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- Title
Water-participated mild oxidation of ethane to acetaldehyde.
- Authors
Li, Bin; Mu, Jiali; Long, Guifa; Song, Xiangen; Huang, Ende; Liu, Siyue; Wei, Yao; Sun, Fanfei; Feng, Siquan; Yuan, Qiao; Cai, Yutong; Song, Jian; Dong, Wenrui; Zhang, Weiqing; Yang, Xueming; Yan, Li; Ding, Yunjie
- Abstract
The direct conversion of low alkane such as ethane into high-value-added chemicals has remained a great challenge since the development of natural gas utilization. Herein, we achieve an efficient one-step conversion of ethane to C2 oxygenates on a Rh1/AC-SNI catalyst under a mild condition, which delivers a turnover frequency as high as 158.5 h−1. 18O isotope-GC–MS shows that the formation of ethanol and acetaldehyde follows two distinct pathways, where oxygen and water directly participate in the formation of ethanol and acetaldehyde, respectively. In situ formed intermediate species of oxygen radicals, hydroxyl radicals, vinyl groups, and ethyl groups are captured by laser desorption ionization/time of flight mass spectrometer. Density functional theory calculation shows that the activation barrier of the rate-determining step for acetaldehyde formation is much lower than that of ethanol, leading to the higher selectivity of acetaldehyde in all the products. The direct conversion of low alkane-like ethane into high-value chemicals has posed a significant challenge. Herein, the authors successfully accomplish a one-step conversion of ethane to C2 oxygenates using a Rh single-atom catalyst under mild conditions.
- Subjects
ACETALDEHYDE; ETHANES; VINYL polymers; REACTIVE oxygen species; DENSITY functional theory; HYDROXYL group; ETHYL group
- Publication
Nature Communications, 2024, Vol 15, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-024-46884-7