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Mass Spectrometry for Spatially Resolved, Elemental, and Fe, Ni Isotopic Analysis of Metal and Silicate Meteoritic Material

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Mass Spectrometry for Spatially Resolved, Elemental, and Fe, Ni Isotopic Analysis of Metal and Silicate Meteoritic Material Faculty of Sciences Department of Analytical Chemistry Research group “Atomic & Mass Spectrometry” Development and application of analytical methods based on ICP – mass spectrometry for spatially resolved, elemental, and Fe, Ni isotopic analysis of metal and silicate meteoritic material Thesis submitted in fulfillment of the requirements for the degree of Doctor of Science: Chemistry by Stepan M. Chernonozhkin Academic year 2015-2016 Supervisor: Prof. Dr. Frank Vanhaecke Supervisor: Prof. Dr. Philippe Claeys For my family and my wife Contents 5 Contents Goals ............................................................................................................................................................................. 7 Chapter 1. General Introduction ............................................................................................................................. 15 1. Meteorites and their parent bodies ...................................................................................................................... 15 1.1. Classification of meteorites ......................................................................................................................... 16 1.2. Triple-oxygen isotope ratios ........................................................................................................................ 23 2. Isotopic variability in the Solar System .............................................................................................................. 24 3. Principles of ICP-mass spectrometry and its cosmochemical applications ......................................................... 28 3.1. Principle design of ICP-MS ......................................................................................................................... 29 3.2. Multi-collector ICP-MS ............................................................................................................................... 33 3.3. Correction for instrumental mass discrimination ......................................................................................... 34 3.4. Spectral interference and matrix effects....................................................................................................... 36 3.5. Ion exchange chromatography for isotopic analysis .................................................................................... 37 3.6. Laser ablation in-situ sample introduction ................................................................................................... 38 3.7. Complementary techniques .......................................................................................................................... 40 4. List of references ................................................................................................................................................. 42 Chapter 2. Evaluation of pneumatic nebulization and ns-laser ablation ICP-MS for bulk elemental analysis and 2-dimensional element mapping of iron meteorites .................................................................... 49 1. Abstract ............................................................................................................................................................... 49 2. Introduction ......................................................................................................................................................... 50 3. Experimental ....................................................................................................................................................... 51 4. Results and discussion ........................................................................................................................................ 55 5. Conclusions ......................................................................................................................................................... 65 6. Appendix ............................................................................................................................................................. 67 7. Acknowledgments ............................................................................................................................................... 70 8. List of references ................................................................................................................................................. 71 Chapter 3. Quantitative laser ablation ICP-MS and μXRF element mapping of zoned olivines of main group pallasites .................................................................................................................................................... 75 1. Abstract ............................................................................................................................................................... 75 2. Introduction ......................................................................................................................................................... 76 3. Experimental ....................................................................................................................................................... 77 4. LA-ICP-MS data reduction protocol ................................................................................................................... 78 5. Results ................................................................................................................................................................. 79 6. Discussion ........................................................................................................................................................... 82 7. Implications ......................................................................................................................................................... 86 8. Appendices .......................................................................................................................................................... 87 9. Acknowledgements ............................................................................................................................................. 94 10. List of references ............................................................................................................................................... 95 6 Chapter 4. Development of an isolation procedure and MC-ICP-MS measurement protocol for the study of stable isotope ratio variations of nickel ............................................................................................... 97 1. Abstract ............................................................................................................................................................... 97 2. Introduction ......................................................................................................................................................... 98 3. Experimental ....................................................................................................................................................... 99 4. Results and discussion ...................................................................................................................................... 102 5. Conclusions ....................................................................................................................................................... 110 6. Appendices........................................................................................................................................................ 111 7. Acknowledgments............................................................................................................................................. 114 8. List of references............................................................................................................................................... 115 Chapter 5. Evaluation of the use of cold plasma conditions for Fe isotopic analysis via MC-ICP-MS: effect on spectral interferences and instrumental mass discrimination ........................................................ 119 1. Abstract ............................................................................................................................................................. 119 2. Introduction ....................................................................................................................................................... 120 3. Experimental ..................................................................................................................................................... 120 4. Results ............................................................................................................................................................... 121 5. Summary ........................................................................................................................................................... 125 6. List of references............................................................................................................................................... 127 Chapter 6. Effect of parent body evolution on equilibrium and kinetic isotope fractionation: a combined Ni and Fe isotope study of iron and stony-iron meteorites ........................................................... 129 1. Abstract ............................................................................................................................................................
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