AbstractA major cost consideration in the use of anaerobic digestion to convert biomass and waste to utility‐grade gas is the expense of separating CO2from the product gas. Anaerobic digestion has a number of inherent properties that can be exploited to increase the methane content of the gas directly produced by the digester, the most important of which is the high solubility of CO2(40‐60 times that of methane) in water under digestion conditions. The methane enrichment concept examined in this study involved the recirculation of a liquid stream from the digester through a CO2desorption process and the return of the liquid stream back to the digester for absorption of additional CO2produced by the conversion of organic materials. A steady‐state equilibrium model predicted that a digester gas methane content exceeding 94% could be achieved with this scheme using modest recirculation rates provided a desorption process could be designed to achieve a 60+% CO2removal efficiency in the degassing of the liquid recycle stream. Using fixed‐film laboratory digesters operated on synthetic feedstocks, the technique of methane enrichment was tested under pressurized and unpressurized conditions. A 93 + 2% methane gas stream was produced from a volatile‐acid‐fed bench‐scale digester simulating the methanogenic stage of two‐phase digestion under conditions of (1) a pH swing achieved without caustic addition that allowed digestion at pH 7. 5 and air stripping at pH 6. 5‐7. 0, (2) digester pressurization to 30 psig, and (3) a recycle rate of 0. 33 L/L reactor/day. Significant but lower levels of methane enrichment were achieved with the single‐stage digester at the low experimental recycle rate. However, the narrow range among all experiments of CO2desorption efficiencies achieved in air stripping the recycle stream (35‐60% CO2removal) suggests that comparable methane enrichment‐may be achieved with unpressurized single‐stage digestion using greater recycle rates. A materials balance analysis of data from an unpressurized, single‐stage digester employing no chemical addition and using laboratory degassing efficiencies indicated that 94% methane could be produced at recycle rates of less than 1. 4 L/L reactor/day with a m