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Vandekerckhove, T.; Courtens, E.N.P.; Prat, D.; Vilchez-Vargas, R.; Vital, M.; Pieper, D.H.; Meerbergen, K.; Lievens, B.; Boon, N.; Vlaeminck, S.E. |
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Title |
Transitioning from mesophilic to thermophilic nitrification: shaping a niche for archaeal ammonia oxidizers |
Type |
P3 Proceeding |
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Year |
2016 |
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9 p.
T2 - WEF/IWA Nutrient Removal and Recovery Co |
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P3 Proceeding; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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Call Number |
UA @ admin @ c:irua:151126 |
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8697 |
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Author |
Mishra, V.K.; Dons, E.; Panis, L.I.; Frijns, E.; van Poppel, M.; Berghmans, P.; Bleux, N.; Wuyts, K.; Samson, R. |
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Title |
Understanding ultrafine particles dynamics within a one km urban grid |
Type |
P3 Proceeding |
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Year |
2010 |
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P3 Proceeding; Sustainable Energy, Air and Water Technology (DuEL) |
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Call Number |
UA @ admin @ c:irua:88671 |
Serial |
8709 |
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Author |
de Gendt, S.; Kenis, K.; Mertens, P.W.; Heyns, M.M.; Claes, M.; Van Grieken, R.E.; Bailleul, A.; Knotter, M.; de Bokx, P.K. |
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Title |
Use of grazing emission XRF spectrometry for silicon wafer surface contamination measurements |
Type |
P3 Proceeding |
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Year |
1996 |
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Abbreviated Journal |
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P3 Proceeding; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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no |
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Call Number |
UA @ admin @ c:irua:14679 |
Serial |
8720 |
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Author |
Amiri-Aref, M. |
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Title |
Utilization of magnetic nanoparticles and carbon nanotubes to fabrication electrochemical sensors for determination of some important biological and pharmaceutical compounds |
Type |
Doctoral thesis |
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Year |
2015 |
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Pages |
137 p. |
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Keywords |
Doctoral thesis; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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no |
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Call Number |
UA @ admin @ c:irua:128299 |
Serial |
8727 |
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Author |
Vanmeert, F.; Van der Snickt, G.; Legrand, S.; Janssens, K. |
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Title |
Velázquez? A portrait of Pope Innocent X : an X-ray imaging investigation (II) |
Type |
H3 Book chapter |
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Year |
2019 |
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Abbreviated Journal |
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Pages |
132-141
T2 - Velázquez : Anregungen, Vorschläge, L |
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Keywords |
H3 Book chapter; Art; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Encompassing a broad spectrum of methodological approaches and aims, the scholars contributing to this volume offer renewed perspectives on the multifaceted oeuvre of Diego Velázquez. The seventeenth-century artist’s exceptional religious works as well as his numerous portraits are examined within the social and historical context of Velázquez’s milieu which included both the Spanish court as well as circles comprising important intellectual figures of his time. Following a close investigation of his works, which also includes the results of recent technological examinations on his paintings, the contributors to this volume offer new, exciting findings and discussions on the inspirations, sources and possible intentions of Velázquez. |
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978-3-99020-155-8 |
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Call Number |
UA @ admin @ c:irua:190783 |
Serial |
8736 |
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Author |
Lindeboom, R.E.F.; Clauwaert, P.; Alloul, A.; Coessens, W.; Christiaens, M.; Vanoppen, M.; Rabaey, K.; Verliefde, A.R.D.; Vlaeminck, S.E. |
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Title |
Water and nutrient recovery from combined urine and grey water treatment in Space |
Type |
P3 Proceeding |
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Year |
2015 |
Publication |
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Abbreviated Journal |
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Pages |
3 p.
T2 - IWA Resource Recovery Conference, 30 Aug |
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Keywords |
P3 Proceeding; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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Call Number |
UA @ admin @ c:irua:151143 |
Serial |
8747 |
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Author |
Han, M.; Seuntjens, D.; Al-Omari, A.; Takacs, I.; Meerburg, F.; Murthy, S.; Vlaeminck, S.E.; De Clippeleir, H. |
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Title |
Water and process parameters as controllers for the ammonia to nitrite oxidation rate ratio in activated sludge |
Type |
P3 Proceeding |
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Year |
2017 |
Publication |
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Abbreviated Journal |
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Volume |
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Pages |
3 p.
T2 - IWA 2017 Conference on Sustainable Waste |
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Keywords |
P3 Proceeding; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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no |
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Call Number |
UA @ admin @ c:irua:151110 |
Serial |
8748 |
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Author |
de Paepe, J.; Lindeboom, R.E.F.; Vanoppen, M.; Alonso Farinas, B.; Coessens, W.; Abbas, A.; Christiaens, M.; Dotremont, C.; Beckers, H.; Lamaze, B.; Demey, D.; Rabaey, K.; Clauwaert, P.; Verliefde, A.R.D.; Vlaeminck, S.E. |
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Title |
Water treatment unit breadboard : ground test facility for the recycling of urine and shower water for one astronaut |
Type |
P3 Proceeding |
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Year |
2017 |
Publication |
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Abbreviated Journal |
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Pages |
2 p.
T2 - 5th IWA Benelux Young Water Professional |
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Keywords |
P3 Proceeding; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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no |
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Call Number |
UA @ admin @ c:irua:151114 |
Serial |
8749 |
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Author |
Delalieux, F.; Sweevers, H.; Van Grieken, R. |
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Title |
Weathering mechanism of Pentelic marble under ambient atmospheric conditions derived from runoff studies |
Type |
P3 Proceeding |
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Year |
1997 |
Publication |
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Abbreviated Journal |
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Keywords |
P3 Proceeding; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Approved |
no |
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Call Number |
UA @ admin @ c:irua:18791 |
Serial |
8751 |
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Author |
Vleugels, G.; Van Grieken, R. |
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Title |
Weathering of bare and treated limestones under ambient conditions using runoff water analysis and microanalysis |
Type |
P3 Proceeding |
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Year |
1992 |
Publication |
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Abbreviated Journal |
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Keywords |
P3 Proceeding; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Approved |
no |
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Call Number |
UA @ admin @ c:irua:2865 |
Serial |
8752 |
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Author |
Roekens, E.; Van Raemdonck, C.; Leysen, L.; Chakravorty, R.; Van Grieken, R. |
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Title |
Weathering products and surface recession rates for sandy limestones exposed to air pollution |
Type |
H3 Book chapter |
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Year |
1987 |
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Abbreviated Journal |
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Volume |
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Pages |
707-714
T2 - Acid rain : scientific and technical |
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Keywords |
H3 Book chapter; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Approved |
no |
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| |
Call Number |
UA @ admin @ c:irua:117536 |
Serial |
8756 |
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Author |
Van Grieken, R. |
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Title |
Working close to the detection limits: XRF |
Type |
Minutes and reports |
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Year |
1998 |
Publication |
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Abbreviated Journal |
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Volume |
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Keywords |
Minutes and reports; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Approved |
no |
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| |
Call Number |
UA @ admin @ c:irua:20973 |
Serial |
8761 |
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Author |
Samek, L.; Worobiec, A.; Van Grieken, R.; van Meel, K.; Kontozova, V.; Karaszkiewicz, P.; Wiłkojć, E. |
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Title |
Wpływ zwiedzajacych na zanieczyszczenia wnetrz muzealnych |
Type |
H3 Book chapter |
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Year |
2007 |
Publication |
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Abbreviated Journal |
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Volume |
|
Issue |
|
Pages |
209-218
T2 - Konserwacja zapobiegawcza w muzeach |
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| |
Keywords |
H3 Book chapter; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Laboratory Experimental Medicine and Pediatrics (LEMP) |
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Approved |
no |
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| |
Call Number |
UA @ admin @ c:irua:67628 |
Serial |
8762 |
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| Permanent link to this record |
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Author |
Injuk, J.; Van Grieken, R.E. |
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Title |
X-ray fluorescence |
Type |
H3 Book chapter |
| |
Year |
2001 |
Publication |
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Abbreviated Journal |
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| |
Volume |
|
Issue |
|
Pages |
151-178
T2 - Non-destructive elemental analysis / |
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Keywords |
H3 Book chapter; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Approved |
no |
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| |
Call Number |
UA @ admin @ c:irua:34107 |
Serial |
8764 |
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Author |
Margu'i', E.; Queralt, I.; Van Grieken, R. |
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Title |
X-ray fluorescence analysis, sample preparation for |
Type |
H1 Book chapter |
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Year |
2009 |
Publication |
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Abbreviated Journal |
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Volume |
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Issue |
|
Pages |
1-20
T2 - Sncyclopedia of analytical chemistry / M |
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Keywords |
H1 Book chapter; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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|
ISBN |
978-0-471-97670-7 |
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Approved |
no |
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| |
Call Number |
UA @ admin @ c:irua:81641 |
Serial |
8765 |
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Author |
Vincze, L.; Vekemans, B.; Szaloki, I.; Brenker, F.E.; Falkenberg, G.; Rickers, K.; Aerts, K.; Van Grieken, R.; Adams, F. |
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| |
Title |
X-ray fluorescence microtomography and polycapillary based confocal imaging using synchrotron radiation |
Type |
P1 Proceeding |
| |
Year |
2004 |
Publication |
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Abbreviated Journal |
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Volume |
|
Issue |
|
Pages |
220-231
T2 - 4th Conference on Developments in X-R |
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P1 Proceeding; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
Ibis work illustrates the development of X-ray fluorescence tomography and polycapillary based confocal imaging towards a three-dimensional (313), quantitative analytical method with lateral resolution levels down to the 2-20 mum scale. Detailed analytical characterization is given for polycapillary based confocal XRF imaging, which is a new variant of the 3D micro-XRF technique. Applications for 2D/3D micro-XR-F are illustrated for the analysis of biological (zooplankton) and geological samples (microscopic inclusions in natural diamonds and fluid inclusions in quartz). Based on confocal imaging, fully three-dimensional distributions of trace elements could be obtained, representing a significant generalization of the regular 2D scanning technique for micro-XRF spectroscopy. The experimental work described in this paper has been carried out at the ESRF ID18F microfluorescence end-station and at HASYLAB Beam Line L. |
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000225665000023 |
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2004-11-02 |
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0-8194-5473-7 |
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UA @ admin @ c:irua:94812 |
Serial |
8767 |
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Author |
Marguí, E.; Van Grieken, R. |
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Title |
X-ray fluorescence spectrometry and related techniques : an introduction |
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MA3 Book as author |
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Year |
2013 |
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148 p. |
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MA3 Book as author; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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978-1-60650-391-1 |
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UA @ admin @ c:irua:106179 |
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8768 |
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Author |
Van Grieken, R.E. |
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Title |
X-ray spectrometry |
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2000 |
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15 |
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13269-13443
T2 - Encyclopedia of analytical chemis |
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H3 Book chapter; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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UA @ admin @ c:irua:31650 |
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8775 |
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Author |
Van Grieken, R.; Delalieux, F. |
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Title |
X-ray spectrometry for air pollution and cultural heritage research |
Type |
P3 Proceeding |
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2004 |
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P3 Proceeding; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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UA @ admin @ c:irua:51259 |
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8783 |
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Author |
Van Grieken, R.; Makarovska, Y.; van Meel, K.; Worobiec, A. |
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Title |
X-ray spectrometry for analysis of atmospheric particulate matter: detection limits versus legal levels |
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H3 Book chapter |
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2007 |
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153-161
T2 - Topics in X-ray spectrometry / Vázque |
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H3 Book chapter; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Laboratory Experimental Medicine and Pediatrics (LEMP) |
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no |
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UA @ admin @ c:irua:64402 |
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8784 |
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Author |
Tsuji, K.; Injuk, J.; Van Grieken, R. |
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Title |
X-ray spectrometry: recent technological advances |
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ME1 Book as editor or co-editor |
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2004 |
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616 p. |
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ME1 Book as editor or co-editor; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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0-471-48640-x |
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UA @ admin @ c:irua:43876 |
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8786 |
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Author |
Mendonça Verbinnen, C.D. |
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Title |
Development of semiconductor-based photoelectrochemical sensing strategies for phenolic compounds in natural and supply water |
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Doctoral thesis |
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2022 |
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152 p. |
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Doctoral thesis; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
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Abstract |
A wide variety of organic and inorganic compounds have been frequently released into the environment without control by industries and agricultural activities. This has caused significant impact on the development and health of living organisms, and biodiversity. Therefore, the challenge of monitoring and/or remediation of these contaminants remains. This thesis presents the development of three sensing strategies based on photoelectrochemical sensors to monitor phenolic contaminants. The well-known semiconductors TiO2 and ZnO were used for building novel setups for nM analysis of phenolic compounds in water. The setups employing TiO2-based photosensors were integrated into a photoelectrochemical flow cell. The flow system favored higher sensitivity of the method by periodic wash sequences of the electrode, significantly reducing the electrode fouling. Firstly, a straightforward method was developed based on the immobilization of TiO2 on screen printed graphite electrodes. Under UV light, the developed photosensor presented high performance for the detection of 4- aminophenol. A second study was developed by impregnating gold nanoparticles into TiO2 structure. The incorporation of gold nanoparticles can broaden the light absorption region of TiO2 and improve its photocatalytic activity for the detection of hydroquinone under visible light. In both systems, the detection was possible due to the presence of reactive oxygen species at the surface of TiO2 upon light, which participate in the oxidation process of the analyte. By applying a reductive potential, the oxidized form of the analyte gets reduced and a measurable amperometric response proportional to the initial analyte concentration is recorded. The third proposed setup is a ZnO-based photosensor for the quantification of 4-nitrophenol under UVA light. Nanostructured ZnO was electrochemically synthesized on FTO glass without the use of catalysts or seed layer. A post-growth annealing treatment significantly improved ZnO nanorods physicochemical properties. Subsequent modification of ZnO nanorods with a photosensitizer (perylene acid) increased the photocurrent response and the sensitivity. In this system, the detection mechanism is based on the decrease of the photocurrent response at the presence of an electron harvesting molecule, such as 4-nitrophenol. The decrease in photocurrent is proportional to the increase of 4-nitrophenol concentration in the solution. The applicability of the photoelectrochemical semiconductor-based sensing setups was verified to analyze phenolic compounds in natural and supply water samples. The proposed robust and sensitive approaches were designed for the on-site monitoring of phenolic compounds. The encouraging results confirm the potential of these photosensors as promising tools for tracelevel sensing purposes. |
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UA @ admin @ c:irua:186763 |
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8850 |
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Author |
Thiruvottriyur Shanmugam, S. |
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Title |
Singlet oxygen-based photoelectrochemical detection of nucleic acids |
Type |
Doctoral thesis |
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Year |
2022 |
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Abbreviated Journal |
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Volume |
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217 p. |
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Keywords |
Doctoral thesis; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
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Abstract |
MicroRNAs (miRNAs) are small oligonucleotides (18-25 bases) that play a key role in epigenetic regulation. Since the discovery of miRNAs in 1993, their role in biological processes has been extensively investigated. By now, it has been evidenced that monitoring and detection of miRNAs can improve (early) disease diagnosis. The existing diagnostic approaches have limitations such as the need for complex multistep protocols for sample preparation, analysis, data interpretation, high cost of equipment, the need for highly qualified personnel, and high laboratory standards. As opposed to this, point-of-care biosensors and chips aim to facilitate the procedure and avoid sending samples into centralized laboratories, which saves time, reduces the chance of sample degradation, and enables analysis of patient samples in remote areas, directly at home or primary and secondary care facilities (i.e. general practitioners and specialists). The latter is essential for therapy assessment and follow-up monitoring of patients with chronic diseases and cancer. Nevertheless, the development of such sensors is lagging compared to the projections of 10 – 20 years ago, mainly due to insufficient sensitivity, poor reproducibility, and the complexity of the sensors’ design reported in the research literature. This motivates the development of new detection strategies and technologies such as photoelectrochemical sensors that combine the best features of different sensing approaches. The primary concern when developing detection technologies for miRNA is the need for a highly sensitive and selective platform. This thesis explores a novel photoelectrochemical (PEC) method that is distinctive owing to its sensitive nature and simple and robust design. Firstly, we focused on the usage of recently emerging commercial gold-sputtered electrode systems for the detection of short nucleic acid with enzymatic amplification. Importantly, cleaning such electrodes is a challenge since the standard procedures known for regular disk electrodes such as polishing cannot be employed here, since it will damage the protective layer on the electrode. However, the electrodes can be washed and pretreated chemically and/or electrochemically. Thus, a procedure to effectively clean and modify the gold-sputtered electrode has been developed, resulting in high-performance gold-sputtered nucleic acid sensors. Next, the usage of molecular photosensitizers as an alternative to enzymatic amplification has been evaluated. We took advantage of the singlet oxygen production by photosensitizers upon photoexcitation, leading to a photocurrent response due to the singlet oxygen-induced (electro)chemical conversions. Following the demonstration of the detection strategy, the analytical performance of the sensing system was evaluated using magnetic beads-based nucleic acid assay on disposable electrode platforms, with a focus to enhance the sensitivity and robustness of the technique in detecting complementary nucleic acid targets. Following the fundamental evaluation of the singlet oxygen-based PEC detection of nucleic acids, we further optimized the assay and measurement parameters and employed the sensing strategy for a polymerase chain reaction-free (PCR-free) quantification of miRNAs related to prostate cancer. By successfully detecting and quantifying low-picomolar range concentrations (< 10 pM) in plasma samples from prostate cancer patients, we successfully showed the applicability of the novel sensing strategy. We have also compared and positioned the performance of our developed PEC strategy with an existing state-of-art technique, i.e. electrochemiluminescence (ECL). Our PEC strategy performed on par with ECL, both yielding low-picomolar detection limits in serum matrices, however quicker and cheaper than ECL. Owing to the versatility of this PEC technique, the final study explored its multiplexing capability. As a starting point in this branch of the research, we have investigated two possible ways for multiplexing. To perform multiple measurements at the same time, constructing calibration plots and quantifying unknown miRNA concentrations in patient samples at the same time, we have developed a high-throughput detection with 96X multi-channel electrode systems and in-house designed and constructed 96XLED illumination sources. Secondly, to detect more than one target miRNA in a single measurement, intra-vial multiplexing where the samples were analyzed for different targets in one vial was also explored. Altogether, this thesis presents the fundamentals, development and application of a novel PEC strategy for detecting short (< 25 bases) nucleic acid sequences, in particular, miRNA. With an aim to serve as a distinctive technique to function as a clinical testing platform without any need for PCR, this work adds value to the development of nucleic acid-based sensors for miRNAs and other short-stranded nucleic acid biomarkers, and benefits in the early detection of diseases like cancer. |
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UA @ admin @ c:irua:191753 |
Serial |
8931 |
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Author |
Neven, L. |
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Title |
Singlet oxygen-based photoelectrochemical detection of phenolic contaminants |
Type |
Doctoral thesis |
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Year |
2022 |
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Abbreviated Journal |
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Volume |
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234 p. |
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Doctoral thesis; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
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Abstract |
Phenolic compounds can be found everywhere in our daily lives but exhibit high toxicity, low (bio)degradability and hormone-disrupting effects when they are released in the environment. It is for this reason imperative to develop detection strategies for these pollutants. A promising approach involves the use of a photoelectrochemical (PEC) sensor. In this sensor, a photosensitiser (PS) type II, which generates 1O2 under illumination, is used to oxidise phenolic compounds present in the sample. The oxidised phenols are reduced at the electrode surface leading to the generation of an electrocatalytic redox cycle. In this thesis, an in-depth understanding, through the identification of the reactive oxygen species (ROS) in the PEC sensing mechanism, is obtained. The detection strategy is optimised by choosing the PS with the highest 1O2 production and by optimising the detection parameters so that the PEC sensor can be successfully applied for the detection of phenols in industrial samples. First, it was determined that the use of highly fluorinated zinc phthalocyanine derivatives, F52PcZn and F64PcZn, as photocatalysts was optimal for the sensing of phenol due to their high 1O2 production and improved single-site isolation. However, next to 1O2, it was shown that the ROS O2•- and H2O2 were also generated in the PEC sensor. Their contribution to the photocurrent response was studied by rotating disk electrode measurements in function of the pH and applied potential. After this, the PEC detection strategy was optimised in terms of pH and applied potential for the detection of doxycycline, cefadroxil, and phenol. It was found that the use of alkaline pH-levels led to nmol L-1-level detection limits. The combination with square wave voltammetry (SWV) was, also, proposed to allow the quantification and identification of phenolic compounds in a specific sample. At last, the developed PEC and SWV sensors were applied for the measurement of phenolic compounds in industrial water samples. The PEC sensor could follow the decrease of the phenolic concentration throughout the wastewater treatment process while the SWV sensor provided the electrochemical fingerprints of these samples. The thesis concluded that the use of the PEC sensor was advantageous in the measurement of lower concentrated phenolic samples due to its high sensitivity and fast measurement time in comparison to commercial test kits. |
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UA @ admin @ c:irua:187029 |
Serial |
8932 |
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Ahmadi Eshtehardi, H. |
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Combined computational-experimental study on plasma and plasma catalysis for N2 fixation |
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Doctoral thesis |
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2024 |
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160 p. |
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Doctoral thesis; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Humanity feels the urge of shifting to a sustainable society more than at any other time in its history. Electrification of chemical industry plays a key role in this transition. The possibility of producing fertilizers from air using renewable electricity, and simultaneously, no greenhouse gas emission, resulted in an increasing interest toward plasma technology as a solution for electrification of a part of the chemical industry in the past few years. Additionally, the activation of nitrogen molecules by vibrational and electronic excitation reactions in plasma can lead to an energy-efficient process. Last but not least, the modularity (fast on/off characteristic) of plasma technology makes it capable of using intermittent renewable electricity on site for the production of fertilizers using air. All these advantages offered by plasma technology make it a potential solution for the on-site production of fertilizers in small and decentralized plants using air and renewable electricity, which leads to a considerable reduction in fertilizer production and transportation costs. However, industrialization of plasma-based NF suffers from several challenges, including challenges of plasma catalysis for the selective production of desired species, the high energy cost of plasma-based NF compared to current industrial processes, and the design and development of scaled up and energy-efficient plasma reactors for industrial purposes. In the framework of this thesis we have tried to add to the state-of-the-art (SOTA) in plasma-based NOx production and deal with its limitations using a combination of experimental and modelling work. |
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2024-06-14 |
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UA @ admin @ c:irua:205246 |
Serial |
9139 |
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Cioni, M.; Delle Piane, M.; Polino, D.; Rapetti, D.; Crippa, M.; Arslan Irmak, E.; Pavan, G.M.; Van Aert, S.; Bals, S. |
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Title |
Data for Sampling Real‐Time Atomic Dynamics in Metal Nanoparticles by Combining Experiments, Simulations, and Machine Learning |
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2024 |
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Dataset; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Even at low temperatures, metal nanoparticles (NPs) possess atomic dynamics that are key for their properties but challenging to elucidate. Recent experimental advances allow obtaining atomic‐resolution snapshots of the NPs in realistic regimes, but data acquisition limitations hinder the experimental reconstruction of the atomic dynamics present within them. Molecular simulations have the advantage that these allow directly tracking the motion of atoms over time. However, these typically start from ideal/perfect NP structures and, suffering from sampling limits, provide results that are often dependent on the initial/putative structure and remain purely indicative. Here, by combining state‐of‐the‐art experimental and computational approaches, how it is possible to tackle the limitations of both approaches and resolve the atomistic dynamics present in metal NPs in realistic conditions is demonstrated. Annular dark‐field scanning transmission electron microscopy enables the acquisition of ten high‐resolution images of an Au NP at intervals of 0.6 s. These are used to reconstruct atomistic 3D models of the real NP used to run ten independent molecular dynamics simulations. Machine learning analyses of the simulation trajectories allows resolving the real‐time atomic dynamics present within the NP. This provides a robust combined experimental/computational approach to characterize the structural dynamics of metal NPs in realistic conditions. |
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UA @ admin @ c:irua:205843 |
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9143 |
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De Luca, F.; Abate, S.; Bogaerts, A.; Centi, G. |
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Electrified CO2 conversion : integrating experimental, computational, and process simulation methods for sustainable chemical synthesis |
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2024 |
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Doctoral thesis; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Nowadays, the burning of fossil fuels, particularly petroleum, natural gas, and coal, meets the rising need for power and fuels for automobiles and industries. This has given rise to ecological and climate challenges. This thesis explores these issues from three distinct perspectives: (i) experimental, (ii) computational, and (iii) process simulation, with a focus on studying CO2 as an alternative and economically viable raw material. Firstly, the experimental study is focused on the synthesis, characterization, and testing of novel catalysts for electroreduction of CO2 and oxalic acid, an intermediate product of CO2. Electrocatalysts based on Cu supported by citrus (orange and lemon) peel biomass are prepared. These catalysts exhibit activity in the electrochemical reduction of CO2, emphasizing the effectiveness of biomasses, particularly orange peels, as environmentally friendly precursors for sustainable and efficient electrocatalysts. In addition, graphitic carbon nitrides/TiO2 nanotubes (g-C3N4/TiNT) composites are prepared for the electrocatalytic reduction of oxalic acid to glycolic acid, revealing superior electrocatalytic properties compared to pristine TiNT. Characterization by X-ray diffraction, X-ray photoelectron spectroscopy, and scanning electronic microscopy were performed for all the prepared electrocatalysts. Delving into the reduction of CO2 on Cu catalysts, a computational study about the synthesis of methanol on Cu(111) surface is performed by using the Vienna Ab initio Simulation Package. A systematic study is carried out to define the activation energies of the elementary reactions by using mGGA DF. Consequently, it is shown that the rate-controlling step is CH3O* hydrogenation and the formate pathway on Cu(111) proceeds through the HCOOH* intermediate. Finally, the process simulation, performed by using the software Aspen Plus 11 from AspenTech Inc., is based on the comparison of a catalytic (oxidation of ethylene glycol) and an electrocatalytic process (CO2 electroreduction chain) to synthesize glycolic acid. An economic analysis of the operational and investment costs reveals that the catalytic process is more cost-effective due to the current instability of electrocatalysts and proton exchange membranes, resulting in increased maintenance costs and, consequently, higher prices for the product. |
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UA @ admin @ c:irua:205262 |
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9147 |
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Vlasov, E. |
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Exploiting secondary electrons in transmission electron microscopy for 3D characterization of nanoparticle morphologies |
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2024 |
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x, 118 p. |
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Doctoral thesis; Electron microscopy for materials research (EMAT) |
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Electron tomography (ET) is an indispensable tool for determining the three-dimensional (3D) structure of nanomaterials in (scanning) transmission electron microscopy ((S)TEM). ET enables 3D characterization of a variety of nanomaterials across different fields, including life sciences, chemistry, solid-state physics, and materials science down to atomic resolution. However, the acquisition of a conventional tilt series for ET is a time-consuming process and thus cannot capture fast transformations of materials in realistic conditions. Moreover, only a limited number of nanoparticles (NPs) can be investigated, hampering a general understanding of the average properties of the material. Therefore, alternative characterization techniques that allow for high-resolution characterization of the surface structure without the need to acquire a full tilt series in ET are required which would enable a more time-efficient investigation with better statistical value. In the first part of this work, an alternative technique for the characterization of the morphology of NPs to improve the throughput and temporal resolution of ET is presented. The proposed technique exploits surface-sensitive secondary electron (SE) imaging in STEM employed using a modification of electron beam-induced current (EBIC) setup. The time- and dose efficiency of SEEBIC are tested in comparison with ET and superior spatial resolution is shown compared to conventional scanning electron microscopy. Finally, contrast artefacts arising in SEEBIC images are described, and their origin is discussed. The second part of my thesis focuses on real applications of the proposed technique and introduces a high-throughput methodology that combines images acquired by SEEBIC with quantitative image analysis to retrieve information about the helicity of gold nanorods. It shows that SEEBIC imaging overcomes the limitation of ET providing a general understanding of the connection between structure and chiroptical properties. |
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2024-06-17 |
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UA @ admin @ c:irua:204905 |
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Kummamuru, N.B. |
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Methane and hydrogen storage in clathrate hydrates |
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2024 |
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XXV, 260 p. |
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Doctoral thesis; Engineering sciences. Technology; Antwerp engineering, PhotoElectroChemistry & Sensing (A-PECS) |
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In a world increasingly reliant on alternative energy sources, the quest for efficient and secure storage solutions is paramount. This doctoral thesis explores the exciting potential of a familiar material – water – to act as a vault for next-generation energy sources like hydrogen (H2) and methane (CH4). Nature offers a solution in the form of clathrate hydrates, fascinating cage-like structures formed from water molecules that can trap these gas molecules within their framework. This research investigates on improving the formation kinetics and gas storage capabilities of clathrate hydrates utilizing porous materials and the interstitial space between non-porous materials to augment the contact between gas and water thereby catalysing the growth of hydrates and unlocking their full potential as efficient and secure energy storage reservoirs. A key outcome of this research is the formulation of an empirical correlation, offering predictive insights into CH4 hydrate phase equilibrium conditions. Innovative approaches utilizing thermally conductive beads have yielded substantial enhancements in CH4 uptake. Furthermore, the identification of optimal water content within porous materials showcases a pathway to maximize CH4 storage capacity and hydrate growth kinetics. In the domain of hydrogen storage, attention is also directed towards unstirred systems, where the integration of functionalized porous materials has demonstrated a significant improvement in the rate of hydrate formation and the overall H2 storage capacity. A noteworthy achievement of this research lies in the successful storage of H2 within confined CH4 hydrates through a gas exchange process and the preliminary results show the potential for safer and more sustainable method for H2 storage at mild thermodynamic conditions, offering promising prospects for future energy systems. |
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UA @ admin @ c:irua:206258 |
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9160 |
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Lu, Q. |
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Precipitation behavior and heat resistance properties of Al-Cu-Mg-Ag-(Si) alloy |
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2024 |
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VIII, 212 p. |
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Doctoral thesis; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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With the rapid increase in the speed of new-generation aerospace vehicles, conventional heat-resistant aluminum alloys cannot meet the long-term service of the equipment. Therefore, the development of new high-strength heat-resistant aluminum alloys is of great strategic for the sustainable and high-quality development of industries. Al-Cu-Mg-Ag alloy is an age-hardenable heat-resistant aluminum alloy and has high strength and heat resistance. The addition of alloying elements such as Si and Sc to Al-Cu-Mg-Ag alloy introduces a competitive relationship among the σ-Al5Cu6Mg2, θ′-Al2Cu, and Ω phases. Therefore, a systematic investigation of precipitation behavior and heat resistance of Al-Cu-Mg-Ag-(Si) is essential for guiding the design of high-strength heat-resistant aluminum alloys. Combined characterization testing methods such as scanning electron microscopy, transmission electron microscopy, atom probe tomography, microhardness testing, and tensile testing with simulation calculation methods such as calculation of phase diagram, first-principles calculations, and Ab initio molecular dynamics, the effects of heat treatment processes and element content on the precipitation behavior, mechanical properties, and heat resistance of Al-Cu-Mg-Ag-(Si) alloys were systematically investigated. Furthermore, a multiple interface segregation structure was constructed at the θ′/Al interface, and a new Al-Cu-Mg-Ag-Si-Sc alloy with synergistically improved strength and heat resistance was developed. The main conclusions are as follows: (1) Based on the Kampmann-Wagner-Numerical theory, the relationship between the coarsening rate of the Ω phase and the aging process was analyzed, revealing for the first time that the critical size of Ω phase ( ) under thermal exposure temperature was the key factor determining the coarsening rate of Ω phase during long time thermal exposure heat treatment. After artificial ageing, when the size of Ω phase was smaller than the critical size , the dissolution of smaller Ω phase leaded to a rapid decrease in the number density of Ω phases, thereby reducing the heat resistance of the alloy. When the size of Ω phase was greater than or equal to the critical size , the coarsening rate of Ω phase was consistent, but a larger initial size would result in a larger final size after long-term thermal exposure. Therefore, the closer the size of Ω phase in the alloy is to the critical size under heat exposure temperature, the better the heat resistance of the alloy. (2) A concept of constructing a multiple interface segregation structure at the precipitate/matrix interface was proposed, and based on this concept, a multiple interface segregation structure containing the C/L-AlMgSiCu interfacial phase, newly discovered χ-AgMg interfacial phase, and Sc segregation layer was successfully constructed at the θ′/Al interface. The existence of the multiple interface segregation structure ensured that the designed Al-Cu-Mg-Ag-Si-Sc alloy maintains a yield strength of 400 MPa after thermal exposure at 200 C for 100 h, with a strength retention rate of 97%, creating a new record for the synergistic improvement of strength and heat resistance in aluminum alloys. In addition, combining transmission electron microscopy ex-situ/in-situ characterization with first-principles calculations, it is shown that the χ-AgMg interface phase will be destroyed due to the diffusion of the outer Ag layer during thermal exposure, and gradually dissolve into the matrix, but it can still delay the coarsening behavior of θ′-Al2Cu phase. (3) The criteria for determining whether Ω phase can precipitate are updated in Al-Cu-Mg-Ag-Si alloys with low Mg/Si ratio based on phase diagram thermodynamic calculations and multi-scale structural characterization. When W(Mg)/W(Si) > 1.4 and X(Ag)/X(Mgexcess) > 1, Ω phase can precipitate in Al-Cu-Mg-Ag-Si alloys, where X(Mgexcess) represents the atomic percentage of residual Mg elements after the formation of the AlMgSiCu quaternary precipitate phase C/L phase in the supersaturated solid solution, and the W(Mg) is the mass fraction of Mg in the supersaturated solid solution before artificial ageing. (4) The effects of alloy element content on precipitation behavior and heat resistance of Al-Cu-Mg-Ag-Si alloys were systematically analyzed. Critical conditions for the precipitation of σ-Al5Cu6Mg2 and Ω phase in Al-Cu-Mg-Ag-Si alloys are revealed. Based on calculation of phase diagram results, the conditions for precipitating σ-Al5Cu6Mg2 phase in the alloy are: ① W(Mg)/W(Si) > 1.8; ② W(Cu) > 2.7W(Mg) – 5W(Si). When W(Mg)/W(Si) < 1.8, the alloy is mainly precipitated with C/L/Q′-AlMgSiCu. When W(Cu) < 2.7W(Mg) – 5W(Si), the alloy will generate GPB zone. In addition, W(Ag)/W(Si) > 4 is the critical condition which the Ω phase can the main precipitates in Al-Cu-Mg-Ag-Si alloys. Furthermore, the correlation between precipitate types and heat resistance was summarized, showing that Al-Cu-Mg-Ag-(Si) alloys with Ω phase as the main strengthening phase are more suitable for the preparation of structures with short service time but high temperature, while Al-Cu-Mg-Ag-(Si) alloys with low Mg content and multiple segregation structures are more suitable for structures requiring long-term service at medium to high temperatures. This study, for the first time, combines calculation of phase diagram with multi-scale microstructure characterization, systematically unraveling the effects of element content on precipitation behavior, strength, and heat resistance of Al-Cu-Mg-Ag-(Si) alloys. In addition, a concept of constructing a multiple interface segregation structure at the precipitate/matrix interface was proposed to synergistically improve alloy strength and heat resistance. This work provides theoretical guidance for optimizing the composition and processing of Al-Cu-Mg-Ag-(Si) alloy and regulating the microstructure. Furthermore, it also offers new ideas and theoretical guidance for the development of novel high-strength heat-resistant alloys in other systems. |
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UA @ admin @ c:irua:206180 |
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