A hydrogen utilizing exoelectrogenic bacterium (Geobacter sulfurreducens) was compared to both a nonhydrogen oxidizer (Geobacter metallireducens) and a mixed consortium in order to compare the hydrogen production rates and hydrogen recoveries of pure and mixed cultures in microbial electrolysis cells (MECs). At an applied voltage of 0.7 V, both G. sulfurreducens and the mixed culture generated similar current densities (ca. 160 A/m 3 ), resulting in hydrogen production rates of ca. 1.9 m 3 H 2 /m 3 /day, whereas G. metallireducens exhibited lower current densities and production rates of 110 ؎ 7 A/m 3 and 1.3 ؎ 0.1 m 3 H 2 /m 3 /day, respectively. Before methane was detected in the mixed-culture MEC, the mixed consortium achieved the highest overall energy recovery (relative to both electricity and substrate energy inputs) of 82% ؎ 8% compared to G. sulfurreducens (77% ؎ 2%) and G. metallireducens (78% ؎ 5%), due to the higher coulombic efficiency of the mixed consortium. At an applied voltage of 0.4 V, methane production increased in the mixed-culture MEC and, as a result, the hydrogen recovery decreased and the overall energy recovery dropped to 38% ؎ 16% compared to 80% ؎ 5% for G. sulfurreducens and 76% ؎ 0% for G. metallireducens. Internal hydrogen recycling was confirmed since the mixed culture generated a stable current density of 31 ؎ 0 A/m 3 when fed hydrogen gas, whereas G. sulfurreducens exhibited a steady decrease in current production. Community analysis suggested that G. sulfurreducens was predominant in the mixed-culture MEC (72% of clones) despite its relative absence in the mixed-culture inoculum obtained from a microbial fuel cell reactor (2% of clones). These results demonstrate that Geobacter species are capable of obtaining similar hydrogen production rates and energy recoveries as mixed cultures in an MEC and that high coulombic efficiencies in mixed culture MECs can be attributed in part to the recycling of hydrogen into current.Electrohydrogenesis is an efficient method for generating hydrogen gas from organic matter in reactors known as microbial electrolysis cells (MECs) (17,18,26). MECs differ from air-cathode microbial fuel cells (MFCs) in that the cathode remains anaerobic, and voltage is added in order to generate hydrogen at the cathode. Under the biological conditions in MECs, hydrogen evolution is not a thermodynamically favorable reaction. However, combining the hydrogen formation reaction potential of Ϫ0.41 V at the cathode (E CAT ) with the anode potential (E AN ) typically obtained in MFCs with an E AN of Ϫ0.30 V (1 g of acetate/liter) results in a minimum required voltage of only 0.14 V. Applied voltages (E AP ) of 0.2 V (0.45 kWh/m 3 H 2 ) or larger are needed in practice to produce measurable quantities of hydrogen, but this input is substantially less than the average of 2.3 V (5.1 kWh/m 3 H 2 ) required for water electrolysis (13).Recent improvements in designs and materials have substantially improved hydrogen yields, production rates, and energy recoveries (3,18,(27)(2...