A Hybrid Fluidized-bed Reactor (HFBR) Based on Arrayed Ceramic Membranes (ACMs) Coupled with Powdered Activated Carbon (PAC) for Efficient Catalytic Ozonation: A Comprehensive Study on a Pilot Scale

Taking advantage of the high mass transfer in the bulk solution of fluidized-bed reactor (FBR), and the benefits of simultaneous particle separation and ozone catalysis on ceramic membranes, we proposed a hybrid fluidized-bed reactor (HFBR) based on arrayed ceramic membranes (ACMs) coupled with powdered activated carbon (PAC) for efficient catalytic ozonation. The optimum HFBR performance on a pilot scale was found at PAC addition of 3 g/L, ozone dosage of 25 mg/L, hydraulic retention time of 60 min and auxiliary aeration strength of 5 m/h. During the 30-day treatment of coal-gasification secondary effluent (200 L/h), the HFBR system revealed not only a 117% increase in ozone utilization efficiency (ΔCOD/ΔO) upon pure ozonation but also a highly purified effluent with better sterilization and low residual bromate (∼11 μg/L). Low-molecular-weight organic fragments and acids, as well as phthalate esters were identified as the main products in this process. By density functional theory (DFT) calculations, it was found the main functional groups (carbonyls, -C=O) on the PAC could be protected from direct ozonation in the presence of ozone-degradable organics (e.g. phenolic and aliphatic compounds) in the wastewater through an ozone-competing reaction, which prevented the rapid inactivation of the PAC in catalytic ozonation. A longer service life and cheaper materials for ceramic membranes would benefit low operation costs for the HFBR. Moreover, the addition of PAC could greatly reduce ozone demand by ∼60% in the HFBR, and therefore decrease energy consumption by ∼30%. Hence, the HFBR was proved to be a highly competitive technology for wide application in the near future.