Physico-chemical properties of silicate melts [Elektronische Ressource] / vorgelegt von Marcel Potužák

Marcel Potužák

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• Publié par: ludwig-maximilians-universitat_munchen
• Publié le: 01 janvier 2006
• Nombre de lectures: 32
• Poids de l'ouvrage: 2 Mo

Extrait

Physico-Chemical Properties of Silicate Melts





INAUGURALDISSERTATION
ZUR ERLANGUNG DES DOKTORGRADES
DER FAKULTÄT FÜR GEOWISSENSCHAFTEN
DER LUDWIG-MAXIMILIANS-UNIVERSITÄT MÜNCHEN










VORGELEGT VON
MARCEL POTUŽÁK


München, May 2006 ii iii

“No matter how much you do, you never do enough…”










Die vorliegende Arbeit wurde in der Zeit von Dezember 2001 bis Dezember 2005 am
Department für Geo und Umweltwissenschaften der Ludwig-Maximilians-Universität,
München angerichtet.








Tag des Rigorosums: 07. 07. 2006

Promotionskomissions-
vorsitzender: Prof. Dr. H. Igel

1. Berichterstatter: Prof. Dr. D.B. Dingwell
2. Berichterstatter: Priv. Doz. Dr. T. Kunzmann

Übrige Promotions- Prof. Dr. P. Gille
komissionsmitglieder: Prof. T. Fehr iv v
Content

Thanks to………………………………………………………………………………………ix
Preamble……………………………………………………………………………………….xi
Zuzammenfassung……………………………………………………………………………13
Abstract ……………………………………………………………………………………….19
1. Introduction…………………………………………………………………………...25

2. Theoretical Background……………………………………………………………...27
2.1. Relaxation theory………………………………………………………………...27
2.2. Structure of silicate melts………………………………………………………..30
2.3. Viscosity…………………………………………………………………….…….32
2.4. Experimental methods and analytical hardware………………………………33
2.4.1. Low temperature viscometry…………………………………………..33
2.4.2. High temperature viscom
2.4.3. Low temperature densitometry…………………………………………36
2.4.4. High temperature densitometry………………………………………...36
2.4.5. Calorimetry……………………………………………………………..38
2.4.6. Dilatometry……………………………………………………………..40
2.4.7. Electron microprobe……………………………………………………42
2.4.8. Potassium dichromate titration…………………………………………42
2.4.9. X-Ray analysis…………………………………………………………44

3. History of Density and Expansivity Determination…………………………………….45
3.1. Combining dilatometric/calorimetric methods – Web et al., (1992) method...47

4. A Partial Molar Volume for ZnO in Silicate Melts ……………………………………51
4.1. Background……………………………………………………………………….52
4.2. Experimental methods…………………………………………………………...53
4.2.1. Sample separation……………………………………………………...53
4.2.2. Room temperature densitometry………………………….……………54
4.2.3. High tempetry……………………………….………..55
4.3. Results……………………………………………………………………………55 vi
4.3.1. Room temperature densitometry…………………………………….…55
4.3.2. High tempetry………………………………………...55
4.3.3. Molar volume of liquids………………………………………………..56
4.3.4. Compositional dependence of the molar volume of
the present liquids……………………………………………………...57
4.3.5. Partial molar volume of ZnO…………………………………………..58
4.4. Discussion………………………………………………………………………...61
4.4.1. Comparison with previous literature data……………………………...61
5. Temperature Independent Thermal Expansivities of Calcium Aluminosilicate Melts
between 1150 and 1973 K in the System Anorthite-Wollastonite-Gehlenite (An-Wo-
Geh): A density model……………………………………………………………………65
5.1. Experimental methods…………………………………………………………...66
5.1.1. Sample preparation……………………………………………………..66
5.1.2. Low temperature dilatometric/calorimetric method……………………67
5.1.3. Room temperature densitometry……………………………………….69
5.1.4. Partial molar volumes…………………………………………………..69
5.2. Results…………………………………………………………………………….71
5.2.1. Room temperature densitometry……………………………………….71
5.2.2. Molar volume of glasses (low temperature densitometry).…………….71
5.2.3. e of liquids………………………………………………..72
5.2.4. Partial molar volumes and molar thermal expansivities……………….75
5.3 Discussion………………………………………………………………………….76

6. Temperature Dependent Thermal Expansivities of Multicomponent Natural Melts
Between 993 and 1803 K …………………………………………………………………79
6.1. Introduction………………………………………………………………………79
6.2. Experimetal methods……………….……………………………………………80
6.2.1. Sample preparation…………………………………………………...…80
6.2.2. High temperature densitometry…………………………...…………….81
6.2.3. Calorimetry……………………………………………………………...82
6.2.4. Dilatometry……………………………………………………………..82
6.2.5. Room temperature densitometry……………………………………….83
6.3. Results…………………...…………………………….………….………………84
6.3.1. Sample composition and Fe oxidation state……………………………84 vii
6.3.2. Room temperature densitometry……………………………………….84
6.3.3. Low temperature calorimetry and dilatometry…………………………85
6.3.4. Molar volume of liquids………………………………………………..85
6.4. Discussion……………………………………………………………………….90

7. An Expanded non-Arhenian Model for Silicate Melt Viscosity: A Treatment for
Metaluminous, Peraluminous and Peralkaline Liquids……………………………...95
7.1. Introduction ………….………………………………………………………...95
7.2. Exparimental rationale…….………………………………………………….97
7.3. Results and numerical strategy…….…………………………………………99
7.4. Viscosity model…….………………………………………………………….102
7.5. Extension to peralkaline and peraluminous melts…….……………………105
7.6. Discussion…….…………………………………….………………………….108

8. Outlook………………………………………………………………………………...111

Reference List…….…………………………………….………………………………..113
APPENDIX…….…………………………………….…………………………………..125
Curriculum Vitae…….…………………………………….……………………………143 viii ix
Thanks to
Prof. Dr. Donald Bruce Dingwell to accept me in Munich, offering and supervising this
very interesting study. Many thanks to him for finding a sources to cover expenses of the
scientific conferences and for rare but very intensive, useful and open discussions. My first
supervisor p.g. Petr Jakeš PhD to sending me to Munich. I am very sad that I can not to tell him
personally how much I appreciate his introduction to the problems of „Simulating the Earth“.
My parents, František and Blanka, who enabled this scientific life by always supporting
me. My grandmother Marie to keep my mind open even if my life situation was critical. My
sister Dominika and brother Lukáš for going through the Potužák´s way of education.
My colleagues in office, lab and field Daniele Giordano, Philippe Courtial, Kai-Uwe
Hess, Werner Ertel-Ingrisch, Alex Rocholl, Oliver Spieler, Ben Kennedy, Lothar Schwarzkopf,
Betty Scheu, Sebastian Müller, Alfonso Davila, Jacopo Taddeucci, Benoit Cordonnier, Thomas
Dorfner, Antonia Wimmer, Yan Lavallée, Dominique Richard, Jan Pawlowski, Conrad
Gennaro and many more unmentioned but not forgotten.
Special thanks to Alex Nichols alias “Sir Bamboo” for his specific British humour and
countless English correction of my very first article. Many thanks to Ulli Küppers for listening
me and for frequent help and assistance in any kind of never-ending bureaucratic tasks.
Very special thanks to Anny Mangiacapra for her strong support during a good and
even during a bad period of my stay in Germany.
Kelley J. Rusell, R.S.J. Sparks, G. Boudon, B. Villemant, Claudia Romano, Mette
Solvang, Dave Clague, Roberto Moretti, Jonathan Castro, François Beauducel, Cliff Shaw,
Brenda Ledda, Joe Gottsmann, Meritxell Aulinas I Junca, Antonio Costa, Andrea Di Muro,
Luca Caricchi for their help, sample providing, collaboration and scientific discussion.
The institute’s secretaries and mechanics Wolfgang and Martin for helping me out
whenever something had broken or got stuck.
Libor Stránský alias ”Švartna“ and Pavel Chromý alias “Paša“ with his family to stay
as a friends across the distance and the life-roads which divided us.
This work was funded by the projects CO 212 1-1, CO 212 1-2 from the German
Science Foundation (DFG), the EU Volcano Dynamics RTN project as well as general
University funds.
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