Research progress and prospect of accelerating reduction of FeⅢ to FeⅡ in Fenton reaction

doi:10.19965/j.cnki.iwt.2020-1236

Abstract

Abstract:

As a representative of advanced oxidation technology nowadays，Fenton reaction has been widely used in the treatment of refractory organic wastewater. However，engineering practice witnesses masses of troublesome iron sludge produced because Fe^Ⅱ is fast consumed while Fe^Ⅲ is rapidly accumulated，which constraints further promotion and application of the Fenton reaction. One promising solution to break this shackle in the future is accelerating Fe^Ⅲ reduction to Fe^Ⅱ，which makes the Fe^Ⅲ/Fe^Ⅱ cycling possible，also reduces Fe^Ⅱ dosage and iron sludge. Studies on the topic of accelerating Fe^Ⅲ reduction to Fe^Ⅱ recent years can be divided into two groups：energy input and substance adding. The effects of different substances and energy forms on the catalytic degradation ability of the reaction system were reviewed，including the increase of Fe^Ⅱ/Fe^Ⅲ ratio，the improvement of pollutant removal efficiency and the acceleration of degradation rate. Meanwhile the reaction principles were analyzed. Finally，based on the problems existed in the practical application，it was proposed that increasing energy utilization and optimizing selection of substances would be the focus of future research.

Key words: Fenton reaction, refractory organic wastewater, cycling of iron, energy applied

摘要：

Fenton反应作为当今高级氧化技术的代表，已被广泛应用于难降解有机废水的处理。但工程实践中发现，因体系内Fe^Ⅱ迅速消耗、Fe^Ⅲ快速积累产生大量难以处置的铁泥，成为Fenton技术进一步推广应用的桎梏。加速Fenton反应中Fe^Ⅲ还原为Fe^Ⅱ，尽可能实现体系内Fe^Ⅲ/Fe^Ⅱ循环，以此减少Fe^Ⅱ投加和铁泥产生是未来有望实现突破的一种解决思路。近年来关于加速Fenton反应中Fe^Ⅲ还原为Fe^Ⅱ的研究主要分为2个方面：输入能量和投加物质。回顾了不同物质和能量形式对于反应体系催化降解能力的强化作用，如Fe^Ⅱ/Fe^Ⅲ比例增大、污染物去除率提高、降解速率加快等，同时分析了其中的反应原理。最后基于相关技术在实际应用中存在的一些问题，指出提高能量利用率和优化物质选择是未来研究的重点。

关键词: Fenton反应, 难降解有机废水, 铁价态循环, 输入能量

CLC Number:

X703

Ziyan ZHU, Xiaowen WANG, Yundong WANG, Hailiang YANG, Yong LI, Xin LIU. Research progress and prospect of accelerating reduction of Fe^Ⅲ to Fe^Ⅱ in Fenton reaction[J]. Industrial Water Treatment, 2022, 42(2): 1-10.

朱紫燕, 王孝文, 王允东, 杨海亮, 李勇, 刘忻. Fenton反应中加速Fe^Ⅲ还原为Fe^Ⅱ的研究进展及展望[J]. 工业水处理, 2022, 42(2): 1-10.

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References 65

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物质种类		投加量	Fe^Ⅲ/Fe^Ⅱ循环	参考文献
有机物	原儿茶酸（PCA）	0.1 mmol/L	Fe^Ⅱ在Fe^Ⅲ/PCA/H₂O₂中再生速率是（279±6） L/（mol·s）；在Fe^Ⅱ/H₂O₂中仅为63~76 L/（mol·s）	〔32〕
	抗坏血酸（Acs）	1.0×10^-3 mol/L	投加0.4 g/L赤铁矿纳米片，经300 min还原产生40 μmol/L Fe^Ⅱ，甲草胺降解率可提高到70%	〔33〕
	巯基乙酸（TGA）	2 mmol/L	c（TGA）/c（Fe^Ⅲ）=2.0，30 min可产生160 μmol/L Fe^Ⅱ	〔34〕
	聚多巴胺（PDA）	0.2 g/L Fe₃O₄@PDA	Fe^Ⅱ有效再生，初始投加量低至0.18 mmol/L	〔36〕
	三乙醇胺（TEA）	200 mg/L TEA/GO@Fe₃O₄	反应35 min后，Fe^Ⅱ/Fe^Ⅲ仅降低了2.3%	〔37〕
	氢醌（HQ），对苯醌（1，4-BQ）	5 mmol/L	反应40 min，Fe^Ⅱ浓度可维持在总铁的90%，而传统Fenton产生占总铁95%的Fe^Ⅲ	〔46〕
	富勒醇	10 mg/L	投加40 μmol/L Fe^Ⅲ，经30 min还原产生10 μmol/L Fe^Ⅱ	〔48〕
	3-羟基邻氨基苯甲酸（3-HAA）	10 μmol/L	Fe^Ⅲ与H₂O₂反应的表观活化能从106.8 kJ/mol降低到64.8 kJ/mol，亚甲基蓝脱色率提高了30%	〔49〕
无机物	MoS₂	0.3 g/L	Fe^Ⅱ有效再生，初始投加量低至0.07 mmol/L	〔53〕
	Mo⁰	50 mg/L钼粉	30 min后体系中Fe^Ⅱ占总铁近1/2	〔56〕
	NiFe₂O₄	2 g/L	Ni²⁺/Ni³⁺与Fe^Ⅱ/Fe^Ⅲ双循环，体系在330 min内降解95%的苯酚	〔57〕
	CeO₂	100 mg/L nano⁃Fe⁰-CeO₂	Ce³⁺/Ce⁴⁺和Fe^Ⅱ/Fe^Ⅲ双循环，体系在10 min内降解40%的双氯芬酸	〔58〕
	Pd@Fe₃O₄@MOF	0.5 g/L	反应150 min，Pd@Fe₃O₄表面的Fe^Ⅱ仅降低了5%	〔59〕
	H₂	0.1 MPa	Fe^Ⅱ有效再生，初始投加量低至1 mg/L	〔9〕
	H₂	85 mL/min	投加25 μmol/L Fe^Ⅲ，180 min还原产生24 μmol/L Fe^Ⅱ，对氯苯酚完全降解	〔63〕
	HSO₃ ^-	0.3 mmol/L	投加0.1 mmol/L Fe^Ⅲ，5 min即可产生0.08 mmol/L Fe^Ⅱ	〔64〕
	B	100 mg/L硼晶体	投加20 μmol/L Fe^Ⅲ，15 min内可还原产生7 μmol/L Fe^Ⅱ	〔65〕

物质种类		投加量	Fe^Ⅲ/Fe^Ⅱ循环	参考文献
有机物	原儿茶酸（PCA）	0.1 mmol/L	Fe^Ⅱ在Fe^Ⅲ/PCA/H₂O₂中再生速率是（279±6） L/（mol·s）；在Fe^Ⅱ/H₂O₂中仅为63~76 L/（mol·s）	〔32〕
	抗坏血酸（Acs）	1.0×10^-3 mol/L	投加0.4 g/L赤铁矿纳米片，经300 min还原产生40 μmol/L Fe^Ⅱ，甲草胺降解率可提高到70%	〔33〕
	巯基乙酸（TGA）	2 mmol/L	c（TGA）/c（Fe^Ⅲ）=2.0，30 min可产生160 μmol/L Fe^Ⅱ	〔34〕
	聚多巴胺（PDA）	0.2 g/L Fe₃O₄@PDA	Fe^Ⅱ有效再生，初始投加量低至0.18 mmol/L	〔36〕
	三乙醇胺（TEA）	200 mg/L TEA/GO@Fe₃O₄	反应35 min后，Fe^Ⅱ/Fe^Ⅲ仅降低了2.3%	〔37〕
	氢醌（HQ），对苯醌（1，4-BQ）	5 mmol/L	反应40 min，Fe^Ⅱ浓度可维持在总铁的90%，而传统Fenton产生占总铁95%的Fe^Ⅲ	〔46〕
	富勒醇	10 mg/L	投加40 μmol/L Fe^Ⅲ，经30 min还原产生10 μmol/L Fe^Ⅱ	〔48〕
	3-羟基邻氨基苯甲酸（3-HAA）	10 μmol/L	Fe^Ⅲ与H₂O₂反应的表观活化能从106.8 kJ/mol降低到64.8 kJ/mol，亚甲基蓝脱色率提高了30%	〔49〕
无机物	MoS₂	0.3 g/L	Fe^Ⅱ有效再生，初始投加量低至0.07 mmol/L	〔53〕
	Mo⁰	50 mg/L钼粉	30 min后体系中Fe^Ⅱ占总铁近1/2	〔56〕
	NiFe₂O₄	2 g/L	Ni²⁺/Ni³⁺与Fe^Ⅱ/Fe^Ⅲ双循环，体系在330 min内降解95%的苯酚	〔57〕
	CeO₂	100 mg/L nano⁃Fe⁰-CeO₂	Ce³⁺/Ce⁴⁺和Fe^Ⅱ/Fe^Ⅲ双循环，体系在10 min内降解40%的双氯芬酸	〔58〕
	Pd@Fe₃O₄@MOF	0.5 g/L	反应150 min，Pd@Fe₃O₄表面的Fe^Ⅱ仅降低了5%	〔59〕
	H₂	0.1 MPa	Fe^Ⅱ有效再生，初始投加量低至1 mg/L	〔9〕
	H₂	85 mL/min	投加25 μmol/L Fe^Ⅲ，180 min还原产生24 μmol/L Fe^Ⅱ，对氯苯酚完全降解	〔63〕
	HSO₃ ^-	0.3 mmol/L	投加0.1 mmol/L Fe^Ⅲ，5 min即可产生0.08 mmol/L Fe^Ⅱ	〔64〕
	B	100 mg/L硼晶体	投加20 μmol/L Fe^Ⅲ，15 min内可还原产生7 μmol/L Fe^Ⅱ	〔65〕

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