Abstract:
Organophosphate flame retardants (OPFRs), as emerging contaminants, are difficult to remove effectively in traditional wastewater treatment processes. The iron-carbon micro-electrolysis (ICME) constructed wetland system (ICME-CWs), as a novel water treatment technology, can remove emerging contaminants through enhanced adsorption by fillers, plant uptake, and microbial degradation. However, research on its efficacy in removing OPFRs remains insufficient. Therefore, this study selected three filler combinations (biochar-sponge iron (BC+SI), activated carbon-iron filings (AC+Fe), and commercial iron-carbon material (FeC)) to construct ICME-CWs, with a pure gravel constructed wetland (CW) as the control group. The study systematically investigated the effects of different fillers, hydraulic retention time (HRT, 0.5-2.0 d), and influent OPFRs loading (300-1 500 μg/L) in ICME-CWs on the removal of three typical OPFRs (triphenyl phosphate (TPHP), tris(2-chloroethyl) phosphate (TCEP), and tris(chloropropyl) phosphate (TCPP)), as well as the removal performance of conventional pollutants. The results showed that the BC+SI combination achieved the highest performance, with average removal rates exceeding 82% for all three OPFRs. The system also demonstrated excellent removal of conventional pollutants, with the highest average removal rates of 85.5% for COD, 75.5% for TN, and 93.6% for TP, meeting the Grade 1 A standard of China's
Discharge Standard of Pollutants for Municipal Waste-water Treatment Plant (GB 18918-2002). Mechanism analysis revealed that the ICME substrates significantly altered the system's microenvironment, increasing the effluent pH to 8.0-8.5 and decreasing the dissolved oxygen in the intensified layer to 0.3-0.9 mg/L, thereby creating favorable conditions for pollutant degradation. Shortening the HRT from 2.0 d to 0.5 d or increasing the influent OPFRs concentration to 1 500 μg/L reduced OPFRs removal rates by approximately 30% and 35%, respectively. The BC+SI combination, through the synergistic effects of adsorption and micro-electrolysis, can efficiently and stably remove both typical OPFRs and conventional pollutants from water.