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https://hdl.handle.net/2440/139115
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Type: | Journal article |
Title: | Mild Methane Electrochemical Oxidation Boosted via Plasma Pre-Activation |
Author: | Sun, X. Wang, P. Davey, K. Zheng, Y. Qiao, S.-Z. |
Citation: | Small, 2023; 19(45):2303428-1-2303428-7 |
Publisher: | Wiley-VCH GmbH |
Issue Date: | 2023 |
ISSN: | 1613-6810 1613-6829 |
Statement of Responsibility: | Xiaogang Sun, Pengtang Wang, Kenneth Davey, Yao Zheng, and Shi-Zhang Qiao |
Abstract: | Obtaining partial methane oxidation reaction (MOR) with various oxygenates via a mild electrochemical method is practically difficult because of activation of stable C─H bond and consequent reaction pathway regulation. Here, a real-time tandem MOR with cascaded plasma and electrocatalysis to activate and convert the methane (CH₄) synergistically is reported for the first time. Boosted CH₄ conversion is demonstrated toward value-added products including, alcohols, carboxylates, and ketone via use of commercial Pd-based electrocatalysts. Compared with hash industrial processes, a mild condition, that is, anode potential < 1.0 V versus RHE (reversible hydrogen electrode) is used that mitigates overoxidation of oxygenates and obviates competing reaction(s). One evidence that Pd(II) sites and surface adsorbed hydroxyls are important in facilitating activated-CH₄ species conversion, and establish a reaction mechanism for conversion(s) that involves coupling reactions between adsorbed hydroxyls, carbon monoxide and C₁/C₂ alkyls. One conclude that pre-activation is important in boosting electrochemical partial MOR under mild conditions and will be of benefit in the development of sustainable CH₄ |
Keywords: | dielectric barrier discharges plasma electrochemical tandem palladium electrocatalysis partial methane oxidation pre-activation |
Description: | Published online: July 11, 2023 |
Rights: | © 2023 Wiley-VCH GmbH |
DOI: | 10.1002/smll.202303428 |
Grant ID: | http://purl.org/au-research/grants/arc/FL170100154 http://purl.org/au-research/grants/arc/LP210301397 http://purl.org/au-research/grants/arc/DP220102596 http://purl.org/au-research/grants/arc/DP190103472 http://purl.org/au-research/grants/arc/FT200100062 |
Published version: | http://dx.doi.org/10.1002/smll.202303428 |
Appears in Collections: | Chemical Engineering publications |
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