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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摘要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.

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	王泽君
	杨志兵
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	陈益峰

关键词 ：非水相液体, 氧化修复, 多相渗流, 三氯乙烯, 微流控

Abstract：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.

Key words： DNAPL oxidative remediation multiphase flow trichloroethylene microfluidics

收稿日期: 2024-01-25

PACS:	X13
	X523

基金资助:国家自然科学基金资助项目(41877203,42377066)

作者简介: 王泽君(1996-),男,河南洛阳人,博士,主要从事地下水渗流与修复研究.发表论文12篇.wangzejun@hhu.edu.cn.

引用本文:

王泽君, 杨志兵, 胡冉, 陈益峰. 基于微流控技术的重质非水相液体氧化修复机理[J]. 中国环境科学, 2024, 44(8): 4530-4538. WANG Ze-jun, YANG Zhi-bing, HU Ran, CHEN Yi-Feng. Pore-scale mechanisms of DNAPL oxidative remediation in a microfluidic device. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(8): 4530-4538.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2024/V44/I8/4530

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