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Enhanced methane chlorination via RuO2-gas convection electrode with in-situ generated dynamical three-phase
Ziyan Fu1,2,3, Yunpeng Zhou1,2,3, Ziming Cao1,2,3
1State Key Laboratory of Soil Pollution Control and Safety, College of Environmental and Resource Sciences, Zhejiang University, Hangzhou, PR China.
Abstract:
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.
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