Nitrogen-doped metal-free carbon catalysts for aerobic oxidation of xanthene

被引:25
|
作者
Fujita, Shin-Ichiro [1 ]
Yamada, Katsuaki [1 ]
Katagiri, Ayaka [1 ]
Watanabe, Hiroyuki [1 ]
Yoshida, Hiroshi [1 ]
Arai, Masahiko [1 ]
机构
[1] Hokkaido Univ, Fac Engn, Div Chem Proc Engn, Sapporo, Hokkaido 0608628, Japan
关键词
Carbon; Nitrogen doping; Oxidation; Xanthene; Xanthone; OXYGEN REDUCTION REACTION; KNOEVENAGEL CONDENSATION; NITRIDE MATERIALS; NANOTUBES;
D O I
10.1016/j.apcata.2014.09.049
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
N-doped carbons were prepared from a commercial activated carbon (AC) by heat treatments in pure NH3, an NH3-air mixture, and NO and these were used for a model reaction of aerobic oxidation of xanthene to xanthone (XO). The catalytic activity of AC for the title reaction was greatly enhanced by N-doping and the enhancement in the activity depended on the N source gasses used. The effectiveness of the three gases for both N-doping and enhancing the activity was in an order of NH3-air > NH3 > NO. The temperature of N-doping also affected the catalyst activity but not so significantly. X-ray photoelectron spectroscopy (XPS) indicated the presence of pyridine-type and pyrrole-fpyridone-type N species. The catalytic activity of N-doped carbon was correlated with the ratio of the amount of pyridine-type N against that of ether-type O species. The structures of the active sites were discussed on the basis of the XPS and reaction results. Metal-free N-doped AC was less active than a commercial Rut AC catalyst but more active than a commercial Pd/AC one. The activity of N-carbon slightly decreased after the first recycling but it remained almost the same during the following two-time recycling. (C) 2014 Elsevier B.V. All rights reserved.
引用
收藏
页码:171 / 175
页数:5
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