The present invention provides a method for generating methane from a carbonaceous feedstock with simultaneous in situ sequestration of carbon dioxide to afford a biogas comprising at least 85 percent by volume methane, the method comprising anaerobically incubating a particulate additive in contact with a carbonaceous feedstock in a neutral or alkaline aqueous culture medium containing a culture of methanogenic consortia and collecting methane generated therefrom. The additive comprises at least one material selected from a biochar, an ash produced by gasification or combustion of a carbonaceous material, a black carbon soil, and a Terra Preta soil.