高春阳1,2,3,
陈昌照1,,
宋权威1,
陈宏坤1,
陈家玮2
1.中国石油安全环保技术研究院,石油石化污染物控制与处理国家重点实验室,北京 102206
2.中国地质大学北京地球科学与资源学院,北京 100083
3.中国地质科学院水文地质环境地质研究所,石家庄 050061
Degradation of PAHs in contaminated soil by zero valent iron activated sodium persulfate system
ZHANG Yu1,2,,GAO Chunyang1,2,3,
CHEN Changzhao1,,
SONG Quanwei1,
CHEN Hongkun1,
CHEN Jiawei2
1.State Key Laboratory of Petroleum Pollution Control, Research Institute of Safety and Environment Technology of China National Petroleum Corporation, Beijing 102206, China
2.School of Earth Sciences and Resources, China University of Geosciences Beijing, Beijing 100083, China
3.Institute of Hydrogeology and Environmental Geology, Chinese Academy of Geological Sciences, Shijiazhuang 050061, China
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摘要:采用Fe0活化Na2S2O8体系降解污染土壤中的PAHs,其代表化学物为NAP、PHE、FLA和BAP。分别研究了Na2S2O8的添加量、Na2S2O8与Fe0的物质的量比、水土比和温度对降解效果的影响,同时探讨了PAHs的降解动力学;并利用电子顺磁共振法(EPR)验证了Fe0活化Na2S2O8的自由基产生情况。结果表明,当1 mol·L-1的Na2S2O8添加量为10 mL、Na2S2O8与Fe0物质量之比为200∶1、水土比为2∶1、温度为60 ℃时反应36 h后,NAP、PHE、FLA、BAP的降解率分别为98.15%、78.41%、93.47%和97.64%。PAHs的降解符合一级反应动力学,且BAP的反应速率常数最大为0.030 5 h-1。EPR谱图表明,Fe0活化Na2S2O8降解PAHs污染的土壤是SO4-·和·OH共存的反应体系。该研究可为Fe0活化Na2S2O8体系降解PAHs污染土壤的机理提供一定的依据。
关键词: 土壤修复/
零价铁活化/
过硫酸钠/
多环芳烃污染土壤/
自由基共存体系
Abstract:In this study, Fe0 was used to activate Na2S2O8 to degrade NAP, PHE, FLA and BAP in PAH contaminated soil. The effects of Na2S2O8 addition, the ratio of Na2S2O8 to Fe0, soil-water ratio and temperature on the degradation rate were studied, as well as PAHs degradation kinetics. The free radical production in Fe0 activated Na2S2O8 system was verified by electron paramagnetic resonance (EPR). The results showed that the degradation rates of NAP, PHE, FLA and BAP were 98.15%, 78.41%, 93.47% and 97.64%, respectively, after 36 h reaction under the following conditions: 10 mL 1 mol·L-1 Na2S2O8 addition, Na2S2O8 to Fe0 molar ratio of 200∶1, the soil to water ratio of 2∶1, and 60 ℃. The PAHs degradation accorded with the first-order kinetics, and the maximum reaction rate constant for BAP was 0.030 5 h-1. EPR spectra identified that the coexistence system of SO4-·and·OH produced from Fe0 activated Na2S2O8 reaction contributed to PAHs degradation in contaminated soils. This study may provide a basis for the PAHs degradation mechanism in contaminated soil by Fe0 activated Na2S2O8 system.
Key words:soil remediation/
zero valent iron activation/
sodium persulfate/
polycyclic aromatic hydrocarbons contaminated soil/
free radical coexistence system.
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刊出日期:2019-04-15
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零价铁活化过硫酸钠体系降解污染土壤中的多环芳烃
张羽1,2,,高春阳1,2,3,
陈昌照1,,
宋权威1,
陈宏坤1,
陈家玮2
1.中国石油安全环保技术研究院,石油石化污染物控制与处理国家重点实验室,北京 102206
2.中国地质大学北京地球科学与资源学院,北京 100083
3.中国地质科学院水文地质环境地质研究所,石家庄 050061
基金项目:
关键词: 土壤修复/
零价铁活化/
过硫酸钠/
多环芳烃污染土壤/
自由基共存体系
摘要:采用Fe0活化Na2S2O8体系降解污染土壤中的PAHs,其代表化学物为NAP、PHE、FLA和BAP。分别研究了Na2S2O8的添加量、Na2S2O8与Fe0的物质的量比、水土比和温度对降解效果的影响,同时探讨了PAHs的降解动力学;并利用电子顺磁共振法(EPR)验证了Fe0活化Na2S2O8的自由基产生情况。结果表明,当1 mol·L-1的Na2S2O8添加量为10 mL、Na2S2O8与Fe0物质量之比为200∶1、水土比为2∶1、温度为60 ℃时反应36 h后,NAP、PHE、FLA、BAP的降解率分别为98.15%、78.41%、93.47%和97.64%。PAHs的降解符合一级反应动力学,且BAP的反应速率常数最大为0.030 5 h-1。EPR谱图表明,Fe0活化Na2S2O8降解PAHs污染的土壤是SO4-·和·OH共存的反应体系。该研究可为Fe0活化Na2S2O8体系降解PAHs污染土壤的机理提供一定的依据。
English Abstract
Degradation of PAHs in contaminated soil by zero valent iron activated sodium persulfate system
ZHANG Yu1,2,,GAO Chunyang1,2,3,
CHEN Changzhao1,,
SONG Quanwei1,
CHEN Hongkun1,
CHEN Jiawei2
1.State Key Laboratory of Petroleum Pollution Control, Research Institute of Safety and Environment Technology of China National Petroleum Corporation, Beijing 102206, China
2.School of Earth Sciences and Resources, China University of Geosciences Beijing, Beijing 100083, China
3.Institute of Hydrogeology and Environmental Geology, Chinese Academy of Geological Sciences, Shijiazhuang 050061, China
Keywords: soil remediation/
zero valent iron activation/
sodium persulfate/
polycyclic aromatic hydrocarbons contaminated soil/
free radical coexistence system
Abstract:In this study, Fe0 was used to activate Na2S2O8 to degrade NAP, PHE, FLA and BAP in PAH contaminated soil. The effects of Na2S2O8 addition, the ratio of Na2S2O8 to Fe0, soil-water ratio and temperature on the degradation rate were studied, as well as PAHs degradation kinetics. The free radical production in Fe0 activated Na2S2O8 system was verified by electron paramagnetic resonance (EPR). The results showed that the degradation rates of NAP, PHE, FLA and BAP were 98.15%, 78.41%, 93.47% and 97.64%, respectively, after 36 h reaction under the following conditions: 10 mL 1 mol·L-1 Na2S2O8 addition, Na2S2O8 to Fe0 molar ratio of 200∶1, the soil to water ratio of 2∶1, and 60 ℃. The PAHs degradation accorded with the first-order kinetics, and the maximum reaction rate constant for BAP was 0.030 5 h-1. EPR spectra identified that the coexistence system of SO4-·and·OH produced from Fe0 activated Na2S2O8 reaction contributed to PAHs degradation in contaminated soils. This study may provide a basis for the PAHs degradation mechanism in contaminated soil by Fe0 activated Na2S2O8 system.