Publications by authors named "Shotaro Tada"

Interest is growing in transition metal-free compounds for small molecule activation and catalysis. We discuss the opportunities arising from synthesizing sodium-doped amorphous silicon-boron-nitride (Na-doped a-SiBN). Na cations and 3-fold coordinated B moieties were incorporated into an amorphous silicon nitride network via chemical modification of a polysilazane followed by pyrolysis in ammonia (NH) at 1000 °C.

View Article and Find Full Text PDF

Herein, nanocomposites made of Ni nanoparticles distributed in an amorphous silicon nitride (Ni/a-SiN) matrix, on the one hand, and within an amorphous silicon dioxide (Ni/a-SiO) matrix, on the other hand, were synthesized from the same Ni-modified polysilazane precursor. In both compounds, the Ni/Si atomic ratio (0.06-0.

View Article and Find Full Text PDF
Article Synopsis
  • The study explores how nickel (Ni) nanocrystallites are formed during the creation of amorphous silicon nitride at low temperatures (400 °C), using perhydropolysilazane (PHPS) and nickel chloride (NiCl) as key materials.
  • Nickel chloride acts as a catalyst to initiate reactions that combine silicon and nitrogen components in PHPS, ultimately creating a nanocomposite by forming silylamino groups and coordinating them with Ni(II) ions.
  • During pyrolysis, a nucleophilic reaction forms Ni-N bonds, leading to Ni nanocrystallite growth below 300 °C, which is enhanced by hydrogen-rich conditions resulting from the prior reactions, culminating in a strong SiN
View Article and Find Full Text PDF

This work highlights the first demonstration of a low-temperature in situ formation of Co nanocrystallites embedded within an amorphous silicon nitride matrix through careful control of the chemistry behind material design using perhydropolysilazane (PHPS) as a Si3N4 precursor further coordinated with CoCl2 and ammonia as a pyrolysis atmosphere. The Co nucleation was allowed to proceed at temperatures as low as 400 °C via thermal decomposition of Co2N pre-formed in situ by the reaction of CoCl2 with the Si centers of PHPS at the early stage of pyrolysis (220-350 °C).

View Article and Find Full Text PDF

This paper reports on a unique reversible reducing and oxidizing (redox) property of Co(III) in Co-doped amorphous SiO/γ-AlO composites. The Fenton reaction during the HO-catalyzed sol-gel synthesis utilized in this study lead to the partial formation of Co(III) in addition to Co(II) within the composites. High-resolution transmission electron microscopy (HRTEM) and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) analyses for the composite powder sample with a composition of Al:Si:Co = 85:10:5 showed the amorphous state of the Co-doped SiO that modified γ-AlO nanocrystalline surfaces.

View Article and Find Full Text PDF