氧合物
甲烷
催化作用
化学
单体
选择性
部分氧化
甲烷厌氧氧化
电子顺磁共振
多相催化
X射线光电子能谱
烷烃
化学工程
无机化学
光化学
有机化学
聚合物
工程类
物理
核磁共振
作者
Zhenghan Fang,Meng‐Yuan Huang,Bing Liu,Jie Chen,Feng Jiang,Yuebing Xu,Xiaohao Liu
出处
期刊:Chemcatchem
[Wiley]
日期:2022-04-29
卷期号:14 (13)
被引量:4
标识
DOI:10.1002/cctc.202200218
摘要
Abstract Direct oxidation of methane to value‐added products under mild conditions remains a grand challenge due to the problem of selective CH 4 activation. Here we report a Fe‐MOR‐F catalyst prepared via freeze‐drying method, indicating excellent catalytic performance for the direct partial oxidation of methane using H 2 O 2 under mild conditions. Various characterizations including XRD, NH 3 ‐TPD, H 2 ‐TPR, UV‐Vis, XPS, and EPR studies revealed that Fe‐MOR‐F catalyst possesses more highly dispersed monomeric and dimeric iron species, which is strongly correlated to its high catalytic activity for direct methane oxidation. The DFT calculations indicate the highly dispersed monomeric and dimeric iron species can effectively homogenize H 2 O 2 into active hydroxyl groups, while iron clusters can decompose H 2 O 2 into inactive O 2 . The EPR experiments show more ⋅OH was generated on Fe‐MOR‐F catalyst, which is in line with DFT calculation results. These structural characteristics endow Fe‐MOR‐F catalyst with superior catalytic performance for direct methane oxidation in terms of oxygenates yield (9.8 mol kg cat −1 h −1 ) and selectivity (91.8 %) at 80 °C. This work not only highlights the excellent catalytic performance of methane activation on the highly dispersed monomeric and dimeric iron species, but also promotes the potential application by freeze‐drying method for the preparation of the highly dispersed active species.
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