1,532 research outputs found

    Iodide-mediated Cu catalyst restructuring during CO<sub>2</sub> electroreduction

    Get PDF
    Catalyst restructuring during electrochemical reactions is a critical but poorly understood process that determines the underlying structure–property relationships during catalysis. In the electrocatalytic reduction of CO2 (CO2RR), it is known that Cu, the most favorable catalyst for hydrocarbon generation, is highly susceptible to restructuring in the presence of halides. Iodide ions, in particular, greatly improved the catalyst performance of Cu foils, although a detailed understanding of the morphological evolution induced by iodide remains lacking. It is also unclear if a similar enhancement transfers to catalyst particles. Here, we first demonstrate that iodide pre-treatment improves the selectivity of hexagonally ordered Cu-island arrays towards ethylene and oxygenate products. Then, the morphological changes in these arrays caused by iodide treatment and during CO2RR are visualized using electrochemical transmission electron microscopy. Our observations reveal that the Cu islands evolve into tetrahedral CuI, which then become 3-dimensional chains of copper nanoparticles under CO2RR conditions. Furthermore, CuI and Cu2O particles re-precipitated when the samples are returned to open circuit potential, implying that iodide and Cu+ species are present within these chains. This work provides detailed insight into the role of iodide, and its impact on the prevailing morphologies that exist during CO2RR

    Growth Dynamics and Processes Governing the Stability of Electrodeposited Size-Controlled Cubic Cu Catalysts

    Get PDF
    The renewable energy-powered conversion of industrially generated CO2 into useful chemicals and fuels is considered a promising technology for the sustainable development of our modern society. The electrochemical reduction of CO2 (CO2RR) is one of the possible conversion processes that can be employed to close the artificial carbon cycle, mimicking nature’s photosynthesis. Nevertheless, to enable green catalytic processes, selectivity for the desired products must be achieved. In the case of CO2RR, the selectivity is strongly dependent on the electrocatalyst structure. Here, we explore the phase space of synthesis parameters required for the electrodeposition of Cu cubes with {100} facets on glassy carbon substrates and elucidate their influence on the size, shape, coverage, and uniformity of the cubes. We found that the concentration of Cl– ions in solution controls the cube size, shape, and coverage, whereas the ratio of the reduction versus oxidation time and number of cycles in the alternating potential electrodeposition protocol can be used to further tune the cube size. Cyclic voltammetry experiments were complemented with in situ electrochemical scanning electron microscopy to follow the growth dynamics and ex situ transmission electron microscopy and electron diffraction. Our results indicate that the cube growth starts from nuclei formed during the first cycle, followed by a layered deposition and partial dissolution of new material in subsequent cycles

    The Role of Solar Wind Hydrogen in Space Weathering: Insights from Laboratory-Irradiated Northwest Africa 12008

    Get PDF
    Micrometeoroid impacts, solar wind plasma interactions, and regolith gardening drive the complicated and nuanced mechanism of space weathering (or optical maturation); a process by which a materials optical properties are changed as a result of chemical and physical alterations at the surface of grains on airless bodies. Reddened slopes, attenuated absorption bands, and an overall reduction in albedo in the visible and near-IR wavelength ranges are primarily the result of native iron nanoparticle (npFe0) production within glassy rims that form from sputtering and vaporization. The sizes and abundance of these particles provide information about the relative surface exposure age of a particular grain. In addition, many studies have indicated that composition greatly affects the rate at which optical maturation occurs. Despite our understanding of how npFe0 affects optical signatures, the relative roles of micrometeoroid bombardment and solar wind interactions remains undetermined. To simulate the early effects of weathering by the solar wind and to determine thresholds for optical change with respect to a given mineral phase, we irradiated a fine-grained lunar basalt with 1 keV H+ to a fluence of 6.4 x 1016 H+ per sq.cm. Surface alterations within four phases have been evaluated using transmission electron microscopy (TEM). We found that for a given fluence of H+, the extent of damage acquired by each grain was dependent on its composition. No npFe(0) was produced in any of the phases evaluated in this study. These results are consistent with many previous studies conducted using ions of similar energy, but they also provide valuable information about the onset of space weathering and the role of the solar wind during the early stages of optical maturation

    Understanding the performance increase of catalysts supported on N-functionalized carbon in PEMFC catalyst layers

    Get PDF
    Applying nitrogen-modified carbon support in PEMFCs has been attracting arising interest due to the resulting performance enhancement. In the present study, we attempt to uncover the origin and gain a deeper understanding of the different N-modification processes, whose influences are responsible for the performance improvement. By utilizing chemically modified Ketjenblack supports comprising altered fraction of N-functionalities, we investigate the underlying mechanism of the drastically reduced voltage losses under fuel cell operation conditions. In all, we demonstrate the key role of support modification induced by ammonia in strengthened support/ionomer interactions and alter physico-chemical properties of the carbon support contributing towards enhanced MEA performance. With the use of X-ray photoelectron spectroscopy (XPS), we show unambiguous evidences that not all N modified surfaces yield the desired performance increase. Rather, the latter depends on a complex interplay between different electrochemical parameter and catalyst properties. We want to emphasize the ionomer/support interaction as one important factor for enhanced ionomer distribution and present a prove of a direct interaction between the ionomers´ sidechains and N-functional groups of the support

    Quality parameters and technological properties of pasta enriched with a fish by-product: A healthy novel food

    Get PDF
    The effect of incorporating a fish (D. labrax) by-product on pasta quality was evaluated to assess its technological viability in comparison with a common pasta. Two enriched pastas, both dried and fresh and including or not a natural antioxidant (R. officinalis) were analyzed and compared to traditional pasta (durum and spelt). Findings indicated that enriched pasta showed a decrease in their texture properties, except for adhesiveness which was higher compared to traditional pasta. The addition of fish caused slight changes in color. Regarding the technological quality, it was moderately affected by fish inclusion, presenting lower gains in weight respect to control pasta (>15% of difference). Therefore, enriched pasta appears to be a good alternative to offer food with an improved nutritional profile with a low impact on the quality of the product from a technological point of view since the introduction of fish does not extensively affect pasta quality. Novelty impact statement: The enrichment of pasta from fish by-product is a good alternative to improve its nutritional value. The cooking had a beneficial effect on the bioavailability of nutrients in enriched pasta with fish. Technological properties of enriched pasta with fish after cooking was similar to traditional pasta made with durum wheat. © 2021 The Authors. Journal of Food Processing and Preservation published by Wiley Periodicals LLC

    Vacuum Polarization and Dynamical Chiral Symmetry Breaking: Phase Diagram of QED with Four-Fermion Contact Interaction

    Full text link
    We study chiral symmetry breaking for fundamental charged fermions coupled electromagnetically to photons with the inclusion of four-fermion contact self-interaction term. We employ multiplicatively renormalizable models for the photon dressing function and the electron-photon vertex which minimally ensures mass anomalous dimension = 1. Vacuum polarization screens the interaction strength. Consequently, the pattern of dynamical mass generation for fermions is characterized by a critical number of massless fermion flavors above which chiral symmetry is restored. This effect is in diametrical opposition to the existence of criticality for the minimum interaction strength necessary to break chiral symmetry dynamically. The presence of virtual fermions dictates the nature of phase transition. Miransky scaling laws for the electromagnetic interaction strength and the four-fermion coupling, observed for quenched QED, are replaced by a mean-field power law behavior corresponding to a second order phase transition. These results are derived analytically by employing the bifurcation analysis, and are later confirmed numerically by solving the original non-linearized gap equation. A three dimensional critical surface is drawn to clearly depict the interplay of the relative strengths of interactions and number of flavors to separate the two phases. We also compute the beta-function and observe that it has ultraviolet fixed point. The power law part of the momentum dependence, describing the mass function, reproduces the quenched limit trivially. We also comment on the continuum limit and the triviality of QED.Comment: 9 pages, 10 figure

    Antibody-Antigen Binding Interface Analysis in the Big Data Era

    Get PDF
    Antibodies have become the Swiss Army tool for molecular biology and nanotechnology. Their outstanding ability to specifically recognise molecular antigens allows their use in many different applications from medicine to the industry. Moreover, the improvement of conventional structural biology techniques (e.g., X-ray, NMR) as well as the emergence of new ones (e.g., Cryo-EM), have permitted in the last years a notable increase of resolved antibody-antigen structures. This offers a unique opportunity to perform an exhaustive structural analysis of antibody-antigen interfaces by employing the large amount of data available nowadays. To leverage this factor, different geometric as well as chemical descriptors were evaluated to perform a comprehensive characterization.Fil: Reis, Pedro B. P. S.. Istituto Italiano Di Technologie; Italia. Universidade Nova de Lisboa; PortugalFil: Barletta Roldan, Patricio German. The Abdus Salam; Italia. The Abdus Salam. International Centre for Theoretical Physics; Italia. Universidad Nacional de Quilmes; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Gagliardi, Lucas. Istituto Italiano Di Technologie; ItaliaFil: Fortuna, Sara. Istituto Italiano Di Technologie; ItaliaFil: Soler, Miguel A.. Istituto Italiano Di Technologie; ItaliaFil: Rocchia, Walter. Istituto Italiano Di Technologie; Itali
    • …
    corecore