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Boron-modified perhydropolysilazane towards facile synthesis of amorphous SiBN ceramic with excellent thermal stability

Zhan, Ying ; Li, Wei ; Jiang, Tianshu ; Fasel, Claudia ; Ricohermoso, Emmanuel ; Bernauer, Jan ; Yu, Zhaoju ; Wu, Zhenghao ; Müller-Plathe, Florian ; Molina-Luna, Leopoldo ; Grottenmüller, Ralf ; Riedel, Ralf (2022):
Boron-modified perhydropolysilazane towards facile synthesis of amorphous SiBN ceramic with excellent thermal stability.
In: Journal of Advanced Ceramics, 11 (7), pp. 1104-1116. Springer, ISSN 2226-4108, e-ISSN 2227-8508,
DOI: 10.1007/s40145-022-0597-z,
[Article]

Abstract

SiBN ceramics are widely considered to be the most promising material for microwave-transparent applications in harsh environments owing to its excellent thermal stability and low dielectric constant. This work focuses on the synthesis and ceramization of single-source precursors for the preparation of SiBN ceramics as well as the investigation of the corresponding microstructural evolution at high temperatures including molecular dynamic simulations. Carbon- and chlorine-free perhydropolysilazanes were reacted with borane dimethyl sulfide complex at different molar ratios to synthesize single-source precursors, which were subsequently pyrolyzed and annealed under N-2 atmosphere (without ammonolysis) to prepare SiBN ceramics at 1100, 1200, and 1300 degrees C with high ceramic yield in contrast to previously widely-used ammonolysis synthesis process. The obtained amorphous SiBN ceramics were shown to have remarkably improved thermal stability and oxidation resistance compared to amorphous silicon nitride. Particularly, the experimental results have been combined with molecular dynamics simulation to further study the amorphous structure of SiBN and the atomic-scale diffusion behavior of Si, B, and N at 1300 degrees C. Incorporation of boron into the Si-N network is found to suppress the crystallization of the formed amorphous silicon nitride and hence improves its thermal stability in N-2 atmosphere.

Item Type: Article
Erschienen: 2022
Creators: Zhan, Ying ; Li, Wei ; Jiang, Tianshu ; Fasel, Claudia ; Ricohermoso, Emmanuel ; Bernauer, Jan ; Yu, Zhaoju ; Wu, Zhenghao ; Müller-Plathe, Florian ; Molina-Luna, Leopoldo ; Grottenmüller, Ralf ; Riedel, Ralf
Title: Boron-modified perhydropolysilazane towards facile synthesis of amorphous SiBN ceramic with excellent thermal stability
Language: English
Abstract:

SiBN ceramics are widely considered to be the most promising material for microwave-transparent applications in harsh environments owing to its excellent thermal stability and low dielectric constant. This work focuses on the synthesis and ceramization of single-source precursors for the preparation of SiBN ceramics as well as the investigation of the corresponding microstructural evolution at high temperatures including molecular dynamic simulations. Carbon- and chlorine-free perhydropolysilazanes were reacted with borane dimethyl sulfide complex at different molar ratios to synthesize single-source precursors, which were subsequently pyrolyzed and annealed under N-2 atmosphere (without ammonolysis) to prepare SiBN ceramics at 1100, 1200, and 1300 degrees C with high ceramic yield in contrast to previously widely-used ammonolysis synthesis process. The obtained amorphous SiBN ceramics were shown to have remarkably improved thermal stability and oxidation resistance compared to amorphous silicon nitride. Particularly, the experimental results have been combined with molecular dynamics simulation to further study the amorphous structure of SiBN and the atomic-scale diffusion behavior of Si, B, and N at 1300 degrees C. Incorporation of boron into the Si-N network is found to suppress the crystallization of the formed amorphous silicon nitride and hence improves its thermal stability in N-2 atmosphere.

Journal or Publication Title: Journal of Advanced Ceramics
Volume of the journal: 11
Issue Number: 7
Publisher: Springer
Uncontrolled Keywords: polymer-derived ceramics (PDCs), SiBNcrystallization, molecular dynamics,oxidation resistance, single-source-precursor, silicon-nitride, oxidation behavior, molecular dynamics, atomic structure, nanocomposites, nitrogen, carbon, composites, pyrolysis
Divisions: 11 Department of Materials and Earth Sciences
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences > Material Science > Dispersive Solids
11 Department of Materials and Earth Sciences > Material Science > In-situ electron microscopy
07 Department of Chemistry
07 Department of Chemistry > Physical Chemistry
TU-Projects: DFG|TRR146|TP A08 Müller-Plathe
Date Deposited: 05 Jul 2022 05:37
DOI: 10.1007/s40145-022-0597-z
PPN: 496362712
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