Coupling advanced oxidative pretreatment with subsequent biodegradation demonstrates potential for treating wastewaters containing biorecalcitrant and inhibitory organic constituents. However, advanced oxidation is indiscriminate, producing a range of products that can be too oxidized, unavailable for biodegradation, or toxic themselves. This problem could be overcome if advanced oxidation and biodegradation occurred together, an orientation called intimate coupling; then, biodegradable organics are removed as they are formed, focusing the chemical oxidant on the non-biodegradable fraction. Intimate coupling has seemed impossible because the conditions of advanced oxidation, for example, hydroxyl radicals and sometimes UV-light, are severely toxic to microorganisms. Here, we demonstrate that a novel photocatalytic circulating-bed biofilm reactor (PCBBR), which utilizes macro-porous carriers to protect biofilm from toxic reactants and UV light, achieves intimate coupling. We demonstrate the viability of the PCBBR system first with UV only and acetate, where the carriers grew biofilm and sustained acetate biodegradation despite continuous UV irradiation. Images obtained by scanning electron microscopy and confocal laser scanning microscopy show bacteria living behind the exposed surface of the cubes. Second, we used slurry-form Degussa P25 TiO2 to initiate photocatalysis of inhibitory 2,4,5-trichlorophenol (TCP) and acetate. With no bacterial carriers, photocatalysis and physical processes removed TCP and COD to 32% and 26% of their influent levels, but addition of biofilm carriers decreased residuals to 2% and 4%, respectively. Biodegradation alone could not remove TCP. Photomicrographs clearly show that biomass originally on the exterior of the carriers was oxidized (charred), but biofilm a short distance within the carriers was protected. Finally, we coated TiO2 directly onto the carrier surface, producing a hybrid photocatalytic-biological carrier. These carriers likewise demonstrated the concept of photocatalytic degradation of TCP coupled with biodegradation of acetate, but continued TCP degradation required augmentation with slurry-form TiO2.

Chlorinated aromatic compounds challenge our environment and wastewater treatment processes due to their biorecalcitrance and inhibition. In particular, 2,4,5-trichlorophenol (TCP) seems to demonstrate greater resistance to biodegradation than other trichlorophenols and is a known uncoupler of the electron transport chain, although little work addresses this compound specifically. Here, we investigate the biorecalcitrance, inhibition, and adaptation to 2,4,5-trichlorophenol by aerobic mixed microbial communities. We show that 2,4,5-trichlorophenol is strongly resistant to biodegradation at concentrations greater than 40 microM, demonstrates inhibition to respiration in direct proportion to 2,4,5-trichlorophenol concentration (with 50% inhibition projected near 85 microM 2,4,5-trichlorophenol), and does not sustain biomass in continuous reactors, even when all input 2,4,5-trichlorophenol is degraded. Communities showed consistent adaptation patterns to 2,4,5-trichlorophenol at concentrations of 10 microM and 20 microM, but these patterns diverged at concentrations greater than 40 microM. Finally, thermodynamic approximations were used to estimate the yield of 2,4,5-trichlorophenol as 0.165 gVSS/gCOD, a low value that partially explains why biodegradation of 2,4,5-trichlorophenol did not sustain the biomass. In particular, we estimated that the minimum concentration to support steady-state biomass (S (min)) is approximately 180 microM, a value much larger than the 40-microM concentration that is strongly resistant to biodegradation. Thus, readily biodegradable concentrations of 2,4,5-trichlorophenol are too low to sustain the biomass that biodegrades it.

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