AbstractA novel binary transition metal oxide (NiFe2O4) nanosphere catalyst with a diameter of 500 nm has been synthesized by the hydrothermal reaction, which can efficiently catalyze the formation of hexagonal boron nitride nanotubes (BNNTs) with high‐yield and large aspect ratio. Based on the temperature dependence of the product phase composition and microstructure, combined with results generated using single‐component catalysts, the BNNTs formation process can be summarized as follows: NiFe2O4 reacts with NH3 to generate Fe0.64Ni0.36, which dissolves to form a liquid‐phase Ni‐Fe alloy at high temperatures, where the B component in the precursor and the N atom formed by the decomposition of NH3 diffuse on the surface of the Ni‐Fe alloy; when the concentration of B and N exceed the saturation threshold, hollow BNNTs containing catalyst at the tips are precipitated. The formation process is dominated by a vapor‐liquid‐solid mechanism with tip‐growth mode, where the synergistic catalytic effect of the Ni‐Fe binary system promotes a high yield of large aspect ratio BNNTs.
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