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Author |
Ramachandran, R.K.; Filez, M.; Solano, E.; Poelman, H.; Minjauw, M.M.; Van Daele, M.; Feng, J.-Y.; La Porta, A.; Altantzis, T.; Fonda, E.; Coati, A.; Garreau, Y.; Bals, S.; Marin, G.B.; Detavernier, C.; Dendooven, J. |
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Title |
Chemical and Structural Configuration of Pt Doped Metal Oxide Thin Films Prepared by Atomic Layer Deposition |
Type |
A1 Journal article |
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Year  |
2019 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
31 |
Issue |
31 |
Pages |
9673-9683 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
Pt doped semiconducting metal oxides and Pt metal clusters embedded in an oxide matrix are of interest for applications such as catalysis and gas sensing, energy storage and memory devices. Accurate tuning of the dopant level is crucial for adjusting the properties of these materials. Here, a novel atomic layer deposition (ALD) based method for doping Pt into In2O3 in specific, and metals in metal oxides in general, is demonstrated. This approach combines alternating exposures of Pt and In2O3 ALD processes in a single ‘supercycle’, followed by supercycle repetition leading to multilayered nanocomposites. The atomic level control of ALD and its conformal nature make the method suitable for accurate dopant control even on high surface area supports. Oxidation state, local structural environment and crystalline phase of the embedded Pt dopants were obtained by means of X-ray characterization methods and high angle annular dark-field scanning transmission electron microscopy (HAADF-STEM). In addition, this approach allows characterization of the nucleation stages of metal ALD processes, by stacking those states multiple times in an oxide matrix. Regardless of experimental conditions, a few Pt ALD cycles leads to the formation of oxidized Pt species due to their highly dispersed nature, as proven by X-ray absorption spectroscopy (XAS). Grazing-incidence small-angle X-ray scattering (GISAXS) and highresolution scanning transmission electron microscopy, combined with energy dispersive X-ray spectroscopy (HR-STEM/EDXS) show that Pt is evenly distributed in the In2O3 metal oxide matrix without the formation of clusters. For a larger number of Pt ALD
cycles, typ. > 10, the oxidation state gradually evolves towards fully metallic, and metallic Pt clusters are obtained within the In2O3 metal oxide matrix. This work reveals how tuning of the ALD supercycle approach for Pt doping allows controlled engineering of the Pt compositional and structural configuration within a metal oxide matrix. |
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Wos |
000502418000010 |
Publication Date |
2019-11-11 |
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Edition |
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ISSN |
0897-4756 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
6 |
Open Access |
OpenAccess |
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Notes |
This research was supported by the Flemish Research Foundation (FWO-Vlaanderen), the Flemish Government (Long term structural funding – Methusalem funding and Medium scale research infrastructure funding-Hercules funding), the Special Research Fund BOF of Ghent University (GOA 01G01513) and the CALIPSO Trans National Access Program funded by the European Commission in supplying financing of travel costs. We are grateful to the SIXS and SAMBA-SOLEIL staff for smoothly running the beamline facilities. J.D. and R.K.R. are postdoctoral fellows of the FWO. |
Approved |
Most recent IF: 9.466 |
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Call Number |
EMAT @ emat @c:irua:164056 |
Serial |
5380 |
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Author |
Dendooven, J.; Ramachandran, R.K.; Solano, E.; Kurttepeli, M.; Geerts, L.; Heremans, G.; Ronge, J.; Minjauw, M.M.; Dobbelaere, T.; Devloo-Casier, K.; Martens, J.A.; Vantomme, A.; Bals, S.; Portale, G.; Coati, A.; Detavernier, C. |
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Title |
Independent tuning of size and coverage of supported Pt nanoparticles using atomic layer deposition |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
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Volume |
8 |
Issue |
8 |
Pages |
1074 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Synthetic methods that allow for the controlled design of well-defined Pt nanoparticles are highly desirable for fundamental catalysis research. In this work, we propose a strategy that allows precise and independent control of the Pt particle size and coverage. Our approach exploits the versatility of the atomic layer deposition (ALD) technique by combining two ALD processes for Pt using different reactants. The particle areal density is controlled by tailoring the number of ALD cycles using trimethyl(methylcyclopentadienyl) platinum and oxygen, while subsequent growth using the same Pt precursor in combination with nitrogen plasma allows for tuning of the particle size at the atomic level. The excellent control over the particle morphology is clearly demonstrated by means of in situ and ex situ X-ray fluorescence and grazing incidence small angle X-ray scattering experiments, providing information about the Pt loading, average particle dimensions, and mean center-to-center particle distance. |
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Wos |
000413353500023 |
Publication Date |
2017-10-16 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2041-1723 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.124 |
Times cited |
88 |
Open Access |
OpenAccess |
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Notes |
; This research was funded by the Research Foundation-Flanders (FWO), the Special Research Fund BOF of Ghent University (GOA 01G01513) and the Flemish Government (Medium-scale research infrastructure funding-Hercules funding). J. D., T. D. and M. M. M. acknowledge the FWO for a research fellowship. S. B. acknowledges the European Research Council, ERC grant no. 335078-Colouratom. For the GISAXS and XRF measurements at SOLEIL, the authors received funding from the European Community's Trans National Access Program CALIPSO. We are also grateful to the SOLEIL and ESRF staff for smoothly running the facilities. The authors thank G. Verellen for his help with drawing the 3D sketches. ; ecas_Sara |
Approved |
Most recent IF: 12.124 |
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Call Number |
UA @ lucian @ c:irua:146668UA @ admin @ c:irua:146668 |
Serial |
4786 |
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