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<p>Chloromethane (CH<sub>3</sub>Cl) is a crucial chemical intermediate conventionally synthesized under harsh conditions. Electrocatalytic methane (CH<sub>4</sub>) chlorination enables a sustainable alternative by utilizing abundant CH<sub>4</sub> and chlor-alkali feedstocks under ambient conditions. However, the high stability and low solubility of CH<sub>4</sub> limit CH<sub>3</sub>Cl’s production. To address these issues, we develop a hierarchical system integrating catalyst and electrode designs. RuO<sub>2</sub> catalyst is applied for surface adsorbed chlorine (*Cl) generation and CH<sub>4</sub> activation. We also design a gas convection electrode (GCE), achieving a CH<sub>3</sub>Cl yield of 547.5 ± 33.4 mmol cm<sup>-2</sup> h<sup>-1</sup> and a 19-fold enhancement in faradaic efficiency compared to gas diffusion electrodes. This enhancement is attributed to efficient *Cl production by RuO<sub>2</sub>, coupled with the convection-dominated mass transport and the GCE’s in-situ generation of dynamic three-phase boundaries. Here, we demonstrate an efficient catalyst for electrocatalytic CH<sub>4</sub> chlorination and propose a broadly applicable strategy to enhance reaction efficiency involving less soluble gaseous reactants.</p>

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Enhanced methane chlorination via RuO2-gas convection electrode with in-situ generated dynamical three-phase boundaries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月31日

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  • Ziyan Fu,
  • Yunpeng Zhou,
  • Ziming Cao,
  • Sen Yang,
  • Liu Huang,
  • Zhongbiao Wu,
  • Yunhao Lu,
  • Wei Chen,
  • Xiaole Weng,
  • Zheng Wang,
  • Le Shi

摘要

Chloromethane (CH3Cl) is a crucial chemical intermediate conventionally synthesized under harsh conditions. Electrocatalytic methane (CH4) chlorination enables a sustainable alternative by utilizing abundant CH4 and chlor-alkali feedstocks under ambient conditions. However, the high stability and low solubility of CH4 limit CH3Cl’s production. To address these issues, we develop a hierarchical system integrating catalyst and electrode designs. RuO2 catalyst is applied for surface adsorbed chlorine (*Cl) generation and CH4 activation. We also design a gas convection electrode (GCE), achieving a CH3Cl yield of 547.5 ± 33.4 mmol cm-2 h-1 and a 19-fold enhancement in faradaic efficiency compared to gas diffusion electrodes. This enhancement is attributed to efficient *Cl production by RuO2, coupled with the convection-dominated mass transport and the GCE’s in-situ generation of dynamic three-phase boundaries. Here, we demonstrate an efficient catalyst for electrocatalytic CH4 chlorination and propose a broadly applicable strategy to enhance reaction efficiency involving less soluble gaseous reactants.