Citation: XIA Long-Fei, JIANG Zhi, SHANGGUAN Wen-Feng, GU Shun-Chao, HIRANO Shinichi. Influence of Oxidation State of Nickel Supported on TiO2 on Gas-Phase Hydrogenation of Acetonitrile[J]. Acta Physico-Chimica Sinica, ;2015, 31(5): 941-947. doi: 10.3866/PKU.WHXB201503051
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Nickel catalysts supported on TiO2 were prepared using an impregnation method. Changes in the reduction temperature from 200 to 400 ℃ resulted in dispersion of nickel with different oxidation states on TiO2. The gas-phase hydrogenation of acetonitrile was found to be influenced by the nickel oxidation state. Nickel reduced at 300 ℃ gave the highest acetonitrile conversion ratio, i.e., about 100%, when the reaction temperature was 100 ℃. The product yields depend on the amount of acidic sites on Ni/TiO2 catalysts; this can be influenced not only by the TiO2 support, but also by the properties of the supported nickel nanoparticles. The triethylamine yield increased to a maximum (from 34% to about 48%) with increasing reduction temperature; this corresponded to the gradual appearance of Ni0 in Ni/TiO2 and a decrease in the intrinsic acidity of the Ni/TiO2 catalyst. Triethylamine was the initial product in the hydrogenation of acetonitrile with Ni/TiO2. The oxidation state of nickel influenced not only the conversion of acetonitrile but also desorption of the final products. Amechanism for the first step in this reaction is proposed.
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Keywords:
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Gas-phase hydrogenation of acetonitrile
, - Impregnation method,
- TiO2,
- Ni,
- Amine
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