鲁中碳酸盐岩区土壤重金属污染特征及来源分析

姜冰; 孙增兵; 张德明; 王建; 刘阳

doi:10.11932/karst20250410

鲁中碳酸盐岩区土壤重金属污染特征及来源分析

doi: 10.11932/karst20250410

姜冰^{1, 2,},
孙增兵^{1, 2, ,},
张德明¹,
王建¹,
刘阳¹

1.
山东省第四地质矿产勘查院, 山东潍坊 261021
2.
山东省地质矿产勘查开发局海岸带地质环境保护重点实验室, 山东潍坊 261021

基金项目: 山东省地质矿产勘查开发局地质勘查引领示范项目(KC202207)

详细信息

作者简介:
姜冰（1984－），男，高级工程师，主要从事生态环境地球化学调查与研究。E-mail：jbing08@163.com

通讯作者:
孙增兵（1974－），男，教授级高级工程师，主要从事基础地质与地球化学研究。E-mail：sunzb0721@163.com。

中图分类号: X142；X53
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出版历程
- 收稿日期: 2022-07-20
- 录用日期: 2024-10-15
- 修回日期: 2024-07-28
- 网络出版日期: 2025-11-07
- 刊出日期: 2025-08-25

Pollution characteristics and sources of soil heavy metals in the carbonate rock region of central Shandong

JIANG Bing^{1, 2
,},
SUN Zengbing^{1, 2
, ,},
ZHANG Deming¹,
WANG Jian¹,
LIU Yang¹

1.
Shandong Provincial No.4 Institute of Geological and Mineral Survey, Weifang, Shandong 261021, China
2.
Key Laboratory of Coastal Zone Geological Environment Protection, Shandong Geology and Mineral Exploration and Development Bureau, Weifang, Shandong 261021, China

摘要

摘要: 碳酸盐岩区土壤重金属含量通常具有天然的高背景特征，会对土壤健康、农产品安全和生态环境构成威胁，因此，在土壤重金属高背景区开展污染特征研究和重金属来源识别，对环境保护和人类健康发展具有重要意义。以鲁中碳酸盐岩分布区为研究区域，分析测试了岩石、土壤、大气降尘中的重金属含量特征，采用富集因子法、主成分分析、模拟计算和相关分析等方法，研究了土壤重金属污染特征，探究了其来源，阐明了其影响因素。结果表明，研究区属土壤重金属含量高背景区，土壤重金属含量是岩石的2.76~6.82倍，大气降尘中As、Cr、Ni含量低于土壤，Cu、Pb、Zn、Hg、Cd含量高于土壤。土壤重金属污染程度低，平均污染程度由大到小依次为Hg、Cd、Ni、Cu、As、Zn、Pb、Cr。大气降尘对土壤重金属有所贡献，其导致的表层土壤Cd、Hg的年增长速率最大，分别为0.55%和0.20%。土壤有机质与Cd、Hg相关性最为显著，阳离子交换量与Cu、Pb、Zn、Cr、Ni、As相关性最为显著。总体来看，Cd、Hg主要受控于有机质，并叠加了降尘积累，Cu、Pb、Zn、Cr、Ni、As主要受控于成土母岩。
- 重金属 /
- 土壤 /
- 碳酸盐岩 /
- 大气降尘
Abstract: Soil heavy metals in carbonate rock regions often exhibit natural high-background characteristics due to secondary enrichment during pedogenesis, posing potential risks to soil health, agricultural product safety, and ecological sustainability. Understanding the pollution patterns and sources of heavy metals in such high-background zones is critical for formulating targeted environmental protection strategies and safeguarding human health. This study focused on the carbonate rock region of central Shandong, a typical northern Chinese karst region dominated by Cambrian-Ordovician limestone and dolomite as parent rocks. A comprehensive investigation was conducted by collecting and analyzing samples of rock, surface soil, vertical soil profile, and atmospheric dustfall. Multiple analytical methods, including Enrichment Factor (EF) analysis, Principal Component Analysis (PCA), annual heavy metal increment simulation from dustfall, and Pearson correlation analysis, were employed to explore the pollution characteristics, sources, and influencing factors of soil heavy metals. Carbonate rock regions are globally significant for their unique pedogenic processes, where heavy metals undergo secondary enrichment due to intense chemical weathering and leaching of carbonate minerals. This natural enrichment, combined with potential anthropogenic inputs (e.g., atmospheric dustfall), complicates the identification of heavy metal sources and their ecological impacts. Previous studies have primarily focused on single-medium (soil-only or rock-soil) analyses, lacking systematic multi-medium investigations. This study aimed to bridge this gap by integrating data on rock, soil, and atmospheric dustfall to comprehensively characterize the behavior of heavy metals in carbonate rock regions. The study area, located at the junction of the mountainous area in central Shandong and the northern Shandong plain, experiences a semi-humid continental monsoon climate characterized by distinct seasonal precipitation. Parent rocks are primarily carbonate (limestone and dolomite), with soil development dominated by chemical weathering. Soil samples were collected from natural woodlands and wilderness grasslands with minimal human disturbance. Rock samples were collected at the outcrop of bedrock. Atmospheric dustfall samples were collected over a one-year period of dry deposition. All samples were processed and analyzed in a certified laboratory, with heavy metal concentrations measured by Inductively Coupled Plasma Mass Spectrometry (ICP-MS), X-ray Fluorescence (XRF), and Atomic Fluorescence Spectrometry (AFS). Additionally, physicochemical properties, including pH, cation exchange capacity, and organic matter, were determined. The results show as follows: (1) The contents of soil heavy metals (Cu, Pb, Zn, Cr, Ni, As, Cd, and Hg) are 2.76 to 6.82 times higher than those in parent rocks. The contents of As, Cr, and Ni in atmospheric dustfall is lower than those in soil (enrichment coefficient between 0.47 and 0.65), while the contents of Cu, Pb, Zn, Hg, and Cd are higher (enrichment coefficient between 1.17 and 8.67), with Cd being the most significantly enriched. (2) The average pollution degree of soil heavy metals, ranked by EF values, is: Hg > Cd > Ni > Cu > As > Zn > Pb > Cr. Most metals exhibit low pollution levels (EF< 2), except for minor Hg cases (EF> 5). Cr and Ni show negligible anthropogenic influence (all EF< 2), while Cd and Hg have relatively higher EF values, indicating potential external inputs. (3) Atmospheric dustfall contribute to the accumulation of soil heavy metals, with annual growth rates calculated as follows: Cd (0.55%), Hg (0.20%), Zn (0.16%), and Pb (0.09%). Cd and Hg, with the highest growth rates, were more significantly affected by dust deposition. (4) Soil Organic Matter (SOM) is strongly correlated with Cd and Hg (P<0.01), showing similar vertical distribution patterns (surface accumulation). Cation Exchange Capacity (CEC) is significantly correlated with Cu, Pb, Zn, Cr, Ni, and As (P<0.01), with stable vertical variations. These results indicate that Cd and Hg are primarily controlled by SOM and superimposed by dustfall inputs, while Cu, Pb, Zn, Cr, Ni, and As are mainly derived from parent rock weathering. This study provides a systematic multi-media (rock-soil-dustfall) analysis of heavy metal behavior in carbonate rock regions, emphasizing the combined effects of natural parent materials and anthropogenic dustfall. By integrating enrichment factor analysis, PCA, dustfall increment simulation, and correlation analysis, we identified the sources and controlling factors of soil heavy metals. These findings provide scientific support for strategies of evidence-based soil pollution control in similar carbonate rock regions, particularly prioritizing the management of Cd and Hg based on their higher accumulation rates and anthropogenic contributions.
- heavy metals /
- soil /
- carbonate rock /
- atmospheric dustfall

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图 1 地质简图及采样点位

Figure 1. Geologic sketch map and sampling sites

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图 2 岩石重金属含量分布特征小提琴图

Figure 2. Violin plot of distribution characteristics of heavy metal contents in rock

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图 3 土壤重金属含量分布特征小提琴图

Figure 3. Violin plot of distribution characteristics of heavy metal contents in soil

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图 4 土壤理化性质与重金属在垂向上的变化规律

Figure 4. Vertical variation of soil physicochemical properties and heavy metals

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图 5 大气降尘重金属含量分布特征小提琴图

Figure 5. Violin plot of distribution characteristics of heavy metal contents in atmospheric dustfall

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图 6 土壤重金属富集因子箱线图

Figure 6. Box plot of enrichment factors of soil heavy metals

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图 7 旋转后的主成分空间载荷

Figure 7. Space load of main constituent after rotation

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图 8 土壤理化性质与重金属的相关性热图

Figure 8. Heat map of the correlation between soil physicochemical properties and heavy metals

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表 1 重金属含量及土壤理化性质特征

Table 1. Characteristics of heavy metal contents and soil physicochemical properties

重金属	岩石(n = 60)				土壤(n = 100)				大气降尘(n = 17)
重金属	最大值	最小值	平均值	变异系数	最大值	最小值	平均值	变异系数	最大值	最小值	平均值	变异系数
Cu/mg·kg⁻¹	20.90	3.69	7.72	0.44	78.50	16.90	29.57	0.29	62.0	11.2	34.55	0.37
Pb/mg·kg⁻¹	42.40	1.10	5.75	0.98	68.30	7.40	26.25	0.28	64.6	4.5	40.68	0.40
Zn/mg·kg⁻¹	53.60	3.70	16.09	0.69	243.00	42.90	77.13	0.31	427.0	50.0	202.88	0.49
Cr/mg·kg⁻¹	38.10	2.60	10.61	0.67	101.00	51.50	69.45	0.09	95.3	7.5	41.09	0.54
Cd/mg·kg⁻¹	0.180	0.010	0.033	0.85	0.340	0.067	0.170	0.26	2.16	0.54	1.48	0.31
Ni/mg·kg⁻¹	9.50	2.10	4.97	0.33	41.90	22.00	33.22	0.11	40.7	5.0	21.55	0.41
As/mg·kg⁻¹	19.80	0.21	2.83	1.01	22.50	4.87	11.71	0.22	14.08	1.37	5.50	0.62
Hg/mg·kg⁻¹	0.0419	0.0063	0.0131	0.51	0.273	0.010	0.038	0.86	0.190	0.022	0.110	0.40
SOM/g·kg⁻¹	/	/	/	/	59.20	3.40	20.36	0.44	/	/	/	/
CEC/cmol·kg⁻¹	/	/	/	/	29.69	7.76	17.58	0.22	/	/	/	/
pH	/	/	/	/	8.47	7.19	8.19	0.02	/	/	/	/

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表 2 主成分旋转载荷

Table 2. Rotational load of main constituent

重金属	第1主成分	第2主成分
Cr	0.832	0.098
As	0.698	0.366
Cu	0.656	−0.238
Pb	0.647	0.572
Zn	0.638	0.500
Ni	0.553	0.059
Cd	0.030	0.844
Hg	0.039	0.670
特征根	3.378	1.309
方差/%	42.224	16.358
贡献率/%	42.224	58.582

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表 3 大气降尘年沉降通量参数统计与比较

Table 3. Statistics and comparison of flux parameters for annual sedimentation of heavy metals in atmospheric dustfall

重金属	最大值	最小值	均值	标准差	变异系数	济南^[8]	长江三角洲^[28]	北京平原区^[29]	江西石城^[30]
Cu/mg·m⁻²	9.42	2.61	5.45	1.73	0.32	26.4	13.9	14.2	10.32
Pb/mg·m⁻²	9.18	1.03	6.23	2.10	0.34	43.3	35.9	21.0	5.24
Zn/mg·m⁻²	43.08	14.57	30.11	8.23	0.27	148	89.5	54.49	28.07
Cr/mg·m⁻²	7.37	2.40	5.95	1.52	0.26	57.8	13.2	11.86	50.12
Cd/mg·m⁻²	0.408	0.124	0.236	0.081	0.34	0.85	0.41	0.236	0.281
Ni/mg·m⁻²	4.61	1.60	3.26	0.85	0.26	12.47	4.6	6.6	5.87
As/mg·m⁻²	3.90	0.37	0.90	0.80	0.89	4.53	1.57	2.9	0.33
Hg/mg·m⁻²	0.028	0.007	0.017	0.006	0.35	0.085	0.03	0.024	0.005

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表 4 大气降尘导致的表层土壤重金属年增量

Table 4. Annual increment of heavy metals in topsoil caused by atmospheric dustfall

重金属	最大值	最小值	均值	标准差	变异系数	表层土壤均值	年增长速率/%
Cu/mg·kg⁻¹	0.0368	0.0102	0.0213	0.0068	0.32	28.74	0.07
Pb/mg·kg⁻¹	0.0359	0.0040	0.0243	0.0082	0.34	25.82	0.09
Zn/mg·kg⁻¹	0.1683	0.0569	0.1176	0.0321	0.27	74.43	0.16
Cr/mg·kg⁻¹	0.0288	0.0094	0.0232	0.0059	0.26	69.13	0.03
Cd/mg·kg⁻¹	0.0016	0.0005	0.0009	0.0003	0.34	0.168	0.55
Ni/mg·kg⁻¹	0.0180	0.0062	0.0128	0.0033	0.26	33.22	0.04
As/mg·kg⁻¹	0.0153	0.0014	0.0035	0.0031	0.89	11.60	0.03
Hg/mg·kg⁻¹	0.00011	0.00003	0.00007	0.00002	0.35	0.034	0.20

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