Insights into the decomposition of zirconium acetylacetonate using synchrotron radiation: Routes to the formation of volatile Zr-intermediates

The thermal decomposition of Zr(acac) 4 is studied in a SiC-microreactor on the micro-second time scale. By utilizing synchrotron radiation and photoelectron photoion coincidence spectroscopy, six important zirconium intermediates, as for instance Zr(C 5 H 7 O 2 ) 2 (C 5 H 6 O 2 ), and Zr(C 5 H 6 O...

Full description

Saved in:
Bibliographic Details
Published in:Journal of materials research 2022-05, Vol.37 (9), p.1558-1575
Main Authors: Grimm, Sebastian, Baik, Seung-Jin, Hemberger, Patrick, Kasper, Tina, Kempf, Andreas M., Atakan, Burak
Format: Article
Language:English
Subjects:
Acetylacetone
Applied and Technical Physics
Argon
Biomaterials
Ceramic coatings
Chemistry and Materials Science
Decomposition
Dilution
Functional materials
Inorganic Chemistry
Invited Paper
Ionization
Materials Engineering
Materials research
Materials Science
Microreactors
Nanomaterials
Nanotechnology
Photoelectrons
Pyrolysis
Radiation
Synchrotron radiation
Synchrotrons
Temperature profiles
Thermal decomposition
Uniform flow
Vapor phases
Zirconium
Citations: Items that this one cites
Items that cite this one
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary:The thermal decomposition of Zr(acac) 4 is studied in a SiC-microreactor on the micro-second time scale. By utilizing synchrotron radiation and photoelectron photoion coincidence spectroscopy, six important zirconium intermediates, as for instance Zr(C 5 H 7 O 2 ) 2 (C 5 H 6 O 2 ), and Zr(C 5 H 6 O 2 ) 2 , are identified in the gas phase for the first time. The adiabatic ionization thresholds of intermediately formed zirconium species are estimated and the main products of their thermal decomposition, acetylacetone, acetylallene and acetone are characterized unambiguously and isomer-selectively. Based on all detected intermediates, we deduce the predominant pyrolysis pathways of the precursor in the temperature range from 400 to 900 K. Our findings are complemented by numerical simulations of the flow field in the microreactor, which show that the choice of dilution gas significantly influences the temperature profile and residence times in the microreactor, such that helium provides a more uniform flow field than argon and should preferentially be used. Graphical abstract Using a soft ionization method coupled to velocity map imaging (VMI), leads to valuable insights in the thermal decomposition of Zr(C 5 H 7 O 2 ) 4 , used in the synthesis of functional nanomaterials and ceramic coatings. Thanks to the use of a microreactor, important gas
ISSN:0884-2914
2044-5326
DOI:10.1557/s43578-022-00566-6