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Author |
Theofanidis, S.A.; Galvita, V.V.; Poelman, H.; Dharanipragada, N.V.R.A.; Longo, A.; Meledina, M.; Van Tendeloo, G.; Detavernier, C.; Marin, G.B. |
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Title |
Fe-containing magnesium aluminate support for stability and carbon control during methane reforming |
Type |
A1 Journal article |
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Year |
2018 |
Publication  |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
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Volume |
8 |
Issue |
7 |
Pages |
5983-5995 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
We report a MgFexAl2-xO4 synthetic spinel, where x varies from 0 to 0.26, as support for Ni-based catalysts, offering stability and carbon control under various conditions of methane reforming. By incorporation of Fe into a magnesium aluminate spine!, a support is created with redox functionality and high thermal stability, as concluded from temporal analysis of products (TAP) experiments and redox cycling, respectively. A diffusion coefficient of 3 x 10(-17) m(2) s(-1) was estimated for lattice oxygen at 993 K from TAP experiments. X-ray diffraction (XRD) and extended X-ray absorption fine structure (EXAFS) modeling identified that the incorporation of iron occurs as Fe3+ in the octahedral sites of the spinel lattice, replacing aluminum. Simulation of the X-ray absorption near edge structure (XANES) spectrum of the reduced support showed that 60 +/- 10% of iron was reduced from 3+ to 2+ at 1073 K, while there was no formation of metallic iron. A series of Ni/MgFexAl2-xO4 catalysts, where x varies from 0 to 0.26, was synthesized and reduced, yielding a supported Ni-Fe alloy. The evolution of the catalyst structure during H-2 temperature-programmed reduction (TPR) and CO2 temperature-programmed oxidation (TPO) was examined using time-resolved in situ XRD and XANES. During reforming, iron in both the support and alloy keeps control of carbon accumulation, as confirmed by O-2-TPO on the spent catalysts. By fine tuning the amount of Fe in MgFexAl2-xO4, a supported alloy was obtained with a Ni/Fe molar ratio of similar to 10, which was active for reforming and stable. By comparison of the performance of Ni-based catalysts with Fe either incorporated into or deposited onto the support, the location of Fe within the support proved crucial for the stability and carbon mitigation under reforming conditions. |
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Wos |
000438475100034 |
Publication Date |
2018-05-22 |
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ISSN |
2155-5435 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
10.614 |
Times cited |
18 |
Open Access |
OpenAccess |
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Notes |
; This work was supported by the FAST industrialization by Catalyst Research and Development (FASTCARD) project, which is a Large Scale Collaborative Project supported by the European Commission in the 7th Framework Programme (GA no 604277), the “Long Term Structural Methusalem Funding by the Flemish Government”, the Interuniversity Attraction Poles Programme, IAP7/5, Belgian State – Belgian Science Policy, and the Fund for Scientific Research Flanders (FWO-Vlaanderen) in supplying financing of travel costs and beam time at the DUBBLE beamline of the ESRF. The authors acknowledge the assistance from the DUBBLE (ESRF, XAS campaign 26-01-1048) and ROCK staff (SOLEIL, proposal 201502561). The authors equally acknowledge support from a public grant overseen by the French National Research Agency (ANR) as part of the “Investissements d'Avenir” program (reference: ANR-10-EQPX-45) for the ROCK beamline and from Lukas Buelens and Rakesh Batchu (Laboratory for Chemical Technology, Ghent University) for the STEM measurements and TAP experiments, respectively. ; |
Approved |
Most recent IF: 10.614 |
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Call Number |
UA @ lucian @ c:irua:153178 |
Serial |
5102 |
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Author |
Asapu, R.; Claes, N.; Ciocarlan, R.-G.; Minjauw, M.; Detavernier, C.; Cool, P.; Bals, S.; Verbruggen, S.W. |
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Title |
Electron Transfer and Near-Field Mechanisms in Plasmonic Gold-Nanoparticle-Modified TiO2Photocatalytic Systems |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
ACS applied nano materials |
Abbreviated Journal |
ACS Appl. Nano Mater. |
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Volume |
2 |
Issue |
2 |
Pages |
4067-4074 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
The major mechanism responsible for plasmonic enhancement of titanium dioxide photocatalysis using gold nanoparticles is still under contention. This work introduces an experimental strategy to disentangle the significance of the charge transfer and near-field mechanisms in plasmonic photocatalysis. By controlling the thickness and conductive nature of a nanoparticle shell that acts as a spacer layer separating the plasmonic metal core from the TiO2 surface, field enhancement or charge transfer effects can be selectively repressed or evoked. Layer-by-layer and in situ polymerization methods are used to synthesize gold core–polymer shell nanoparticles with shell thickness control up to the sub-nanometer level. Detailed optical and electrical characterization supported by near-field simulation models corroborate the trends in photocatalytic activity of the different systems. This approach mainly points at an important contribution of the enhanced near field. |
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000477917700006 |
Publication Date |
2019-05-31 |
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Edition |
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ISSN |
2574-0970 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
32 |
Open Access |
OpenAccess |
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Notes |
This work was supported by Research Foundation Flanders (FWO). P.C. and R-G.C. acknowledge financial support from FWO (Project No. G038215N). N.C. and S.B. acknowledge financial support from the European Research Council (ERC Starting Grant No. 335078-COLOURATOM). |
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Most recent IF: NA |
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Call Number |
EMAT @ emat @UA @ admin @ c:irua:160579 |
Serial |
5184 |
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Author |
Kurttepeli, M.; Deng, S.; Mattelaer, F.; Cott, D.J.; Vereecken, P.; Dendooven, J.; Detavernier, C.; Bals, S. |
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Title |
Heterogeneous TiO2/V2O5/Carbon Nanotube Electrodes for Lithium-Ion Batteries |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
Acs Appl Mater Inter |
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Volume |
9 |
Issue |
9 |
Pages |
8055-8064 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Vanadium pentoxide (V2O5) is proposed and investigated as a cathode material for lithium-ion (Li-ion) batteries. However, the dissolution of V2O5 during the charge/discharge remains as an issue at the V2O5–electrolyte interface. In this work, we present a heterogeneous nanostructure with carbon nanotubes supported V2O5/titanium dioxide (TiO2) multilayers as electrodes for thin-film Li-ion batteries. Atomic layer deposition of V2O5 on carbon nanotubes provides enhanced Li storage capacity and high rate performance. An additional TiO2 layer leads to increased morphological stability and in return higher electrochemical cycling performance of V2O5/carbon nanotubes. The physical and chemical properties of TiO2/V2O5/carbon nanotubes are characterized by cyclic voltammetry and charge/discharge measurements as well as electron microscopy. The detailed mechanism of the protective TiO2 layer to improve the electrochemical cycling stability of the V2O5 is unveiled. |
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Wos |
000396186000021 |
Publication Date |
2017-03-08 |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.504 |
Times cited |
28 |
Open Access |
OpenAccess |
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Notes |
European Research Council, 239865 335078 ; Fonds Wetenschappelijk Onderzoek; Agentschap voor Innovatie door Wetenschap en Technologie, 18142 ; Bijzonder Onderzoeksfonds, GOA – 01G01513 ; This research was funded by the Flemish research foundation FWO-Vlaanderen, by the European Research Council (Starting Grant No. 239865 and No. 335078), by IWT-Flanders (SBO project IWT 18142 “SoS-Lion”) and by the Special Research Fund BOF of Ghent University (GOA – 01G01513); colouratoms (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); ECAS_Sara |
Approved |
Most recent IF: 7.504 |
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Call Number |
EMAT @ emat @ c:irua:142446UA @ admin @ c:irua:142446 |
Serial |
4572 |
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Author |
Asapu, R.; Ciocarlan, R.-G.; Claes, N.; Blommaerts, N.; Minjauw, M.; Ahmad, T.; Dendooven, J.; Cool, P.; Bals, S.; Denys, S.; Detavernier, C.; Lenaerts, S.; Verbruggen, S.W. |
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Title |
Plasmonic Near-Field Localization of Silver Core–Shell Nanoparticle Assemblies via Wet Chemistry Nanogap Engineering |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
Acs Appl Mater Inter |
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Volume |
9 |
Issue |
9 |
Pages |
41577-41585 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Silver nanoparticles are widely used in the field of plasmonics because of their unique optical properties. The wavelength-dependent surface plasmon resonance gives rise to a strongly enhanced electromagnetic field, especially at so-called hot spots located in the nanogap in-between metal nanoparticle assemblies. Therefore, the interparticle distance is a decisive factor in plasmonic applications, such as surface-enhanced Raman spectroscopy (SERS). In this study, the aim is to engineer this interparticle distance for silver nanospheres using a convenient wet-chemical approach and to predict and quantify the corresponding enhancement factor using both theoretical and experimental tools. This was done by building a tunable ultrathin polymer shell around the nanoparticles using the layer-by-layer method, in which the polymer shell acts as the separating interparticle spacer layer. Comparison of different theoretical approaches and corroborating the results with SERS analytical experiments using silver and silver−polymer core−shell nanoparticle clusters as SERS substrates was also done. Herewith, an approach is provided to estimate the extent of plasmonic near-field enhancement both theoretically as well as experimentally. |
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Wos |
000417005900057 |
Publication Date |
2017-11-29 |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.504 |
Times cited |
29 |
Open Access |
OpenAccess |
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Notes |
financial support through a research fellowship. C.D. wishes to thank the Hercules foundation for the financial support (SPINAL). P.C. and R.-G.C. acknowledge financial support by FWO Vlaanderen (project no. G038215N). N.C. and S.B. acknowledge the financial support from the European Research Council (ERC starting grant #335078-COLOURATOM). (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); saraecas; ECAS_Sara; |
Approved |
Most recent IF: 7.504 |
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Call Number |
EMAT @ emat @c:irua:147243 |
Serial |
4804 |
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