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抗坏血酸强化含水层介质Fenton降解PNP研究
引用本文:肖超,张东国,张晓雪,牛远,袁英,汪洋,唐军,鹿豪杰,李娟.抗坏血酸强化含水层介质Fenton降解PNP研究[J].环境科学研究,2021,34(12):2907-2916.
作者姓名:肖超  张东国  张晓雪  牛远  袁英  汪洋  唐军  鹿豪杰  李娟
作者单位:桂林理工大学环境科学与工程学院,广西环境污染控制理论与技术重点实验室,广西 桂林 541004;中国环境科学研究院,环境基准与风险评估国家重点实验室,北京 100012;中国环境科学研究院,国家环境保护地下水污染模拟与控制重点实验室,北京 100012;天津市生态环境科学研究院绿色与低碳发展研究中心,天津 300191;天津环科环境咨询有限公司,天津 300191;中国环境科学研究院,环境基准与风险评估国家重点实验室,北京 100012;中国环境科学研究院,国家环境保护地下水污染模拟与控制重点实验室,北京 100012;生态环境部土壤与农业农村生态环境监管技术中心,北京 100012
基金项目:国家水体污染控制与治理科技重大专项2018ZX07109-001
摘    要:为解决Fenton技术在地下水有机污染的原位修复中铁基材料难注入、降低二次污染的问题,并拓宽适用的pH范围. 以含水层介质(aquifer medium,简称“AM”)中的铁矿物为铁源,综合考虑区域地下水系统分区、地质类型和地质时代,采集京津冀5处典型地区浅层含水层介质,以天然还原剂/配体-抗坏血酸(ascorbic acid,简称“AA”)为强化试剂,构建了AM/AA/H2O2体系,并探究该体系对硝基苯酚(PNP)的降解效能以及环境pH对PNP降解的影响,同时揭示了AM/AA/H2O2体系降解污染物的机制. 结果表明:①五处含水层介质主要为长石类介质和碳酸盐类介质,表面都均匀分布了一定量的铁矿物,且以长石类介质催化H2O2分解降解PNP效果较好. ②抗坏血酸可显著促进含水层介质催化H2O2分解降解PNP,反应40 h内PNP的去除率最高可在89.00%以上(TOC的去除率为84.03%),与未加抗坏血酸的体系相比提升了6.82倍. ③降解PNP的主要功能自由基为·OH,是由液相中经抗坏血酸络合的铁离子催化H2O2分解产生的. ④与传统Fenton体系相比,抗坏血酸可有效拓宽AM/H2O2体系适用的pH范围,初始pH在5~10的范围内对PNP的降解无显著影响. 研究显示,AM/AA/H2O2体系在地下水有机污染的原位修复中具有较大的应用潜能. 

关 键 词:含水层介质  抗坏血酸  地下水  Fenton氧化  有机污染物
收稿时间:2021-04-08

Research on Degradation of PNP with Enhanced Aquifer Media Fenton System by Ascorbic Acid
Abstract:In order to solve the problems of difficulty in injecting iron-based materials and the secondary pollution in the in-situ remediation of organic contaminated groundwater by Fenton technology, and to broaden the applicable pH range, iron minerals in aquifer medium (AM) were taken as the iron sources in this study. Considering the groundwater system, geological type and geologic age, shallow aquifer media in five typical areas of Beijing, Tianjin and Hebei were taken. The natural reducing agent/ligand-ascorbic acid (AA) was used as the strengthening reagent to construct the AM/AA/H2O2 system. The degradation efficiency of organic pollutants (p-nitrophenol, PNP), effect of environmental pH were explored, and the degradation mechanism of PNP by the AM/AA/H2O2 system was also revealed. The results show that: (1) The main rock types of the five aquifer medium were feldspar and carbonate, and iron was distributed evenly on their surface. Among the five aquifer medium, feldspar media showed good catalytic efficiency for PNP degradation. (2) Ascorbic acid significantly promoted the catalytic decomposition of H2O2 in aquifer medium, therefore promoting the degradation rate of PNP. The maximum removal rate of PNP reached more than 89.00% within 40 h (the remove rate of TOC=84.03%), which is 6.82 times higher than that without ascorbic acid. (3) The main functional radical for PNP degradation is ·OH, which is mainly produced by the catalytic decomposition of H2O2 by ascorbic acid complexed iron ions in the liquid phase. (4) Compared with the traditional Fenton system, ascorbic acid can significantly broaden the applicable pH range of AM/H2O2 system, and the initial pH in the range of 5-10 has no obvious effect on PNP degradation. These results indicate that the AM/AA/H2O2 system has a great application potential in the in-situ remediation of organic contaminated groundwater. 
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