Water-participated mild oxidation of ethane to acetaldehyde

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 C 2 oxygenates on a Rh 1 /AC-SNI catalyst under a mild condition, which...

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Bibliographic Details
Published in:Nature communications 2024-03, Vol.15 (1), p.2555-2555, Article 2555
Main 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
Format: Article
Language:English
Subjects:
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Acetaldehyde
Alkanes
Catalysts
Density functional theory
Direct conversion
Ethane
Ethanol
Free radicals
Humanities and Social Sciences
Hydroxyl radicals
Ionization
multidisciplinary
Natural gas
Oxidation
Oxygen
Science
Science (multidisciplinary)
Single atom catalysts
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Summary: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 C 2 oxygenates on a Rh 1 /AC-SNI catalyst under a mild condition, which delivers a turnover frequency as high as 158.5 h −1 . 18 O 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.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-024-46884-7