scholarly journals Tracking dynamic structural changes in catalysis by rapid 2D-XANES microscopy

2021 ◽  
Vol 28 (5) ◽  
Author(s):  
Saba Alizadehfanaloo ◽  
Jan Garrevoet ◽  
Martin Seyrich ◽  
Vadim Murzin ◽  
Johannes Becher ◽  
...  
Keyword(s):  
Partial Oxidation ◽  
Structural Changes ◽  
Functional Materials ◽  
Methane Combustion ◽  
Spectroscopic Characterization ◽  
Frame Rate ◽  
High Time Resolution ◽  
Imaging Method ◽  
Full Field ◽  
Oxidation Of Methane

Many processes and materials in heterogeneous catalysis undergo dynamic structural changes depending on their chemical environment. Monitoring such dynamic changes can be challenging using conventional spectroscopic characterization tools, due to the high time resolution required. Here, a high-resolution 2D X-ray camera operating at 50 Hz full-frame rate was synchronized with a QEXAFS monochromator, enabling rapid spectro-microscopic imaging with chemical contrast over individual pixels. This was used to monitor chemical gradients within a model Pt/Al2O3 catalyst during catalytic partial oxidation of methane to synthesis gas. The transition from methane combustion (partly oxidized Pt) to combustion-reforming and partial oxidation (fully reduced Pt) was observed by a characteristic reduction front, which progressed from the end of the catalyst bed towards its beginning on the second time scale. The full-field QEXAFS imaging method applied here allows acquisition of entire XANES spectra `on the fly' in a rapid and spatially resolved manner. The combination of high spatial and temporal resolution with spectroscopic data offers new opportunities for observing dynamic processes in catalysts and other functional materials at work. The methodology is flexible and can be applied at beamlines equipped with a QEXAFS or other fast-scanning monochromators and a suitable sample environment for gas phase analytics to allow for catalytic studies at the same time.

scholarly journals New SiO2/Caffeic Acid Hybrid Materials: Synthesis, Spectroscopic Characterization, and Bioactivity

Materials ◽  
2020 ◽  
Vol 13 (2) ◽  
pp. 394 ◽  
Author(s):  
Michelina Catauro ◽  
Federico Barrino ◽  
Giovanni Dal Poggetto ◽  
Giuseppina Crescente ◽  
Simona Piccolella ◽  
...  
Keyword(s):  
Caffeic Acid ◽  
Hybrid Materials ◽  
Structural Changes ◽  
Sol Gel ◽  
Functional Materials ◽  
Spectroscopic Characterization ◽  
Silica Matrix ◽  
Materials Synthesis ◽  
Vis Spectroscopy ◽  
Ft Ir

The sol–gel route represents a valuable technique to obtain functional materials, in which organic and inorganic members are closely connected. Herein, four hybrid materials, containing caffeic acid entrapped in a silica matrix at 5, 10, 15, and 20 wt.%, were synthesized and characterized through Fourier-Transform Infrared (FT-IR) and Ultraviolet-Visible (UV–Vis) spectroscopy. FT-IR analysis was also performed to evaluate the ability to induce the hydroxyapatite nucleation. Despite some structural changes occurring on the phenol molecular skeleton, hybrid materials showed scavenging properties vs. 2,2-diphenyl-1-picrylhydrazyl (DPPH) radical and 2,2′-azinobis-(3-ethylbenzothiazolin-6-sulfonic acid) radical cation (ABTS•+), which was dependent on the tested dose and on the caffeic acid wt.%. The SiO2/caffeic acid materials are proposed as valuable antibacterial agents against Escherichia coli and Enterococcus faecalis.

scholarly journals New SiO2/Caffeic Acid Hybrid Materials: Synthesis, Spectroscopic Characterization and Bioactivity

2019 ◽  
Author(s):  
Michelina Catauro ◽  
Federico Barrino ◽  
Giovanni Dal Poggetto ◽  
Giuseppina Crescente ◽  
Simona Piccolella ◽  
...  
Keyword(s):  
Caffeic Acid ◽  
Hybrid Materials ◽  
Structural Changes ◽  
Sol Gel ◽  
Functional Materials ◽  
Spectroscopic Characterization ◽  
Silica Matrix ◽  
Materials Synthesis ◽  
Vis Spectroscopy ◽  
Ft Ir

Sol-gel route represents a valuable technique to obtain functional materials, in which organic and inorganic members are closely connected. Herein four hybrid materials, containing caffeic acid entrapped in a silica matrix at 5, 10, 15 and 20 wt%, were synthesized and characterized through FT-IR and UV-Vis spectroscopy. FT-IR analysis was also performed to evaluate the ability to induce the hydroxyapatite nucleation. Despite some structural changes occurred on the phenol molecular skeleton, hybrid materials showed scavenging properties vs DPPH and ABTS+ radicals, which was dependent on the tested dose and on the caffeic acid wt%. Finally, the SiO2/caffeic acid materials have been proposed as valuable antibacterial agents against Escherichia coli and Enterococcus faecalis.

Partial oxidation of methane over bimetallic nickel–lanthanide oxides

2010 ◽  
Vol 489 (1) ◽  
pp. 316-323 ◽  
Author(s):  
Ana C. Ferreira ◽  
A.M. Ferraria ◽  
A.M. Botelho do Rego ◽  
António P. Gonçalves ◽  
M. Rosário Correia ◽  
...  
Keyword(s):  
Partial Oxidation ◽  
Partial Oxidation Of Methane ◽  
Lanthanide Oxides ◽  
Oxidation Of Methane

scholarly journals Oscillatory Behaviour of Ni Supported on ZrO2 in the Catalytic Partial Oxidation of Methane as Determined by Activation Procedure

Materials ◽  
2021 ◽  
Vol 14 (10) ◽  
pp. 2495
Author(s):  
Daniela Pietrogiacomi ◽  
Maria Cristina Campa ◽  
Ida Pettiti ◽  
Simonetta Tuti ◽  
Giulia Luccisano ◽  
...  
Keyword(s):  
Catalytic Activity ◽  
Partial Oxidation ◽  
Active Sites ◽  
Direct Reduction ◽  
Partial Oxidation Of Methane ◽  
Catalytic Partial Oxidation ◽  
Oxidation Of Methane ◽  
Short Contact Time ◽  
Oxidation Reduction ◽  
Ni Species

Ni/ZrO2 catalysts, active and selective for the catalytic partial oxidation of methane to syngas (CH4-CPO), were prepared by the dry impregnation of zirconium oxyhydroxide (Zhy) or monoclinic ZrO2 (Zm), calcination at 1173 K and activation by different procedures: oxidation-reduction (ox-red) or direct reduction (red). The characterization included XRD, FESEM, in situ FTIR and Raman spectroscopies, TPR, and specific surface area measurements. Catalytic activity experiments were carried out in a flow apparatus with a mixture of CH4:O2 = 2:1 in a short contact time. Compared to Zm, Zhy favoured the formation of smaller NiO particles, implying a higher number of Ni sites strongly interacting with the support. In all the activated Ni/ZrO2 catalysts, the Ni–ZrO2 interaction was strong enough to limit Ni aggregation during the catalytic runs. The catalytic activity depended on the activation procedures; the ox-red treatment yielded very active and stable catalysts, whereas the red treatment yielded catalysts with oscillating activity, ascribed to the formation of Niδ+ carbide-like species. The results suggested that Ni dispersion was not the main factor affecting the activity, and that active sites for CH4-CPO could be Ni species at the boundary of the metal particles in a specific configuration and nuclearity.

scholarly journals Sample Environment for Operando Hard X-ray Tomography—An Enabling Technology for Multimodal Characterization in Heterogeneous Catalysis

Catalysts ◽  
2021 ◽  
Vol 11 (4) ◽  
pp. 459
Author(s):  
Johannes Becher ◽  
Sebastian Weber ◽  
Dario Ferreira Sanchez ◽  
Dmitry E. Doronkin ◽  
Jan Garrevoet ◽  
...  
Keyword(s):  
Heterogeneous Catalysis ◽  
Synchrotron Radiation ◽  
Contrast Imaging ◽  
Co2 Methanation ◽  
Full Field ◽  
X Ray ◽  
Spatially Resolved ◽  
Oxidation Of Methane ◽  
Unique Source ◽  
Sample Environment

Structure–activity relations in heterogeneous catalysis can be revealed through in situ and operando measurements of catalysts in their active state. While hard X-ray tomography is an ideal method for non-invasive, multimodal 3D structural characterization on the micron to nm scale, performing tomography under controlled gas and temperature conditions is challenging. Here, we present a flexible sample environment for operando hard X-ray tomography at synchrotron radiation sources. The setup features are discussed, with demonstrations of operando powder X-ray diffraction tomography (XRD-CT) and energy-dispersive tomographic X-ray absorption spectroscopy (ED-XAS-CT). Catalysts for CO2 methanation and partial oxidation of methane are shown as case studies. The setup can be adapted for different hard X-ray microscopy, spectroscopy, or scattering synchrotron radiation beamlines, is compatible with absorption, diffraction, fluorescence, and phase-contrast imaging, and can operate with scanning focused beam or full-field acquisition mode. We present an accessible methodology for operando hard X-ray tomography studies, which offer a unique source of 3D spatially resolved characterization data unavailable to contemporary methods.

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