铁碳微电解人工湿地对典型有机磷阻燃剂的去除效能

Removal of typical organophosphate flame retardants by iron-carbon micro-electrolysis constructed wetlands

  • 摘要: 有机磷阻燃剂(OPFRs)作为一种新污染物在传统污水处理过程中难以被有效去除,而铁碳微电解(ICME)人工湿地系统(ICME-CWs)作为一种新型水处理技术,能够通过填料强化吸附、植物吸收和微生物降解等方式去除新污染物,但目前对其去除OPFRs的效能研究不足。选取生物炭-海绵铁(BC+SI)、活性炭-铁屑(AC+Fe)及商品铁碳材料(FeC)3种填料组合构建了ICME-CWs,以砾石人工湿地(CW)作为对照组,系统考察了ICME-CWs中不同填料、水力停留时间(0.5~2.0 d)及进水OPFRs负荷(300~1 500 μg/L)对磷酸三苯酯(TPHP)、磷酸三(2-氯乙基)酯(TCEP)和磷酸三(氯丙基)酯(TCPP)3种典型OPFRs去除的影响与常规污染物去除性能。结果表明:BC+SI组合的去除效能最优,对TPHP、TCEP和TCPP的平均去除率均超过82%,出水COD、TN和TP的平均去除率最高分别达85.5%、75.5%和93.6%,出水水质优于GB 18918—2002《城镇污水处理厂污染物排放标准》一级A标准。ICME填料的加入显著改变了CWs微环境,出水pH升至8.0~8.5,强化层溶解氧浓度降至0.3~0.9 mg/L,为污染物降解创造了有利条件。水力停留时间(HRT)从2.0 d缩短至0.5 d或进水OPFRs浓度增至1 500 μg/L时,OPFRs去除率分别下降约30%和35%。BC+SI组合通过吸附与微电解的协同作用,能高效稳定地去除水中典型OPFRs及常规污染物。

     

    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.

     

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