Degradation of reactive yellow K-RN by electricity/potassium permanganate/peroxymonosulfate system and its mechanism

doi:10.16085/j.issn.1000-6613.2023-1697

Abstract

Abstract:

The removal of organic dyes in printing and dyeing wastewater has been a difficult problem in water treatment technology for a long time. Electricity/potassium permanganate/peroxymonosulfate (EC/PM/PMS) system can efficiently degrade refractory organic dyes, such as reactive yellow K-RN. However, the degradation mechanism, especially the activation mechanism of Mn in relation to PMS, remains unclear. Therefore, this paper studied the types and production pathways of active substances in EC/PM/PMS system, and determined the action mechanism of Mn and the activation process of PMS during printing and dyeing wastewater treatment. Results showed that EC/PM/PMS system is a composite system including free radical oxidation and non-free radical oxidation. During this process, PMS activates Mn (‍Ⅴ), Mn (‍Ⅵ) and amorphous manganese dioxide, resulting in the reduction of PM. In addition, reactive oxygen radical oxidation is the main degradation path accounting for 95.3%, while electrode direct oxidation and non-free radical oxidation account for 2.1% and 2.6%, respectively.

Key words: electrochemical, potassium permanganate, peroxymonosulfate, reactive yellow K-RN, radical

摘要：

印染废水中的有机染料处理在水处理技术中长久以来都是一大难题，电/高锰酸钾/过一硫酸盐体系（EC/PM/PMS体系）可以高效地降解活性黄K-RN等难降解有机污染物，但其降解机制还尚未明确，且锰类物质能否活化PMS产生活性物质以及PMS活化机理还需进一步探究。因此，本文研究了EC/PM/PMS体系在降解印染废水时活性物质的类别和产生途径，同时确定了锰类物质在其中的作用机理和PMS的活化过程。结果表明，EC/PM/PMS体系是一种包含自由基氧化和非自由基氧化的复合体系，体系中由PM还原生成五价锰、六价锰和无定形二氧化锰活化PMS。此外，明确了活性氧类自由基氧化是活性黄K-RN降解的主要路径，占比为95.3%，电极直接氧化占比2.1%，非自由基氧化占比仅为2.6%。

关键词: 电化学, 高锰酸钾, 过一硫酸盐, 活性黄K-RN, 自由基

CLC Number:

X703.5

MA Chao, SUN Zhihua, WANG Lei, JI Yu, CHEN Cuizhong, WANG Jiankang, ZHAO Chun. Degradation of reactive yellow K-RN by electricity/potassium permanganate/peroxymonosulfate system and its mechanism[J]. Chemical Industry and Engineering Progress, 2024, 43(10): 5958-5968.

马超, 孙志华, 王蕾, 姬钰, 陈翠忠, 王健康, 赵纯. 电/高锰酸钾/过一硫酸盐体系降解活性黄K-RN及其机理[J]. 化工进展, 2024, 43(10): 5958-5968.

Figures/Tables 22

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体系	5min去除率/%	120min矿化率/%
EC	2.06	1.7
PM	0.23	0.47
PMS	1.83	3.60
EC/PM	4.57	6.69
EC/PMS	5.64	4.54
PM/PMS	24.18	12.41
EC/PM/PMS	60.53	47.96

体系	5min去除率/%	120min矿化率/%
EC	2.06	1.7
PM	0.23	0.47
PMS	1.83	3.60
EC/PM	4.57	6.69
EC/PMS	5.64	4.54
PM/PMS	24.18	12.41
EC/PM/PMS	60.53	47.96

捕获剂	反应速率常数/L²·mol^-1·s^-1
捕获剂	^•OH	SO₄^-•	¹O₂	^•O₂^-	PM
MeOH	9.7×10⁸	2.5×10⁷	3.0×10³	1.1×10⁷	—
TBA	6.0×10⁸	7.6×10⁵	1.8×10³	<10³	—

捕获剂	反应速率常数/L²·mol^-1·s^-1
捕获剂	^•OH	SO₄^-•	¹O₂	^•O₂^-	PM
MeOH	9.7×10⁸	2.5×10⁷	3.0×10³	1.1×10⁷	—
TBA	6.0×10⁸	7.6×10⁵	1.8×10³	<10³	—

反应体系	降解路径	k_obs/10^-3min^-1	占比/%
EC	—	5.30	—
EC（MeOH）	甲	5.30	2.1
—	乙	—	95.3
—	丙	—	2.6
EC/PM/PMS（MeOH）	甲+丙	11.84	4.8
EC/PM/PMS	甲+乙+丙	249.52	100