黑龙江省海伦地区浅层地下水中“三氮”分布特征及来源解析

李丽君; 刘强

doi:10.15898/j.ykcs.202208270160

黑龙江省海伦地区浅层地下水中“三氮”分布特征及来源解析

李丽君,
刘强^,

中国地质调查局沈阳地质调查中心，辽宁沈阳 110034

基金项目: 中国地质调查局地质调查项目“松嫩平原水文地质调查”（DD20190340）

详细信息

作者简介: 李丽君，硕士，正高级工程师，从事岩矿测试及地质矿产方法研究。E-mail：475876904@qq.com

通讯作者: 刘强，硕士，正高级工程师，从事水文地质及水资源调查评价。E-mail：94778933@qq.com

中图分类号: X523；X131.2

收稿日期: 2022-08-27

修回日期: 2022-10-09

录用日期: 2023-05-29

刊出日期: 2023-08-31

Distribution Characteristics and Source Analysis of “Three Nitrogen” in Shallow Groundwater in Hailun Area of Heilongjiang Province

LI Lijun,
LIU Qiang^,

Shenyang Center of China Geological Survey, Shenyang 110034, China

More Information

Corresponding author: LIU Qiang, 94778933@qq.com

Received Date: 27 August 2022

Revised Date: 09 October 2022

Accepted Date: 29 May 2023

Publish Date: 31 August 2023

摘要

摘要:
近年来随着人类活动增加、工业废水的大量排放以及农业氮肥过量施用，使得地下水中“三氮”（即硝酸盐氮、氨氮、亚硝酸盐氮）污染问题愈加严重，对人体带来潜在健康风险。通过地下水“三氮”污染分布及来源作出解析，对于开展污染源头防控具有重要的现实意义。本文以黑龙江省海伦地区浅层地下水作为研究对象，采用气相分子吸收光谱法（GMA）及电感耦合等离子体质谱法（ICP-MS）测定了地下水中“三氮”及其他金属元素的检出情况，应用内梅罗综合污染指数法对地下水中“三氮”划分水质污染等级，综合运用Pearson相关性分析、正定矩阵因子分析法（PMF）等方法，识别和定量解析污染源及贡献。结果表明：①研究区地下水中硝酸盐氮含量范围在0.021～123.05mg/L之间，平均浓度为15.27mg/L；氨氮含量范围在 ND～3.91mg/L之间，平均浓度为0.33mg/L；亚硝酸盐含量范围在ND～0.65mg/L之间。与《地下水质量标准》（GB/T 14848—2017）Ⅲ类水指标对比，硝酸盐氮超标率为20.0%，氨氮超标率为12.5%。②内梅罗综合污染指数评价结果表明，研究区地下水水质污染等级一级至三级中度污染地下水占比为92.5%，整体上水质“三氮”污染较轻。海伦地区“三氮”空间分布整体上呈现出氨氮、硝酸盐氮流域中心区近端含量高、远端含量低的趋势。硝酸盐氮及氨氮超标点主要分布在研究区中部的人类活动密集区域。亚硝酸盐氮在空间分布上沿海伦河流向呈现出北高南低的趋势。③正定矩阵因子分析模型（PMF）源解析结果表明，硝酸盐氮主要来源于生活与工业复合源；亚硝酸盐氮主要来源于自然源；氨氮主要来源于生活与农业复合源。与中南部长三角武进地区太湖平原、西南部成都平原及东南部广花盆地地下水相比，海伦地区氨氮含量偏低，硝酸盐氮均值则均高于中南部地区。“三氮”的源解析结果呼应了东三省尤其是黑龙江部分地区“三氮”含量较高的分布特征。海伦地区地下水“三氮”污染程度整体上相对较轻，人类活动对地下水中“三氮”分布的影响较大。
- 海伦地区 /
- 地下水 /
- 三氮 /
- 分布特征 /
- 源解析 /
- 气相分子吸收光谱法 /
- 电感耦合等离子体质谱法
Abstract: BACKGROUND
With the increase of population, urbanization development, the large discharge of industrial wastewater and the excessive application of agricultural nitrogen fertilizer, the problem of “three nitrogen” (nitrate nitrogen, ammonia nitrogen, and nitrite nitrogen) pollution in groundwater has become increasingly serious. Due to the slow flow, weak alternation degree and poor self-purification ability, the nitrogen polluted groundwater is difficult to rehabilitate and the repair cost is high. It is of great practical significance to carry out prevention and control from the pollution source. With the concealment, complexity and hysteretic groundwater pollution property, it is difficult to conduct the source analysis of nitrate in groundwater. Positive matrix factorization (PMF) model, as a new type of source analysis model, has more interpretable and clear physical significance in terms of factor load and source factor score. At present, the application of the PMF model in the source analysis of “three nitrogen” in groundwater media is rarely reported, and the research in this field needs to be deepened. Gas-phase molecular absorption spectrometry is a practical analytical method for nitrogen compounds with high accuracy, wide linear range without color and turbidity interference. This method does not require chemical separation, and uses few chemical reagents and innoxious reagents. At present, this method has been widely used in the analysis and determination of water quality, nitrite nitrogen, ammonia nitrogen, nitrate nitrogen, total nitrogen, and other substances.
OBJECTIVES
To identify the source and distribution characteristics of the “three nitrogen” in shallow groundwater in the Hailun area.
METHODS
(1) Determination of “three nitrogen” and other elements in groundwater samples. With GPS coordinates, the 40 shallow groundwater samples were collected in Helen River Basin and Zaying River Basin. The collection and preservation of groundwater samples were performed in accordance with the environmental standards HJ/T 164—2004, HJ/T 195—2005, HJ/T 197—2005 and the ecological industry standards DZ/T 0064—2021. The quality control of the “three nitrogen” test in groundwater was based on the requirements of the national standard GB/T 14848—2017, the technical requirements for analytical quality control of groundwater pollution investigation (DD 2014-15), and the specification of testing quality management for geological laboratories (DZ/T 0130—2006). Each batch contained twenty samples and the test process of each batch was equipped with laboratory blank, reference materials, laboratory duplicate samples and quality control of external monitoring samples. All of the laboratory blank results were less than 2 times the detection limit of the method. The added standard recovery rate of the sample matrix was between 80%-120%, with the relative deviation (RD) of the laboratory repeat samples under 15%. The qualified rate of external quality control sample was 100%.　　(2) Analysis of detection data. Statistics and analysis of “three nitrogen”, heavy metal content correlation and principal components in groundwater were carried out using WPS Office 2016 and SPSS 22.0. The spatial distribution map of “three nitrogen” content in groundwater was obtained by CoreDRAW X5.0 software. The Ⅲ class water criterion in Standard for Groundwater Quality (GB/T 14848—2017) was used as the criterion for drinking water source and industrial and agricultural water. The Nemerow pollution index was calculated and compared with the corresponding grade standard index. The PMF model was used to identify and quantify the contribution rate of each nitrogen source to comprehensively judge the source of “three nitrogen”.
RESULTS
(1) The contents of “three nitrogen” and other elements in the groundwater samples in the study area were determined. According to the contents of “three nitrogen” and related parameters shown in Table 3, the detection rates of the nitrate nitrogen, ammonia nitrogen and nitrite nitrogen were 100%, 77.5% and 90.0%, respectively. The maximum detection content of nitrate nitrogen was 123.05mg/L, and average content was 15.27mg/L. The maximum detection content of ammonia nitrogen was 3.91mg/L, and average content was 0.33mg/L. The maximum detection content of nitrite nitrogen was 0.65mg/L, and average content was 0.12mg/L. Compared with the Ⅲ class water criterion, the nitrate nitrogen over standard rate was 20%, with the maximum value 6.18 times; the ammonia nitrogen over standard rate was 12.5%, with its maximum value 7.8 times; the nitrite nitrogen did not exceed the Ⅲ class water criterion. The content of Mn was ND-3.20mg/L, and the proportion of Mn in I-III class water range was 40%. The contents of 8 heavy metals including Cd were within 10 times the detection limit, with 100% Ⅰ-Ⅲ class water. The content of anion F⁻ was 0.029-0.69mg/L. The content of anion Cl⁻ ranged from 0.0027 to 310mg/L, with the 97.5% Ⅰ-Ⅲ class and 2.5% over standard rate. The content of SO₄ ²⁻ was 0.46-433mg/L, with the 95% Ⅰ-Ⅲ class and 5% over standard rate.　　(2) The pollution and spatial distribution of groundwater were studied. The results of Nemerow comprehensive pollution evaluation showed that the pollution degree of “three nitrogen” in the study area was relatively low. The proportion of unpolluted samples, mild pollution samples, heavy pollution samples and serious pollution samples was 65%, 25%, 2.5% and 0, respectively (Table 4). “Three nitrogen” spatial distribution is shown in Fig.1a-c. Samples with ammonia nitrogen content ranging in Ⅰ-Ⅲ class water was mainly concentrated in the north, west, east and central; the Ⅳ class water samples were concentrated in the middle; the class V water samples were concentrated in the center. Fig.1a shows the trend of high ammonia nitrogen in the middle and low ammonia nitrogen on both sides. In Fig.1b, Ⅰ-Ⅲ class water samples of nitrate nitrogen were mainly concentrated in the central, east and north, with the Ⅳ class water in the middle and the class V water in the west. The samples with the highest and sub highest nitrate nitrogen content were located in the center of the study area, radially distributing along the Helen River Basin and the Zaying River Basin. The nitrate nitrogen content was high near the central area, with the low content far from the central area. The nitrite nitrogen in Fig.1c was Ⅰ-Ⅲ class water. The spatial distribution of the nitrite nitrogen shows the trend of high in the north and low in the south along the Helen River Basin.　　(3) Multivariate statistical analysis and source of “three nitrogen” in groundwater were studied. Multivariate statistical analysis of Pearson correlation coefficient showed that nitrate nitrogen had some homology with Cd, Co, Ni. Nitrate nitrogen in groundwater was significantly correlated with Cl⁻ and SO₄ ²⁻, while ammonia nitrogen and nitrite nitrogen showed no correlation with anion. Sample detection data imported into EPA PMF5.0 software for PMF source analysis, and the industrial source, agricultural source, living source and natural factor source were taken as the four source analysis factors of “three nitrogen” in the groundwater in the study area. The PMF source analysis results are presented in Table 6 and Fig.2. The main sources of “three nitrogen” in the groundwater in the study area were the compound source of living and industrial source, which further indicated that human activity was the root cause of “three nitrogen” pollution in the groundwater in Helen area. According to the spatial distribution of “three nitrogen” in groundwater, the highest point of nitrate nitrogen pollution was distributed in the center of the research area, with the relatively developed human life and industrial activities in this area. The ammonia nitrogen pollution samples were related to the dense human activities in the middle of the study area. The over-standard area of nitrate nitrogen was higher than the ammonia nitrogen, which indicated that the compound source of living and industrial source was the main factor affecting the “three nitrogen” content in the groundwater in study area.
CONCLUSIONS
The nitrate nitrogen and ammonia nitrogen are the nitrogen pollution components in the groundwater in the study area. Compared with the water index in groundwater quality standard (GB/T 14848—2017), the over standard rates of the nitrate nitrogen and ammonia nitrogen are 20% and 12.5% respectively. The groundwater quality with pollution evaluation grade I （unpolluted） to grade Ⅲ （moderate polluted）accounts for 92.5%, which indicates relatively light pollution.　　The spatial distribution of ammonia nitrogen in the study area shows a trend of high in the middle and low on both sides. Nitrate nitrogen and ammonia nitrogen pollution samples are mainly distributed in the center of the intensive human activity research area. The quantitative analysis results of the “three nitrogen” PMF analysis model show that the compound source of living and industry are the main source of nitrate nitrogen pollution in the study area, and the compound source of living and agricultural production is the main source of ammonia nitrogen pollution. Combining the situation with the source of the “three nitrogen” pollution in the research area, the project of the “three nitrogen” pollution prevention can be carried out to strengthen protection, sustainable development and utilization of groundwater resources in the Helen area.
- Hailun area /
- groundwater /
- three nitrogen /
- distribution characteristics /
- source apportionment /
- gas-phase molecular absorption spectrometry /
- inductively coupled plasma-mass spectrometry

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图 1 研究区地下水采样点及“三氮”含量空间分布示意图

Figure 1.

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图 2 基于PMF的各因子对地下水中“三氮”及重金属等含量分布的贡献率

Figure 2.

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表 1 样品测试质量控制结果统计

Table 1. Statistics of recovery rate and relative deviation.

分析项目	加标回收率（80%～120%）	实验室重复样相对偏差（≤15%）
Mn	90.9%～110.6%	3.40
Cd	89.6%～113.6%	2.40
Pb	85.0%～105.0%	5.10
Zn	85.6%～90.2%	12.6
Cu	83.0%～95.0%	11.4
Co	84.0%～94.0%	11.2
Ni	82.0%～89.0%	11.8
As	97.0%～107.0%	4.10
Hg	85.0%～98.3%	14.5
NO₃ ⁻-N	82.1%～96.0%	11.0
NH₄ ⁺-N	83.0%～89.0%	11.9
NO₂ ⁻-N	82.2%～92.0%	13.4
F⁻	82.3%～91.1%	13.2
Cl⁻	85.0%～92.5%	12.4
SO₄ ²⁻	83.0%～90.0%	13.0

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表 2 内梅罗综合污染指数分级标准^［16］

Table 2. Nemerow comprehensive pollution index classification standard^［16］.

内梅罗综合污染指数 F	污染等级	污染程度	内梅罗综合污染指数 F	污染等级	污染程度
F≤0.8	Ⅰ	未污染	4.25＜F≤7.2	Ⅳ	较重污染
0.80＜F≤2.5	Ⅱ	轻度污染	F≥7.2	Ⅴ	严重污染
2.5＜F≤4.25	Ⅲ	中度污染

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表 3 研究区地下水中“三氮”含量统计

Table 3. Statistics of ammonia nitrogen, nitrate nitrogen, and nitrite nitrogen contents in groundwater.

统计项目	硝酸盐氮含量	氨氮含量	亚硝酸盐氮含量
最大值（mg/L）	123.05	3.91	0.65
最小值（mg/L）	0.021	ND（未检出）	ND（未检出）
平均值（mg/L）	15.27	0.33	0.12
标准偏差	28.56	0.79	0.26
变异系数（100%）	1.87	2.42	2.27
《地下水质量标准》（GB/T 14848—2017）Ⅲ类水（mg/L）	20	0.5	1.0
偏度	2.52	3.66	2.43
峰度	6.47	13.66	5.94
检出率（%）	100	77.5	90.0
超标率（%）	20	12.5	0

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表 4 研究区地下水内梅罗综合污染指数（F）评价结果

Table 4. Evaluation results of Nemerow comprehensive pollution index in groundwater in the study area.

内梅罗综合污染指数（F）范围	污染等级	污染程度	样品数量（件）	占比（%）
F≤0.8	Ⅰ	未污染	26	65
0.80＜F≤2.5	Ⅱ	轻度污染	10	25
2.5＜F≤4.25	Ⅲ	中度污染	1	2.5
4.25＜F≤7.2	Ⅳ	较重污染	3	7.5
F≥7.2	Ⅴ	严重污染	0	0

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表 5 地下水中“三氮”与重金属及阴离子的Pearson相关性系数

Table 5. Pearson correlation coefficient of heavy metals and negative ions in the groundwater.

组分	Mn	Cd	Pb	Zn	Cu	Co	Ni	As	Hg	NO₃ ⁻−N	NH₄ ⁺−N	NO₂ ⁻−N	F⁻	Cl⁻	SO₄ ²⁻
Mn	1
Cd	−0.166	1
Pb	0.151	0.220	1
Zn	0.086	0.191	0.172	1
Cu	0.085	−0.037	0.469^**	0.196	1
Co	0.380^*	0.196	0.423^**	0.137	0.112	1
Ni	−0.026	0.103	0.191	0.155	0.009	0.400^*	1
As	0.302	−0.160	0.396^*	−0.135	0.020	0.326^*	0.031	1
Hg	−0.103	−0.047	−0.090	0.005	0.014	−0.016	0.385^*	−0.103	1
NO₃ ⁻−N	−0.304	0.370^*	−0.038	−0.204	0.060	0.329^*	0.319^*	−0.146	−0.117	1
NH₄ ⁺−N	0.059	−0.107	−0.055	0.040	−0.067	−0.138	−0.157	0.106	−0.075	−0.132	1
NO₂ ⁻−N	0.181	−0.146	−0.101	−0.212	−0.028	0.327^*	−0.095	0.167	0.003	−0.169	−0.033	1
F⁻	0.082	0.195	0.189	0.509^**	0.080	−0.029	−0.195	0.312^*	−0.116	−0.287	0.193	−0.009	1
Cl⁻	−0.051	−0.049	0.169	−0.212	0.106	0.440^**	0.485^**	0.087	0.198	0.605^**	−0.122	−0.098	−0.098	1
SO₄ ²⁻	−0.157	0.244	0.044	−0.236	0.104	0.376^*	0.288	−0.041	−0.024	0.897^**	−0.153	−0.182	−0.157	0.796^**	1
注： “*”表示在 0.01水平（双侧）上显著相关，“”表示在 0.05水平（双侧）上显著相关。

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表 6 地下水中“三氮”及重金属含量实测值与模拟预测值的拟合结果

Table 6. Fitting results of measured value and simulated predicted value of three nitrogen and heavy metal contents in the groundwater.

分析项目	R²	截距	斜率	P/O
Mn	0.672	10.139	0.369	0.894
Cd	0.901	10.667	0.548	0.779
Pb	0.605	5.161	0.237	0.802
Co	0.870	−10.208	0.856	0.804
Ni	0.557	75.286	0.786	0.781
As	0.733	45.310	0.812	0.870
NO₃ ⁻−N	0.749	−1.193	0.752	0.775
NH₄ ⁺−N	0.797	0.186	0.756	0.896
NO₂ ⁻−N	0.750	0.114	0.756	0.887
Cl⁻	0.773	−10.369	0.835	0.791
SO₄ ²⁻	0.531	−9.631	0.921	0.809

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