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Nanoporous Silicon Oxycarbonitride Ceramics Derived from Polysilazanes In situ Modified with Nickel Nanoparticles

Seifollahi Bazarjani, Mahdi and Kleebe, Hans-Joachim and Müller, Mathis M. and Fasel, Claudia and Baghaie Yazdi, Mehrdad and Gurlo, Aleksander and Riedel, Ralf (2011):
Nanoporous Silicon Oxycarbonitride Ceramics Derived from Polysilazanes In situ Modified with Nickel Nanoparticles.
In: Chemistry of Materials, ACS, pp. 4112-4123, 23, (18), ISSN 0897-4756, [Online-Edition: http://dx.doi.org/10.1021/cm200589n],
[Article]

Abstract

Ni–polysilazane precursors were synthesized from polysilazane and trans- [bis(2-aminoetanol-N,O)diacetato-nickel(II)]. The Ni–polysilazane precursors are superparamagnetic indicating formation of nanosized nickel particles (2−3 nm) confirmed by HRTEM as well. The as-obtained Ni–polysilazane precursors were thermolized at 700 °C and transformed to ceramic nanocomposites, manifesting a nanoporous structure, revealing a BET surface area of 215 m2 g–1, a micropore surface area of 205 m2 g–1, and a micropore volume of 0.113 cm3 g–1. Although Si–C–N–(O) ceramics derived from the native polysilazane are nonporous, the pronounced development of porosity in the Ni/Si–C–N–(O) system was attributed to (i) the stabilizing effect of carbosilane bonds, which prohibit the formation of macropores during thermolysis; (ii) the reduced barrier for heterogeneous pore nucleation as a result of in situ created nickel nanoparticles; and (iii) the reduced viscous flow of the pores due to the presence of nickel nanoparticles and turbostratic carbon. The formation of turbostratic carbon is due to the reactions catalyzed by nickel nanoparticles that result in graphene stacking as inferred from the STA–MS studies.

Item Type: Article
Erschienen: 2011
Creators: Seifollahi Bazarjani, Mahdi and Kleebe, Hans-Joachim and Müller, Mathis M. and Fasel, Claudia and Baghaie Yazdi, Mehrdad and Gurlo, Aleksander and Riedel, Ralf
Title: Nanoporous Silicon Oxycarbonitride Ceramics Derived from Polysilazanes In situ Modified with Nickel Nanoparticles
Language: English
Abstract:

Ni–polysilazane precursors were synthesized from polysilazane and trans- [bis(2-aminoetanol-N,O)diacetato-nickel(II)]. The Ni–polysilazane precursors are superparamagnetic indicating formation of nanosized nickel particles (2−3 nm) confirmed by HRTEM as well. The as-obtained Ni–polysilazane precursors were thermolized at 700 °C and transformed to ceramic nanocomposites, manifesting a nanoporous structure, revealing a BET surface area of 215 m2 g–1, a micropore surface area of 205 m2 g–1, and a micropore volume of 0.113 cm3 g–1. Although Si–C–N–(O) ceramics derived from the native polysilazane are nonporous, the pronounced development of porosity in the Ni/Si–C–N–(O) system was attributed to (i) the stabilizing effect of carbosilane bonds, which prohibit the formation of macropores during thermolysis; (ii) the reduced barrier for heterogeneous pore nucleation as a result of in situ created nickel nanoparticles; and (iii) the reduced viscous flow of the pores due to the presence of nickel nanoparticles and turbostratic carbon. The formation of turbostratic carbon is due to the reactions catalyzed by nickel nanoparticles that result in graphene stacking as inferred from the STA–MS studies.

Journal or Publication Title: Chemistry of Materials
Volume: 23
Number: 18
Publisher: ACS
Uncontrolled Keywords: micropores, polymer-derived ceramics, polysilazane, nanocomposite, superparamagnetic, graphene stacking, nanosized nickel
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
Date Deposited: 04 Apr 2012 08:10
Official URL: http://dx.doi.org/10.1021/cm200589n
Identification Number: doi:10.1021/cm200589n
Funders: This work has been performed within the framework of the project “Thermoresistant ceramic membrane with integrated gas sensor for high temperature separation and detection of hydrogen and carbon monoxide” of the priority program “Adapting surfaces for hig, Fonds der Chemischen Industrie, Frankfurt, Germany: financial support, Alexander-von-Humboldt Foundation: financial support
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