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Journal of Advanced Ceramics 2022, 11(7): 1104-1116 https://doi.org/10.1007/s40145-022-0597-z
Research Article | Open Access | Issue | Published: 28 May 2022

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

Show Author's Information Ying ZHANa,†,  Wei LIa,†,  Tianshu JIANGa,  Claudia FASELa,  Emmanuel III RICOHERMOSOa,  Jan BERNAUERa,  Zhaoju YUb( ),  Zhenghao WUc( ),  Florian MÜLLER-PLATHEc,  Leopoldo MOLINA-LUNAa,  Ralf GROTTENMÜLLERd,  Ralf RIEDELa
Department of Materials and Earth Sciences, Technical University of Darmstadt, D-64287 Darmstadt, Germany
College of Materials, Key Laboratory of High Performance Ceramic Fibers (Xiamen University), Ministry of Education, Xiamen 361005, China
Eduard-Zintl-Institut für Anorganische und Physikalische Chemie, Technical University of Darmstadt, D-64287 Darmstadt, Germany
Merck KGaA, Performance Materials, D-64293, Darmstadt, Germany

† Ying Zhan and Wei Li contributed equally to this work.

Keywords:
molecular dynamics, polymer-derived ceramics (PDCs), oxidation resistance, crystallization, SiBN
Cite this article:
ZHAN Y, LI W, JIANG T, et al. Boron-modified perhydropolysilazane towards facile synthesis of amorphous SiBN ceramic with excellent thermal stability. Journal of Advanced Ceramics, 2022, 11(7): 1104-1116. https://doi.org/10.1007/s40145-022-0597-z
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Abstract Full text Electronic supplementary material About this article

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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About this article

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

Show Author's information Ying ZHANa,†, Wei LIa,†, Tianshu JIANGa, Claudia FASELa, Emmanuel III RICOHERMOSOa, Jan BERNAUERa, Zhaoju YUb( ), Zhenghao WUc( ), Florian MÜLLER-PLATHEc, Leopoldo MOLINA-LUNAa, Ralf GROTTENMÜLLERd, Ralf RIEDELa
Department of Materials and Earth Sciences, Technical University of Darmstadt, D-64287 Darmstadt, Germany
College of Materials, Key Laboratory of High Performance Ceramic Fibers (Xiamen University), Ministry of Education, Xiamen 361005, China
Eduard-Zintl-Institut für Anorganische und Physikalische Chemie, Technical University of Darmstadt, D-64287 Darmstadt, Germany
Merck KGaA, Performance Materials, D-64293, Darmstadt, Germany

† Ying Zhan and Wei Li contributed equally to this work.

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.

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

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Received: 14 November 2021
Revised: 01 April 2022
Accepted: 03 April 2022
Published: 28 May 2022
Issue date: July 2022

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© The Author(s) 2022.

Acknowledgements

The authors would like to acknowledge Merck KGaA for the financial support of this research project. Wei Li acknowledges financial support from China Scholarship Council (No. 201907040060) during his research at TU Darmstadt. Zhenghao Wu acknowledges the funding of Deutsche Forschungsgemeinschaft via the SFB-TRR 146 "Multiscale Simulation Methods for Soft Matter Systems", Project A8.

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