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Pyrolysis of different polysilazanes has been used to prepare novel covalent amorphous ceramics composed of silicon, carbon, and nitrogen. The formation and structure of the as‐pyrolyzed amorphous state and its devitrification into stable crystalline phases have been investigated by means of nuclear magnetic resonance spectroscopy, infrared spectroscopy, thermogravimetry, mass spectroscopy, X‐ray and neutron diffraction, and by transmission electron microscopy. Additionally, the electrical conductivity and the compression creep behaviour of the as‐received materials have been analyzed.

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