Original Data for Efficient Co-Removal of Urea and Diclofenac via Spatial Redox Decoupling in a Modified Microbial Fuel Cell

This study proposes a spatial redox-decoupled dual-chamber microbial fuel cell (MFC) equipped with a Pd-Ni/Pt-Ti hybrid cathode to address the thermodynamic incompatibility (ΔG = +221 kJ·mol⁻¹) between urea hydrolysis and diclofenac (DCF) degradation in complex wastewater. The system achieves synergistic removal of 85.3 ± 2.1% urea and 70% DCF within 15 hours, representing a 3.2-fold kinetic enhancement compared to conventional aerobic processes, while generating a power density of 0.81 W·m⁻². Microbial community analysis reveals that Geobacter (38.2 ± 2.1%) dominates the electroactive consortium, facilitating direct interspecies electron transfer (DIET) via 2.5-fold upregulation of the omcZ cytochrome. Mechanistic investigations using electron paramagnetic resonance (EPR) spectroscopy confirm hydroxyl radical (·OH)-mediated demethylation as the primary DCF degradation pathway, with ·OH contributing 78 ± 3% to degradation efficiency. The spatial decoupling of anodic urea hydrolysis and cathodic ·OH generation resolves substrate competition and kinetic mismatches, enabling energy-positive treatment of nitrogenous and pharmaceutical co-contaminated wastewater.

本研究提出一种搭载Pd-Ni/Pt-Ti复合阴极的空间氧化还原分离式双室微生物燃料电池（MFC），以解决复杂废水中尿素水解与双氯芬酸（DCF）降解之间的热力学不相容性（ΔG = +221 kJ·mol⁻¹）。该系统可在15小时内实现85.3 ± 2.1%的尿素与70%双氯芬酸的协同去除，较传统好氧工艺的动力学性能提升达3.2倍，同时可输出0.81 W·m⁻²的功率密度。微生物群落分析结果表明，地杆菌属（Geobacter）在电活性菌群中占比达38.2 ± 2.1%，为优势菌群，通过将omcZ细胞色素的表达量上调2.5倍，介导种间直接电子转移（DIET）。采用电子顺磁共振（EPR）光谱开展的机制研究证实，羟基自由基（·OH）介导的脱甲基反应是双氯芬酸降解的主要途径，羟基自由基对降解效率的贡献占比达78 ± 3%。阳极侧尿素水解与阴极侧羟基自由基生成的空间分离策略，解决了底物竞争与动力学不匹配的问题，可实现含氮与药物复合污染废水的能量正效益处理。