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Controlling disinfection byproducts from treated wastewater using adsorption with granular activated carbon: Impact of pre-ozonation and pre-chlorination

ABSTRACT: This study measured chlorine- and chloramine-reactive precursors using formation potential (FP) tests of nine U.S. Environmental Protection Agency (EPA) regulated and 57 unregulated disinfection byproducts (DBPs) in tertiary-filtered wastewater before and after pilot-scale granular activated carbon (GAC) adsorption. Using breakthrough of precursor concentration and of concentration associated calculated cytotoxicity and genotoxicity (by correlating known lethal concentrations reported elsewhere), the performance of three parallel GAC treatment trains were compared against tertiary-filtered wastewater: ozone/GAC, chlorine/GAC, and GAC alone. Results show GAC alone was the primary process, versus ozone or chlorine alone, to remove the largest fraction of total chlorine- and chloramine-reactive DBP precursors and calculated cytotoxicity and genotoxicity potencies. GAC with pre-ozonation removed the most chlorine- and chloramine-reactive DBP precursors followed by GAC with pre-chlorination and lastly GAC without pre-treatment. GAC with pre-ozonation produced an effluent with cytotoxicity and genotoxicity of DBPs from FP that generally matched that of GAC without pre-oxidation; meanwhile removal of toxicity was greater by GAC with pre-chlorination. The cytotoxicity and genotoxicity of DBPs from FP tests did not scale with DBP concentration; for example, more than 90% of the calculated cytotoxicity resulted from 20% of the DBPs, principally from haloacetaldehydes, haloacetamides, and haloacetonitriles. The calculated cytotoxicity and genotoxicity from DBPs associated with FP-chloramination were at times higher than with FP-chlorination though the concentration of DBPs was five times higher with FP-chlorination. The removal of DBP precursors using GAC based treatment was at least as effective as removal of DOC (except for halonitromethanes for GAC without pre-oxidation and with pre-chlorination), indicating DOC can be used as an indicator for DBP precursor adsorption efficacy. However, the DOC was not a good surrogate for total cytotoxicity and genotoxicity breakthrough behavior, therefore, unregulated DBPs could have negative health implications that are disconnected from general water quality parameters, such as DOC, and regulated classes of DBPs. Instead, cytotoxicity and genotoxicity correlate with the concentration of specific classes of unregulated DBPs. Graphical abstract Image 1 Highlights • Ozonation followed by GAC yielded the lowest DBP formation potential.• Chlorination followed by GAC yielded the lowest DBP-associated calculated toxicity.• Breakthrough of DOC matched that of DBP concentration but not of toxicity.• Breakthrough of DOC was faster than most types of DBP precursors.

SUBMITTER: Verdugo E

PROVIDER: S-EPMC7522497 | biostudies-literature | 2020 Sep

REPOSITORIES: biostudies-literature

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Project description:Nitrification and distillation of urine allow for the recovery of all nutrients in a highly concentrated fertilizer solution. However, pharmaceuticals excreted with urine are only partially removed during these two process steps. For a sustainable and safe application, more extensive removal of pharmaceuticals is necessary. To enhance the pharmaceutical removal, which is already occurring during urine storage, nitrification and distillation, an adsorption column with granular activated carbon (GAC) can be included in the treatment train. We executed a pilot-scale study to investigate the adsorption of eleven indicator pharmaceuticals on GAC. During 74 days, we treated roughly 1000 L of pre-filtered and nitrified urine spiked with pharmaceuticals in two flow-through GAC columns filled with different grain sizes. We compared the performance of these columns by calculating the number of treated bed volumes until breakthrough and carbon usage rates. The eleven spiked pharmaceuticals were candesartan, carbamazepine, clarithromycin, diclofenac, emtricitabine, hydrochlorothiazide, irbesartan, metoprolol, N4-acetylsulfamethoxazole, sulfamethoxazole and trimethoprim. At the shortest empty bed contact time (EBCT) of 25 min, immediate breakthrough was observed in both columns shortly after the start of the experiments. Strong competition by natural organic material (NOM) could have caused the low pharmaceutical removal at the EBCT of 25 min. At EBCTs of 70, 92 and 115 min, more than 660 bed volumes could be treated until breakthrough in the column with fine GAC. The earliest breakthrough was observed for candesartan and clarithromycin. On coarse GAC, only half the number of bed volumes could be treated until breakthrough compared to fine GAC. The probable reason for the later breakthrough with fine GAC is the smaller intraparticle diffusive path length. DOC and UV absorbance measurements at 265 nm indicated that both parameters can be used as indicators for the breakthrough of pharmaceuticals. In contrast to pharmaceuticals and DOC, the nutrient compounds ammonium, nitrate, phosphate, potassium and sulfate were not removed significantly. A comparison with literature values suggests that the amount of GAC needed to remove pharmaceuticals from human excreta could be reduced by nearly two orders of magnitude, if urine were treated on site instead of being discharged and treated in a centralized wastewater treatment plant.

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Controlling disinfection byproducts from treated wastewater using adsorption with granular activated carbon: Impact of pre-ozonation and pre-chlorination

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