A novel electrochemical oxidation-methanogenesis system for simultaneously degrading antibiotics and reducing CO_2 to CH_4 with low energy costs

摘要

A novel electrochemical oxidation-methanogenesis (EO-M) system was proposed for the first time to simultaneously achieve antibiotic degradation and a bioelectrochemical conversion of CO_2 to CH_4 with low energy costs. A dual-chamber system was installed with an antimony-doped tin oxide anode (Ti/SnO_2-Sb) for the elec-trocatalytic generation of hydroxyl radicals to degrade ciprofloxacin (CIP), and a CO_2-reducing methanogenic biocathode was enriched based on a three-dimensional (3D) graphitized granular activated carbon (CGAC) for microbial electromethanogenesis. The anode achieved removal efficiencies as high as 99.99% and 90.53% for CIP (14 mL, 50 mg L~(-1)) and the chemical oxygen demand (COD, 89 mg L~(-1)). respectively. The biocathode was rapidly enriched within 15 days and exhibited a methane production rate that stabilized at 15.12 ± 1.82 m~3 m~(-3) d~(-1); additionally, the cathodic coulombic efficiency reached 71.76 ± 17.24%. The energy consumption of CIP degradation was reduced by 3.03 Wh L~(-1) compared to that of a single electrochemical oxidation system due to the lower cathodic overpotential of CO_2 bioelectrochemical reduction in the EO-M system. A detailed analysis of the biofilm evolution in the 3D biocathode during the start-up process demonstrated that the enhanced absorption of extracellular polymeric substances by the GGAC cathode accelerated the enrichment of methanogens and induced the formation of methanogens with a large number of flagella. An analysis of the microbial community showed that a high relative abundance of Methanobacterium movens could promote a flagella-mediated direct electron transfer of the biocathode, eventually reducing the cathodic overpotential and energy costs of the EO-M system.