Methanol-linked synergy between aerobic methanotrophs and denitrifiers enhanced nitrate removal efficiency in a membrane biofilm reactor under a low O2:CH4 ratio

Abstract

Nitrate removal efficiency of aerobic methane oxidation coupled with denitrification (AME-D) process was elevated by enhancing the methanol-linked synergy in a membrane biofilm reactor (MBfR) under a low O₂:CH₄ ratio. After 140 days' enrichment, the nitrate removal rate increased significantly from 3 to 4 mg-N L^-1 d^-1 to 22.09 ± 1.21 mg-N L^-1 d^-1 and the indicator, mol CH₄ consumed/mol reduced NO₃^--N (C/N ratio), decreased to 1.79 which was very close to the theoretical minimum value (1.27-1.39). The increased nitrate removal efficiency was largely related to the enhanced relationship between aerobic methanotrophs and methanol-utilizing denitrifiers. Type I methanotrophs and some denitrifiers, especially those potential methanol-utilizing denitrifiers from Methylobacillus, Methylotenera, Methylophilus and Methyloversatilis, were abundant in the MBfR sludge. Aerobic methanotrophs and potential methanol-utilizing denitrifiers were closely associated in many globular aggregates (5-10 μm diameter) in the MBfR sludge, which may have promoted the denitrifiers to capture methanol released by methanotrophs efficiently. If we assume methanol is the only cross-feeding intermediate in the MBfR, about 38-60% of the CH₄ supplied would be converted to methanol and secreted rather than continuing to be oxidized. At least 63% of this secreted methanol should be utilized for denitrification instead of being oxidized by oxygen in the MBfR. These findings suggest that the nitrate removal efficiency of the AME-D process could be significantly improved.

Keywords: Aerobic methane oxidation coupled to denitrification; Membrane biofilm reactor; Methanol-linked synergy; Nitrate removal efficiency; O(2):CH(4) ratio.