紫外活性铁碳微电解和过硫酸钾降解含聚丙烯酰胺废水

doi:10.13809/j.cnki.cn32-1825/te.2025.05.017

摘要/Abstract

摘要：

聚丙烯酰胺（PAM）是一种常用的直链有机聚合物，具有良好的抗剪切性、絮凝性、分散性、减阻等特性。PAM主要用于土壤改良、医学、石油化工和环保。预测至2030年，化石燃料和可再生能源仍将是主要能源（67.8×10¹⁶ J，其中化石燃料占总能源消耗的78%）。过去的40 a里，聚合物驱油技术已经在边际油田进行，并已被证明在许多情况下是成功的。大多数聚合物驱油项目都选择了部分水解的聚丙烯酰胺和石油磺酸盐。然而，聚丙烯酰胺可以自然降解为芳环酰胺单体，有很大的毒性。含PAM废水的净化方法主要包括物理方法（絮凝、热降解、机械剪切降解、膜分离）、生物法和化学方法。铁/碳（Fe/C）微电解是高级氧化工艺中广泛应用的水处理技术之一，已成功证明是一种高效、低成本的方法处理各种废水和土壤，包括染料废水、有机废水、含砷、氟废水。研究通过紫外活性铁碳微电解测定了聚丙烯酰胺溶液在不同pH值、反应时间、K₂S₂O₈浓度和紫外线功率的COD（化学需氧量）去除率。实验结果表明，365 nm紫外光下的COD去除率分别高于395 nm和405 nm。通过测定COD去除率和氧化铁沉淀质量，K₂S₂O₈添加水平的浮动确定为1 mmol/L。中心复合材料设计响应面显示，pH值、反应时间、K₂S₂O₈浓度和紫外线功率对COD去除率有显著影响。回归模型表明，决定系数R²为0.778 9，表明该模型与实验结果相吻合。聚丙烯酰胺溶液降解的最佳工艺条件为：pH值为3.01，反应时间为3 h，K₂S₂O₈浓度为1.4 mmol/L，紫外线功率为30 W。在此条件下，COD去除率为90.2%，实现了聚丙烯酰胺有效的清除。

关键词: 聚丙烯酰胺, 铁/碳微电解, K₂S₂O₈, 紫外反应面法, COD去除率

Abstract:

Polyacrylamide (PAM) is a commonly used straight-chain organic polymer with good shear resistance, flocculation, dispersibility, and drag-reducing effect. It is mainly used in soil improvement, medicine, petrochemical industry, and environmental protection. By 2030, fossil fuels and renewable energy are projected to remain the primary energy sources (67.8×10¹⁶ J in total, with fossil fuels accounting for 78% of the total energy consumption). Over the past 40 years, polymer flooding technology has been applied in marginal oil fields and has proven effective in many cases. Most polymer flooding projects have employed partially hydrolyzed PAM and petroleum sulfonates. However, PAM can naturally degrade into aromatic amide monomers, which are highly toxic to humans. The purification methods of PAM-containing wastewater mainly include physical methods (flocculation, thermal degradation, mechanical shear degradation, and membrane separation), biological methods, and chemical methods. Among them, iron/carbon (Fe/C) micro-electrolysis, one of the widely used water treatment technologies in advanced oxidation processes, has been demonstrated as an efficient and low-cost method to treat various types of wastewaters and contaminated soils, including dye wastewater, organic wastewater, arsenic-containing, and fluoride-containing wastewater. Using ultraviolet (UV)-activated Fe/C micro-electrolysis, the study determined the chemical oxygen demand (COD) removal rates of PAM solution under different pH values, reaction times, K₂S₂O₈ concentrations, and UV powers. The experimental results showed that the COD removal rate under 365 nm UV irradiation was higher than that under 395 nm and 405 nm. Based on the measurements of the COD removal rate and the mass of iron oxide precipitates, the K₂S₂O₈ dosage fluctuation range was determined to be 1 mmol/L. The central composite design (CCD) approach-based response surface methodology (RSM) analysis showed that pH, reaction time, K₂S₂O₈ concentration, and UV power had significant effects on COD removal rate. The regression model yielded a coefficient of determination (R₂) of 0.778 9, indicating good agreement between the model and experimental results. The optimal conditions for PAM solution degradation were identified as pH 3.01, a reaction time of 3 h, a K₂S₂O₈ concentration of 1.4 mmol/L, and a UV power of 30 W. Under these conditions, the COD removal rate reached 90.2%, achieving effective removal of PAM.

Key words: Polyacrylamide, Iron/carbon microelectrolysis, K₂S₂O₈, UV reaction surface method, COD removal rate

中图分类号:

TE53

黄尧奇,赵忠敏. 紫外活性铁碳微电解和过硫酸钾降解含聚丙烯酰胺废水[J]. 油气藏评价与开发, 2025, 15(5): 881-890.

HUANG Yaoqi,ZHAO Zhongmin. Degradation of polyacrylamide-containing wastewater by ultraviolet-activated iron-carbon micro-electrolysis and potassium persulfate[J]. Petroleum Reservoir Evaluation and Development, 2025, 15(5): 881-890.

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变量	编码级别
变量	-2	-1	0	1	2
pH值	3.0	3.5	4.0	4.5	5.0
反应时间/h	1.0	1.5	2.0	2.5	3.0
K₂S₂O₈剂量/（mmol/L）	0.6	0.8	1.0	1.2	1.4
紫外线功率/W	6	12	18	24	30

序号	pH值	反应时间/h	K₂S₂O₈剂量/（mmol/L）	紫外线功率/W	COD 去除率/%
1	3.5	1.5	1.2	12	50.20
2	4.0	2.0	1.0	18	57.32
3	4.0	2.0	1.0	18	53.40
4	4.0	2.0	1.0	18	56.63
5	4.5	2.5	1.2	12	57.49
6	4.0	1.0	1.0	18	29.00
7	4.0	2.0	1.4	18	62.49
8	4.5	1.5	1.2	24	47.20
9	4.5	1.5	0.8	24	34.51
10	3.5	1.5	1.2	24	60.74
11	4.5	1.5	0.8	12	31.62
12	3.5	2.5	1.2	24	80.91
13	4.0	2.0	1.0	6	38.43
14	3.5	2.5	0.8	12	65.26
15	4.0	2.0	1.0	30	62.60
16	4.0	3.0	1.0	18	71.81
17	4.5	1.5	1.2	12	45.60
18	3.5	2.5	1.2	12	73.69
19	4.5	2.5	1.2	24	73.26
20	3.5	1.5	0.8	24	48.09
21	4.5	2.5	0.8	24	52.69
22	4.5	2.5	0.8	12	49.37
23	3.5	1.5	0.8	12	48.00
24	3.0	2.0	1.0	18	62.50
25	4.0	2.0	1.0	18	57.21
26	5.0	2.0	1.0	18	26.64
27	3.5	2.5	0.8	24	69.81
28	4.0	2.0	1.0	18	58.71
29	4.0	2.0	0.6	18	49.83
30	4.0	2.0	1.0	18	57.31

参数类别	平方和	自由度	均方值	方差比例值	概率值
COD去除率模型	4 753.47	10	475.35	18.24	<0.000 1	重要的
pH值	1 300.66	1	1 300.66	49.90	<0.000 1
反应时间	2 442.99	1	2 442.99	93.72	<0.000 1
K₂S₂O₈浓度	551.62	1	551.62	21.16	0.000 2
紫外线功率	370.68	1	370.68	14.22	0.001 3
pH值-反应时间	4.80	1	4.80	0.18	0.672 8
pH值-K₂S₂O₈浓度	27.51	1	27.51	1.06	0.317 2
pH值-紫外线功率	0.087	1	0.087	0.003	0.954 5
反应时间-K₂S₂O₈浓度	2.81	1	2.81	0.11	0.746 4
反应时间-紫外线功率	15.48	1	15.48	0.59	0.450 3
K₂S₂O₈剂量-紫外线功率	36.84	1	36.84	1.41	0.249 1
残余	495.27	19	26.07
缺乏适应度	479.34	14	34.24	10.75	0.008 0	重要的
纯错误	15.93	5	3.19
总计	5 248.74	29