On the catalytic activity of Co3O4 in low-temperature CO oxidation

On the catalytic activity of Co3O4 in low-temperature CO oxidation
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DOI:
10.1006/jcat.2002.3738
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发表时间:
2002-10-25
影响因子:
7.3
通讯作者:
Langer, V
Langer, V
中科院分区:
化学1区
文献类型:
--
作者:
Jansson, J;Palmqvist, AEC;Langer, V

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用流动反应器实验、原位光谱和结构分析方法研究了CO在Co3O4上的常温氧化反应。催化剂在反应过程中失活。失活速率随CO或CO2气相浓度的增加而增加,随O2浓度的增加或温度的升高而减小。在10%O-2/Ar中再生比单独在Ar中再生更有效。TPO实验表明,失活催化剂上存在碳酸盐和表面碳。然而,这些物种中没有一个与催化剂的失活有关。原位傅里叶变换红外光谱显示表面存在碳酸盐、羰基和氧物种。用原位X射线衍射仪、原位XANES、XPS和流动床实验研究了催化剂结构和氧化状态的变化。催化剂失活的一个可能解释是表面重建阻碍了反应的氧化还原循环。(C)2002年埃尔塞维尔科学公司(美国)。
Oxidation of CO over Co3O4 at ambient temperature was studied with flow reactor experiments, and in-situ spectroscopic and structural methods. The catalyst deactivates during the reaction. The rate of deactivation increased with increasing CO or CO2 gas-phase concentration but decreased with increased 02 concentration or increased temperature. Regeneration of the catalyst in 10% O-2/Ar was more efficient than regeneration in Ar alone. The presence of carbonates and surface carbon on the deactivated catalyst was concluded from TPO experiments. None of these species could, however, be correlated with the deactivation of the catalyst. In-situ FTIR showed the presence of surface carbonates, carbonyl, and oxygen species. The change in structure and oxidation state of the catalyst was studied by in-situ XRD, in-situ XANES, XPS, and flow reactor experiments. One possible explanation for the deactivation of the catalyst is a surface reconstruction hindering the redox cycle of the reaction. (C) 2002 Elsevier Science (USA).