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Methane oxidation with low O-2/CH4 ratios in the present of water: Combustion or reforming

机译:在水中存在低O-2 / CH4比例的甲烷氧化:燃烧或重整

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This paper investigates the reaction of methane over copper and cobalt catalysts under oxygen-deficient conditions with added water. A fixed-bed reactor, TPD analysis, in situ DRIFTS study, and temperature detection were used to test the activity of the methane reaction, water adsorption on the metal surface, OH group behavior, and the endothermic and exothermic processes of the reaction. The results show that the inhibitory effect of water mainly occurs at a low temperature and methane conversion decreases when water is introduced into the feed. Water easily adsorbs on metal clusters and forms OH groups at low temperatures. Copper tends to adsorb more water than cobalt and shows a stronger inhibitory effect. The DRIFTS spectra of the Cu catalyst show strong OH peaks during the reaction, of which the magnitudes increase with the water pressure. When the reaction temperature rises (750 degrees C), water begins to serve as an oxidant and participates in the reforming reaction. Both catalysts show a transition process between the oxidation and reforming reactions as the temperature increases. Co displays a better catalytic performance in the reforming reaction. Oxidation precedes reforming; water does not participate in the reaction if the oxygen is not fully consumed. (C) 2016 Elsevier Ltd. All rights reserved.
机译:本文研究了缺氧条件下加水在铜和钴催化剂上甲烷的反应。使用固定床反应器,TPD分析,原位DRIFTS研究和温度检测来测试甲烷反应的活性,金属表面的水吸附,OH基团行为以及反应的吸热和放热过程。结果表明,水的抑制作用主要发生在低温下,当将水引入进料中时甲烷转化率降低。水在低温下容易吸附在金属簇上并形成OH基团。铜往往比钴吸收更多的水,并且显示出更强的抑制作用。 Cu催化剂的DRIFTS光谱在反应过程中显示出很强的OH峰,其幅度随水压而增加。当反应温度升高(750℃)时,水开始充当氧化剂并参与重整反应。两种催化剂都随着温度的升高而在氧化和重整反应之间显示出过渡过程。 Co在重整反应中显示出更好的催化性能。氧化先于重整;如果氧气没有完全消耗,则水不会参与反应。 (C)2016 Elsevier Ltd.保留所有权利。

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