Temperature and time dependence of the water inhibition effect on supported palladium catalyst for methane combustion

Temperature and time dependence of the water inhibition effect on supported palladium catalyst for methane combustion
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DOI:
10.1016/s0926-860x(01)00558-0
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发表时间:
2001-08-01
影响因子:
5.5
通讯作者:
Pfefferle, L
Pfefferle, L
中科院分区:
化学2区
文献类型:
--
作者:
Ciuparu, D;Katsikis, N;Pfefferle, L

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在脉冲流和连续流实验条件下,定性研究了不同反应温度下氧化锆负载钯催化剂上甲烷燃烧过程中水吸附/解吸平衡的时间常数。水对甲烷氧化的抑制作用很大程度上取决于水的吸附/解吸平衡的时间常数,而时间常数又是温度的重要函数。在脉冲实验中,在低于723 K的温度下,发现水抑制作用是重要的,这与先前报道的结果一致,也与其他作者报道的结果一致。这也与测量的二氧化碳和水峰值之间的解吸时间差距消失的温度相吻合。发现对水浓度变化的反应是缓慢的,因此在低温下不平衡。但在连续流动条件下,水中毒的重要原因是高温下的再吸附。(C) 2001 Elsevier Science B.V.版权所有
The time constant for equilibration of water adsorption/desorption during methane combustion over zirconia supported palladium catalyst was qualitatively studied at different reaction temperatures under both pulsed and continuous flow experiments. Water inhibition of methane oxidation was found to depend strongly on the time constant for equilibration of the adsorption/desorption of water, which, in turn, is a strong function of temperature. In pulsed experiments, at temperatures below 723 K the water inhibition effect was found to be important, in agreement with previously reported results and consistent with results reported by other authors. This also coincides with the temperature at which the desorption time gap between the measured CO2 and water peaks disappears. Response to changes in water concentration was found to be slow, thus not equilibrated at low temperatures. However, under continuous flow water poisoning is important to higher temperatures due to readsorption. (C) 2001 Elsevier Science B.V. All rights reserved.