好氧颗粒污泥对页岩气返排水中的典型多环芳烃的去除、解毒作用及机制  

Performance and mechanism of removal and detoxification of typical polycyclic aromatic hydrocarbons in shale gas flowback water by aerobic granular sludge

作　　者：孙靖蕾 卢培利[1,2,3] 丁阿强 刘阳[1,2,3] 佟宇浩 李仕康 SUN Jinglei;LU Peili;DING Aqiang;LIU Yang;TONG Yuhao;LI Shikang(State Key Laboratory of Coal Mine Disaster Dynamics and Control,Chongqing University,Chongqing 400044,China;Department of Environmental Science,College of Environment and Ecology,Chongqing University,Chongqing 400045,China;Key Laboratory of the Three Gorges Reservoir Region’s Eco-Environments(Ministry of Education),Chongqing University,Chongqing 400045,China)

机构地区：[1]重庆大学煤矿灾害动力学与控制全国重点实验室,重庆400044 [2]重庆大学三峡库区生态环境教育部重点实验室,重庆400045 [3]重庆大学环境与生态学院环境科学系,重庆400045

出　　处：《环境工程学报》2024年第8期2176-2188,共13页Chinese Journal of Environmental Engineering

基　　金：国家自然科学面上基金资助项目(52070025);国家自然科学青年基金资助项目(52200086);煤矿灾害动力学与控制国家重点实验室面上资助项目(2011DA105287-MS202213);国家重点研发计划(2019YFC1805503)。

摘　　要：页岩气开发是我国重大能源战略的关键组成部分,返排水的处理是该行业面临的主要挑战。目前,在返排水中普遍存在的多环芳烃由于具有高环境风险而备受关注。本研究采用具有页岩气返排水处理能力的好氧颗粒污泥探究其对典型多环芳烃萘和菲的处理能力及其行为特征,并通过HPLC和GC-MS分析降解过程中的中间产物探究降解路径,及好氧颗粒污泥对多环芳烃毒性的缓解效应。结果显示,该好氧颗粒污泥对萘和菲的去除率达到93.8%和91.3%,并能保持长期稳定。生物降解是该好氧颗粒污泥系统长期稳定去除典型多环芳烃的主要途径,对萘和菲的去除贡献率分别达到64.1%和72.2%。受限于吸附容量,吸附作用仅在初期发挥短期贡献,且具有不同的吸附机制:萘的吸附过程主要表现为多分子层的化学吸附,而菲的吸附表现为物理吸附和静电力作用下的化学吸附。伴随着萘和菲的去除,含萘和菲的废水经该好氧颗粒污泥处理之后生物毒性显著降低,分别降至1%和16%。萘降解生成的中间体包括2,4-二甲基苯甲醛、2,4-二叔丁基苯酚和2,2'-亚甲基双-(4-甲基-6-叔丁基苯酚),而菲的降解中间体则包括萘、三(2,4-二叔丁基苯基)亚磷酸酯、2,4-二甲基苯甲醛、2,4-二叔丁基苯酚和2,2'-亚甲基双-(4-甲基-6-叔丁基苯酚),这些中间体最终转化为水杨酸和邻苯二甲酸,通过三羧酸循环实现矿化并缓解毒性。上述结果暗示处理页岩气返排水的好氧颗粒污泥系统能够对返排水中的多环芳烃进行有效去除进而缓解其毒性效应,为好氧颗粒污泥技术应用于页岩气返排水处理提供了技术支撑。Shale gas development is a crucial element of China's significant energy strategy,and managing flowback water presents a substantial challenge for the industry.The presence of PAHs in flowback water has received particularly concerns due to their high environmental risks.This study utilizes aerobic granular sludge,which is capable of treating shale gas flowback water,to explore its effectiveness in processing typical PAHs such as naphthalene and phenanthrene,and examine the behavior of these compounds and their degradation pathways by analyzing the intermediates via HPLC and GC-MS.Additionally,the capacity of aerobic granular sludge to reduce the toxicity associated with PAHs was evaluated,highlighting its potential benefits in environmental remediation.The results showed that the aerobic granular sludge could remove 93.8%of naphthalene and 91.3%of phenanthrene with a sustained efficacy over time.Biodegradation served as the primary pathway for a long-term stable removal of typical PAHs by this AGS system,contributing 64.1%to naphthalene removal and 72.2%to phenanthrene removal.Constrained by adsorption capacity,adsorption only played a fleeting yet crucial role at the initial stage with the distinct pathways:chemisorption for naphthalene in a multimolecular layer and a combination of physisorption and chemisorption influenced by electrostatic forces for phenanthrene.Notably,the treatment significantly reduced the biotoxicity of PAH-laden wastewater to 1%and 16%for naphthalene and phenanthrene,respectively.Degradation intermediates such as 2,4-dimethylbenzaldehyde,2,4-di-tert-butylphenol,and 2,2'-methylenebis(4-methyl-6-tert-butylphenol)for naphthalene,while those for phenanthrene degradation included naphthalene,tris(2,4-di-tert-butylphenyl)phosphite,2,4-dimethylbenzaldehyde,2,4-di-tert-butylphenol,and 2,2'-methylenebis(4-methyl-6-tertbutylphenol),ultimately transformed into salicylic acid and phthalic acid,facilitating detoxification and mineralization through the tricarboxylic acid cycle.These insights affirme

关 键 词：页岩气返排水 好氧颗粒污泥 多环芳烃 吸附 生物降解 生物毒性 

分 类 号：X703[环境科学与工程—环境工程]