In this study, we analyzed 27 pharmaceuticals in liquid and solid phase samples collected from the unit processes of four different sewage treatment plants (STPs) to evaluate their distribution and behavior of the pharmaceuticals. The examination of the relative distributions of various categories of pharmaceuticals in the influent showed that non-steroidal anti-inflammatory drugs (NSAIDs) were the most dominant. While the relative distribution of antibiotics in the influent was not high (i.e., 3%-5%), it increased to 14%-30% in the effluent. In the four STPs, the mass load of the target pharmaceuticals was reduced by 88%-95% mainly in the biological treatment process, whereas the ratio of pharmaceuticals in waste sludge to those in the influent (w/w) was only 2%. In all the STPs, the removal efficiencies for the stimulant caffeine, NSAIDs (acetaminophen, naproxen, and acetylsalicylic acid), and the antibiotic cefradine were high; they were removed mainly by biological processes. Certain compounds, such as the NSAID ketoprofen, contrast agent iopromide, lipid regulator gemfibrozil, and antibiotic sulfamethoxazole, showed varying removal efficiencies depending on the contribution of biodegradation and sludge sorption. In addition, a quantitative meta-analysis was performed to compare the pharmaceutical removal efficiencies of the biological treatment processes in the four STPs, which were a membrane bioreactor (MBR) process, sequencing batch reactor (SBR) process, anaerobic-anoxic-oxic (A2O) process, and moving-bed biofilm reactor (MBBR) process. Among the biological processes, the removal efficiency was in the order of MBR > SBR > A2O > MBBR. Among the tertiary treatment processes investigated, powdered activated carbon showed the highest removal efficiency of 18%-63% for gemfibrozil, ibuprofen, ketoprofen, atenolol, cimetidine, and trimethoprim.
Keywords: biological treatment processes; mass balance; pharmaceuticals; sewage treatment plant.