Unappreciated role of secondary metabolism-derived small mediators in degrading bisphenol A and antibiotics by a laccase-expressing fungus

Fungal laccase producers can effectively address bisphenol A (BPA) and antibiotic-contaminated water. However, the role of small mediators produced by fungal secondary metabolism in enhancing the removal of refractory contaminants is often overlooked. In this work, an efficient laccase-producing strain, Trametes hirsuta La-7, was activated to simultaneously treat BPA and antibiotics. Coexisting tetracycline, ciprofloxacin, sulfadiazine, or roxithromycin inhibited fungal cell growth, reducing laccase biosynthesis but largely increasing the formation of syringaldehyde (SYR), 4-hydroxybenzoic acid (HBA), and vanillin (VAN) through a complex regulatory network. These specialized metabolites ( i.e. , small mediators) acted as diffusible electron carriers for laccase, enabling the oxidative decomposition of the four antibiotics with high redox potentials. According to laccase-mediator-regulated radical random polymerization and decomposition, the identified intermediates of copollutants were parallelly concentrated in oligomeric coupling products and oxidative cleavage species. By inoculating logarithmic phase cell pellets in conjunction with an artificially added small mediator (SYR, HBA, or VAN), the removal efficiencies of BPA and the four antibiotics within 5 d reached 100% and 69–100% in artificial wastewater, respectively. The low and ultimately non-biotoxic intermediate products generated in the fungus-mediator systems mitigated the eco-environmental risks of the parent compounds. This work highlights the previously underappreciated role of secondary metabolism-derived small mediators in enhancing the degradation of BPA and antibiotics by a laccase-expressing fungus and is beneficial to the rational design of a robust fungus-mediator system for environmental bioremediation.