Suppressing COx in oxidative dehydrogenation of propane with dual-atom catalysts

Oxidative dehydrogenation of propane (ODHP) is a promising route for propylene production, but achieving high selectivity towards propylene while minimizing CO<sub>x</sub> byproducts remains a significant challenge for conventional metal oxide catalysts. Here we propose a solution to this challenge by employing atomically dispersed dual-atom catalysts (M<sub>1</sub>M'<sub>1</sub>-TiO<sub>2</sub> DACs). Ni<sub>1</sub>Fe<sub>1</sub>-TiO<sub>2</sub> DACs exhibit an ultralow CO<sub>x</sub> selectivity of 5.2% at a high propane conversion of 46.1% and 520 °C, with stable performance for over 1000 hours. Mechanistic investigations reveal that these catalysts operate via a cooperative Langmuir-Hinshelwood mechanism, distinct from the Mars-van Krevelen mechanism typical of metal oxides. This cooperative pathway facilitates efficient conversion of propane and oxygen into propylene at the dual-atom interface. The superior selectivity arises from facile olefin desorption from the dual-atom sites and suppressed formation of electrophilic oxygen species, which are preferentially adsorbed on Fe<sub>1</sub> sites rather than oxygen vacancies. This work highlights the potential of dual-atom catalysts for highly selective ODHP and provides insights into their unique catalytic mechanism.

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Publication Details

Journal
Nature Communications
Published
2025-05-19
DOI
https://doi.org/10.1038/s41467-025-59376-z
Citations
10
Primary Topic
Catalysis and Oxidation Reactions
Type
article
Field-Weighted Citation Impact
3.89

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article

Suppressing COx in oxidative dehydrogenation of propane with dual-atom catalysts

Jingnan Wang, Sanjaya D. Senanayake, Yongbin Yao, Wensheng Yan et al.
10 citations
Nature Communications
Catalysis and Oxidation Reactions
3.89
article

Suppressing COx in oxidative dehydrogenation of propane with dual-atom catalysts

Jingnan Wang, Sanjaya D. Senanayake, Yongbin Yao, Wensheng Yan, Fei Lu, Bingbao Mei, Fangli Yuan, Guiyuan Jiang, Lifeng Zhang, Xi Wang, Wenlin Li
article en
10 citations

Abstract

Oxidative dehydrogenation of propane (ODHP) is a promising route for propylene production, but achieving high selectivity towards propylene while minimizing CO<sub>x</sub> byproducts remains a significant challenge for conventional metal oxide catalysts. Here we propose a solution to this challenge by employing atomically dispersed dual-atom catalysts (M<sub>1</sub>M'<sub>1</sub>-TiO<sub>2</sub> DACs). Ni<sub>1</sub>Fe<sub>1</sub>-TiO<sub>2</sub> DACs exhibit an ultralow CO<sub>x</sub> selectivity of 5.2% at a high propane conversion of 46.1% and 520 °C, with stable performance for over 1000 hours. Mechanistic investigations reveal that these catalysts operate via a cooperative Langmuir-Hinshelwood mechanism, distinct from the Mars-van Krevelen mechanism typical of metal oxides. This cooperative pathway facilitates efficient conversion of propane and oxygen into propylene at the dual-atom interface. The superior selectivity arises from facile olefin desorption from the dual-atom sites and suppressed formation of electrophilic oxygen species, which are preferentially adsorbed on Fe<sub>1</sub> sites rather than oxygen vacancies. This work highlights the potential of dual-atom catalysts for highly selective ODHP and provides insights into their unique catalytic mechanism.

Nature CommunicationsVol. 16(1)
University of Science and Technology of China (CN), Chinese Academy of Sciences (CN), Brookhaven National Laboratory (US), China University of Petroleum, Beijing (CN), Beijing Jiaotong University (CN), Shantou University (CN), Ji Hua Laboratory (CN), Shanghai Institute of Applied Physics (CN), Institute of Process Engineering (CN), National Synchrotron Radiation Laboratory (CN), Yangzhou University (CN), Fuzhou University (CN), Taiyuan University of Technology (CN)
U.S. Department of Energy, Salt Science Research Foundation, Chinese Academy of Sciences, National Synchrotron Radiation Laboratory, Office of Science, Fundamental Research Funds for the Central Universities, Beijing Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Basic Energy Sciences, Brookhaven National Laboratory
Openalex Percentile: Top 6%
Catalysis and Oxidation Reactions
3.89
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