Water-participated mild oxidation of ethane to acetaldehyde

Li，Bin1,2; Mu，Jiali1; Long，Guifa3; Song，Xiangen1; Huang，Ende1,2; Liu，Siyue1,2; Wei，Yao4; Sun，Fanfei4; Feng，Siquan1; Yuan，Qiao1,2; Cai，Yutong1,2; Song，Jian1,2; Dong，Wenrui5,6; Zhang，Weiqing5; Yang，Xueming5,7; Yan，Li1; Ding，Yunjie1,8

2024-12-01

10.1038/s41467-024-46884-7

Nature Communications   影响因子和分区

2041-1723

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 oxygenates on a Rh/AC-SNI catalyst under a mild condition, which delivers a turnover frequency as high as 158.5 h. 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.

SCI

英语

其他

2-s2.0-85188456248

Scopus

1.Dalian National Laboratory for Clean Energy,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,China
2.University of Chinese Academy of Sciences,Beijing,China
3.Guangxi Key Laboratory of Chemistry and Engineering of Forest Products,School of Chemistry and Chemical Engineering,Guangxi Minzu University,Nanning,China
4.Shanghai Synchrotron Radiation Facility,Shanghai Advanced Research Institute,Chinese Academy of Sciences,Shanghai,China
5.State Key Laboratory of Molecular Reaction Dynamics,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,China
6.Hefei National Laboratory,Hefei,China
7.Department of Chemistry,Southern University of Science and Technology,Shenzhen,China
8.State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,China

Li，Bin,Mu，Jiali,Long，Guifa,et al. Water-participated mild oxidation of ethane to acetaldehyde[J]. Nature Communications,2024,15(1).

Li，Bin.,Mu，Jiali.,Long，Guifa.,Song，Xiangen.,Huang，Ende.,...&Ding，Yunjie.(2024).Water-participated mild oxidation of ethane to acetaldehyde.Nature Communications,15(1).

Li，Bin,et al."Water-participated mild oxidation of ethane to acetaldehyde".Nature Communications 15.1(2024).