Polydopamine‐Mediated Contact‐Electro‐Catalysis for Efficient Partial Oxidation of Methane

Abstract The direct conversion and efficient utilization of methane pose a critical scientific challenge. Indirect activation via reactive oxygen species (ROS) offers a high probability of contact with methane and conversion efficiency under mild conditions. However, reported product yields are suboptimal due to challenges in activating oxygen and facilitating mass transfer in suspension systems. We propose the use of contact‐electro‐catalysis (CEC), employing polydopamine (PDA) as a catalyst that undergoes electron transfer with oxygen under ultrasound, generating ROS that drives the partial oxidation of methane (POM). Corresponding experimental results indicate that CH 3 OH and most HCHO are produced directly from CH 4 . Furthermore, through in situ characterizations, we have shown that light pretreatment of the catalysts in an oxygenated atmosphere facilitates the forming of more C=O functional groups with strong electron‐withdrawing properties, thereby significantly enhancing overall product yields, particularly for CH 3 OH. Within two hours, product yields reach 1.5 mmol g cat −1 for HCHO and 0.9 mmol g cat −1 for CH 3 OH. This work introduces a novel approach for efficient POM, while highlighting the distinctive catalytic properties of PDA.

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Publication Details

Journal
Angewandte Chemie
Published
2024-10-17
DOI
https://doi.org/10.1002/ange.202413343
Primary Topic
Polymer Surface Interaction Studies
Type
article
Field-Weighted Citation Impact
0.00

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article

Polydopamine‐Mediated Contact‐Electro‐Catalysis for Efficient Partial Oxidation of Methane

Chuanqi Zhang, Taikang Jia, Wenjing Wang, Wenzhong Wang et al.
Angewandte Chemie
Polymer Surface Interaction Studies
article

Polydopamine‐Mediated Contact‐Electro‐Catalysis for Efficient Partial Oxidation of Methane

Chuanqi Zhang, Taikang Jia, Wenjing Wang, Wenzhong Wang, Ling Zhang
article en

Abstract

Abstract The direct conversion and efficient utilization of methane pose a critical scientific challenge. Indirect activation via reactive oxygen species (ROS) offers a high probability of contact with methane and conversion efficiency under mild conditions. However, reported product yields are suboptimal due to challenges in activating oxygen and facilitating mass transfer in suspension systems. We propose the use of contact‐electro‐catalysis (CEC), employing polydopamine (PDA) as a catalyst that undergoes electron transfer with oxygen under ultrasound, generating ROS that drives the partial oxidation of methane (POM). Corresponding experimental results indicate that CH 3 OH and most HCHO are produced directly from CH 4 . Furthermore, through in situ characterizations, we have shown that light pretreatment of the catalysts in an oxygenated atmosphere facilitates the forming of more C=O functional groups with strong electron‐withdrawing properties, thereby significantly enhancing overall product yields, particularly for CH 3 OH. Within two hours, product yields reach 1.5 mmol g cat −1 for HCHO and 0.9 mmol g cat −1 for CH 3 OH. This work introduces a novel approach for efficient POM, while highlighting the distinctive catalytic properties of PDA.

Angewandte ChemieVol. 137(1)
Chinese Academy of Sciences (CN), Shanghai Institute of Ceramics (CN), University of Chinese Academy of Sciences (CN)
National Natural Science Foundation of China
Openalex Percentile: Top 82%
Polymer Surface Interaction Studies
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