Facile synthesis of N-doped carbon supported iron species for highly efficient methane conversion with H2O2 at ambient temperature

Abstract

A series of N-doped carbon supported highly-dispersed Fe catalysts are prepared, and their catalytic performances for the direct conversion of methane to CH3OH and HCOOH with by-product CO2 are tested at ambient temperature. The nitrogen doping can greatly improve the metal-support interaction, and anchor the Fe species on the support. The catalytic activity of the catalyst is further enhanced by the modification of hydroxylamine hydrochloride. The optimized 2.5 wt%Fe/NC−HH catalyst shows 475 μmol/gcat for CH3OH and 832 μmol/gcat for HCOOH after 1 h reaction. The effect of the type of nitrogen species on the catalytic performance of the catalyst has been studied in detail. In addition, other transition metals (Ni, Co, Cu and Mn) as active centers have been also studied, and none of them is effective for the conversion of methane. Additionally, it is found that the methane conversion over the prepared catalysts proceed via a radical mechanism.