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Journal of Advanced Ceramics

Authors

Ying ZHAN, Department of Materials and Earth Sciences, Technical University of Darmstadt, D-64287 Darmstadt, Germany
Wei LI, Department of Materials and Earth Sciences, Technical University of Darmstadt, D-64287 Darmstadt, Germany
Tianshu JIANG, Department of Materials and Earth Sciences, Technical University of Darmstadt, D-64287 Darmstadt, Germany
Claudia FASEL, Department of Materials and Earth Sciences, Technical University of Darmstadt, D-64287 Darmstadt, Germany
Emmanuel III RICOHERMOSO, Department of Materials and Earth Sciences, Technical University of Darmstadt, D-64287 Darmstadt, Germany
Jan BERNAUER, Department of Materials and Earth Sciences, Technical University of Darmstadt, D-64287 Darmstadt, Germany
Zhaoju YU, College of Materials, Key Laboratory of High Performance Ceramic Fibers (Xiamen University), Ministry of Education, Xiamen 361005, China
Zhenghao WU, Eduard-Zintl-Institut für Anorganische und Physikalische Chemie, Technical University of Darmstadt, D-64287 Darmstadt, Germany
Florian MÜLLER-PLATHE, Eduard-Zintl-Institut für Anorganische und Physikalische Chemie, Technical University of Darmstadt, D-64287 Darmstadt, Germany
Leopoldo MOLINA-LUNA, Department of Materials and Earth Sciences, Technical University of Darmstadt, D-64287 Darmstadt, Germany
Ralf GROTTENMÜLLER, Merck KGaA, Performance Materials, D-64293, Darmstadt, Germany
Ralf RIEDEL, Department of Materials and Earth Sciences, Technical University of Darmstadt, D-64287 Darmstadt, Germany

Keywords

polymer-derived ceramics (PDCs), SiBN, crystallization, molecular dynamics, oxidation resistance

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 N2 atmosphere (without ammonolysis) to prepare SiBN ceramics at 1100, 1200, and 1300 ℃ 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 ℃. 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 N2 atmosphere.

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