Water-participated mild oxidation of ethane to acetaldehyde

Bin Li, Jiali Mu, Guifa Long, Xiangen Song (), Ende Huang, Siyue Liu, Yao Wei, Fanfei Sun, Siquan Feng, Qiao Yuan, Yutong Cai, Jian Song, Wenrui Dong, Weiqing Zhang, Xueming Yang (), Li Yan and Yunjie Ding ()
Additional contact information
Bin Li: Chinese Academy of Sciences
Jiali Mu: Chinese Academy of Sciences
Guifa Long: Guangxi Minzu University
Xiangen Song: Chinese Academy of Sciences
Ende Huang: Chinese Academy of Sciences
Siyue Liu: Chinese Academy of Sciences
Yao Wei: Chinese Academy of Sciences
Fanfei Sun: Chinese Academy of Sciences
Siquan Feng: Chinese Academy of Sciences
Qiao Yuan: Chinese Academy of Sciences
Yutong Cai: Chinese Academy of Sciences
Jian Song: Chinese Academy of Sciences
Wenrui Dong: Chinese Academy of Sciences
Weiqing Zhang: Chinese Academy of Sciences
Xueming Yang: Chinese Academy of Sciences
Li Yan: Chinese Academy of Sciences
Yunjie Ding: Chinese Academy of Sciences

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-46884-7

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