京津冀地区工业区土壤中多环芳烃的污染特征、源解析及生物因子相关性

doi:10.16258/j.cnki.1674-5906.2023.11.006

生态环境学报 ›› 2023, Vol. 32 ›› Issue (11): 1952-1963.DOI: 10.16258/j.cnki.1674-5906.2023.11.006

京津冀地区工业区土壤中多环芳烃的污染特征、源解析及生物因子相关性

许明(), 张馥颖, 孙露露, 周增幸, 林超霸, 朱雪竹^*()

南京农业大学资源与环境科学学院，江苏南京 210095

收稿日期:2022-03-24 出版日期:2023-11-18 发布日期:2024-01-17
通讯作者: * 朱雪竹。E-mail: zhuxuezhu@njau.edu.cn
作者简介:许明（1996年生），男，硕士研究生，研究方向为环境污染控制与生物修复研究。E-mail: 3220225213@bit.edu.cn
基金资助:
国家重点研发计划项目(2019YFC1804301)

Pollution Characteristics, Source Analysis and Correlation of Biological Factors of Polycyclic Aromatic Hydrocarbons in Soils of Industrial Areas in Beijing-Tianjin-Hebei Region

XU Ming(), ZHANG Fuying, SUN Lulu, ZHOU Zengxing, LIN Chaoba, ZHU Xuezhu^*()

School of Resources and Environmental Sciences, Nanjing Agricultural University, Nanjing 210095, P. R. China

Received:2022-03-24 Online:2023-11-18 Published:2024-01-17

摘要/Abstract

摘要：

调查京津冀地区工业土壤污染的状况及其与土壤生物因子的相互关系，为后续环境监测及修复提供参考。在京津冀地区代表性工业园区采集土壤样品，分析其中半挥发有机污染和土壤生物状况。土壤采集点周边的工业产业涵盖了金属冶炼及压延加工业，石油加工业、炼焦及核燃料加工业，交通运输设备制造业，化学原料及化学制品制造业等北方地区典型重工业产业。结果表明，芘（Pyrene，Pyr）、荧蒽（Fluoranthene，Flu）、邻苯二甲酸二（2-二乙基己基）酯（Bis(2-diethylhexyl) Phthalate，DEHP）检出排名前3，分别有98.4%、98.4%、96.9%的点位浓度高于检出限，其最高质量分数分别为2.84、2.79、5.72 mg∙kg⁻¹。土壤中多环芳烃（Polycyclic Aromatic Hydrocarbons，PAHs）以4－6环PAHs为主，∑₁₆PAHs质量分数中位值为0.67 mg∙kg⁻¹，约有90.6%的样品中苯并[a]芘（Benzo[a]pyrene，BaP）的浓度高于检出限。荧蒽、芘、苯并[a]蒽（Benzo[a]anthracene，BaA）、䓛（Chrysene，Chr）、苯并[b]荧蒽（Benzo[b]fluoranthene，BbF）、苯并[k]荧蒽（Benzo[k]fluoranthene，BkF）、BaP对土壤中PAHs污染方差的贡献率高达52.9%。结合特征比值法与主成分分析法得出液体化石燃料燃烧产生的PAHs占土壤PAHs来源的79.7%。微生物量碳（Microbial Biomass Carbon，MBC）、微生物量氮（Microbial Biomass Nitrogen，MBN）在0－20 cm处与2－3环和∑₁₆PAHs呈显著负相关（r= −0.4，P=0.023），在20－40 cm土壤中蔗糖酶活性与LMW-PAHs（r=0.51，P=0.006）和HMW-PAHs（r=0.53，P=0.005）呈显著正相关。研究成果可为评估土壤有机污染环境归趋提供依据。

关键词: 京津冀, 产业类型, 土壤有机污染, PAHs源解析, 生物因子

Abstract:

In order to investigate the pollution of industrial soils and its relationship with soil biological factors, and to provide a reference for subsequent environmental monitoring and remediation. Soil samples were collected from the representative industrial parks in Beijing-Tianjin-Hebei region to analyze the semi-volatile organic pollution and soil biological factor activity. The industries around the soil sample sites included metal smelting and rolling processing industry, petroleum processing, coking and nuclear fuel processing industry, transportation equipment manufacturing industry, chemical raw material and chemical product manufacturing industry, which are four typical heavy industries in northern China. The results showed that the detection rates of pyrene (Pyr), fluoranthene (Flu), and bis (2-diethylhexyl) phthalate (DEHP) were the top three among the semi-volatile organic pollutants, with the detection rates of 98.4%, 98.4%, and 96.9%, and the maximum mass fractions were 2.84, 2.79 and 5.72 mg∙kg⁻¹, respectively. PAHs with 4‒6 rings were the popular PAHs, and the detection rate of benzo(a)pyrene (BaP), a type of carcinogen, was 90.6%. The median mass fraction of ∑₁₆PAHs was 0.67 mg∙kg⁻¹. The variance contribution rate of Flu, Pyr, benzo[a]anthracene (BaA), chrysene (Chr), benzo[b]fluoranthene (BbF), benzo[k]fluoranthene (BkF) and BaP to PAHs pollution in soils was 52.9%. According to the results of the characteristic ratio method and the principal component analysis, the PAHs produced by combustion of liquid fossil fuels accounted for 79.7% of the source of soil PAHs. Microbial biomass carbon (MBC) and microbial biomass nitrogen (MBN) were significantly and negatively correlated with the concentrations of PAHs with 2‒3 rings and ∑₁₆PAHs in soils with depth at 0‒20 cm (r=−0.4, P=0.023). The activity of invertase was significantly and negatively correlated with the concentrations of LMW PAHs (r=0.51，P=0.006), HMW PAHs (r=0.53, P=0.005) in 20‒40 cm soils. These results would provide a basis for evaluating the environmental fate of soil organic pollution.

Key words: Beijing-Tianjin-Hebei, industry types, soil organic pollution, PAHs source analysis, biological factors

中图分类号:

许明, 张馥颖, 孙露露, 周增幸, 林超霸, 朱雪竹. 京津冀地区工业区土壤中多环芳烃的污染特征、源解析及生物因子相关性[J]. 生态环境学报, 2023, 32(11): 1952-1963.

XU Ming, ZHANG Fuying, SUN Lulu, ZHOU Zengxing, LIN Chaoba, ZHU Xuezhu. Pollution Characteristics, Source Analysis and Correlation of Biological Factors of Polycyclic Aromatic Hydrocarbons in Soils of Industrial Areas in Beijing-Tianjin-Hebei Region[J]. Ecology and Environment, 2023, 32(11): 1952-1963.

图/表 11

图1 京津冀采样点位布置示意图

Figure 1 Layout of sampling sites in Beijing-Tianjin-Hebei

表1 特征比值和排放源的关系

Table 1 Relationship between characteristic ratio and emission source

特征比值	比值范围	指示污染物
m_(An)/m_(An+Phe)	<0.1	石油源
	>0.1	燃烧源
	<0.4	石油源
m_(Flu)/m_(Flu+Pry)	0.4‒0.5	液体化石燃料燃烧
	>0.5	煤、生物质燃烧
	<0.2	石油源
m_(InP)/m_(InP+BgP)	0.2‒0.4	液体化石燃料燃烧
	>0.4	煤、生物质燃烧
	<0.2	石油源
m_(BaA)/m_(BaA+Chr)	0.2‒0.5	液体化石燃料燃烧
m_(BaA)/m_(BaA+Chr)	>0.5	煤、生物质燃烧

表2 各行业周边土壤污染状况

Table 2 Pollutants in the soil around different industries

行业类型	污染物高于检出限的点位占比	BaP高于检出限的点位占比	质量分数最高的污染物		污染指数最高的污染物
行业类型	污染物高于检出限的点位占比	BaP高于检出限的点位占比	名称	w/(mg∙kg⁻¹)	名称	污染指数
金属冶炼及压延加工制造业	100	84.21	BgP	2.16	BaP	0.40
石油加工、炼焦及核燃料加工制造业	100	92.86	BgP	18.92	BaP	1.48
交通运输设备制造业	100	88.89	BbF	6.12	BaP	2.99
化学原料和化学制品制造业	100	100	DEHP	5.72	BaP	1.36

图2 各采样点土壤中PAHs污染将16种PAHs分成三类：低分子量PAHs为（Low Molecular Weight Polycyclic Aromatic Hydrocarbons，LMW-PAHs），包含2环和3环；中分子量PAHs为（Medium Molecular Weight Polycyclic Aromatic Hydrocarbons，MMW-PAHs），为4环；高分子量PAHs为（High Molecular Weight Polycyclic Aromatic Hydrocarbons，HMW-PAHs），包含5环和6环（Wang et al.，2020）

Figure 2 Polycyclic aromatic hydrocarbon pollution in the soil of the industrial park

表3 工业区周边土壤PAH10质量分数及BaP毒性当量质量分数

Table 3 Mass fraction of PAH10 and BaP toxic equivalent concentration in the surrounding soil of the industrial area mg?kg?1

PAHs	荷兰最大允许质量分数	均值	毒性当量因子	超标率/%	最大超标倍数
Nap	0.14	0.037	0.001	3.1	11.31
Phe	0.51	0.178	0.001	12.5	3.56
An	0.12	0.027	0.01	9.4	2.88
Flu	2.6	0.249	0.001	1.6	1.07
BaA	0.25	0.138	0.1	17.2	9.55
Chr	10.7	0.180	0.01	0	－
BkF	2.4	0.123	0.1	0	－
BaP	0.26	0.242	1	20.3	17.26
InP	7.5	0.284	0.1	0	－
BgP	5.9	0.894	0.01	3.1	3.21
∑₁₀PAHs	－	2.337	－	－	－
TEQ(BaP)₁₀	0.033	0.308	－	65.6	150.48

图3 不同城市（a）和不同行业（b）的PAHs组成

Figure 3 Composition of PAHs in different cities (a) and industries (b)

图4 特征比值法分析土壤PAHs来源

Figure 4 Source analysis of PAHs in soils by characteristic ratio method

表4 土壤中PAHs主成分方差贡献率

Table 4 Principal component variance contribution rate

PAHs	PC1	PC2	PC3
Nap	−0.073	0.698	0.006
Ace	0.185	0.951	−0.055
Acy	0.24	0.882	−0.044
Fl	0.161	0.955	−0.021
Phe	0.409	0.878	−0.034
An	0.475	0.748	−0.033
Flu	0.872	0.423	−0.033
Pyr	0.947	0.229	−0.028
BaA	0.962	0.177	−0.048
Chr	0.937	0.264	−0.056
BbF	0.952	0.14	0.181
BkF	0.965	0.1	0.161
BaP	0.972	0.056	0.143
Inp	0.072	−0.036	0.995
DBA	0.058	−0.041	0.996
BgP	0.053	−0.038	0.994
特征值	8.463	3.550	2.608
方差贡献率/%	52.893	22.186	16.297
累积方差贡献率/%	52.893	75.080	91.377

图5 主成分分析法分析土壤PAHs来源用KMO和巴特利特球形度检验描述相关性矩阵，最大收敛迭代次数为25，提取特征值大于1的数值，并进行方差最大正交旋转。正交旋转后结果KMO取样适切性量数为0.703，巴特利特球形度检验显著性为0.000

Figure 5 Source analysis of PAHs in soils by principal component analysis method

图6 PAHs与生物因子主成分分析

Figure 6 Principal component analysis of PAHs and biological factors

图7 PAHs与生物因子相关性分析

Figure 7 Correlation analysis between PAHs and biological factors

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京津冀地区工业区土壤中多环芳烃的污染特征、源解析及生物因子相关性

Pollution Characteristics, Source Analysis and Correlation of Biological Factors of Polycyclic Aromatic Hydrocarbons in Soils of Industrial Areas in Beijing-Tianjin-Hebei Region

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