<p>The electrochemical oxidative coupling of methane (EOCM), integrated with CO<sub>2</sub> electrolysis enabled by high-temperature electrolysis technology, represents a promising pathway for methane utilization and carbon neutrality. However, progress in methane activation remains hindered by low C<sub>2</sub> product selectivity and limited reaction activity, primarily due to the lack of efficient and stable catalysts and rational design strategies. A critical focus of current research is the development of catalysts capable of stabilizing reactive oxygen species to facilitate C-H bond activation and subsequent C-C bond formation. Herein, an easily fabricated composite electrode consisting of perovskite La<sub>0.6</sub>Sr<sub>0.4</sub>MnO<sub>3-<i>γ</i></sub> and Ce-Mn-W materials with (Ce<sub>0.90</sub>Gd<sub>0.10</sub>)O<sub>1.95</sub> as the support was developed, demonstrating efficient activate methane activation. Combined theoretical and experimental investigations reveal that the designed composite electrode stabilizes active oxygen species during the oxygen evolution reaction (OER) while exhibiting superior methane adsorption capability. This design, leveraging oxygen species engineering and interfacial synergy, significantly enhances electrochemical methane coupling efficiency, establishing a strategic framework for advancing high-performance catalyst development.</p>

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Efficient electrochemical methane coupling enabled by stabilized oxygen species during oxygen evolution in a solid oxide electrolyzer integrated with CO2 electrolysis

  • Chunsong Li,
  • Lingxiu Li,
  • Fan Bai,
  • Hui Gao,
  • Yunzhu Liu,
  • Zhongyuan Liu,
  • Shixian Zhang,
  • Yuhui Jin,
  • Wenxi Ji,
  • Longgui Zhang,
  • Yifeng Li,
  • Bo Yu

摘要

The electrochemical oxidative coupling of methane (EOCM), integrated with CO2 electrolysis enabled by high-temperature electrolysis technology, represents a promising pathway for methane utilization and carbon neutrality. However, progress in methane activation remains hindered by low C2 product selectivity and limited reaction activity, primarily due to the lack of efficient and stable catalysts and rational design strategies. A critical focus of current research is the development of catalysts capable of stabilizing reactive oxygen species to facilitate C-H bond activation and subsequent C-C bond formation. Herein, an easily fabricated composite electrode consisting of perovskite La0.6Sr0.4MnO3-γ and Ce-Mn-W materials with (Ce0.90Gd0.10)O1.95 as the support was developed, demonstrating efficient activate methane activation. Combined theoretical and experimental investigations reveal that the designed composite electrode stabilizes active oxygen species during the oxygen evolution reaction (OER) while exhibiting superior methane adsorption capability. This design, leveraging oxygen species engineering and interfacial synergy, significantly enhances electrochemical methane coupling efficiency, establishing a strategic framework for advancing high-performance catalyst development.