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基于微流控技术的重质非水相液体氧化修复机理

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为揭示重非水相污染物(DNAPL)氧化修复中多相渗流-化学反应-相演变耦合过程的物理化学机理,利用新兴的微流控技术开展了高锰酸钾(KMnO4)氧化修复三氯乙烯(TCE)的实验。结果表明:当浓度3g/L以上的KMnO4氧化TCE时,二氧化锰(MnO2)固相产物会在流道深度方向上产生"固体墙",后续MnO4-只能缓慢渗入墙内对TCE进行氧化,此时MnO4-成为限制性因素并转化为Mn2+,而Mn2+扩散出墙外后再次被氧化为MnO2固相,形成一个负反馈系统并造成修复效率急剧降低。当3g/L以下的KMnO4氧化TCE时,MnO2固相产物附着在流道壁面上,后续MnO4—可以和TCE持续反应并生成MnO2,KMnO4溶液-DNAPL界面不断后退且修复效率较高。当加入磷酸氢盐后,MnO2固相产物被显著抑制从而提高了修复效率,且1~2g/L是孔隙尺度TCE修复的理想KMnO4浓度。
Pore-scale mechanisms of DNAPL oxidative remediation in a microfluidic device
To elucidate pore-scale mechanisms governing the coupled process of multiphase flow,chemical reactions,and phase transformations during the oxidation remediation of dense non-aqueous phase liquids(DNAPLs),we conducted 48microfluidic experiments to investigate the trichloroethylene(TCE)oxidation by potassium permanganate(KMnO4).The results show that when KMnO4 concentration exceeded 3g/L,the manganese dioxide(MnO2)solid products during TCE oxidation formed a"solid wall",which hindered the contact between MnO4-and TCE.Under such conditions,the residual TCE oxidation proceeded only via the slow penetration of KMnO4 solution through the MnO2 wall,where limited MnO4-was converted to Mn2+.As Mn2+diffused out of the MnO2 wall,it was re-oxidized to MnO2 solid phase,creating a negative feedback loop and significantly reducing remediation efficiency.At KMnO4 concentrations below 3g/L,the MnO2 solid products were able to attach to the channel surfaces,permitting continuous reaction between MnO4-and TCE,thereby resulting in a higher remediation efficiency.The introduction of phosphate significantly suppressed the formation of MnO2 solid products and improved remediation efficiency,with an optimal KMnO4 concentration for TCE remediation determined to be 1~2g/L.

DNAPLoxidative remediationmultiphase flowtrichloroethylenemicrofluidics

王泽君、杨志兵、胡冉、陈益峰

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武汉大学水利水电学院,水资源工程与调度全国重点实验室,水工岩石力学教育部重点实验室,湖北武汉 430072

非水相液体 氧化修复 多相渗流 三氯乙烯 微流控

国家自然科学基金资助项目国家自然科学基金资助项目

4187720342377066

2024

中国环境科学
中国环境科学学会

中国环境科学

CSTPCDCHSSCD北大核心
影响因子:2.174
ISSN:1000-6923
年,卷(期):2024.44(8)