生物炭负载纳米铁活化过硫酸盐去除土壤中的五氯联苯

doi:10.16258/j.cnki.1674-5906.2024.02.012

生态环境学报 ›› 2024, Vol. 33 ›› Issue (2): 282-290.DOI: 10.16258/j.cnki.1674-5906.2024.02.012

• 研究论文【环境科学】 • 上一篇下一篇

生物炭负载纳米铁活化过硫酸盐去除土壤中的五氯联苯

丛鑫(), 曹平, 王晓博

辽宁工程技术大学环境科学与工程学院，辽宁阜新 123000

收稿日期:2023-10-31 出版日期:2024-02-18 发布日期:2024-04-03
作者简介:丛鑫（1976年生）女，教授，博士，研究方向为土壤环境化学和生态修复。E-mail: congxin1800@163.com
基金资助:
国家重点研发计划项目(2019YFC1803800)

Degradation of Pentachlorobiphenyl in Soil Using Persulfate Activated by Biochar-supported Nano Zero-valent Iron

CONG Xin(), CAO Ping, WANG Xiaobo

College of Environmental Science and Engineering, Liaoning Technical University, Fuxin 123000, P. R. China

Received:2023-10-31 Online:2024-02-18 Published:2024-04-03

摘要/Abstract

摘要：

以污染土壤中检出量较高的PCB118为目标污染物，采用银杏叶提取液绿色合成纳米铁材料（nZVI）、玉米秸秆制备生物炭（BC），将nZVI负载在BC表面合成生物炭负载纳米零价铁复合材料（BC-nZVI），利用制备的BC-nZVI复合材料催化活化过硫酸盐（PS）去除土壤中PCB118。主要探讨了在生物炭负载纳米零价铁活化过硫酸盐体系（BC-nZVI/PS）中复合材料BC-nZVI碳铁比及其投加量、PS浓度、pH值、温度等因素对PCB118去除速率的影响。结果表明，反应时间为24 h时，碳铁比为2꞉1时BC-nZVI反应体系对土壤中PCB118去除效果优于其他3种比例。实验条件下，随着BC-nZVI的投加量由0.002 g增加到0.500 g，PS浓度由0.05 mol·L⁻¹增至0.35 mol·L⁻¹，温度由15 ℃升高到45 ℃，土壤中PCB118的去除率分别增加了32.4%、10.6%及14.7%。随着溶液初始pH值由3升到9，土壤中PCB118的去除率降低了11.4%。单因素实验数据显示，在BC-nZVI的投加量为0.500 g，PS浓度为0.35 mol·L⁻¹，pH值为3，温度为45 ℃的条件下，土壤中PCB118去除效果最佳。为分析不同因素及其交互作用对土壤中PCB118去除率的影响，采用Box-Behnken响应面法设计了三因素三水平试验，建立了PS浓度、温度和pH等3个变量的二次多项式回归模型，得到土壤中PCB118最佳去除条件为：PS浓度0.23 mol·L⁻¹、pH 3.11、温度45 ℃。在此条件下，土壤中的PCB118在BC-nZVI/PS体系中去除率为71.6%。实验验证结果与模型预测值的相对偏差<5%，表明可使用此模型对BC-nZVI/PS体系中PCB118的去除率进行预测。该研究可为土壤中PCB118污染治理提供一些基础数据，为绿色环保修复土壤中有机污染物提供理论参考。

关键词: 五氯联苯, 生物炭, 植物提取液, 纳米零价铁, 过硫酸盐

Abstract:

The biochar-supported nano zero-valent iron composite materials (BC-nZVI), synthesized by loading nano zero-valent iron (nZVI) on the surface of biochar (BC), was used to remediate soil contaminated with polychlorinated biphenyls (PCBs). The green nZVI was prepared with the extraction solution from ginkgo leaves, and the BC was prepared with corn straw. The prepared BC-nZVI composite material was used to catalyze the activation reaction of persulfate (PS) to remove PCB118, which was highly detected in soil. Various factors affecting the removal rate of PCB118 in the activated persulfate system (BC-nZVI/PS) were mainly discussed, such as the iron-carbon ratio and its dosage in composite material BC-nZVI, PS concentration, pH value, and temperature. The results showed that when the reaction time was 24 h and the carbon-iron ratio was 2꞉1, the BC-nZVI reaction system had a better removal effect on PCB118 compared to the other three ratios. Under experimental conditions, as the dosage of BC-nZVI increased from 0.002 g to 0.500 g, the PS concentration increased from 0.05 mol·L⁻¹ to 0.35 mol·L⁻¹, and temperature increased from 15 ℃ to 45 ℃, the removal rate of PCB118 increased by 32.4%, 10.6%, and 14.7%, respectively. As the initial pH value of the solution increased from 3 to 9, the removal rate of PCB118 decreased by 11.4%. Experimental data of single factor showed that the removal effect of PCB118 in the soil was the best under conditions of BC-nZVI dosage of 0.500 g, PS concentration of 0.35 mol·L⁻¹, pH value of 3, and temperature of 45 ℃. To analyze the impact of different factors and their interactions on the removal rate of PCB118 in soil, the Box Behnken response surface method was used to design a three-factor three-level experiment. A quadratic polynomial regression model was established for three variables: PS concentration, temperature, and pH. According to the model, the optimal removal conditions for PCB118 were as follows: PS concentration of 0.23 mol·L⁻¹, pH of 3.11, temperature of 45 ℃. Under these conditions, the removal rate of PCB118 in the BC-nZVI/PS system was 71.6%. The relative deviation between the experimental verification results and the predicted values of the model was less than 5%, suggesting that this model could be used to predict the removal rate of PCB118 in the BC-nZVI/PS system. This study might provide some basic data for the control of PCB118 in soil and provide theoretical references for the green and environmentally friendly remediation of organic pollutants in soil.

Key words: pentachlorobiphenyl, biochar, plant extract, nano zero-valent iron, persulfate

中图分类号:

丛鑫, 曹平, 王晓博. 生物炭负载纳米铁活化过硫酸盐去除土壤中的五氯联苯[J]. 生态环境学报, 2024, 33(2): 282-290.

CONG Xin, CAO Ping, WANG Xiaobo. Degradation of Pentachlorobiphenyl in Soil Using Persulfate Activated by Biochar-supported Nano Zero-valent Iron[J]. Ecology and Environment, 2024, 33(2): 282-290.

图/表 9

表1 响应面优化实验因素水平表

Table 1 The factors and levels of response surface optimization test

水平	实验因素
水平	A: PS浓度/(mol·L⁻¹)	B: 温度/℃	C: pH
−1	0.05	25	1
0	0.20	35	3
1	0.35	45	5

图1 3种制备材料扫描电镜图片

Figure 1 Scanning electron microscopy images of three preparation materials

图2 BC-nZVI不同碳铁比及投加量条件下土壤中PCB118去除曲线

Figure 2 Removal curve of PCB118 in soil at different BC-nZVI dosages and different carbon iron ratio

图3 不同PS浓度条件下土壤中PCB118去除曲线

Figure 3 Removal curve of PCB118 in soil at different PS concentration

图4 不同pH条件下土壤中PCB118去除曲线

Figure 4 Removal curve of PCB118 in soil at different pH

图5 不同温度条件下土壤中PCB118去除曲线

Figure 5 Removal curve of PCB118 in soil at different temperatures

表2 响应面实验设计与结果

Table 2 Experiment design and results of response surface

实验序号	PS浓度/(mol·L⁻¹)	温度/℃	pH	去除率/%	实验序号	PS浓度/(mol·L⁻¹)	温度/℃	pH	去除率/%
1	0.05	25	3	20.62	10	0.20	45	1	56.64
2	0.35	25	3	45.79	11	0.20	25	5	38.61
3	0.05	45	3	50.42	12	0.20	45	5	58.72
4	0.35	45	3	61.81	13	0.20	35	3	59.68
5	0.05	35	1	24.49	14	0.20	35	3	59.15
6	0.35	35	1	36.23	15	0.20	35	3	58.32
7	0.05	35	5	18.85	16	0.20	35	3	60.69
8	0.35	35	5	46.78	17	0.20	35	3	60.33
9	0.20	25	1	32.47

表3 回归模型方差分析

Table 3 The variance analysis of regression model

方差来源	模型	A	B	C	AB	AC	BC	失拟项
平方和	3645.38	726.38	1014.75	21.55	47.47	65.53	4.12	2.87
自由度	9	1	1	1	1	1	1	3
均方	405.04	726.38	1014.75	21.55	47.47	65.53	4.12	0.9583
F值	440.43	789.85	1103.42	23.43	51.62	71.25	4.48	1.08
P值	<0.0001	<0.0001	<0.0001	0.0019	0.0002	<0.0001	0.0721	0.4538
显著性	极显著	极显著	极显著	极显著	极显著	极显著	不显著	不显著

图6 反应温度、PS浓度与pH交互作用对PCB118去除率影响响应曲面及等高线图左侧为响应面图，右侧为等高线图

Figure 6 Response surface and contour plot of the interaction of reaction temperature, PS concentration, and pH on the removal rate of PCB118

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生物炭负载纳米铁活化过硫酸盐去除土壤中的五氯联苯

Degradation of Pentachlorobiphenyl in Soil Using Persulfate Activated by Biochar-supported Nano Zero-valent Iron

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