煤气化渣活化过硫酸盐体系氧化去除菲  

Removal of phenanthrene by coal gasification slag activated persulfate system

作　　者：郭凯 王嘉琪 李亚男[1] 武亚宁 GUO Kai;WANG Jiaqi;LI Yanan;WU Yaning(College of Environmental Science and Engineering,Taiyuan University of Technology,Jinzhong 030600,China)

机构地区：[1]太原理工大学环境科学与工程学院,山西晋中030600

出　　处：《精细化工》2024年第5期1108-1115,1134,共9页Fine Chemicals

基　　金：自然资源部生态地球化学重点实验室开放基金项目(ZSDHJJ201804);山西省应用基础研究计划项目(20210302123121);山西省回国留学人员科研教研资助项目(2023-054)。

摘　　要：采用固体废弃物煤气化渣(CGS)作为过硫酸盐(PS)的活化剂,考察CGS/PS对菲的去除性能。使用SEM-EDS、XPS表征了CGS的微观结构和元素组成;通过自由基掩蔽实验和电子顺磁共振(EPR)实验确定自由基种类;考察了CGS质量浓度、PS初始浓度、初始pH、共存离子对CGS/PS体系中菲去除率的影响,探讨了反应机理并推测降解路径,并使用ECOSAR软件评估菲及其产物的毒性。结果表明,CGS中Fe元素质量分数为11.9%,可有效活化PS。在菲质量浓度为1 mg/L、pH=3、CGS质量浓度为0.7 g/L、PS初始浓度为1 mmol/L的条件下,60 min后CGS/PS体系对菲的去除率可达95.34%,PS的利用率为29.18%。菲降解过程符合伪一级动力学模型,CGS/PS体系产生了SO_(4)^(–)•和•OH,且SO_(4)^(–)•在菲降解过程中起主要作用,共存离子HCO_(3)^(–)、NO_(3)^(–)对反应的抑制作用较显著。菲主要通过去羰基、羟基化、脱碳等反应分解为长链酸、酯,最终转化为CO_(2)和H_(2)O。ECOSAR模型评估发现,菲降解的中间产物毒性普遍低于菲。Coal gasification slag(CGS),a kind of solid waste generated during the coal gasification process,was used as persulfate(PS)activator.And the removal performance of CGS/PS for phenanthrene was evaluated,while the microstructure and elemental composition of CGS were characterized by SEM-EDS and XPS.Moreover,the species of free radicals were determined by free radical masking experiment and electron paramagnetic resonance(EPR)experiment.The effects of CGS mass concentration,PS initial concentration,initial pH and co-existing ions on the removal rate of phenanthrene in CGS/PS system were further investigated.The reaction mechanism and degradation path were discussed,and the toxicity of phenanthrene as well as its products were evaluated by ECOSAR software.The results showed that Fe element with a mass fraction of 11.9%was identified in CGS,indicating CGS an effective PS activator.The removal rate of phenanthrene reached 95.34%and the utilization rate of PS reached 29.18%after 60 min of reaction under the conditions of mass concentration 1 mg/L phenanthrene,pH=3,mass concentration 0.7 g/L CGS and 1 mmol/L PS initial concentration.The degradation process of phenanthrene conformed to pseudo first-order reaction kinetics,with CGS/PS producing SO_(4)^(–)•and•OH,and SO_(4)^(–)•playing a dominant role during the oxidation.The coexisting ions of HCO_(3)^(–)and NO_(3)^(–)exhibited significant inhibitory effect on the reaction.Phenanthrene was decomposed into long-chain acids and esters through decarbonylation,hydroxylation and decarbonization,and ultimately converted into CO_(2)and H_(2)O.Meanwhile,the ECOSAR model evaluation indicated that the toxicity of intermediate products from phenanthrene decomposition was generally lower than that of phenanthrene.

关 键 词：菲 煤气化渣 过硫酸盐 活性自由基 共存离子 水处理技术 

分 类 号：X784[环境科学与工程—环境工程]