基于稳定同位素的珠江口近岸海域硝酸盐来源解析

林巧云; 王昕; 陈仲晗; 韩丽丽; 杨静; 赵庄明

基于稳定同位素的珠江口近岸海域硝酸盐来源解析

1.
生态环境部华南环境科学研究所，广州 510530
2.
海南大学，南海海洋资源利用国家重点实验室，海口 570228

基金项目: 中央级公益性科研院所基本科研业务专项（PM-zx097-202406-195）；广州市科技计划项目（2025A04J4494）。

详细信息

作者简介:
林巧云（1993—），女，福建省泉州市人，工程师，主要研究方向为河口氮循环及其同位素研究，E-mail：linqiaoyun@scies.org

通讯作者:
赵庄明，男，副研究员，主要研究方向为海洋数值模拟，E-mail：zhaozhuangming@scies.org

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出版历程
- 网络出版日期: 2025-07-07

Source apportionment of nitrate in the Pearl River Estuary based on dual stable isotope

1.
South China Institute of Environmental Science, Ministry of Ecology and Environment, Guangzhou 510530, China
2.
State Key Laboratory of Marine Resources Utilization in the South China Sea, Hainan University, Haikou 570228, China

摘要

摘要: 为了解珠江口氮循环过程及氮污染主要来源，于2020年7月在珠江口近岸海域（伶仃洋西部、磨刀门和黄茅海）系统采集了40个站位的海水样品，耦合水化学基本参数与硝酸盐氮氧稳定同位素示踪技术，定量解析${\mathrm{NO}}_3^- $污染的主要来源，揭示其空间梯度变化与迁移转化机制。结果表明，珠江口近岸海域${\mathrm{NO}}_3^- $平均浓度为44.05 ± 27.85 μmol/L，δ¹⁵N-${\mathrm{NO}}_3^- $和δ¹⁸O-${\mathrm{NO}}_3^- $值分别为10.8 ± 2.6‰ 和6.1 ± 4.5‰。三个海域的${\mathrm{NO}}_3^- $、δ¹⁵N-${\mathrm{NO}}_3^- $和δ¹⁸O-${\mathrm{NO}}_3^- $均不遵循保守混合特征，δ¹⁸O-${\mathrm{NO}}_3^- $和δ¹⁵N-${\mathrm{NO}}_3^- $的回归斜率表明，浮游植物同化作用和硝化作用是珠江口硝酸盐同位素组成变化的主要调控过程，而无机氮（Dissolved Inorganic Nitrogen，DIN）的显著去除则表现出沉积物反硝化作用对珠江口氮储库的影响。贝叶斯模型溯源结果进一步揭示生活污水是三个海域${\mathrm{NO}}_3^- $的最大来源，平均占比达到51.97%，水产养殖是磨刀门和黄茅海${\mathrm{NO}}_3^- $第二大主要来源，这可能与珠江口西岸城市较高的水产养殖面积有关。本研究结果可为近岸海域氮污染综合治理提供科学依据。
- 硝酸盐氮氧同位素组成 /
- 氮循环 /
- 溯源 /
- 珠江口
Abstract: To elucidate nitrogen cycling processes and identify dominant nitrogen pollution sources in the Pearl River Estuary (PRE), seawater samples were systematically collected from 40 stations in coastal waters (the western of Lingdingyang, Modaomen and Huangmaohai) during July 2020. By integrating hydrochemistry parameters and nitrogen-oxygen dual stable isotope (δ¹⁵N-${\mathrm{NO}}_3^- $ and δ¹⁸O-${\mathrm{NO}}_3^- $), we quantitatively analyzed the main sources of nitrate pollution and elucidated spatial gradient variation and transformation mechanism. The results showed an average nitrate concentration of 44.05 ± 27.85 μmol/L in the PRE, with the nitrogen-oxygen isotope value of 10.8 ± 2.6‰ and 6.1 ± 4.5‰, respectively. ${\mathrm{NO}}_3^- $, δ¹⁵N-${\mathrm{NO}}_3^- $ and δ¹⁸O-${\mathrm{NO}}_3^- $ values in the three areas deviated from conservative mixing behavior, with regression slopes between δ¹⁵N-${\mathrm{NO}}_3^- $ and δ¹⁸O-${\mathrm{NO}}_3^- $ indicating phytoplankton assimilation and nitrification are the dominant processes governing isotopic variations in the PRE. Additionally, incomplete sedimentary denitrification also significantly contributes to nitrogen reservoir dynamics. The Bayesian mixing model results revealed that domestic sewage represents the largest nitrate source in Lingdingyang, Modaomen and Huangmaohai, accounting for an average of 51.97% + 25.1%. Aquaculture emerged as the secondary source, which may linked to extensive aquaculture activities along the Pearl River Delta (PRD). These findings provide scientific basis for integrated nitrogen pollution control and water quality management in coastal ecosystems.
- Nitrogen and oxygen isotopic composition of nitrate /
- Nitrogen cycling /
- Source tracking /
- Pearl River Estuary

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图 1 (a) 采样站位图；(b)～(f) 珠江口近岸海域盐度、不同形态氮的空间分布图

Fig. 1 (a) Sampling stations; (b)～(f) Spatial distribution of salinity and different forms of nitrogen in the Pearl River Estuary

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图 2 珠江口近岸海域硝酸盐氮氧同位素值的空间分布图

Fig. 2 Spatial distribution of nitrate δ¹⁵N and δ¹⁸O in the Pearl River Estuary

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图 3 珠江口近岸海域 (a) ${\mathrm{NO}}_3^- $，(b) DIN，(c) δ¹⁵N-${\mathrm{NO}}_3^- $，(d) δ¹⁸O-${\mathrm{NO}}_3^- $与盐度关系图（浅蓝色五角星表示两端元，两端元间的浅蓝色虚线表示保守混合线）

Fig. 3 Relationship between (a) ${\mathrm{NO}}_3^- $ and (b) DIN and (c) δ¹⁵N-${\mathrm{NO}}_3^- $ and (d) δ¹⁸O-${\mathrm{NO}}_3^- $ versus salinity in the Pearl River Estuary (light blue star represent the two end-members, the light blue dotted line indicate the conservative mixing lines of two end-members)

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图 4 (a, b) 珠江口近岸海域 Δδ¹⁵N-${\mathrm{NO}}_3^- $、Δδ¹⁸O-${\mathrm{NO}}_3^- $与 Δ[${\mathrm{NO}}_3^- $] 关系图；(c) Δδ¹⁵N-${\mathrm{NO}}_3^- $ 与 Δδ¹⁸O-${\mathrm{NO}}_3^- $ 关系图；(d) Δ[$ {\mathrm{NH}}_4^+ $] 与 Δ[${\mathrm{NO}}_2^- $] 关系图

Fig. 4 (a, b) Scatter plots for Δδ¹⁵N-${\mathrm{NO}}_3^- $ and Δδ¹⁸O-${\mathrm{NO}}_3^- $ versus Δ[${\mathrm{NO}}_3^- $]; (c) Relationship between Δδ¹⁵N-${\mathrm{NO}}_3^- $ versus Δδ¹⁸O-${\mathrm{NO}}_3^- $ in the Pearl River Estuary; (d) Scatter plots for Δ[${\mathrm{NH}}_4^+ $] versus Δ[${\mathrm{NO}}_2^- $]

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图 5 珠江口近岸海域 Δδ_r与lnf关系图：(a) 伶仃洋西部；(b) 磨刀门；(c) 黄茅海

Fig. 5 Relationship between Δδ_r versus lnf in the Pearl River Estuary, (a) the western of Lingdingyang；(b) Modaomen；(c) Huangmaohai

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图 6 (a) 不同硝酸盐来源的δ¹⁵N-${\mathrm{NO}}_3^- $和δ¹⁸O-${\mathrm{NO}}_3^- $值典型范围示意图（虚线方框表示以往研究中采用的硝酸盐来源的δ¹⁵N-${\mathrm{NO}}_3^- $和δ¹⁸O-${\mathrm{NO}}_3^- $典型范围值^{[9, 23]}，十字表示珠三角地区实测的不同硝酸盐来源的平均值和标准差）；(b) 利用SIAR模型计算的4种端元对于珠江口近岸海域不同区域硝酸盐的贡献比例（数字百分比表示不同端元的贡献）

Fig. 6 (a) Schematic showing typical ranges of δ¹⁵N-${\mathrm{NO}}_3^- $ and δ¹⁸O-${\mathrm{NO}}_3^- $ in various sources. The boxes bordered by dotted lines delineate the typical ranges of δ¹⁵N-${\mathrm{NO}}_3^- $ and δ¹⁸O-${\mathrm{NO}}_3^- $ values for nitrate sources adopted from previous studies^{[9, 23]}. The cross represents the means and standard deviations measured in the site-specific nitrate sources in the Pearl River region; (b) Proportion of the contribution of the four ${\mathrm{NO}}_3^- $ sources in the Pearl River Estuary calculated using the SIAR model (The percentage of figures indicates the contribution of different sources)

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表 1 两端元盐度、${\mathrm{NO}}_3^- $浓度和同位素组成特征值

Tab. 1 Characteristics of riverine and marine end-members

端元	站位	盐度 / psu	${\mathrm{NO}}_3^- $/μmol/L	δ¹⁵N-${\mathrm{NO}}_3^- $/‰	δ¹⁸O-${\mathrm{NO}}_3^- $/‰
河水	S62 - 64	0.84	114.99	7.1	2.7
海水	S39	32.71	2.90	13.0	16.8
注： S62-64站位布设于鸡啼门和磨刀门上游。

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表 2 不同端元硝酸盐来源的氮氧同位素特征值

Tab. 2 Isotopic compositions of nitrogen and oxygen in nitrate from different sources

硝酸盐来源	δ¹⁵N-${\mathrm{NO}}_3^- $/‰	δ¹⁸O-${\mathrm{NO}}_3^- $/‰	样品数量 / 个
生活污水	10.9 ± 4.1	3.0 ± 2.6	n = 22
化肥	3.1 ± 6.8	13.7 ± 5.6	n = 8
水产养殖	6.0 ± 4.5	1.1 ± 0.9	n = 13
外海水	9.1 ± 6.1	13.7 ± 4.1	n = 6

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