full Text PDFAn amendment to this paper has been published and can be accessed via a link at the top of the paper.
View Article and Find Full Text PDFAlloying in group V 2D materials and heterostructures is an effective degree of freedom to tailor and enhance their physical properties. Up to date, black arsenic-phosphorus is the only 2D group V alloy that has been experimentally achieved by exfoliation, leaving all other possible alloys in the realm of theoretical predictions. Herein, the existence of an additional alloy consisting of 2D antimony arsenide (2D-As Sb ) grown by molecular beam epitaxy on group IV semiconductor substrates and graphene is demonstrated.
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