Abiotic Methane Production Driven by Ubiquitous Non‐Fenton‐Type Reactive Oxygen Species

Abstract Abiotic CH 4 production driven by Fenton‐type reactive oxygen species (ROS) has been confirmed to be an indispensable component of the atmospheric CH 4 budget. While the chemical reactions independent of Fenton chemistry to ROS are ubiquitous in nature, it remains unknown whether the produced ROS can drive abiotic CH 4 production. Here, we first demonstrated the abiotic CH 4 production at the soil‐water interface under illumination. Leveraging this finding, polymeric carbon nitrides (CN x ) as a typical analogue of natural geobattery material and dimethyl sulfoxide (DMSO) as a natural methyl donor were used to unravel the underlying mechanisms. We revealed that the ROS, photocatalytically produced by CN x , can oxidize DMSO into CH 4 with a high selectivity of 91.5 %. Such an abiotic CH 4 production process was further expanded to various non‐Fenton‐type reaction systems, such as electrocatalysis, pyrocatalysis and sonocatalysis. This work provides insights into the geochemical cycle of abiotic CH 4 , and offers a new route to CH 4 production via integrated energy development.