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A study of FeNx/C catalysts for the selective oxidation of unsaturated alcohols by molecular oxygen

Journal 2018 · IF 6.759 · 发表于 2018 年 9 月 7 日
作者: Jinping Zhang,Shinichi Nagamatsu,Junmou Du,Chaoli Tong,Huihuang Fang,Dehui Deng,Xi Liu,Kiyotaka Asakura,Youzhu Yuan
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摘要

Transition-metal nitrides can exhibit catalytic performance comparable to that of noble metal catalysts in many reactions. However, investigations on the correlation of catalyst structure, performance, and stability are still highly demanded. Here, a series of metal nitrides were prepared and evaluated for the selective oxidation of alcohols by molecular oxygen. Among them, FeN x /C- T catalysts ( T represents the pyrolysis temperature) display above 95% selectivity to the corresponding aldehydes in the selective oxidation of unsaturated alcohols. The optimized FeN x /C-900 catalyst gives the highest TOF of 7.0 h −1 for the conversion of 5-hydroxymethylfurfural to 2,5-diformylfuran. A combination of characterizations and experiments suggests that Fe N 4 species are the main active sites. In addition, we investigate the reasons for the catalyst deactivation and provide an effective approach to regenerating the catalysts. The results indicate that the deactivated catalysts can be regenerated by heat treatment under NH 3 /N 2 after each run. Based on these studies, a plausible reaction mechanism over the FeN x /C catalysts is proposed.

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