氧合物
化学
电催化剂
电化学
阳极
吸附
部分氧化
甲烷
光化学
催化作用
无机化学
电极
有机化学
物理化学
作者
Xiaogang Sun,Pengtang Wang,Kenneth Davey,Yao Zheng,Shi Zhang Qiao
出处
期刊:Small
[Wiley]
日期:2023-07-11
卷期号:19 (45)
被引量:7
标识
DOI:10.1002/smll.202303428
摘要
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 conversion technology.
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