Abstract
Methane is a potent greenhouse gas, and its rapid conversion at low concentrations under ambient conditions is a challenging process where combustion is not an option. Herein, we report an electrochemical method to address this problem. It was achieved by applying an oxidation potential to electrochemically activate methane followed by conducting an anodic cyclic voltammogram to fully oxidize activated methane to carbon dioxide on platinized Pt mesh (Pt/Pt) and carbon paper (Pt/CP). This "dynamic potential" oxidation approach enabled methane conversion with low energy consumption, thanks to the low activation potential. Effects of various experimental conditions (applied potential, reaction time, and methane concentration) were investigated. Pure methane and methane/nitrogen gas mixtures containing a series of low concentrations of methane were tested. It was found that methane conversion is independent of its concentration on both Pt/Pt and Pt/CP. Compared to Pt/Pt electrocatalysis, Pt/CP displayed approximately 10 times higher catalytic activity, which can be attributed to the stronger binding of intermediate CO* to Pt, leading to easier CO* activation in the presence of a carbon substrate. Carbon dioxide was the only compound detected during the electro-oxidation phase for Pt/Pt, while for Pt/CP, carbon dioxide and a small amount of formic acid (after 15 h reaction) were observed. Electrocatalytic conversion of methane to carbon dioxide on Pt/CP using 0.5% methane was measured, giving a methane conversion rate of 7.5 × 10(-8) mol L(-1) s(-1) m(-2), while the methane conversion rate on Pt/Pt with 1% methane was only 8.3 × 10(-9) mol L(-1) s(-1) m(-2).