污泥生物炭耦合臭氧氧化去除渗滤液中多种药物类污染物  

The removal of multiple pharmaceuticals from leachates by sludge biochar combined with ozonation

作　　者：余阳[1] 王园园 阮仁伟 钱雅洁 YU Yang;WANG Yuanyuan;RUAN Renwei;QIAN Yajie(College of Environmental Science and Engineering,Donghua University,Shanghai 201620,China)

机构地区：[1]东华大学环境科学与工程学院,上海201620

出　　处：《环境工程学报》2025年第1期167-177,共11页Chinese Journal of Environmental Engineering

基　　金：国家自然科学基金资助项目(52170069);上海市青年科技启明星计划(21QC1400500)。

摘　　要：臭氧(Ozone,O_(3))作为一种较强的氧化剂,被广泛应用于高级氧化工艺,催化剂的加入能够激活臭氧,产生活性氧物质(如·OH等)从而实现对废水的处理。然而,基于污泥生物炭催化臭氧氧化去除渗滤液中药物类污染物(pharmaceutically active compounds,PhACs)的效能及特性罕有报道。因此本研究通过高温热解法制备污泥生物炭(sludge biochar,SDBC)催化臭氧降解渗滤液中的典型PhACs,包括磺胺类抗生素磺胺甲恶唑(sulfamethoxazole,SMX)、喹诺酮类抗生素环丙沙星(ciprofloxacin,CIP)、四环素类抗生素四环素(tetracycline,TTC)以及抗癫痫药物卡马西平(carbamazepine,CBZ)。研究结果表明,在未调pH的条件下(pH=7.8),SDBC/O_(3)体系能快速去除渗滤液的多种PhACs,在30 min内去除率均超过90%,效果显著优于单独使用O_(3)或SDBC,表明该体系能较好地处理渗滤液中的微污染物。pH实验表明SDBC/O_(3)体系在中性和碱性的条件下降解效果较好,在酸性的条件下效果较差,推测是由于酸性的水环境不利于臭氧分解产生活性物质以及污染物和生物炭之间易产生相斥作用。淬灭实验和电子顺磁共振实验(electron paramagnetic resonance,EPR)显示,体系中主要的活性物质为O_(2)^(·−)和^(1)O_(2),其中^(1)O_(2)起降解主要作用,O_(2)^(·−)起次要作用。SDBC表面上的C=O基团和Fe^(2+)是臭氧活化的主要活性位点。本研究阐明了SDBC在催化臭氧化方面的主要机制,研究结果可以为渗滤液中有机微污染物的处理提供理论依据和技术支撑。Ozone(O_(3)),as an common oxidant,is extensively applied in advanced oxidation processes.Adding catalysts can activate ozone to generate reactive oxygen species(ROS),such as hydroxyl radicals(·OH),thereby enhancing the efficiency of wastewater treatment.However,there is limited researches on the efficiency and mechanism of sludge derived biochar catalyzed ozonation(SDBC/O_(3))for pharmaceutically active compounds(PhACs)removal from leachates.In this study,SDBC was prepared through high temperature pyrolytic cracking method,and SDBC/O_(3) was used to remove typical PhACs in leachates,such as sulfonamide antibiotics of sulfamethoxazole(SMX),the quinolone antibiotics of ciprofloxacin(CIP),the tetracycline antibiotics of tetracycline(TTC),and the antiepileptic drugs of carbamazepine(CBZ).The results showed that under unadjusted pH conditions(pH=7.8),all the PhACs could be rapidly removed by SDBC/O_(3) from leachates,with the removal efficiency exceeding 90%in 30 min,which is significantly higher than O_(3) or SDBC alone.This indicated that SDBC/O_(3) could well treat the micropollutants in the leachates.The effect of pH investigation revealed that higher removal efficiency occurred at neutral and alkaline pHs than acidic pHs,likely due to the unfavorable environment for ozone decomposition into reactive oxygen species and easy production of repulsion between pollutants and biochar in acidic water.Quenching experiments and electron paramagnetic resonance(EPR)indicated that the primary reactive species in the system were O_(2)^(·−)and singlet oxygen ^(1)O_(2),and ^(1)O_(2) played the major role in removing PhACs.The C=O and Fe^(2+)on SDBC were the dominant reactive sites for O_(3) activating.This research elucidates the mechanism of SDBC/O_(3) removing PhACs in leachates and provides a theoretical and technical support for treating organic micropollutants in leachates.

关 键 词：污泥生物炭 臭氧 渗滤液 药物 

分 类 号：X703[环境科学与工程—环境工程]