Enhanced degradation of methanethiol via operational pH regulation in biofilm reactor: Insight of sulfur metabolism pathways and microbial adaptation mechanism

Methanethiol (CH3SH), a typical organic sulfur pollutant, poses significant risks to both human health and ecological stability due to its high toxicity and corrosive properties. Membrane aerated biofilm reactor (MABR) has been regarded as a promising and eco-friendly solution for removing organic sulfur from wastewater. However, the oxidation of CH3SH might lead to spontaneous acidification, which might affect microbial metabolic activities to influence the CH3SH biotransformation in MABR system. This work demonstrated that operational pH regulation could effectively promote the complete conversion of CH3SH to SO42- in MABR, while the transformation efficiency was only 40.6% under uncontrolled pH condition. Meanwhile, operational pH regulation resulted in 35.2% reduction in the excessive secretion of extracellular polymeric substances, thereby building a stable biofilm structure with sufficient oxygen mass transfer to enhance the CH3SH transformation. Additionally, operational pH regulation favored the enrichment of sulfur-oxidizing microorganisms (e.g., Rhodanobacter and Rhodobacter), while the uncontrolled pH favored the proliferation of microorganisms in harsh environment (e.g., Chitinophagaceae sp. and Sphingobacteriales sp.). Moreover, operational pH regulation enhanced the expression of critical genes involved in sulfur metabolism (e.g., SELENBP1 and SoxA), accompanied with glycolysis (e.g., ppgK and pfkB) and pyruvate metabolism (e.g., ackA and aceE), which could provide sufficient energy and electron. Conversely, these gene expressions were down-regulated in pH unregulation reactor, while the microbial adaptation mechanism was activated through the enhancement of DNA replication, quorum sensing, and two-component system, enabling resistance to extreme acidic conditions. This study would provide the in-depth understanding of operational pH regulation on organic sulfur degradation and transformation in MABR system and offer novel guidance for organic sulfur removal.