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Mechanistic Investigation of the Formation of Nickel Nanocrystallites Embedded in Amorphous Silicon Nitride Nanocomposites

Abstract : Herein, we report the mechanistic investigation of the formation of nickel (Ni) nanocrystallites during the formation of amorphous silicon nitride at a temperature as low as 400 °C, using perhydropolysilazane (PHPS) as a preformed precursor and further coordinated by nickel chloride (NiCl2); thus, forming the non-noble transition metal (TM) as a potential catalyst and the support in an one-step process. It was demonstrated that NiCl2 catalyzed dehydrocoupling reactions between Si-H and N-H bonds in PHPS to afford ternary silylamino groups, which resulted in the formation of a nanocomposite precursor via complex formation: Ni(II) cation of NiCl2 coordinated the ternary silylamino ligands formed in situ. By monitoring intrinsic chemical reactions during the precursor pyrolysis under inert gas atmosphere, it was revealed that the Ni-N bond formed by a nucleophilic attack of the N atom on the Ni(II) cation center, followed by Ni nucleation below 300 °C, which was promoted by the decomposition of Ni nitride species. The latter was facilitated under the hydrogen-containing atmosphere generated by the NiCl2-catalyzed dehydrocoupling reaction. The increase of the temperature to 400 °C led to the formation of a covalently-bonded amorphous Si3N4 matrix surrounding Ni nanocrystallites.
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https://hal-cnrs.archives-ouvertes.fr/hal-03851841
Contributor : Samuel Bernard Connect in order to contact the contributor
Submitted on : Monday, November 14, 2022 - 4:58:01 PM
Last modification on : Saturday, November 19, 2022 - 3:22:15 AM

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Norifumi Asakuma, Shotaro Tada, Erika Kawaguchi, Motoharu Terashima, Sawao Honda, et al.. Mechanistic Investigation of the Formation of Nickel Nanocrystallites Embedded in Amorphous Silicon Nitride Nanocomposites. Nanomaterials, 2022, 12 (10), pp.1644. ⟨10.3390/nano12101644⟩. ⟨hal-03851841⟩

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