State Key Laboratory of Clean Energy, College of Energy Engineering, Zhejiang University, Hangzhou 310027, PR China.
State Key Laboratory of Clean Energy, College of Energy Engineering, Zhejiang University, Hangzhou 310027, PR China.
Sci Total Environ. 2021 Jan 1;750:141732. doi: 10.1016/j.scitotenv.2020.141732. Epub 2020 Aug 15.
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 to CH with low energy costs. A dual-chamber system was installed with an antimony-doped tin oxide anode (Ti/SnO-Sb) for the electrocatalytic generation of hydroxyl radicals to degrade ciprofloxacin (CIP), and a CO-reducing methanogenic biocathode was enriched based on a three-dimensional (3D) graphitized granular activated carbon (GGAC) for microbial electromethanogenesis. The anode achieved removal efficiencies as high as 99.99% and 90.53% for CIP (14 mL, 50 mg L) and the chemical oxygen demand (COD, 89 mg L), respectively. The biocathode was rapidly enriched within 15 days and exhibited a methane production rate that stabilized at 15.12 ± 1.82 m m d; additionally, the cathodic coulombic efficiency reached 71.76 ± 17.24%. The energy consumption of CIP degradation was reduced by 3.03 Wh L compared to that of a single electrochemical oxidation system due to the lower cathodic overpotential of CO 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.
首次提出了一种新型的电化学氧化-产甲烷(EO-M)系统,该系统可同时实现抗生素降解和以低能耗将 CO 生物电化学转化为 CH。安装了一个双室系统,其中掺锑氧化锡阳极(Ti/SnO-Sb)用于电催化生成羟基自由基以降解环丙沙星(CIP),并基于三维(3D)石墨化颗粒活性炭(GGAC)富集 CO 还原产甲烷微生物生物阴极进行微生物电甲烷生成。阳极对 14 mL、50 mg L 的 CIP(14 mL、50 mg L)和化学需氧量(COD,89 mg L)的去除效率分别高达 99.99%和 90.53%。生物阴极在 15 天内迅速富集,并稳定在 15.12±1.82 m m d 的产甲烷速率;此外,阴极库仑效率达到 71.76±17.24%。与单一电化学氧化系统相比,EO-M 系统中 CO 生物电化学还原的阴极过电位较低,因此 CIP 降解的能耗降低了 3.03 Wh L。在启动过程中对 3D 生物阴极中生物膜演化的详细分析表明,GGAC 阴极对细胞外聚合物的增强吸收加速了产甲烷菌的富集,并诱导了大量鞭毛产甲烷菌的形成。微生物群落分析表明,Methanobacterium movens 的相对丰度较高可促进生物阴极的鞭毛介导的直接电子转移,最终降低 EO-M 系统的阴极过电位和能源成本。